Search references:
| 21. | Valente, Gonçalo; Dantas, Raquel; Ferreira, Pedro; Grieco, Rebecca; Patil, Nagaraj; Guillem-Navajas, Ana; Miguel, David Rodríguez-San; Zamora, Félix; Guntermann, Roman; Bein, Thomas; Rocha, João; Braga, Helena M; Strutyński, Karol; Melle-Franco, Manuel; Marcilla, Rebeca; Souto, Manuel: Tetrathiafulvalene-based covalent organic frameworks as high-voltage organic cathodes for lithium batteries. In: Journal of Materials Chemistry A, 2024, ISSN: 20507488, (Cited by: 0). (Type: Journal Article | Abstract | Links | BibTeX) @article{Valente2024, title = {Tetrathiafulvalene-based covalent organic frameworks as high-voltage organic cathodes for lithium batteries}, author = {Gonçalo Valente and Raquel Dantas and Pedro Ferreira and Rebecca Grieco and Nagaraj Patil and Ana Guillem-Navajas and David Rodríguez-San Miguel and Félix Zamora and Roman Guntermann and Thomas Bein and João Rocha and Helena M Braga and Karol Strutyński and Manuel Melle-Franco and Rebeca Marcilla and Manuel Souto}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85201428063&doi=10.1039%2fd4ta04576a&partnerID=40&md5=961b9f8d9b2a7e85f5fa41fbc3c5a440}, doi = {10.1039/d4ta04576a}, issn = {20507488}, year = {2024}, date = {2024-01-01}, journal = {Journal of Materials Chemistry A}, publisher = {Royal Society of Chemistry}, abstract = {Redox-active covalent organic frameworks (COFs) are promising electrode materials for metal-ion batteries owing to their tunable electrochemical properties, adjustable structure, and resource availability. Herein, we report a series of two-dimensional tetrathiafulvalene (TTF)-based COFs incorporating different organic linkers between the electroactive moieties. These COFs were investigated as p-type organic cathode materials for lithium-organic batteries. The electrical conductivity of both neutral and doped TTF-COFs was measured using a van der Pauw setup, and their electronic structures were investigated through quantum-chemical calculations. Binder-free buckypaper TTF-based electrodes were prepared and systematically tested as organic cathodes in lithium half-cells. The results revealed high average discharge potentials (∼3.6 V vs. Li/Li+) and consistent cycling stability (80% capacity retention after 400 cycles at 2C) for the three TTF-COF electrodes. In addition, the specific capacity, rate capability, and kinetics varied depending on the structure of the framework. Our results highlight the potential of TTF-COFs as high-voltage organic cathodes for metal-ion batteries and emphasize the importance of molecular design in optimizing their electrochemical performance. © 2024 The Royal Society of Chemistry.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Redox-active covalent organic frameworks (COFs) are promising electrode materials for metal-ion batteries owing to their tunable electrochemical properties, adjustable structure, and resource availability. Herein, we report a series of two-dimensional tetrathiafulvalene (TTF)-based COFs incorporating different organic linkers between the electroactive moieties. These COFs were investigated as p-type organic cathode materials for lithium-organic batteries. The electrical conductivity of both neutral and doped TTF-COFs was measured using a van der Pauw setup, and their electronic structures were investigated through quantum-chemical calculations. Binder-free buckypaper TTF-based electrodes were prepared and systematically tested as organic cathodes in lithium half-cells. The results revealed high average discharge potentials (∼3.6 V vs. Li/Li+) and consistent cycling stability (80% capacity retention after 400 cycles at 2C) for the three TTF-COF electrodes. In addition, the specific capacity, rate capability, and kinetics varied depending on the structure of the framework. Our results highlight the potential of TTF-COFs as high-voltage organic cathodes for metal-ion batteries and emphasize the importance of molecular design in optimizing their electrochemical performance. © 2024 The Royal Society of Chemistry. |
| 22. | Sirotti, Elise; Böhm, Stefan; Sharp, Ian D: Ultrastable Zn3N2 Thin Films via Integration of Amorphous GaN Protection Layers. In: Advanced Materials Interfaces, 11 (22), 2024, ISSN: 21967350, (Cited by: 0). (Type: Journal Article | Abstract | Links | BibTeX) @article{Sirotti2024, title = {Ultrastable Zn3N2 Thin Films via Integration of Amorphous GaN Protection Layers}, author = {Elise Sirotti and Stefan Böhm and Ian D Sharp}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85196511694&doi=10.1002%2fadmi.202400214&partnerID=40&md5=dc119cc28d4f1c2ccb3c5d6edda495f7}, doi = {10.1002/admi.202400214}, issn = {21967350}, year = {2024}, date = {2024-01-01}, journal = {Advanced Materials Interfaces}, volume = {11}, number = {22}, publisher = {John Wiley and Sons Inc}, abstract = {Zinc nitride (Zn3N2) is a promising semiconductor for a range of optoelectronic and energy conversion applications, offering a direct bandgap of 1.0 eV, large carrier mobilities, and abundant constituent elements. However, the material is prone to bulk oxidation in ambient environments, which has thus far impeded its practical deployment. While previous approaches have focused on stabilizing the material via integration of ZnO surface layers, these strategies introduce additional challenges regarding elevated processing temperatures and limited control of interface properties. In this study, it is shown that amorphous GaN thin films can serve as highly stable protection layers on Zn3N2 surfaces and can be deposited at the same growth temperature and in the same deposition system as the underlying semiconductor. The GaN-capped Zn3N2 structures exhibit long-term stability, surviving over 3 years of exposure to ambient conditions with no discernible alterations in composition, structure, or electrical properties. Notably, the amorphous GaN coatings can even impede Zn3N2 oxidation under prolonged aqueous exposure. Thus, this study offers a solution to stabilize Zn3N2 in ambient conditions, providing a viable pathway to its utilization in robust and high-performance electronic devices, such as thin film transistors and solar energy conversion systems. © 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Zinc nitride (Zn3N2) is a promising semiconductor for a range of optoelectronic and energy conversion applications, offering a direct bandgap of 1.0 eV, large carrier mobilities, and abundant constituent elements. However, the material is prone to bulk oxidation in ambient environments, which has thus far impeded its practical deployment. While previous approaches have focused on stabilizing the material via integration of ZnO surface layers, these strategies introduce additional challenges regarding elevated processing temperatures and limited control of interface properties. In this study, it is shown that amorphous GaN thin films can serve as highly stable protection layers on Zn3N2 surfaces and can be deposited at the same growth temperature and in the same deposition system as the underlying semiconductor. The GaN-capped Zn3N2 structures exhibit long-term stability, surviving over 3 years of exposure to ambient conditions with no discernible alterations in composition, structure, or electrical properties. Notably, the amorphous GaN coatings can even impede Zn3N2 oxidation under prolonged aqueous exposure. Thus, this study offers a solution to stabilize Zn3N2 in ambient conditions, providing a viable pathway to its utilization in robust and high-performance electronic devices, such as thin film transistors and solar energy conversion systems. © 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH. |
| 23. | Berger, Luca M; Barkey, Martin; Maier, Stefan A; Tittl, Andreas: Metallic and All-Dielectric Metasurfaces Sustaining Displacement-Mediated Bound States in the Continuum. In: Advanced Optical Materials, 12 (5), 2024, ISSN: 21951071, (Cited by: 6; All Open Access, Green Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Berger2024, title = {Metallic and All-Dielectric Metasurfaces Sustaining Displacement-Mediated Bound States in the Continuum}, author = {Luca M Berger and Martin Barkey and Stefan A Maier and Andreas Tittl}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85169339120&doi=10.1002%2fadom.202301269&partnerID=40&md5=e2109c06d6b9ff2112970d07bbc33976}, doi = {10.1002/adom.202301269}, issn = {21951071}, year = {2024}, date = {2024-01-01}, journal = {Advanced Optical Materials}, volume = {12}, number = {5}, publisher = {John Wiley and Sons Inc}, abstract = {Bound states in the continuum (BICs) are localized electromagnetic modes within the continuous spectrum of radiating waves. Due to their infinite lifetimes without radiation losses, BICs are driving research directions in lasing, non-linear optical processes, and sensing. However, conventional methods for converting BICs into leaky resonances, or quasi-BICs, with high-quality factors typically rely on breaking the in-plane inversion symmetry of the metasurface and often result in resonances that are strongly dependent on the angle of the incident light, making them unsuitable for many practical applications. Here, an emerging class of BIC-driven metasurfaces is numerically analyzed and experimentally demonstrated, where the coupling to the far field is controlled by the displacement of individual resonators. In particular, both all-dielectric and metallic as well as positive and inverse displacement-mediated metasurfaces sustaining angular-robust quasi-BICs are investigated in the mid-infrared spectral region. Their optical behavior with regard to changes in the angle of incidence is investigated and experimentally shows their superior performance compared to two conventional alternatives: silicon-based tilted ellipses and cylindrical nanoholes in gold. These findings are anticipated to open exciting perspectives for bio-sensing, conformal optical devices, and photonic devices using focused light. © 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH.}, note = {Cited by: 6; All Open Access, Green Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Bound states in the continuum (BICs) are localized electromagnetic modes within the continuous spectrum of radiating waves. Due to their infinite lifetimes without radiation losses, BICs are driving research directions in lasing, non-linear optical processes, and sensing. However, conventional methods for converting BICs into leaky resonances, or quasi-BICs, with high-quality factors typically rely on breaking the in-plane inversion symmetry of the metasurface and often result in resonances that are strongly dependent on the angle of the incident light, making them unsuitable for many practical applications. Here, an emerging class of BIC-driven metasurfaces is numerically analyzed and experimentally demonstrated, where the coupling to the far field is controlled by the displacement of individual resonators. In particular, both all-dielectric and metallic as well as positive and inverse displacement-mediated metasurfaces sustaining angular-robust quasi-BICs are investigated in the mid-infrared spectral region. Their optical behavior with regard to changes in the angle of incidence is investigated and experimentally shows their superior performance compared to two conventional alternatives: silicon-based tilted ellipses and cylindrical nanoholes in gold. These findings are anticipated to open exciting perspectives for bio-sensing, conformal optical devices, and photonic devices using focused light. © 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH. |
| 24. | Derelli, Davide; Frank, Kilian; Grote, Lukas; Mancini, Federica; Dippel, Ann-Christin; Gutowski, Olof; Nickel, Bert; Koziej, Dorota: Direct Synthesis of CuPd Icosahedra Supercrystals Studied by In Situ X-Ray Scattering. In: Small, 20 (32), 2024, ISSN: 16136810, (Cited by: 0; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Derelli2024, title = {Direct Synthesis of CuPd Icosahedra Supercrystals Studied by In Situ X-Ray Scattering}, author = {Davide Derelli and Kilian Frank and Lukas Grote and Federica Mancini and Ann-Christin Dippel and Olof Gutowski and Bert Nickel and Dorota Koziej}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85188518964&doi=10.1002%2fsmll.202311714&partnerID=40&md5=95bcc8e6ed98322bfb411c2169f05879}, doi = {10.1002/smll.202311714}, issn = {16136810}, year = {2024}, date = {2024-01-01}, journal = {Small}, volume = {20}, number = {32}, publisher = {John Wiley and Sons Inc}, abstract = {Nanocrystal self-assembly into supercrystals provides a versatile platform for creating novel materials and devices with tailored properties. While common self-assembly strategies imply the use of purified nanoparticles after synthesis, conversion of chemical precursors directly into nanocrystals and then supercrystals in simple procedures has been rarely reported. Here, the nucleation and growth of CuPd icosahedra and their consecutive assembly into large closed-packed face-centered cubic (fcc) supercrystals are studied. To this end, the study simultaneously and in situ measures X-ray total scattering with pair distribution function analysis (TS-PDF) and small-angle X-ray scattering (SAXS). It is found that the supercrystals' formation is preceded by an intermediate dense phase of nanocrystals displaying short-range order (SRO). It is further shown that the organization of oleic acid/oleylamine surfactants into lamellar structures likely drives the emergence of the SRO phase and later of the supercrystals by reducing the volume accessible to particle diffusion. The supercrystals' formation as well as their disassembly are triggered by temperature. The study demonstrates that ordering of solvent molecules can be crucial in the direct synthesis of supercrystals. The study also provides a general approach to investigate novel preparation routes of supercrystals in situ and across several length scales via X-ray scattering. © 2024 The Authors. Small published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Nanocrystal self-assembly into supercrystals provides a versatile platform for creating novel materials and devices with tailored properties. While common self-assembly strategies imply the use of purified nanoparticles after synthesis, conversion of chemical precursors directly into nanocrystals and then supercrystals in simple procedures has been rarely reported. Here, the nucleation and growth of CuPd icosahedra and their consecutive assembly into large closed-packed face-centered cubic (fcc) supercrystals are studied. To this end, the study simultaneously and in situ measures X-ray total scattering with pair distribution function analysis (TS-PDF) and small-angle X-ray scattering (SAXS). It is found that the supercrystals' formation is preceded by an intermediate dense phase of nanocrystals displaying short-range order (SRO). It is further shown that the organization of oleic acid/oleylamine surfactants into lamellar structures likely drives the emergence of the SRO phase and later of the supercrystals by reducing the volume accessible to particle diffusion. The supercrystals' formation as well as their disassembly are triggered by temperature. The study demonstrates that ordering of solvent molecules can be crucial in the direct synthesis of supercrystals. The study also provides a general approach to investigate novel preparation routes of supercrystals in situ and across several length scales via X-ray scattering. © 2024 The Authors. Small published by Wiley-VCH GmbH. |
| 25. | Jan, Pei-En; Liang, Hao-Chi; Cheng, Ren-Wei; Greve, Christopher R; Chuang, Yung-Tang; Chiu, Yung-Ling; Tan, Guang-Hsun; Elsenety, Mohamed M; Chang, Chih-Li; Dorrah, Dalia M; Lai, Hoong-Lien; Chiu, Po-Wei; Sun, Sheng-Yuan; Li, Yun-Li; Herzig, Eva M; Chou, Ho-Hsiu; Lin, Hao-Wu: Molecular Design Strategy for Meta-Substituted Aromatic Organic Halides in Zero-Lead-Release Halide Perovskites with Efficient Waterproof Light Emission. In: Advanced Functional Materials, 2024, ISSN: 1616301X, (Cited by: 0). (Type: Journal Article | Abstract | Links | BibTeX) @article{Jan2024, title = {Molecular Design Strategy for Meta-Substituted Aromatic Organic Halides in Zero-Lead-Release Halide Perovskites with Efficient Waterproof Light Emission}, author = {Pei-En Jan and Hao-Chi Liang and Ren-Wei Cheng and Christopher R Greve and Yung-Tang Chuang and Yung-Ling Chiu and Guang-Hsun Tan and Mohamed M Elsenety and Chih-Li Chang and Dalia M Dorrah and Hoong-Lien Lai and Po-Wei Chiu and Sheng-Yuan Sun and Yun-Li Li and Eva M Herzig and Ho-Hsiu Chou and Hao-Wu Lin}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85203043862&doi=10.1002%2fadfm.202408323&partnerID=40&md5=a4d8aa1813df5d142bfe44e08872c17a}, doi = {10.1002/adfm.202408323}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, publisher = {John Wiley and Sons Inc}, abstract = {Halide perovskites have received an immense attention in the field of optoelectronics due to their outstanding photophysical properties. But so far, lead-based halide perovskites still account for most of the research, which raises concerns due to lead toxicity. Herein, a new design strategy is proposed utilizing a super large, energetically higher singlet and triplet energy levels aromatic organic cation to incorporate into the perovskite structure, forming ultra-stable high-performance 2D/3D (quasi-2D) perovskite. The judicious molecular design of connecting all the phenyl groups at their meta sites ensures the simultaneous achievement of a large molecular weight and high singlet and triplet energy levels. The resulting quasi-2D perovskite thin films not only exhibits excellent emission properties but also, surprisingly, show long-term waterproof-level stability. The robustness of these perovskites is confirmed by their extraordinary emission stability upon direct water immersion and almost undetectable lead release in water. Proof-of-concept of a water-resistant color conversion-type perovskite near-infrared (NIR) light-emitting diode (LED) is demonstrated, showing high external quantum efficiency (EQE) and power conversion efficiency (PCE) of 20.5% and 13.3%, respectively. It is believed these results and strategy pave a new way for realizing environmentally friendly lead halide materials and devices. © 2024 Wiley-VCH GmbH.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Halide perovskites have received an immense attention in the field of optoelectronics due to their outstanding photophysical properties. But so far, lead-based halide perovskites still account for most of the research, which raises concerns due to lead toxicity. Herein, a new design strategy is proposed utilizing a super large, energetically higher singlet and triplet energy levels aromatic organic cation to incorporate into the perovskite structure, forming ultra-stable high-performance 2D/3D (quasi-2D) perovskite. The judicious molecular design of connecting all the phenyl groups at their meta sites ensures the simultaneous achievement of a large molecular weight and high singlet and triplet energy levels. The resulting quasi-2D perovskite thin films not only exhibits excellent emission properties but also, surprisingly, show long-term waterproof-level stability. The robustness of these perovskites is confirmed by their extraordinary emission stability upon direct water immersion and almost undetectable lead release in water. Proof-of-concept of a water-resistant color conversion-type perovskite near-infrared (NIR) light-emitting diode (LED) is demonstrated, showing high external quantum efficiency (EQE) and power conversion efficiency (PCE) of 20.5% and 13.3%, respectively. It is believed these results and strategy pave a new way for realizing environmentally friendly lead halide materials and devices. © 2024 Wiley-VCH GmbH. |
| 26. | Reus, Manuel A; Reb, Lennart K; Kosbahn, David P; Roth, Stephan V; Müller-Buschbaum, Peter: INSIGHT: in situ heuristic tool for the efficient reduction of grazing-incidence X-ray scattering data. In: Journal of Applied Crystallography, 57 , pp. 509 – 528, 2024, ISSN: 00218898, (Cited by: 5; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Reus2024509, title = {INSIGHT: in situ heuristic tool for the efficient reduction of grazing-incidence X-ray scattering data}, author = {Manuel A Reus and Lennart K Reb and David P Kosbahn and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189931954&doi=10.1107%2fS1600576723011159&partnerID=40&md5=a928626dbb33d73f92d7880e27a75d81}, doi = {10.1107/S1600576723011159}, issn = {00218898}, year = {2024}, date = {2024-01-01}, journal = {Journal of Applied Crystallography}, volume = {57}, pages = {509 – 528}, publisher = {International Union of Crystallography}, abstract = {INSIGHT is a Python-based software tool for processing and reducing 2D grazing-incidence wide- and small-angle X-ray scattering (GIWAXS/GISAXS) data. It offers the geometric transformation of the 2D GIWAXS/GISAXS detector image to reciprocal space, including vectorized and parallelized pixelwise intensity correction calculations. An explicit focus on efficient data management and batch processing enables full control of large time-resolved synchrotron and laboratory data sets for a detailed analysis of kinetic GIWAXS/ GISAXS studies of thin films. It processes data acquired with arbitrarily rotated detectors and performs vertical, horizontal, azimuthal and radial cuts in reciprocal space. It further allows crystallographic indexing and GIWAXS pattern simulation, and provides various plotting and export functionalities. Customized scripting offers a one-step solution to reduce, process, analyze and export findings of large in situ and operando data sets. © 2024 International Union of Crystallography. All rights reserved.}, note = {Cited by: 5; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } INSIGHT is a Python-based software tool for processing and reducing 2D grazing-incidence wide- and small-angle X-ray scattering (GIWAXS/GISAXS) data. It offers the geometric transformation of the 2D GIWAXS/GISAXS detector image to reciprocal space, including vectorized and parallelized pixelwise intensity correction calculations. An explicit focus on efficient data management and batch processing enables full control of large time-resolved synchrotron and laboratory data sets for a detailed analysis of kinetic GIWAXS/ GISAXS studies of thin films. It processes data acquired with arbitrarily rotated detectors and performs vertical, horizontal, azimuthal and radial cuts in reciprocal space. It further allows crystallographic indexing and GIWAXS pattern simulation, and provides various plotting and export functionalities. Customized scripting offers a one-step solution to reduce, process, analyze and export findings of large in situ and operando data sets. © 2024 International Union of Crystallography. All rights reserved. |
| 27. | Almora, Osbel; Cabrera, Carlos I; Erten-Ela, Sule; Forberich, Karen; Fukuda, Kenjiro; Guo, Fei; Hauch, Jens; Ho-Baillie, Anita W Y; Jacobsson, Jesper T; Janssen, Rene A J; Kirchartz, Thomas; Loi, Maria A; Mathew, Xavier; Mitzi, David B; Nazeeruddin, Mohammad K; Paetzold, Ulrich W; Rand, Barry P; Rau, Uwe; Someya, Takao; Unger, Eva; Vaillant-Roca, Lídice; Brabec, Christoph J: Device Performance of Emerging Photovoltaic Materials (Version 4). In: Advanced Energy Materials, 14 (4), 2024, ISSN: 16146832, (Cited by: 8; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Almora2024, title = {Device Performance of Emerging Photovoltaic Materials (Version 4)}, author = {Osbel Almora and Carlos I Cabrera and Sule Erten-Ela and Karen Forberich and Kenjiro Fukuda and Fei Guo and Jens Hauch and Anita W Y Ho-Baillie and Jesper T Jacobsson and Rene A J Janssen and Thomas Kirchartz and Maria A Loi and Xavier Mathew and David B Mitzi and Mohammad K Nazeeruddin and Ulrich W Paetzold and Barry P Rand and Uwe Rau and Takao Someya and Eva Unger and Lídice Vaillant-Roca and Christoph J Brabec}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85179733522&doi=10.1002%2faenm.202303173&partnerID=40&md5=1c0215d482802ecd01505122d7519361}, doi = {10.1002/aenm.202303173}, issn = {16146832}, year = {2024}, date = {2024-01-01}, journal = {Advanced Energy Materials}, volume = {14}, number = {4}, publisher = {John Wiley and Sons Inc}, abstract = {Following the 3rd release of the “Emerging PV reports”, the best achievements in the performance of emerging photovoltaic (e-PV) devices in diverse e-PV research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2022. Updated graphs, tables, and analyses are provided with several performance parameters, such as power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, for example, the detailed balance efficiency limit. The 4th installment of the “Emerging PV reports” discusses the “PV emergence” classification with respect to the “PV technology generations” and “PV research waves” and highlights the latest device performance progress in multijunction and flexible photovoltaics. Additionally, Dale-Scarpulla's plots of efficiency-effort in terms of cumulative academic publication count are also introduced. © 2023 Wiley-VCH GmbH.}, note = {Cited by: 8; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Following the 3rd release of the “Emerging PV reports”, the best achievements in the performance of emerging photovoltaic (e-PV) devices in diverse e-PV research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2022. Updated graphs, tables, and analyses are provided with several performance parameters, such as power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, for example, the detailed balance efficiency limit. The 4th installment of the “Emerging PV reports” discusses the “PV emergence” classification with respect to the “PV technology generations” and “PV research waves” and highlights the latest device performance progress in multijunction and flexible photovoltaics. Additionally, Dale-Scarpulla's plots of efficiency-effort in terms of cumulative academic publication count are also introduced. © 2023 Wiley-VCH GmbH. |
| 28. | Reus, Manuel A; Baier, Thomas; Lindenmeir, Christoph G; Weinzierl, Alexander F; Buyan-Arivjikh, Altantulga; Wegener, Simon A; Kosbahn, David P; Reb, Lennart K; Rubeck, Jan; Schwartzkopf, Matthias; Roth, Stephan V; Müller-Buschbaum, Peter: Modular slot-die coater for in situ grazing-incidence x-ray scattering experiments on thin films. In: Review of Scientific Instruments, 95 (4), 2024, ISSN: 00346748, (Cited by: 1; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Reus2024b, title = {Modular slot-die coater for in situ grazing-incidence x-ray scattering experiments on thin films}, author = {Manuel A Reus and Thomas Baier and Christoph G Lindenmeir and Alexander F Weinzierl and Altantulga Buyan-Arivjikh and Simon A Wegener and David P Kosbahn and Lennart K Reb and Jan Rubeck and Matthias Schwartzkopf and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85191250978&doi=10.1063%2f5.0204673&partnerID=40&md5=2368b6fa4cd1af9516bc308d5b33c7a5}, doi = {10.1063/5.0204673}, issn = {00346748}, year = {2024}, date = {2024-01-01}, journal = {Review of Scientific Instruments}, volume = {95}, number = {4}, publisher = {American Institute of Physics}, abstract = {Multimodal in situ experiments during slot-die coating of thin films pioneer the way to kinetic studies on thin-film formation. They establish a powerful tool to understand and optimize the formation and properties of thin-film devices, e.g., solar cells, sensors, or LED films. Thin-film research benefits from time-resolved grazing-incidence wide- and small-angle x-ray scattering (GIWAXS/GISAXS) with a sub-second resolution to reveal the evolution of crystal structure, texture, and morphology during the deposition process. Simultaneously investigating optical properties by in situ photoluminescence measurements complements in-depth kinetic studies focusing on a comprehensive understanding of the triangular interdependency of processing, structure, and function for a roll-to-roll compatible, scalable thin-film deposition process. Here, we introduce a modular slot-die coater specially designed for in situ GIWAXS/GISAXS measurements and applicable to various ink systems. With a design for quick assembly, the slot-die coater permits the reproducible and comparable fabrication of thin films in the lab and at the synchrotron using the very same hardware components, as demonstrated in this work by experiments performed at Deutsches Elektronen-Synchrotron (DESY). Simultaneous to GIWAXS/GISAXS, photoluminescence measurements probe optoelectronic properties in situ during thin-film formation. An environmental chamber allows to control the atmosphere inside the coater. Modular construction and lightweight design make the coater mobile, easy to transport, quickly extendable, and adaptable to new beamline environments. © 2024 Author(s).}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Multimodal in situ experiments during slot-die coating of thin films pioneer the way to kinetic studies on thin-film formation. They establish a powerful tool to understand and optimize the formation and properties of thin-film devices, e.g., solar cells, sensors, or LED films. Thin-film research benefits from time-resolved grazing-incidence wide- and small-angle x-ray scattering (GIWAXS/GISAXS) with a sub-second resolution to reveal the evolution of crystal structure, texture, and morphology during the deposition process. Simultaneously investigating optical properties by in situ photoluminescence measurements complements in-depth kinetic studies focusing on a comprehensive understanding of the triangular interdependency of processing, structure, and function for a roll-to-roll compatible, scalable thin-film deposition process. Here, we introduce a modular slot-die coater specially designed for in situ GIWAXS/GISAXS measurements and applicable to various ink systems. With a design for quick assembly, the slot-die coater permits the reproducible and comparable fabrication of thin films in the lab and at the synchrotron using the very same hardware components, as demonstrated in this work by experiments performed at Deutsches Elektronen-Synchrotron (DESY). Simultaneous to GIWAXS/GISAXS, photoluminescence measurements probe optoelectronic properties in situ during thin-film formation. An environmental chamber allows to control the atmosphere inside the coater. Modular construction and lightweight design make the coater mobile, easy to transport, quickly extendable, and adaptable to new beamline environments. © 2024 Author(s). |
| 29. | Huang, Tzu-Yen; Brun, Anton Le P; Sochor, Benedikt; Wu, Chun-Ming; Bulut, Yusuf; Müller-Buschbaum, Peter; Roth, Stephan V; Yang, Yan-Ling: Nanometer-Thick ITIC Bulk Heterojunction Films as Non-Fullerene Acceptors in Organic Solar Cells. In: ACS Applied Nano Materials, 7 (15), pp. 17588 – 17595, 2024, ISSN: 25740970, (Cited by: 0). (Type: Journal Article | Abstract | Links | BibTeX) @article{Huang202417588, title = {Nanometer-Thick ITIC Bulk Heterojunction Films as Non-Fullerene Acceptors in Organic Solar Cells}, author = {Tzu-Yen Huang and Anton P Le Brun and Benedikt Sochor and Chun-Ming Wu and Yusuf Bulut and Peter Müller-Buschbaum and Stephan V Roth and Yan-Ling Yang}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85199690359&doi=10.1021%2facsanm.4c02865&partnerID=40&md5=3a48422082eab27e5ae5e7ac9c337dcd}, doi = {10.1021/acsanm.4c02865}, issn = {25740970}, year = {2024}, date = {2024-01-01}, journal = {ACS Applied Nano Materials}, volume = {7}, number = {15}, pages = {17588 – 17595}, publisher = {American Chemical Society}, abstract = {The nanomorphology of bulk heterojunctions (BHJs) plays a critical role in determining the performance of non-fullerene organic solar cells (OSCs). Thermal annealing is commonly used to reorganize the donor and acceptor phases within the BHJs. In this study, we investigate the vertical morphology of BHJ blend films incorporating the poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3‴-di(2-octyldodecyl)-2,2′;5′,2″;5″,2‴-quaterthiophen-5,5‴-diyl)] (PffBT4T-2OD) polymer as the donor and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC) as the acceptor. Neutron reflectivity patterns and scattering length density profiles reveal that the surface of the BHJ films became diffuse when the annealing temperature was above 150 °C. We further find that mitigated agglomeration of PffBT4T-2OD side chains exhibits minimal impact on morphology post-annealing. Instead, ITIC molecules trigger aggregations, accompanied by interface diffusion and increased film roughness. X-ray scattering confirms a 5-fold increase in aggregated ITIC nanodomains after annealing. Our findings highlight that unstable ITIC phases dominate the BHJ morphology of thin films, leading to the thermal instability of OSCs. This study enhances our understanding of the BHJ morphology and offers insights into improving the performance of energy conversion devices. © 2024 American Chemical Society.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } The nanomorphology of bulk heterojunctions (BHJs) plays a critical role in determining the performance of non-fullerene organic solar cells (OSCs). Thermal annealing is commonly used to reorganize the donor and acceptor phases within the BHJs. In this study, we investigate the vertical morphology of BHJ blend films incorporating the poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3‴-di(2-octyldodecyl)-2,2′;5′,2″;5″,2‴-quaterthiophen-5,5‴-diyl)] (PffBT4T-2OD) polymer as the donor and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC) as the acceptor. Neutron reflectivity patterns and scattering length density profiles reveal that the surface of the BHJ films became diffuse when the annealing temperature was above 150 °C. We further find that mitigated agglomeration of PffBT4T-2OD side chains exhibits minimal impact on morphology post-annealing. Instead, ITIC molecules trigger aggregations, accompanied by interface diffusion and increased film roughness. X-ray scattering confirms a 5-fold increase in aggregated ITIC nanodomains after annealing. Our findings highlight that unstable ITIC phases dominate the BHJ morphology of thin films, leading to the thermal instability of OSCs. This study enhances our understanding of the BHJ morphology and offers insights into improving the performance of energy conversion devices. © 2024 American Chemical Society. |
| 30. | Maier, Thomas L; de Kam, Lucas B T; Golibrzuch, Matthias; Angerer, Tina; Becherer, Markus; Krischer, Katharina: How Metal/Insulator Interfaces Enable an Enhancement of the Hydrogen Evolution Reaction Kinetics. In: ChemElectroChem, 11 (11), 2024, ISSN: 21960216, (Cited by: 0; All Open Access, Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Maier2024, title = {How Metal/Insulator Interfaces Enable an Enhancement of the Hydrogen Evolution Reaction Kinetics}, author = {Thomas L Maier and Lucas B T. de Kam and Matthias Golibrzuch and Tina Angerer and Markus Becherer and Katharina Krischer}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85193040302&doi=10.1002%2fcelc.202400109&partnerID=40&md5=fd23b3506d9f1ab0592cb211f1de3759}, doi = {10.1002/celc.202400109}, issn = {21960216}, year = {2024}, date = {2024-01-01}, journal = {ChemElectroChem}, volume = {11}, number = {11}, publisher = {John Wiley and Sons Inc}, abstract = {The nanostructuring of electrodes is a common way of increasing electrocatalytic activity. Yet, the fact that the presence of insulating material in nanostructured composites can have a positive effect on efficiency was an unexpected recent finding. The rate enhancement has been linked to different electric fields at the insulator and metal interfaces, facilitating enhanced transport of reaction products into the bulk electrolyte. In this article, we further uncover the origin of the rate enhancement with parameter studies and simulations. We experimentally investigate various parameter dependencies of the alkaline Hydrogen Evolution Reaction (HER) on well-defined nanometer-sized Au arrays embedded in a silicon nitride insulating layer. We find a significant enhancement of the HER for all experimental conditions and opposite activity trends with pH, electrolyte concentration and the cationic species compared to a continuous Au electrode. Using a mean field model, we quantify the electrostatic interfacial pressure above the Au and the insulator patches. Combining the double layer simulations with rate equations, we demonstrate that all parameter variations can be consistently explained by the fact that the double layer structure above the insulator patches is much less rigid than above the metal islands and is independent of the applied potential. © 2024 The Authors. ChemElectroChem published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The nanostructuring of electrodes is a common way of increasing electrocatalytic activity. Yet, the fact that the presence of insulating material in nanostructured composites can have a positive effect on efficiency was an unexpected recent finding. The rate enhancement has been linked to different electric fields at the insulator and metal interfaces, facilitating enhanced transport of reaction products into the bulk electrolyte. In this article, we further uncover the origin of the rate enhancement with parameter studies and simulations. We experimentally investigate various parameter dependencies of the alkaline Hydrogen Evolution Reaction (HER) on well-defined nanometer-sized Au arrays embedded in a silicon nitride insulating layer. We find a significant enhancement of the HER for all experimental conditions and opposite activity trends with pH, electrolyte concentration and the cationic species compared to a continuous Au electrode. Using a mean field model, we quantify the electrostatic interfacial pressure above the Au and the insulator patches. Combining the double layer simulations with rate equations, we demonstrate that all parameter variations can be consistently explained by the fact that the double layer structure above the insulator patches is much less rigid than above the metal islands and is independent of the applied potential. © 2024 The Authors. ChemElectroChem published by Wiley-VCH GmbH. |
| 31. | Rasouli, Azam; Kudyba, Artur; Bruzda, Grzegorz; Safarian, Jafar; Tranell, Gabriella: High-Temperature Reactive Wetting of Natural Quartz by Liquid Magnesium. In: Materials, 17 (6), 2024, ISSN: 19961944, (Cited by: 0; All Open Access, Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Rasouli2024, title = {High-Temperature Reactive Wetting of Natural Quartz by Liquid Magnesium}, author = {Azam Rasouli and Artur Kudyba and Grzegorz Bruzda and Jafar Safarian and Gabriella Tranell}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189066882&doi=10.3390%2fma17061302&partnerID=40&md5=9c63350502cd6144c155f86b3c7474f5}, doi = {10.3390/ma17061302}, issn = {19961944}, year = {2024}, date = {2024-01-01}, journal = {Materials}, volume = {17}, number = {6}, publisher = {Multidisciplinary Digital Publishing Institute (MDPI)}, abstract = {High-temperature wetting of natural, high-purity quartz (SiO2) and liquid magnesium (Mg) was investigated at temperatures between 973 and 1273 K. Sessile drop experiments using the capillary purification (CP) procedure were carried out under an Ar gas atmosphere (N6.0), eliminating the native oxide layer on the surface of Mg melt. The results showed that the wetting behavior was strongly dependent on temperature. At 973 and 1073 K, the wetting system displayed relatively large contact angles of 90° and 65°, respectively, demonstrating modest wetting. The wetting increased to some extent by increasing the temperature to 1123 K with a wetting angle of 22°. However, the SiO2/Mg system demonstrated complete wetting at temperatures of 1173 K and above. Furthermore, interface microstructure examination showed different reaction product phases/microstructures, depending on the wetting experiment temperature. © 2024 by the authors.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } High-temperature wetting of natural, high-purity quartz (SiO2) and liquid magnesium (Mg) was investigated at temperatures between 973 and 1273 K. Sessile drop experiments using the capillary purification (CP) procedure were carried out under an Ar gas atmosphere (N6.0), eliminating the native oxide layer on the surface of Mg melt. The results showed that the wetting behavior was strongly dependent on temperature. At 973 and 1073 K, the wetting system displayed relatively large contact angles of 90° and 65°, respectively, demonstrating modest wetting. The wetting increased to some extent by increasing the temperature to 1123 K with a wetting angle of 22°. However, the SiO2/Mg system demonstrated complete wetting at temperatures of 1173 K and above. Furthermore, interface microstructure examination showed different reaction product phases/microstructures, depending on the wetting experiment temperature. © 2024 by the authors. |
| 32. | Tian, Ting; Tu, Suo; Xu, Ang; Yin, Shanshan; Oechsle, Anna Lena; Xiao, Tianxiao; Vagias, Apostolos; Eichhorn, Johanna; Suo, Jinping; Yang, Zhangcan; Bernstorff, Sigrid; Müller-Buschbaum, Peter: Unraveling the Morphology-Function Correlation of Mesoporous ZnO Films upon Water Exposure. In: Advanced Functional Materials, 34 (8), 2024, ISSN: 1616301X, (Cited by: 1; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Tian2024, title = {Unraveling the Morphology-Function Correlation of Mesoporous ZnO Films upon Water Exposure}, author = {Ting Tian and Suo Tu and Ang Xu and Shanshan Yin and Anna Lena Oechsle and Tianxiao Xiao and Apostolos Vagias and Johanna Eichhorn and Jinping Suo and Zhangcan Yang and Sigrid Bernstorff and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85175527704&doi=10.1002%2fadfm.202311793&partnerID=40&md5=c31a4f3b28afc46702547814c531584e}, doi = {10.1002/adfm.202311793}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, volume = {34}, number = {8}, publisher = {John Wiley and Sons Inc}, abstract = {Ubiquitous moisture in synthetic conditions and ambient environments can strongly influence the conductivity of ZnO semiconductors via the chemisorption and physisorption of water molecules on the ZnO surface. Such an intrinsically water-sensitive nature will become more evident in mesoporous ZnO films where a large surface area and active sites are created simultaneously. However, fundamental insights underlying water-mediated ZnO surface chemistry and electrical conductivity and the factors affecting them remain ambiguous due to the complexity of ZnO surfaces and the difficulties of in situ characterizations at multi-dimensions. Here, self-assembling diblock copolymers are exploited as structure-directing agents to achieve mesoporous ZnO thin films with highly tailorable structural characteristics ranging from nanomorphologies, over crystalline levels, to defect contents. As verified by theoretical calculations, the presence of oxygen vacancy will facilitate favorable water adsorption and subsequent dissociation on the polar ZnO surfaces. Upon humidity exposure with progressively increased levels, mesoporous ZnO films are revealed to follow an almost positive relationship between adsorption and electrical conductivity but show superior morphological stability. This work not only elucidates the water-governed ZnO surface chemistry but may also promote a comprehensive understanding of the morphology-function relationship on ZnO-based electronics. © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Ubiquitous moisture in synthetic conditions and ambient environments can strongly influence the conductivity of ZnO semiconductors via the chemisorption and physisorption of water molecules on the ZnO surface. Such an intrinsically water-sensitive nature will become more evident in mesoporous ZnO films where a large surface area and active sites are created simultaneously. However, fundamental insights underlying water-mediated ZnO surface chemistry and electrical conductivity and the factors affecting them remain ambiguous due to the complexity of ZnO surfaces and the difficulties of in situ characterizations at multi-dimensions. Here, self-assembling diblock copolymers are exploited as structure-directing agents to achieve mesoporous ZnO thin films with highly tailorable structural characteristics ranging from nanomorphologies, over crystalline levels, to defect contents. As verified by theoretical calculations, the presence of oxygen vacancy will facilitate favorable water adsorption and subsequent dissociation on the polar ZnO surfaces. Upon humidity exposure with progressively increased levels, mesoporous ZnO films are revealed to follow an almost positive relationship between adsorption and electrical conductivity but show superior morphological stability. This work not only elucidates the water-governed ZnO surface chemistry but may also promote a comprehensive understanding of the morphology-function relationship on ZnO-based electronics. © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. |
| 33. | Kumar, Labeesh; Nandan, Bhanu; Sarkar, Swagato; König, Tobias A F; Pohl, Darius; Tsuda, Takuya; Zainuddin, Muhammad S B; Humenik, Martin; Scheibel, Thomas; Horechyy, Andriy: Enhanced photocatalytic performance of coaxially electrospun titania nanofibers comprising yolk-shell particles. In: Journal of Colloid and Interface Science, 674 , pp. 560 – 575, 2024, ISSN: 00219797, (Cited by: 1; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Kumar2024560, title = {Enhanced photocatalytic performance of coaxially electrospun titania nanofibers comprising yolk-shell particles}, author = {Labeesh Kumar and Bhanu Nandan and Swagato Sarkar and Tobias A F König and Darius Pohl and Takuya Tsuda and Muhammad S B Zainuddin and Martin Humenik and Thomas Scheibel and Andriy Horechyy}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85197361436&doi=10.1016%2fj.jcis.2024.06.133&partnerID=40&md5=80e88d019a726da6fa5ed4a36d48cc7f}, doi = {10.1016/j.jcis.2024.06.133}, issn = {00219797}, year = {2024}, date = {2024-01-01}, journal = {Journal of Colloid and Interface Science}, volume = {674}, pages = {560 – 575}, publisher = {Academic Press Inc.}, abstract = {The present paper reports the fabrication of novel types of hybrid fibrous photocatalysts by combining block copolymer (BCP) templating, sol–gel processing, and coaxial electrospinning techniques. Coaxial electrospinning produces core–shell nanofibers (NFs), which are converted into hollow porous TiO2 NFs using an oxidative calcination step. Hybrid BCP micelles comprising a single plasmonic nanoparticle (NP) in their core and thereof derived silica-coated core–shell particles are utilized as precursors to generate yolk-shell type particulate inclusions in photocatalytically active NFs. The catalytic and photocatalytic activity of calcined NFs comprising different types of yolk-shell particles is systematically investigated and compared. Interestingly, calcined NFs comprising silica-coated yolk-shells demonstrate enhanced catalytic and photocatalytic performance despite the presence of silica shell separating plasmonic NP from the TiO2 matrix. Electromagnetic simulations indicate that this enhancement is caused by a localized surface plasmon resonance and a confinement effect in silica-coated yolk-shells embedded in porous TiO2 NFs. Utilization of the coaxially electrospun TiO2 NFs in combination with yolk-shells comprising plasmonic NPs reveals to be a potent method for the photocatalytic decomposition of numerous pollutants. It is worth noting that this study stands as the first occurrence of combining yolk-shells (Au@void@SiO2) with porous electrospun NFs (TiO2) for photocatalytic purposes and gaining an understanding of plasmon and confinement effects for photocatalytic performance. This approach represents a promising route for fabricating highly active and up-scalable fibrous photocatalytic systems. © 2024 The Authors}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The present paper reports the fabrication of novel types of hybrid fibrous photocatalysts by combining block copolymer (BCP) templating, sol–gel processing, and coaxial electrospinning techniques. Coaxial electrospinning produces core–shell nanofibers (NFs), which are converted into hollow porous TiO2 NFs using an oxidative calcination step. Hybrid BCP micelles comprising a single plasmonic nanoparticle (NP) in their core and thereof derived silica-coated core–shell particles are utilized as precursors to generate yolk-shell type particulate inclusions in photocatalytically active NFs. The catalytic and photocatalytic activity of calcined NFs comprising different types of yolk-shell particles is systematically investigated and compared. Interestingly, calcined NFs comprising silica-coated yolk-shells demonstrate enhanced catalytic and photocatalytic performance despite the presence of silica shell separating plasmonic NP from the TiO2 matrix. Electromagnetic simulations indicate that this enhancement is caused by a localized surface plasmon resonance and a confinement effect in silica-coated yolk-shells embedded in porous TiO2 NFs. Utilization of the coaxially electrospun TiO2 NFs in combination with yolk-shells comprising plasmonic NPs reveals to be a potent method for the photocatalytic decomposition of numerous pollutants. It is worth noting that this study stands as the first occurrence of combining yolk-shells (Au@void@SiO2) with porous electrospun NFs (TiO2) for photocatalytic purposes and gaining an understanding of plasmon and confinement effects for photocatalytic performance. This approach represents a promising route for fabricating highly active and up-scalable fibrous photocatalytic systems. © 2024 The Authors |
| 34. | Xiao, Tianxiao; Tu, Suo; Tian, Ting; Chen, Wei; Cao, Wei; Liang, Suzhe; Guo, Renjun; Liu, Liangzhen; Li, Yanan; Guan, Tianfu; Liu, Haochen; Wang, Kai; Schwartzkopf, Matthias; Fischer, Roland A; Roth, Stephan V; Müller-Buschbaum, Peter: Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell. In: Nano Energy, 125 , 2024, ISSN: 22112855, (Cited by: 3; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Xiao2024b, title = {Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell}, author = {Tianxiao Xiao and Suo Tu and Ting Tian and Wei Chen and Wei Cao and Suzhe Liang and Renjun Guo and Liangzhen Liu and Yanan Li and Tianfu Guan and Haochen Liu and Kai Wang and Matthias Schwartzkopf and Roland A Fischer and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189558263&doi=10.1016%2fj.nanoen.2024.109555&partnerID=40&md5=fe94f06e4335e9dfe56b1d138c4a15ec}, doi = {10.1016/j.nanoen.2024.109555}, issn = {22112855}, year = {2024}, date = {2024-01-01}, journal = {Nano Energy}, volume = {125}, publisher = {Elsevier Ltd}, abstract = {Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems. © 2024 The Authors}, note = {Cited by: 3; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems. © 2024 The Authors |
| 35. | Tu, Suo; Tian, Ting; Xiao, Tianxiao; Yao, Xiangtong; Shen, Sicong; Wu, Yansong; Liu, Yinlong; Bing, Zhenshan; Huang, Kai; Knoll, Alois; Yin, Shanshan; Liang, Suzhe; Heger, Julian E; Pan, Guangjiu; Schwartzkopf, Matthias; Roth, Stephan V; Müller-Buschbaum, Peter: Humidity Stable Thermoelectric Hybrid Materials Toward a Self-Powered Triple Sensing System. In: Advanced Functional Materials, 34 (25), 2024, ISSN: 1616301X, (Cited by: 4; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Tu2024, title = {Humidity Stable Thermoelectric Hybrid Materials Toward a Self-Powered Triple Sensing System}, author = {Suo Tu and Ting Tian and Tianxiao Xiao and Xiangtong Yao and Sicong Shen and Yansong Wu and Yinlong Liu and Zhenshan Bing and Kai Huang and Alois Knoll and Shanshan Yin and Suzhe Liang and Julian E Heger and Guangjiu Pan and Matthias Schwartzkopf and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85184738841&doi=10.1002%2fadfm.202316088&partnerID=40&md5=287dd8d98d9b38231d5a939bd31c8f2c}, doi = {10.1002/adfm.202316088}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, volume = {34}, number = {25}, publisher = {John Wiley and Sons Inc}, abstract = {Highly sensitive and humidity-resistive detection of the most common physical stimuli is of primary importance for practical application in real-time monitoring. Here, a simple yet effective strategy is reported to achieve a highly humidity-stable hybrid composite that enables simultaneous and accurate pressure and temperature sensing in a single sensor. The improved electronic performance is due to the enhanced planarity of poly (3,-4ethylenedioxythiophene) (PEDOT) and charge transfer between PEDOT:polystyrene sulfonate (PEDOT:PSS) and multi-walled carbon nanotubes (CNTs) by strong π–π interaction. The preferred electronic pathway induced by a robust morphology in the hybrid composite is responsible for the high humidity stability. This study also demonstrates that the sensor has tremendous potential for intelligent object identification with a high level of 97.78% accuracy. Together with the position-detection capability of a triboelectric nanogenerator (TENG), advantages for potential industrial applications of the triple sensing system in terms of intelligent classification without seeing are foreseen. © 2024 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.}, note = {Cited by: 4; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Highly sensitive and humidity-resistive detection of the most common physical stimuli is of primary importance for practical application in real-time monitoring. Here, a simple yet effective strategy is reported to achieve a highly humidity-stable hybrid composite that enables simultaneous and accurate pressure and temperature sensing in a single sensor. The improved electronic performance is due to the enhanced planarity of poly (3,-4ethylenedioxythiophene) (PEDOT) and charge transfer between PEDOT:polystyrene sulfonate (PEDOT:PSS) and multi-walled carbon nanotubes (CNTs) by strong π–π interaction. The preferred electronic pathway induced by a robust morphology in the hybrid composite is responsible for the high humidity stability. This study also demonstrates that the sensor has tremendous potential for intelligent object identification with a high level of 97.78% accuracy. Together with the position-detection capability of a triboelectric nanogenerator (TENG), advantages for potential industrial applications of the triple sensing system in terms of intelligent classification without seeing are foreseen. © 2024 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. |
| 36. | Hegner, Franziska S; Cohen, Adi; Rudel, Stefan S; Kronawitter, Silva M; Grumet, Manuel; Zhu, Xiangzhou; Korobko, Roman; Houben, Lothar; Jiang, Chang-Ming; Schnick, Wolfgang; Kieslich, Gregor; Yaffe, Omer; Sharp, Ian D; Egger, David A: The Critical Role of Anharmonic Lattice Dynamics for Macroscopic Properties of the Visible Light Absorbing Nitride Semiconductor CuTaN2. In: Advanced Energy Materials, 14 (19), 2024, ISSN: 16146832, (Cited by: 1; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Hegner2024, title = {The Critical Role of Anharmonic Lattice Dynamics for Macroscopic Properties of the Visible Light Absorbing Nitride Semiconductor CuTaN2}, author = {Franziska S Hegner and Adi Cohen and Stefan S Rudel and Silva M Kronawitter and Manuel Grumet and Xiangzhou Zhu and Roman Korobko and Lothar Houben and Chang-Ming Jiang and Wolfgang Schnick and Gregor Kieslich and Omer Yaffe and Ian D Sharp and David A Egger}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85188909385&doi=10.1002%2faenm.202303059&partnerID=40&md5=8d45614f8e878ca4ff40bda022a028f0}, doi = {10.1002/aenm.202303059}, issn = {16146832}, year = {2024}, date = {2024-01-01}, journal = {Advanced Energy Materials}, volume = {14}, number = {19}, publisher = {John Wiley and Sons Inc}, abstract = {Ternary nitride semiconductors are rapidly emerging as a promising class of materials for energy conversion applications, offering an appealing combination of strong light absorption in the visible range, desirable charge transport characteristics, and good chemical stability. In this work, it is shown that finite-temperature lattice dynamics in CuTaN2 – a prototypical ternary nitride displaying particularly strong visible light absorption – exhibit a pronounced anharmonic character that plays an essential role in defining its macroscopic optoelectronic and thermal properties. Low-frequency vibrational modes that are Raman-inactive from symmetry considerations of the average crystal structure and unstable in harmonic phonon calculations are found to appear as intensive Raman features near room temperature. The atomic contributions to the anharmonic vibrations are characterized by combining Raman measurements with molecular dynamics and density functional theory calculations. This analysis reveals that anharmonic lattice dynamics have large ramifications on the fundamental properties of this compound, resulting in uniaxial negative thermal expansion and the opening of its bandgap to a near-optimal value for solar energy harvesting. The atomic-level understanding of anharmonic lattice dynamics, as well as the finding that they strongly influence key properties of this semiconductor at room temperature, have important implications for design of new functional materials, especially within the emerging class of ternary nitride semiconductors. © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Ternary nitride semiconductors are rapidly emerging as a promising class of materials for energy conversion applications, offering an appealing combination of strong light absorption in the visible range, desirable charge transport characteristics, and good chemical stability. In this work, it is shown that finite-temperature lattice dynamics in CuTaN2 – a prototypical ternary nitride displaying particularly strong visible light absorption – exhibit a pronounced anharmonic character that plays an essential role in defining its macroscopic optoelectronic and thermal properties. Low-frequency vibrational modes that are Raman-inactive from symmetry considerations of the average crystal structure and unstable in harmonic phonon calculations are found to appear as intensive Raman features near room temperature. The atomic contributions to the anharmonic vibrations are characterized by combining Raman measurements with molecular dynamics and density functional theory calculations. This analysis reveals that anharmonic lattice dynamics have large ramifications on the fundamental properties of this compound, resulting in uniaxial negative thermal expansion and the opening of its bandgap to a near-optimal value for solar energy harvesting. The atomic-level understanding of anharmonic lattice dynamics, as well as the finding that they strongly influence key properties of this semiconductor at room temperature, have important implications for design of new functional materials, especially within the emerging class of ternary nitride semiconductors. © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. |
| 37. | Posnjak, Gregor; Yin, Xin; Butler, Paul; Bienek, Oliver; Dass, Mihir; Lee, Seungwoo; Sharp, Ian D; Liedl, Tim: Diamond-lattice photonic crystals assembled from DNA origami. In: Science, 384 (6697), pp. 781 – 785, 2024, ISSN: 00368075, (Cited by: 6; All Open Access, Green Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Posnjak2024781, title = {Diamond-lattice photonic crystals assembled from DNA origami}, author = {Gregor Posnjak and Xin Yin and Paul Butler and Oliver Bienek and Mihir Dass and Seungwoo Lee and Ian D Sharp and Tim Liedl}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85193516157&doi=10.1126%2fscience.adl2733&partnerID=40&md5=6d4f8061bc1a63794487b181922a88ed}, doi = {10.1126/science.adl2733}, issn = {00368075}, year = {2024}, date = {2024-01-01}, journal = {Science}, volume = {384}, number = {6697}, pages = {781 – 785}, publisher = {American Association for the Advancement of Science}, abstract = {Colloidal self-assembly allows rational design of structures on the micrometer and submicrometer scale. One architecture that can generate complete three-dimensional photonic bandgaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable with the wavelength of visible or ultraviolet light. In this work, we demonstrate three-dimensional photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nanometers. This structure serves as a scaffold for atomic-layer deposition of high–refractive index materials such as titanium dioxide, yielding a tunable photonic bandgap in the near-ultraviolet. © 2024 American Association for the Advancement of Science. All rights reserved.}, note = {Cited by: 6; All Open Access, Green Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Colloidal self-assembly allows rational design of structures on the micrometer and submicrometer scale. One architecture that can generate complete three-dimensional photonic bandgaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable with the wavelength of visible or ultraviolet light. In this work, we demonstrate three-dimensional photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nanometers. This structure serves as a scaffold for atomic-layer deposition of high–refractive index materials such as titanium dioxide, yielding a tunable photonic bandgap in the near-ultraviolet. © 2024 American Association for the Advancement of Science. All rights reserved. |
| 38. | Mentzel, Paul; Holzapfel, Marco; Schmiedel, Alexander; Günther, Johanna; Michel, Maximilian; Krummenacher, Ivo; Wodyński, Artur; Kaupp, Martin; Braunschweig, Holger; Lambert, Christoph: Structure and Photophysics of N-Tolanyl-phenochalcogenazines and their Radical Cations. In: Chemistry - A European Journal, 30 (19), 2024, ISSN: 09476539, (Cited by: 0; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Mentzel2024, title = {Structure and Photophysics of N-Tolanyl-phenochalcogenazines and their Radical Cations}, author = {Paul Mentzel and Marco Holzapfel and Alexander Schmiedel and Johanna Günther and Maximilian Michel and Ivo Krummenacher and Artur Wodyński and Martin Kaupp and Holger Braunschweig and Christoph Lambert}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85185108520&doi=10.1002%2fchem.202303782&partnerID=40&md5=b86f6d73ed4a41c13fbe919d29156c99}, doi = {10.1002/chem.202303782}, issn = {09476539}, year = {2024}, date = {2024-01-01}, journal = {Chemistry - A European Journal}, volume = {30}, number = {19}, publisher = {John Wiley and Sons Inc}, abstract = {The study focuses on the structural and photophysical characteristics of neutral and oxidized forms of N-tolanyl-phenochalcogenazines PZX-tolan with X=O, S, Se, and Te. X-ray crystal structure analyses show a pseudo-equatorial (pe) structure of the tolan substituent in the O, S, and Se dyads, while the Te dyad possesses a pseudo-axial (pa) structure. DFT calculations suggest the pe structure for O and S, and the pa structure for Se and Te as stable forms. Steady-state and femtosecond-time resolved optical spectroscopy in toluene solution indicate that the O and S dyads emit from a CT state, whereas the Se and Te dyads emit from a tolan-localized state. The T1 state is tolan-localized in all cases, showing phosphorescence at 77 K. The heavy atom effect of chalcogens induces intersystem crossing from S1 to Tx, resulting in a decreasing S1 lifetime from 2.1 ns to 0.42 ps. The T1 states possess potential for singlet oxygen sensitization with a high quantum yield (ca. 40 %) for the O, S, and Se dyads. Radical cations exhibit spin density primarily localized at the heterocycle. EPR measurements and quasirelativistic DFT calculations reveal a very strong g-tensor anisotropy, supporting the pe structure for the S and Se derivatives. © 2024 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The study focuses on the structural and photophysical characteristics of neutral and oxidized forms of N-tolanyl-phenochalcogenazines PZX-tolan with X=O, S, Se, and Te. X-ray crystal structure analyses show a pseudo-equatorial (pe) structure of the tolan substituent in the O, S, and Se dyads, while the Te dyad possesses a pseudo-axial (pa) structure. DFT calculations suggest the pe structure for O and S, and the pa structure for Se and Te as stable forms. Steady-state and femtosecond-time resolved optical spectroscopy in toluene solution indicate that the O and S dyads emit from a CT state, whereas the Se and Te dyads emit from a tolan-localized state. The T1 state is tolan-localized in all cases, showing phosphorescence at 77 K. The heavy atom effect of chalcogens induces intersystem crossing from S1 to Tx, resulting in a decreasing S1 lifetime from 2.1 ns to 0.42 ps. The T1 states possess potential for singlet oxygen sensitization with a high quantum yield (ca. 40 %) for the O, S, and Se dyads. Radical cations exhibit spin density primarily localized at the heterocycle. EPR measurements and quasirelativistic DFT calculations reveal a very strong g-tensor anisotropy, supporting the pe structure for the S and Se derivatives. © 2024 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH. |
| 39. | de Kam, Lucas B T; Maier, Thomas L; Krischer, Katharina: Electrolyte effects on the alkaline hydrogen evolution reaction: A mean-field approach. In: Electrochimica Acta, 497 , 2024, ISSN: 00134686, (Cited by: 0; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{deKam2024, title = {Electrolyte effects on the alkaline hydrogen evolution reaction: A mean-field approach}, author = {Lucas B T de Kam and Thomas L Maier and Katharina Krischer}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85195863948&doi=10.1016%2fj.electacta.2024.144530&partnerID=40&md5=568a9ec1f88599475525bd6d1a5f6cee}, doi = {10.1016/j.electacta.2024.144530}, issn = {00134686}, year = {2024}, date = {2024-01-01}, journal = {Electrochimica Acta}, volume = {497}, publisher = {Elsevier Ltd}, abstract = {This paper introduces the combination of an advanced double-layer model with electrochemical kinetics to explain electrolyte effects on the alkaline hydrogen evolution reaction. It is known from experimental studies that the alkaline hydrogen evolution current shows a strong dependence on the concentration and identity of cations in the electrolyte, but is independent of pH. To explain these effects, we formulate the faradaic current in terms of the electric potential in the double layer, which is calculated using a mean-field model that takes into account the cation and anion sizes as well as the electric dipole moment of water molecules. We propose that the Volmer step consists of two activated processes: a water reduction sub-step, and a sub-step in which OH− is transferred away from the reaction plane through the double layer. Either of these sub-steps may limit the rate. The proposed models for these sub-steps qualitatively explain experimental observations, including cation effects, pH-independence, and the trend reversal between gold and platinum electrodes. We also assess the quantitative accuracy of the water-reduction-limited current model; we suggest that the predicted functional relationship is valid as long as the hydrogen bonding structure of water near the electrode is sufficiently maintained. © 2024 The Author(s)}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } This paper introduces the combination of an advanced double-layer model with electrochemical kinetics to explain electrolyte effects on the alkaline hydrogen evolution reaction. It is known from experimental studies that the alkaline hydrogen evolution current shows a strong dependence on the concentration and identity of cations in the electrolyte, but is independent of pH. To explain these effects, we formulate the faradaic current in terms of the electric potential in the double layer, which is calculated using a mean-field model that takes into account the cation and anion sizes as well as the electric dipole moment of water molecules. We propose that the Volmer step consists of two activated processes: a water reduction sub-step, and a sub-step in which OH− is transferred away from the reaction plane through the double layer. Either of these sub-steps may limit the rate. The proposed models for these sub-steps qualitatively explain experimental observations, including cation effects, pH-independence, and the trend reversal between gold and platinum electrodes. We also assess the quantitative accuracy of the water-reduction-limited current model; we suggest that the predicted functional relationship is valid as long as the hydrogen bonding structure of water near the electrode is sufficiently maintained. © 2024 The Author(s) |
| 40. | Wang, Qiyou; Gong, Yujie; Zi, Xin; Gan, Lei; Pensa, Evangelina; Liu, Yuxiang; Xiao, Yusen; Li, Hongmei; Liu, Kang; Fu, Junwei; Liu, Jun; Stefancu, Andrei; Cai, Chao; Chen, Shanyong; Zhang, Shiguo; Lu, Ying-Rui; Chan, Ting-Shan; Ma, Chao; Cao, Xueying; Cortés, Emiliano; Liu, Min: Coupling Nano and Atomic Electric Field Confinement for Robust Alkaline Oxygen Evolution. In: Angewandte Chemie - International Edition, 63 (28), 2024, ISSN: 14337851, (Cited by: 8; All Open Access, Hybrid Gold Open Access). (Type: Journal Article | Abstract | Links | BibTeX) @article{Wang2024b, title = {Coupling Nano and Atomic Electric Field Confinement for Robust Alkaline Oxygen Evolution}, author = {Qiyou Wang and Yujie Gong and Xin Zi and Lei Gan and Evangelina Pensa and Yuxiang Liu and Yusen Xiao and Hongmei Li and Kang Liu and Junwei Fu and Jun Liu and Andrei Stefancu and Chao Cai and Shanyong Chen and Shiguo Zhang and Ying-Rui Lu and Ting-Shan Chan and Chao Ma and Xueying Cao and Emiliano Cortés and Min Liu}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85195690153&doi=10.1002%2fanie.202405438&partnerID=40&md5=4185ba4411edd789080ce5e3183b09b5}, doi = {10.1002/anie.202405438}, issn = {14337851}, year = {2024}, date = {2024-01-01}, journal = {Angewandte Chemie - International Edition}, volume = {63}, number = {28}, publisher = {John Wiley and Sons Inc}, abstract = {The alkaline oxygen evolution reaction (OER) is a promising avenue for producing clean fuels and storing intermittent energy. However, challenges such as excessive OH− consumption and strong adsorption of oxygen-containing intermediates hinder the development of alkaline OER. In this study, we propose a cooperative strategy by leveraging both nano-scale and atomically local electric fields for alkaline OER, demonstrated through the synthesis of Mn single atom doped CoP nanoneedles (Mn SA-CoP NNs). Finite element method simulations and density functional theory calculations predict that the nano-scale local electric field enriches OH− around the catalyst surface, while the atomically local electric field improves *O desorption. Experimental validation using in situ attenuated total reflection infrared and Raman spectroscopy confirms the effectiveness of the nano-scale and atomically electric fields. Mn SA-CoP NNs exhibit an ultra-low overpotential of 189 mV at 10 mA cm−2 and stable operation over 100 hours at ~100 mA cm−2 during alkaline OER. This innovative strategy provides new insights for enhancing catalyst performance in energy conversion reactions. © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.}, note = {Cited by: 8; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The alkaline oxygen evolution reaction (OER) is a promising avenue for producing clean fuels and storing intermittent energy. However, challenges such as excessive OH− consumption and strong adsorption of oxygen-containing intermediates hinder the development of alkaline OER. In this study, we propose a cooperative strategy by leveraging both nano-scale and atomically local electric fields for alkaline OER, demonstrated through the synthesis of Mn single atom doped CoP nanoneedles (Mn SA-CoP NNs). Finite element method simulations and density functional theory calculations predict that the nano-scale local electric field enriches OH− around the catalyst surface, while the atomically local electric field improves *O desorption. Experimental validation using in situ attenuated total reflection infrared and Raman spectroscopy confirms the effectiveness of the nano-scale and atomically electric fields. Mn SA-CoP NNs exhibit an ultra-low overpotential of 189 mV at 10 mA cm−2 and stable operation over 100 hours at ~100 mA cm−2 during alkaline OER. This innovative strategy provides new insights for enhancing catalyst performance in energy conversion reactions. © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. |
References (last update: Sept. 23, 2024):
2024 |
Zou, Yuqin; Eichhorn, Johanna; Zhang, Jiyun; Apfelbeck, Fabian A C; Yin, Shanshan; Wolz, Lukas; Chen, Chun-Chao; Sharp, Ian D; Müller-Buschbaum, Peter Microstrain and Crystal Orientation Variation within Naked Triple-Cation Mixed Halide Perovskites under Heat, UV, and Visible Light Exposure Journal Article ACS Energy Letters, 9 (2), pp. 388 – 399, 2024, ISSN: 23808195, (Cited by: 5; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Zou2024388, title = {Microstrain and Crystal Orientation Variation within Naked Triple-Cation Mixed Halide Perovskites under Heat, UV, and Visible Light Exposure}, author = {Yuqin Zou and Johanna Eichhorn and Jiyun Zhang and Fabian A C Apfelbeck and Shanshan Yin and Lukas Wolz and Chun-Chao Chen and Ian D Sharp and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85182585402&doi=10.1021%2facsenergylett.3c02617&partnerID=40&md5=0ea17b72520b6255fc9fccdcc056a6f6}, doi = {10.1021/acsenergylett.3c02617}, issn = {23808195}, year = {2024}, date = {2024-01-01}, journal = {ACS Energy Letters}, volume = {9}, number = {2}, pages = {388 – 399}, publisher = {American Chemical Society}, abstract = {The instability of perovskite absorbers under various environmental stressors is the most significant obstacle to widespread commercialization of perovskite solar cells. Herein, we study the evolution of crystal structure and microstrain present in naked triple-cation mixed CsMAFA-based perovskite films under heat, UV, and visible light (1 Sun) conditions by grazing-incidence wide-angle X-ray scattering (GIWAXS). We find that the microstrain is gradient distributed along the surface normal of the films, decreasing from the upper surface to regions deeper within the film. Moreover, heat, UV, and visible light treatments do not interfere with the crystalline orientations within annealed polycrystalline films. However, when subjected to heat, the naked perovskite films exhibit a rapid component decomposition, induced by phase separation and ion migration. Conversely, under exposure to UV and 1 Sun light soaking, the naked perovskite films undergo a self-optimization structure evolution during degradation and develop into smoother films with reduced surface potential fluctuations. © 2024 The Authors. Published by American Chemical Society.}, note = {Cited by: 5; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The instability of perovskite absorbers under various environmental stressors is the most significant obstacle to widespread commercialization of perovskite solar cells. Herein, we study the evolution of crystal structure and microstrain present in naked triple-cation mixed CsMAFA-based perovskite films under heat, UV, and visible light (1 Sun) conditions by grazing-incidence wide-angle X-ray scattering (GIWAXS). We find that the microstrain is gradient distributed along the surface normal of the films, decreasing from the upper surface to regions deeper within the film. Moreover, heat, UV, and visible light treatments do not interfere with the crystalline orientations within annealed polycrystalline films. However, when subjected to heat, the naked perovskite films exhibit a rapid component decomposition, induced by phase separation and ion migration. Conversely, under exposure to UV and 1 Sun light soaking, the naked perovskite films undergo a self-optimization structure evolution during degradation and develop into smoother films with reduced surface potential fluctuations. © 2024 The Authors. Published by American Chemical Society. |
Li, Yanan; Li, Nian; Harder, Constantin; Yin, Shanshan; Bulut, Yusuf; Vagias, Apostolos; Schneider, Peter M; Chen, Wei; Roth, Stephan V; Bandarenka, Aliaksandr S; Müller-Buschbaum, Peter Factors Shaping the Morphology in Sol-Gel Derived Mesoporous Zinc Titanate Films: Unveiling the Role of Precursor Competition and Concentration Journal Article Advanced Materials Interfaces, 2024, ISSN: 21967350, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Li2024, title = {Factors Shaping the Morphology in Sol-Gel Derived Mesoporous Zinc Titanate Films: Unveiling the Role of Precursor Competition and Concentration}, author = {Yanan Li and Nian Li and Constantin Harder and Shanshan Yin and Yusuf Bulut and Apostolos Vagias and Peter M Schneider and Wei Chen and Stephan V Roth and Aliaksandr S Bandarenka and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85202997412&doi=10.1002%2fadmi.202400215&partnerID=40&md5=24200471c1385cf1b1833f9aaee468ef}, doi = {10.1002/admi.202400215}, issn = {21967350}, year = {2024}, date = {2024-01-01}, journal = {Advanced Materials Interfaces}, publisher = {John Wiley and Sons Inc}, abstract = {Zinc titanate films with mesoporous structures have widespread applications ranging from sensors to supercapacitors and bio-devices owing to their photoelectric properties and specific surface area. The present work investigates the morphology of mesoporous zinc titanate films obtained by calcination of hybrid thin films containing polymer templates and precursor mixtures of zinc acetate dihydrate (ZAD) and titanium isopropoxide (TTIP). ZnO and TiO2 films are fabricated for reference. The influences of hydrochloric acid contents (HCl), the ratios of ZAD and TTIP, and the solution concentrations on the film morphologies are studied. The amphiphilic diblock copolymer, polystyrene-block-polyethylene oxide (PS-b-PEO), plays the role of a structure directing template, as it self-assembles into micelles in a solvent-acid mixture of N, N-dimethylformamide (DMF) and HCl. Thin films are prepared with spin-coating and subsequent calcination. Adjusting the ratio of TTIP and ZAD leads to the structure evolution from order to disorder in a film. It depends on the hydrolysis and condensation processes of the precursors, providing different time-to-growth processes to control the film morphologies. An increase in solution concentration enhances the surface coverage. As probed with grazing-incidence small-angle X-ray scattering, the inner structures are larger than the surface structures seen in scanning electron microscopy. © 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Zinc titanate films with mesoporous structures have widespread applications ranging from sensors to supercapacitors and bio-devices owing to their photoelectric properties and specific surface area. The present work investigates the morphology of mesoporous zinc titanate films obtained by calcination of hybrid thin films containing polymer templates and precursor mixtures of zinc acetate dihydrate (ZAD) and titanium isopropoxide (TTIP). ZnO and TiO2 films are fabricated for reference. The influences of hydrochloric acid contents (HCl), the ratios of ZAD and TTIP, and the solution concentrations on the film morphologies are studied. The amphiphilic diblock copolymer, polystyrene-block-polyethylene oxide (PS-b-PEO), plays the role of a structure directing template, as it self-assembles into micelles in a solvent-acid mixture of N, N-dimethylformamide (DMF) and HCl. Thin films are prepared with spin-coating and subsequent calcination. Adjusting the ratio of TTIP and ZAD leads to the structure evolution from order to disorder in a film. It depends on the hydrolysis and condensation processes of the precursors, providing different time-to-growth processes to control the film morphologies. An increase in solution concentration enhances the surface coverage. As probed with grazing-incidence small-angle X-ray scattering, the inner structures are larger than the surface structures seen in scanning electron microscopy. © 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH. |
Tagliabue, Giulia; Atwater, Harry A; Polman, Albert; Cortés, Emiliano Photonic solutions help fight climate crisis Journal Article Nature Photonics, 18 (9), pp. 879 – 882, 2024, ISSN: 17494885, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Tagliabue2024879, title = {Photonic solutions help fight climate crisis}, author = {Giulia Tagliabue and Harry A Atwater and Albert Polman and Emiliano Cortés}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85203252837&doi=10.1038%2fs41566-024-01509-9&partnerID=40&md5=c8a9f3a9fe0eb2c20eda0700544774e4}, doi = {10.1038/s41566-024-01509-9}, issn = {17494885}, year = {2024}, date = {2024-01-01}, journal = {Nature Photonics}, volume = {18}, number = {9}, pages = {879 – 882}, publisher = {Nature Research}, abstract = {The mitigation of climate change requires major transformations in the ways we generate energy and operate technologies that release carbon dioxide. Photonic concepts and novel light-driven technologies provide many potential solutions, transforming our current modes of energy use into more effective and sustainable ones. © Springer Nature Limited 2024.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } The mitigation of climate change requires major transformations in the ways we generate energy and operate technologies that release carbon dioxide. Photonic concepts and novel light-driven technologies provide many potential solutions, transforming our current modes of energy use into more effective and sustainable ones. © Springer Nature Limited 2024. |
Zeitz, Sabine; Antoniuk, Hanna; Hlukhyy, Viktor; Fässler, T F Electronic Structure Analysis of the A10Tt2P6 System (A=Li−Cs; Tt=Si, Ge, Sn) and Synthesis of the Direct Band Gap Semiconductor K10Sn2P6 Journal Article Chemistry - A European Journal, 30 (22), 2024, ISSN: 09476539, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Zeitz2024, title = {Electronic Structure Analysis of the A10Tt2P6 System (A=Li−Cs; Tt=Si, Ge, Sn) and Synthesis of the Direct Band Gap Semiconductor K10Sn2P6}, author = {Sabine Zeitz and Hanna Antoniuk and Viktor Hlukhyy and T F Fässler}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85186631554&doi=10.1002%2fchem.202400002&partnerID=40&md5=ebb25cbb880a47a7cac2414675521fbf}, doi = {10.1002/chem.202400002}, issn = {09476539}, year = {2024}, date = {2024-01-01}, journal = {Chemistry - A European Journal}, volume = {30}, number = {22}, publisher = {John Wiley and Sons Inc}, abstract = {Investigating the relationship between atomic and electronic structures is a powerful tool to screen the wide variety of Zintl phases for interesting (opto−)electronic properties. To get an insight in such relations, the A10Tt2P6 system (A=Li−Cs; Tt=Si−Sn) was picked as model system to analyse the influence of structural motives, combination of elements and their properties on type and width of the band gaps. Those compounds comprise two interesting structural motives of their anions, which are either monomeric trigonal planar TtP35− units which are isostructural to CO32− or [Tt2P6]10− dimers which correspond to two edge-sharing TtP4 tetrahedra. The A10Tt2P6 compounds were structurally optimized for both polymorphs and subsequent frequency analysis, band structure as well as density of states calculations were performed. The Gibbs free energies were compared to determine temperature dependent stability, where Na10Si2P6, Na10Ge2P6 and K10Sn2P6 were found to be candidates for a high temperature phase transition between the two polymorphs. Additionally, the unknown, but predicted compound K10Sn2P6 was synthesized and characterized by single crystal and powder x-ray diffraction. It crystalizes in the monoclinic space group P 21/n and incorporates [Sn2P6]10− edge sharing double tetrahedra. It was determined to be a direct band gap semiconductor with a band gap of 2.57 eV. © 2024 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Investigating the relationship between atomic and electronic structures is a powerful tool to screen the wide variety of Zintl phases for interesting (opto−)electronic properties. To get an insight in such relations, the A10Tt2P6 system (A=Li−Cs; Tt=Si−Sn) was picked as model system to analyse the influence of structural motives, combination of elements and their properties on type and width of the band gaps. Those compounds comprise two interesting structural motives of their anions, which are either monomeric trigonal planar TtP35− units which are isostructural to CO32− or [Tt2P6]10− dimers which correspond to two edge-sharing TtP4 tetrahedra. The A10Tt2P6 compounds were structurally optimized for both polymorphs and subsequent frequency analysis, band structure as well as density of states calculations were performed. The Gibbs free energies were compared to determine temperature dependent stability, where Na10Si2P6, Na10Ge2P6 and K10Sn2P6 were found to be candidates for a high temperature phase transition between the two polymorphs. Additionally, the unknown, but predicted compound K10Sn2P6 was synthesized and characterized by single crystal and powder x-ray diffraction. It crystalizes in the monoclinic space group P 21/n and incorporates [Sn2P6]10− edge sharing double tetrahedra. It was determined to be a direct band gap semiconductor with a band gap of 2.57 eV. © 2024 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH. |
Martin, Stefan; Henke, Nina A; Lampe, Carola; Döblinger, Markus; Frank, Kilian; Ganswindt, Patrick; Nickel, Bert; Urban, Alexander S Fine-Tuning Blue-Emitting Halide Perovskite Nanocrystals Journal Article Advanced Optical Materials, 12 (8), 2024, ISSN: 21951071, (Cited by: 2; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: Bromine compounds; Lead compounds; Perovskite; Photoluminescence; Sols; 'current; Blue-emission; Blue-emitting; Fine tuning; Halide perovskites; Lead halide perovskite; Red shift; Red-emitting; Visible range; Wavelength ranges; Nanocrystals @article{Martin2024, title = {Fine-Tuning Blue-Emitting Halide Perovskite Nanocrystals}, author = {Stefan Martin and Nina A Henke and Carola Lampe and Markus Döblinger and Kilian Frank and Patrick Ganswindt and Bert Nickel and Alexander S Urban}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85166277902&doi=10.1002%2fadom.202301009&partnerID=40&md5=a48da52a47eb3a44b40bd173bd529c8f}, doi = {10.1002/adom.202301009}, issn = {21951071}, year = {2024}, date = {2024-01-01}, journal = {Advanced Optical Materials}, volume = {12}, number = {8}, publisher = {John Wiley and Sons Inc}, abstract = {Lead halide perovskite nanocrystals (NCs) with narrow, bright emission in the visible range are promising candidates for light-emitting applications. Near-unity quantum yields have been realized for green and red-emitting perovskites, but efficient, stable blue-emitting perovskite materials are scarce. Current methods to synthesize quantum-confined CsPbBr3 NCs with blue emission are limited to specific wavelength ranges and still suffer from inhomogeneously broadened emission profiles. Herein, anisotropic blue-green emitting CsPbBr3 NCs are synthesized in ambient atmosphere using a spontaneous crystallization method. Optical spectroscopy reveals a gradual, asymptotic photoluminescence (PL) redshift of pristine colloidal NCs after synthesis. During this process, the emission quality improves notably as the PL spectra become narrower and more symmetric, accompanied by a PL intensity increase. Electron microscopy indicates that the gradual redshift stems from an isotropic growth of the CsPbBr3 NCs in at least two dimensions, likely due to residual precursor ions in the dispersion. Most importantly, the growth process can be halted at any point by injecting an enhancement solution containing PbBr2 and organic capping ligands. Thus, excellent control over NC size is achieved, allowing for nanometer-precise tunability of the respective emission wavelength in the range between 475 and 500 nm, enhancing the functionality of these already impressive NCs. © 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH.}, note = {Cited by: 2; All Open Access, Hybrid Gold Open Access}, keywords = {Bromine compounds; Lead compounds; Perovskite; Photoluminescence; Sols; 'current; Blue-emission; Blue-emitting; Fine tuning; Halide perovskites; Lead halide perovskite; Red shift; Red-emitting; Visible range; Wavelength ranges; Nanocrystals}, pubstate = {published}, tppubtype = {article} } Lead halide perovskite nanocrystals (NCs) with narrow, bright emission in the visible range are promising candidates for light-emitting applications. Near-unity quantum yields have been realized for green and red-emitting perovskites, but efficient, stable blue-emitting perovskite materials are scarce. Current methods to synthesize quantum-confined CsPbBr3 NCs with blue emission are limited to specific wavelength ranges and still suffer from inhomogeneously broadened emission profiles. Herein, anisotropic blue-green emitting CsPbBr3 NCs are synthesized in ambient atmosphere using a spontaneous crystallization method. Optical spectroscopy reveals a gradual, asymptotic photoluminescence (PL) redshift of pristine colloidal NCs after synthesis. During this process, the emission quality improves notably as the PL spectra become narrower and more symmetric, accompanied by a PL intensity increase. Electron microscopy indicates that the gradual redshift stems from an isotropic growth of the CsPbBr3 NCs in at least two dimensions, likely due to residual precursor ions in the dispersion. Most importantly, the growth process can be halted at any point by injecting an enhancement solution containing PbBr2 and organic capping ligands. Thus, excellent control over NC size is achieved, allowing for nanometer-precise tunability of the respective emission wavelength in the range between 475 and 500 nm, enhancing the functionality of these already impressive NCs. © 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH. |
Wang, Xiao; Song, Zhulu; Tang, Haodong; Li, Yiwen; Zhong, Huaying; Wu, Jiufeng; Wang, Weichao; Chen, Simin; Zhang, Wenjie; Fang, Fan; Hao, Junjie; Wu, Dan; Müller-Buschbaum, Peter; Cao, Leifeng; Tang, Zeguo; Tang, Jun; Zhang, Lei; Wang, Kai; Chen, Wei Synergic Surface Modifications of PbS Quantum Dots by Sodium Acetate in Solid-State Ligand Exchange toward Short-Wave Infrared Photodetectors Journal Article ACS Applied Materials and Interfaces, 16 (33), pp. 44164 – 44173, 2024, ISSN: 19448244, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Wang202444164, title = {Synergic Surface Modifications of PbS Quantum Dots by Sodium Acetate in Solid-State Ligand Exchange toward Short-Wave Infrared Photodetectors}, author = {Xiao Wang and Zhulu Song and Haodong Tang and Yiwen Li and Huaying Zhong and Jiufeng Wu and Weichao Wang and Simin Chen and Wenjie Zhang and Fan Fang and Junjie Hao and Dan Wu and Peter Müller-Buschbaum and Leifeng Cao and Zeguo Tang and Jun Tang and Lei Zhang and Kai Wang and Wei Chen}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85200660501&doi=10.1021%2facsami.4c05201&partnerID=40&md5=baefce52a6b84c4109ba1157021e248e}, doi = {10.1021/acsami.4c05201}, issn = {19448244}, year = {2024}, date = {2024-01-01}, journal = {ACS Applied Materials and Interfaces}, volume = {16}, number = {33}, pages = {44164 – 44173}, publisher = {American Chemical Society}, abstract = {PbS quantum dots (QDs) are promising for short-wave infrared (SWIR) photodetection and imaging. Solid-state ligand exchange (SSLE) is a low-fabrication-threshold QD solid fabrication method. However, QD treatment by SSLE remains challenging in seeking refined surface passivation to achieve the desired device performance. This work investigates using NaAc in the ligand exchange process to enhance the film morphology and electronic coupling configuration of QD solids. By implementing various film and photodetector device characterization studies, we confirm that adding NaAc with a prominent adding ratio of 20 wt % NaAc with tetrabutylammonium iodide (TBAI) in the SSLE leads to an improved film morphology, reduced surface roughness, and decreased trap states in the QD solid films. Moreover, compared to the devices without NaAc treatment, those fabricated with NaAc-treated QD solids exhibit an enhanced performance, including lower dark current density (<100 nA/cm2), faster response speed, higher responsivity, detectivity, and external quantum efficiency (EQE reaching 25%). The discoveries can be insightful in developing efficient, low-cost, and low-fabrication-threshold QD SWIR detection and imager applications. © 2024 American Chemical Society.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } PbS quantum dots (QDs) are promising for short-wave infrared (SWIR) photodetection and imaging. Solid-state ligand exchange (SSLE) is a low-fabrication-threshold QD solid fabrication method. However, QD treatment by SSLE remains challenging in seeking refined surface passivation to achieve the desired device performance. This work investigates using NaAc in the ligand exchange process to enhance the film morphology and electronic coupling configuration of QD solids. By implementing various film and photodetector device characterization studies, we confirm that adding NaAc with a prominent adding ratio of 20 wt % NaAc with tetrabutylammonium iodide (TBAI) in the SSLE leads to an improved film morphology, reduced surface roughness, and decreased trap states in the QD solid films. Moreover, compared to the devices without NaAc treatment, those fabricated with NaAc-treated QD solids exhibit an enhanced performance, including lower dark current density (<100 nA/cm2), faster response speed, higher responsivity, detectivity, and external quantum efficiency (EQE reaching 25%). The discoveries can be insightful in developing efficient, low-cost, and low-fabrication-threshold QD SWIR detection and imager applications. © 2024 American Chemical Society. |
Ye, Junzhi; Ren, Aobo; Dai, Linjie; Baikie, Tomi K; Guo, Renjun; Pal, Debapriya; Gorgon, Sebastian; Heger, Julian E; Huang, Junyang; Sun, Yuqi; Arul, Rakesh; Grimaldi, Gianluca; Zhang, Kaiwen; Shamsi, Javad; Huang, Yi-Teng; Wang, Hao; Wu, Jiang; Koenderink, Femius A; Murciano, Laura Torrente; Schwartzkopf, Matthias; Roth, Stephen V; Müller-Buschbaum, Peter; Baumberg, Jeremy J; Stranks, Samuel D; Greenham, Neil C; Polavarapu, Lakshminarayana; Zhang, Wei; Rao, Akshay; Hoye, Robert L Z Direct linearly polarized electroluminescence from perovskite nanoplatelet superlattices Journal Article Nature Photonics, 18 (6), pp. 586 – 594, 2024, ISSN: 17494885, (Cited by: 7; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Ye2024586, title = {Direct linearly polarized electroluminescence from perovskite nanoplatelet superlattices}, author = {Junzhi Ye and Aobo Ren and Linjie Dai and Tomi K Baikie and Renjun Guo and Debapriya Pal and Sebastian Gorgon and Julian E Heger and Junyang Huang and Yuqi Sun and Rakesh Arul and Gianluca Grimaldi and Kaiwen Zhang and Javad Shamsi and Yi-Teng Huang and Hao Wang and Jiang Wu and Femius A Koenderink and Laura Torrente Murciano and Matthias Schwartzkopf and Stephen V Roth and Peter Müller-Buschbaum and Jeremy J Baumberg and Samuel D Stranks and Neil C Greenham and Lakshminarayana Polavarapu and Wei Zhang and Akshay Rao and Robert L Z Hoye}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85187263533&doi=10.1038%2fs41566-024-01398-y&partnerID=40&md5=bb785e2bc894354da69907057298694e}, doi = {10.1038/s41566-024-01398-y}, issn = {17494885}, year = {2024}, date = {2024-01-01}, journal = {Nature Photonics}, volume = {18}, number = {6}, pages = {586 – 594}, publisher = {Nature Research}, abstract = {Polarized light is critical for a wide range of applications, but is usually generated by filtering unpolarized light, which leads to substantial energy losses and requires additional optics. Here we demonstrate the direct emission of linearly polarized light from light-emitting diodes made of CsPbI3 perovskite nanoplatelet superlattices. The use of solvents with different vapour pressures enables the self-assembly of the nanoplatelets with fine control over their orientation (either face-up or edge-up) and therefore their transition dipole moment. As a result of the highly uniform alignment of the nanoplatelets, as well as their strong quantum and dielectric confinement, large exciton fine-structure splitting is achieved at the film level, leading to pure red light-emitting diodes with linearly polarized electroluminescence exhibiting a high degree of polarization of 74.4% without any photonic structures. This work demonstrates the potential of perovskite nanoplatelets as a promising source of linearly polarized light, opening up the development of next-generation three-dimensional displays and optical communications from a highly versatile, solution-processable system. © The Author(s) 2024.}, note = {Cited by: 7; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Polarized light is critical for a wide range of applications, but is usually generated by filtering unpolarized light, which leads to substantial energy losses and requires additional optics. Here we demonstrate the direct emission of linearly polarized light from light-emitting diodes made of CsPbI3 perovskite nanoplatelet superlattices. The use of solvents with different vapour pressures enables the self-assembly of the nanoplatelets with fine control over their orientation (either face-up or edge-up) and therefore their transition dipole moment. As a result of the highly uniform alignment of the nanoplatelets, as well as their strong quantum and dielectric confinement, large exciton fine-structure splitting is achieved at the film level, leading to pure red light-emitting diodes with linearly polarized electroluminescence exhibiting a high degree of polarization of 74.4% without any photonic structures. This work demonstrates the potential of perovskite nanoplatelets as a promising source of linearly polarized light, opening up the development of next-generation three-dimensional displays and optical communications from a highly versatile, solution-processable system. © The Author(s) 2024. |
Wei, Weifei; Zhang, Cai'e; Chen, Zhanxiang; Chen, Wei; Ran, Guangliu; Pan, Guangjiu; Zhang, Wenkai; Müller-Buschbaum, Peter; Bo, Zhishan; Yang, Chuluo; Luo, Zhenghui Precise Methylation Yields Acceptor with Hydrogen-Bonding Network for High-Efficiency and Thermally Stable Polymer Solar Cells Journal Article Angewandte Chemie - International Edition, 63 (6), 2024, ISSN: 14337851, (Cited by: 19). Abstract | Links | BibTeX | Tags: @article{Wei2024, title = {Precise Methylation Yields Acceptor with Hydrogen-Bonding Network for High-Efficiency and Thermally Stable Polymer Solar Cells}, author = {Weifei Wei and Cai'e Zhang and Zhanxiang Chen and Wei Chen and Guangliu Ran and Guangjiu Pan and Wenkai Zhang and Peter Müller-Buschbaum and Zhishan Bo and Chuluo Yang and Zhenghui Luo}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85181213994&doi=10.1002%2fanie.202315625&partnerID=40&md5=61eda71a3c5910fe8f8ded4ae326377c}, doi = {10.1002/anie.202315625}, issn = {14337851}, year = {2024}, date = {2024-01-01}, journal = {Angewandte Chemie - International Edition}, volume = {63}, number = {6}, publisher = {John Wiley and Sons Inc}, abstract = {Utilizing intermolecular hydrogen-bonding interactions stands for an effective approach in advancing the efficiency and stability of small-molecule acceptors (SMAs) for polymer solar cells. Herein, we synthesized three SMAs (Qo1, Qo2, and Qo3) using indeno[1,2-b]quinoxalin-11-one (Qox) as the electron-deficient group, with the incorporation of a methylation strategy. Through crystallographic analysis, it is observed that two Qox-based methylated acceptors (Qo2 and Qo3) exhibit multiple hydrogen bond-assisted 3D network transport structures, in contrast to the 2D transport structure observed in gem-dichlorinated counterpart (Qo4). Notably, Qo2 exhibits multiple and stronger hydrogen-bonding interactions compared with Qo3. Consequently, PM6 : Qo2 device realizes the highest power conversion efficiency (PCE) of 18.4 %, surpassing the efficiencies of devices based on Qo1 (15.8 %), Qo3 (16.7 %), and Qo4 (2.4 %). This remarkable PCE in PM6 : Qo2 device can be primarily ascribed to the enhanced donor-acceptor miscibility, more favorable medium structure, and more efficient charge transfer and collection behavior. Moreover, the PM6 : Qo2 device demonstrates exceptional thermal stability, retaining 82.8 % of its initial PCE after undergoing annealing at 65 °C for 250 hours. Our research showcases that precise methylation, particularly targeting the formation of intermolecular hydrogen-bonding interactions to tune crystal packing patterns, represents a promising strategy in the molecular design of efficient and stable SMAs. © 2023 Wiley-VCH GmbH.}, note = {Cited by: 19}, keywords = {}, pubstate = {published}, tppubtype = {article} } Utilizing intermolecular hydrogen-bonding interactions stands for an effective approach in advancing the efficiency and stability of small-molecule acceptors (SMAs) for polymer solar cells. Herein, we synthesized three SMAs (Qo1, Qo2, and Qo3) using indeno[1,2-b]quinoxalin-11-one (Qox) as the electron-deficient group, with the incorporation of a methylation strategy. Through crystallographic analysis, it is observed that two Qox-based methylated acceptors (Qo2 and Qo3) exhibit multiple hydrogen bond-assisted 3D network transport structures, in contrast to the 2D transport structure observed in gem-dichlorinated counterpart (Qo4). Notably, Qo2 exhibits multiple and stronger hydrogen-bonding interactions compared with Qo3. Consequently, PM6 : Qo2 device realizes the highest power conversion efficiency (PCE) of 18.4 %, surpassing the efficiencies of devices based on Qo1 (15.8 %), Qo3 (16.7 %), and Qo4 (2.4 %). This remarkable PCE in PM6 : Qo2 device can be primarily ascribed to the enhanced donor-acceptor miscibility, more favorable medium structure, and more efficient charge transfer and collection behavior. Moreover, the PM6 : Qo2 device demonstrates exceptional thermal stability, retaining 82.8 % of its initial PCE after undergoing annealing at 65 °C for 250 hours. Our research showcases that precise methylation, particularly targeting the formation of intermolecular hydrogen-bonding interactions to tune crystal packing patterns, represents a promising strategy in the molecular design of efficient and stable SMAs. © 2023 Wiley-VCH GmbH. |
Bornschlegl, Andreas J; Lichtenegger, Michael F; Luber, Leo; Lampe, Carola; Bodnarchuk, Maryna I; Kovalenko, Maksym V; Urban, Alexander S Dark-Bright Exciton Splitting Dominates Low-Temperature Diffusion in Halide Perovskite Nanocrystal Assemblies Journal Article Advanced Energy Materials, 14 (10), 2024, ISSN: 16146832, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Bornschlegl2024, title = {Dark-Bright Exciton Splitting Dominates Low-Temperature Diffusion in Halide Perovskite Nanocrystal Assemblies}, author = {Andreas J Bornschlegl and Michael F Lichtenegger and Leo Luber and Carola Lampe and Maryna I Bodnarchuk and Maksym V Kovalenko and Alexander S Urban}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85184213678&doi=10.1002%2faenm.202303312&partnerID=40&md5=c6bc3f429d04fb527a68b3f4f6ca965a}, doi = {10.1002/aenm.202303312}, issn = {16146832}, year = {2024}, date = {2024-01-01}, journal = {Advanced Energy Materials}, volume = {14}, number = {10}, publisher = {John Wiley and Sons Inc}, abstract = {Semiconductor nanocrystals can replace conventional bulk materials completely in displays and light-emitting diodes. Exciton transport dominates over charge carrier transport for materials with high exciton binding energies and long ligands, such as halide perovskite nanocrystal films. Here, how beneficial superlattices – nearly perfect 3D assemblies of nanocrystals - are to exciton transport is investigated. Surprisingly, the high degree of order is not as crucial as the individual nanocrystal size, which strongly influences the splitting of the excitonic manifold into bright and dark states. At very low temperatures, the energetic splitting is larger for the smallest nanocrystals, and dark levels with low oscillator strength effectively trap excitons inside individual nanocrystals, suppressing diffusion. The effect is reversed at elevated temperatures, and the larger nanocrystal size becomes detrimental to exciton transport due to enhanced exciton trapping and dissociation. The results reveal that the nanocrystal size must be strongly accounted for in design strategies of future optoelectronic applications. © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Semiconductor nanocrystals can replace conventional bulk materials completely in displays and light-emitting diodes. Exciton transport dominates over charge carrier transport for materials with high exciton binding energies and long ligands, such as halide perovskite nanocrystal films. Here, how beneficial superlattices – nearly perfect 3D assemblies of nanocrystals - are to exciton transport is investigated. Surprisingly, the high degree of order is not as crucial as the individual nanocrystal size, which strongly influences the splitting of the excitonic manifold into bright and dark states. At very low temperatures, the energetic splitting is larger for the smallest nanocrystals, and dark levels with low oscillator strength effectively trap excitons inside individual nanocrystals, suppressing diffusion. The effect is reversed at elevated temperatures, and the larger nanocrystal size becomes detrimental to exciton transport due to enhanced exciton trapping and dissociation. The results reveal that the nanocrystal size must be strongly accounted for in design strategies of future optoelectronic applications. © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. |
Wu, Lin; Holzapfel, Marco; Schmiedel, Alexander; Peng, Fuwei; Moos, Michael; Mentzel, Paul; Shi, Junqing; Neubert, Thomas; Bertermann, Rüdiger; Finze, Maik; Fox, Mark A; Lambert, Christoph; Ji, Lei Optically induced charge-transfer in donor-acceptor-substituted p- and m- C2B10H12 carboranes Journal Article Nature Communications, 15 (1), 2024, ISSN: 20411723, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: absorption; cluster analysis; experimental study; fluorescence; quantum mechanics; absorption; article; chromatophore; conjugation; controlled study; fluorescence; mechanical torsion @article{Wu2024, title = {Optically induced charge-transfer in donor-acceptor-substituted p- and m- C2B10H12 carboranes}, author = {Lin Wu and Marco Holzapfel and Alexander Schmiedel and Fuwei Peng and Michael Moos and Paul Mentzel and Junqing Shi and Thomas Neubert and Rüdiger Bertermann and Maik Finze and Mark A Fox and Christoph Lambert and Lei Ji}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189755489&doi=10.1038%2fs41467-024-47384-4&partnerID=40&md5=ac794280c62a604ec17bc06515d9f169}, doi = {10.1038/s41467-024-47384-4}, issn = {20411723}, year = {2024}, date = {2024-01-01}, journal = {Nature Communications}, volume = {15}, number = {1}, publisher = {Nature Research}, abstract = {Icosahedral carboranes, C2B10H12, have long been considered to be aromatic but the extent of conjugation between these clusters and their substituents is still being debated. m- and p-Carboranes are compared with m- and p-phenylenes as conjugated bridges in optical functional chromophores with a donor and an acceptor as substituents here. The absorption and fluorescence data for both carboranes from experimental techniques (including femtosecond transient absorption, time-resolved fluorescence and broadband fluorescence upconversion) show that the absorption and emission processes involve strong intramolecular charge transfer between the donor and acceptor substituents via the carborane cluster. From quantum chemical calculations on these carborane systems, the charge transfer process depends on the relative torsional angles of the donor and acceptor groups where an overlap between the two frontier orbitals exists in the bridging carborane cluster. © The Author(s) 2024.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {absorption; cluster analysis; experimental study; fluorescence; quantum mechanics; absorption; article; chromatophore; conjugation; controlled study; fluorescence; mechanical torsion}, pubstate = {published}, tppubtype = {article} } Icosahedral carboranes, C2B10H12, have long been considered to be aromatic but the extent of conjugation between these clusters and their substituents is still being debated. m- and p-Carboranes are compared with m- and p-phenylenes as conjugated bridges in optical functional chromophores with a donor and an acceptor as substituents here. The absorption and fluorescence data for both carboranes from experimental techniques (including femtosecond transient absorption, time-resolved fluorescence and broadband fluorescence upconversion) show that the absorption and emission processes involve strong intramolecular charge transfer between the donor and acceptor substituents via the carborane cluster. From quantum chemical calculations on these carborane systems, the charge transfer process depends on the relative torsional angles of the donor and acceptor groups where an overlap between the two frontier orbitals exists in the bridging carborane cluster. © The Author(s) 2024. |
Journal of the American Chemical Society, 2024, ISSN: 00027863, (Cited by: 0). Abstract | Links | BibTeX | Tags: erratum; human @article{2024_60, title = {Erratum: Controlling Interchromophore Coupling in Diamantane-Linked Pentacene Dimers To Create a ‘Binary’ Pair (J. Am. Chem. Soc. 2024, 146 (15) (10875−10888) DOI: 10.1021/jacs.4c01507)}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85203828352&doi=10.1021%2fjacs.4c11416&partnerID=40&md5=8d028a94d920fe55cbf41bd3b4e28c45}, doi = {10.1021/jacs.4c11416}, issn = {00027863}, year = {2024}, date = {2024-01-01}, journal = {Journal of the American Chemical Society}, publisher = {American Chemical Society}, abstract = {Page 10885. A portion of the funding information was omitted from the Acknowledgments section. The complete, corrected Acknowledgments statement is provided below.ACKNOWLEDGMENTS The authors are grateful for financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC), Canada Foundation for Innovation (CFI), the German Research Foundation (DFG) GU 517/27-1, and “Solar Energy goes Hybrid” Initiative of the Bavarian Ministry for Science, Culture, and Education (SolTech). Z.W.S. acknowledges scholarship support from NSERC and Alberta Innovates. We thank Professor Peter R. Schreiner for graciously providing diamantane as the starting material for this project. © 2024 American Chemical Society.}, note = {Cited by: 0}, keywords = {erratum; human}, pubstate = {published}, tppubtype = {article} } Page 10885. A portion of the funding information was omitted from the Acknowledgments section. The complete, corrected Acknowledgments statement is provided below.ACKNOWLEDGMENTS The authors are grateful for financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC), Canada Foundation for Innovation (CFI), the German Research Foundation (DFG) GU 517/27-1, and “Solar Energy goes Hybrid” Initiative of the Bavarian Ministry for Science, Culture, and Education (SolTech). Z.W.S. acknowledges scholarship support from NSERC and Alberta Innovates. We thank Professor Peter R. Schreiner for graciously providing diamantane as the starting material for this project. © 2024 American Chemical Society. |
Zhang, Wenhao; Deng, Meihui; Xiong, Qingqing Evaluation of energy performance in positive energy building: X HOUSE at Solar Decathlon Middle East 2021 Journal Article Renewable and Sustainable Energy Reviews, 192 , 2024, ISSN: 13640321, (Cited by: 2). Abstract | Links | BibTeX | Tags: @article{Zhang2024b, title = {Evaluation of energy performance in positive energy building: X HOUSE at Solar Decathlon Middle East 2021}, author = {Wenhao Zhang and Meihui Deng and Qingqing Xiong}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85180980490&doi=10.1016%2fj.rser.2023.114163&partnerID=40&md5=240248692cb2dc543fa704b9018cdc70}, doi = {10.1016/j.rser.2023.114163}, issn = {13640321}, year = {2024}, date = {2024-01-01}, journal = {Renewable and Sustainable Energy Reviews}, volume = {192}, publisher = {Elsevier Ltd}, abstract = {Internationally known as the “Olympics of Sustainable Building”, Solar Decathlon Middle East 2021 is the first competition linked to a world EXPO. The competition requests teams to design, build and operate a zero-energy house to drive the buildings and cities in the Middle East to transform into sustainable and intelligent ones. X HOUSE took first place in the Solar Decathlon Middle East 2021 and won eight contests. This article analyzes how the simulation optimization guides the design of X HOUSE to achieve higher energy efficiency and comfort conditions in terms of passive and active design strategies and solar energy utilization. It verifies the effectiveness of the simulation by a detailed analysis based on the monitored data at the competition site in Dubai. It also studies how house management strategies can improve the actual energy performance of X HOUSE. The analysis results show that the X HOUSE is a Positive Energy Building with highly efficient comfort and energy performance, it has strong power accommodation ability for peak shaving without relying on the grid, and it provides satisfactory thermal, ventilation, luminous, acoustics and healthy environment as well as a fully functional and flexible space. It provides a reference and methodology for the design of PEBs and sustainable development in the Middle East. © 2023 Elsevier Ltd}, note = {Cited by: 2}, keywords = {}, pubstate = {published}, tppubtype = {article} } Internationally known as the “Olympics of Sustainable Building”, Solar Decathlon Middle East 2021 is the first competition linked to a world EXPO. The competition requests teams to design, build and operate a zero-energy house to drive the buildings and cities in the Middle East to transform into sustainable and intelligent ones. X HOUSE took first place in the Solar Decathlon Middle East 2021 and won eight contests. This article analyzes how the simulation optimization guides the design of X HOUSE to achieve higher energy efficiency and comfort conditions in terms of passive and active design strategies and solar energy utilization. It verifies the effectiveness of the simulation by a detailed analysis based on the monitored data at the competition site in Dubai. It also studies how house management strategies can improve the actual energy performance of X HOUSE. The analysis results show that the X HOUSE is a Positive Energy Building with highly efficient comfort and energy performance, it has strong power accommodation ability for peak shaving without relying on the grid, and it provides satisfactory thermal, ventilation, luminous, acoustics and healthy environment as well as a fully functional and flexible space. It provides a reference and methodology for the design of PEBs and sustainable development in the Middle East. © 2023 Elsevier Ltd |
Petry, Jannik; Erabhoina, Harimohan; Dietel, Markus; Thelakkat, Mukundan Comparative Study of the Mechanical Reinforcement by Blending, Filling, and Block Copolymerization in Bottlebrush Polymer Electrolytes Journal Article ACS Applied Polymer Materials, 6 (9), pp. 5109 – 5120, 2024, ISSN: 26376105, (Cited by: 1). Abstract | Links | BibTeX | Tags: @article{Petry20245109, title = {Comparative Study of the Mechanical Reinforcement by Blending, Filling, and Block Copolymerization in Bottlebrush Polymer Electrolytes}, author = {Jannik Petry and Harimohan Erabhoina and Markus Dietel and Mukundan Thelakkat}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85192170375&doi=10.1021%2facsapm.4c00161&partnerID=40&md5=597ae552d34b94ce7326c6e10b4d4ec9}, doi = {10.1021/acsapm.4c00161}, issn = {26376105}, year = {2024}, date = {2024-01-01}, journal = {ACS Applied Polymer Materials}, volume = {6}, number = {9}, pages = {5109 – 5120}, publisher = {American Chemical Society}, abstract = {Poly(ethylene glycol) (PEG)-based bottlebrush polymer electrolytes exhibit improved room-temperature ionic conductivity and reduced crystallinity compared to those of semicrystalline poly(ethylene oxide) (PEO). However, these graft copolymers suffer from low mechanical stability. Therefore, we synthesized a PEG-based bottlebrush polymer having a polynorbornene backbone using ring-opening metathesis polymerization, and it was mechanically reinforced using three strategies: (a) by blending with a polynorbornene (PNb) homopolymer, (b) filling with TiO2 nanoparticles, or (c) via block copolymerization with a PNb segment. All three systems were converted to solid polymer electrolytes by adding LiTFSI, and their thermal, mechanical, and detailed electrochemical properties in symmetrical Li/SPE/Li cells over a large number of cycles are given. All solid-state lithium metal battery (Li/SPE/LFP) cells were fabricated, and charge/discharge cycles as well as the cycling behavior were comparatively studied. It was found that block copolymerization resulted in the highest storage modulus above 0.1 Hz and overall ionic conductivity (in the whole range of 25 to 80 °C) compared to those of the other two strategies. Furthermore, the highest accessible discharge capacities (159 mA h g-1) and highest capacity retention of 88% after 50 cycles were also achieved with the block copolymer concept. © 2024 The Authors. Published by American Chemical Society.}, note = {Cited by: 1}, keywords = {}, pubstate = {published}, tppubtype = {article} } Poly(ethylene glycol) (PEG)-based bottlebrush polymer electrolytes exhibit improved room-temperature ionic conductivity and reduced crystallinity compared to those of semicrystalline poly(ethylene oxide) (PEO). However, these graft copolymers suffer from low mechanical stability. Therefore, we synthesized a PEG-based bottlebrush polymer having a polynorbornene backbone using ring-opening metathesis polymerization, and it was mechanically reinforced using three strategies: (a) by blending with a polynorbornene (PNb) homopolymer, (b) filling with TiO2 nanoparticles, or (c) via block copolymerization with a PNb segment. All three systems were converted to solid polymer electrolytes by adding LiTFSI, and their thermal, mechanical, and detailed electrochemical properties in symmetrical Li/SPE/Li cells over a large number of cycles are given. All solid-state lithium metal battery (Li/SPE/LFP) cells were fabricated, and charge/discharge cycles as well as the cycling behavior were comparatively studied. It was found that block copolymerization resulted in the highest storage modulus above 0.1 Hz and overall ionic conductivity (in the whole range of 25 to 80 °C) compared to those of the other two strategies. Furthermore, the highest accessible discharge capacities (159 mA h g-1) and highest capacity retention of 88% after 50 cycles were also achieved with the block copolymer concept. © 2024 The Authors. Published by American Chemical Society. |
Miralles, Bernabé; Paredes, María Y; Bragas, Andrea V; Grinblat, Gustavo; Cortés, Emiliano; Scarpettini, Alberto F Arsenic Oxidation Kinetics with Plasmonic Nanocatalysts Journal Article Journal of Physical Chemistry C, 128 (24), pp. 10017 – 10024, 2024, ISSN: 19327447, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Miralles202410017, title = {Arsenic Oxidation Kinetics with Plasmonic Nanocatalysts}, author = {Bernabé Miralles and María Y Paredes and Andrea V Bragas and Gustavo Grinblat and Emiliano Cortés and Alberto F Scarpettini}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85195592462&doi=10.1021%2facs.jpcc.4c02905&partnerID=40&md5=e80a2c1d7391ab3fc7e07287bda49762}, doi = {10.1021/acs.jpcc.4c02905}, issn = {19327447}, year = {2024}, date = {2024-01-01}, journal = {Journal of Physical Chemistry C}, volume = {128}, number = {24}, pages = {10017 – 10024}, publisher = {American Chemical Society}, abstract = {Arsenic is one of the most toxic elements present in natural waters, and prolonged ingestion causes severe damage to health. Its oxidation from highly toxic As(III) to less harmful species involving As(V) is a process included in most remediation methods. The kinetics of this homogeneous redox reaction in the presence of hydrogen peroxide is very slow. We propose the use of metal nanoparticles as plasmonic catalysts for this reaction assisted by solar illumination. In this work, we show that As(III) oxidation to As(V) is accelerated by gold and silver nanoparticles through heterogeneous catalysis, and under plasmon excitation, hot charge carriers are generated that contribute to further increase in the reaction rate. We evaluate the efficiency of these nanocatalysts and their dependence on the excitation wavelength, and we quantify the different contributions to the oxidation process. Our results show that gold nanoparticles are better heterogeneous catalysts than silver nanoparticles; however, the latter increase their efficiency 8 times under resonant illumination, with irradiation powers close to that of sunlight, evidencing that the lower-cost material becomes a more efficient catalyst with light. © 2024 American Chemical Society}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Arsenic is one of the most toxic elements present in natural waters, and prolonged ingestion causes severe damage to health. Its oxidation from highly toxic As(III) to less harmful species involving As(V) is a process included in most remediation methods. The kinetics of this homogeneous redox reaction in the presence of hydrogen peroxide is very slow. We propose the use of metal nanoparticles as plasmonic catalysts for this reaction assisted by solar illumination. In this work, we show that As(III) oxidation to As(V) is accelerated by gold and silver nanoparticles through heterogeneous catalysis, and under plasmon excitation, hot charge carriers are generated that contribute to further increase in the reaction rate. We evaluate the efficiency of these nanocatalysts and their dependence on the excitation wavelength, and we quantify the different contributions to the oxidation process. Our results show that gold nanoparticles are better heterogeneous catalysts than silver nanoparticles; however, the latter increase their efficiency 8 times under resonant illumination, with irradiation powers close to that of sunlight, evidencing that the lower-cost material becomes a more efficient catalyst with light. © 2024 American Chemical Society |
Wagner, Laura I; Sirotti, Elise; Brune, Oliver; Grötzner, Gabriel; Eichhorn, Johanna; Santra, Saswati; Munnik, Frans; Olivi, Luca; Pollastri, Simone; Streibel, Verena; Sharp, Ian D Defect Engineering of Ta3N5 Photoanodes: Enhancing Charge Transport and Photoconversion Efficiencies via Ti Doping Journal Article Advanced Functional Materials, 34 (4), 2024, ISSN: 1616301X, (Cited by: 5; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Wagner2024b, title = {Defect Engineering of Ta3N5 Photoanodes: Enhancing Charge Transport and Photoconversion Efficiencies via Ti Doping}, author = {Laura I Wagner and Elise Sirotti and Oliver Brune and Gabriel Grötzner and Johanna Eichhorn and Saswati Santra and Frans Munnik and Luca Olivi and Simone Pollastri and Verena Streibel and Ian D Sharp}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85174298732&doi=10.1002%2fadfm.202306539&partnerID=40&md5=07d09e9fb76610871d002b052502e616}, doi = {10.1002/adfm.202306539}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, volume = {34}, number = {4}, publisher = {John Wiley and Sons Inc}, abstract = {While Ta3N5 shows excellent potential as a semiconductor photoanode for solar water splitting, its performance is hindered by poor charge carrier transport and trapping due to native defects that introduce electronic states deep within its bandgap. Here, it is demonstrated that controlled Ti doping of Ta3N5 can dramatically reduce the concentration of deep-level defects and enhance its photoelectrochemical performance, yielding a sevenfold increase in photocurrent density and a 300 mV cathodic shift in photocurrent onset potential compared to undoped material. Comprehensive characterization reveals that Ti4+ ions substitute Ta5+ lattice sites, thereby introducing compensating acceptor states, reducing the concentrations of deleterious nitrogen vacancies and reducing Ta3+ states, and thereby suppressing trapping and recombination. Owing to the similar ionic radii of Ti4+ and Ta5+, substitutional doping does not introduce lattice strain or significantly affect the underlying electronic structure of the host semiconductor. Furthermore, Ti can be incorporated without increasing the oxygen donor content, thereby enabling the electrical conductivity to be tuned by over seven orders of magnitude. Thus, Ti doping of Ta3N5 provides a powerful basis for precisely engineering its optoelectronic characteristics and to substantially improve its functional characteristics as an advanced photoelectrode for solar fuels applications. © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.}, note = {Cited by: 5; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } While Ta3N5 shows excellent potential as a semiconductor photoanode for solar water splitting, its performance is hindered by poor charge carrier transport and trapping due to native defects that introduce electronic states deep within its bandgap. Here, it is demonstrated that controlled Ti doping of Ta3N5 can dramatically reduce the concentration of deep-level defects and enhance its photoelectrochemical performance, yielding a sevenfold increase in photocurrent density and a 300 mV cathodic shift in photocurrent onset potential compared to undoped material. Comprehensive characterization reveals that Ti4+ ions substitute Ta5+ lattice sites, thereby introducing compensating acceptor states, reducing the concentrations of deleterious nitrogen vacancies and reducing Ta3+ states, and thereby suppressing trapping and recombination. Owing to the similar ionic radii of Ti4+ and Ta5+, substitutional doping does not introduce lattice strain or significantly affect the underlying electronic structure of the host semiconductor. Furthermore, Ti can be incorporated without increasing the oxygen donor content, thereby enabling the electrical conductivity to be tuned by over seven orders of magnitude. Thus, Ti doping of Ta3N5 provides a powerful basis for precisely engineering its optoelectronic characteristics and to substantially improve its functional characteristics as an advanced photoelectrode for solar fuels applications. © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. |
Hu, Haiyang; Lu, Wenzheng; Antonov, Alexander; Berté, Rodrigo; Maier, Stefan A; Tittl, Andreas Environmental permittivity-asymmetric BIC metasurfaces with electrical reconfigurability Journal Article Nature Communications, 15 (1), 2024, ISSN: 20411723, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Hu2024c, title = {Environmental permittivity-asymmetric BIC metasurfaces with electrical reconfigurability}, author = {Haiyang Hu and Wenzheng Lu and Alexander Antonov and Rodrigo Berté and Stefan A Maier and Andreas Tittl}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85201385846&doi=10.1038%2fs41467-024-51340-7&partnerID=40&md5=acb426c453b453ab7e68a1498440c5a4}, doi = {10.1038/s41467-024-51340-7}, issn = {20411723}, year = {2024}, date = {2024-01-01}, journal = {Nature Communications}, volume = {15}, number = {1}, publisher = {Nature Research}, abstract = {Achieving precise spectral and temporal light manipulation at the nanoscale remains a critical challenge in nanophotonics. While photonic bound states in the continuum (BICs) have emerged as a powerful means of controlling light, their reliance on geometrical symmetry breaking for obtaining tailored resonances makes them highly susceptible to fabrication imperfections, and their generally fixed asymmetry factor fundamentally limits applications in reconfigurable metasurfaces. Here, we introduce the concept of environmental symmetry breaking by embedding identical resonators into a surrounding medium with carefully placed regions of contrasting refractive indexes, activating permittivity-driven quasi-BIC resonances (ε-qBICs) without altering the underlying resonator geometry and unlocking an additional degree of freedom for light manipulation through active tuning of the surrounding dielectric environment. We demonstrate this concept by integrating polyaniline (PANI), an electro-optically active polymer, to achieve electrically reconfigurable ε-qBICs. This integration not only demonstrates rapid switching speeds and exceptional durability but also boosts the system’s optical response to environmental perturbations. Our strategy significantly expands the capabilities of resonant light manipulation through permittivity modulation, opening avenues for on-chip optical devices, advanced sensing, and beyond. © The Author(s) 2024.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Achieving precise spectral and temporal light manipulation at the nanoscale remains a critical challenge in nanophotonics. While photonic bound states in the continuum (BICs) have emerged as a powerful means of controlling light, their reliance on geometrical symmetry breaking for obtaining tailored resonances makes them highly susceptible to fabrication imperfections, and their generally fixed asymmetry factor fundamentally limits applications in reconfigurable metasurfaces. Here, we introduce the concept of environmental symmetry breaking by embedding identical resonators into a surrounding medium with carefully placed regions of contrasting refractive indexes, activating permittivity-driven quasi-BIC resonances (ε-qBICs) without altering the underlying resonator geometry and unlocking an additional degree of freedom for light manipulation through active tuning of the surrounding dielectric environment. We demonstrate this concept by integrating polyaniline (PANI), an electro-optically active polymer, to achieve electrically reconfigurable ε-qBICs. This integration not only demonstrates rapid switching speeds and exceptional durability but also boosts the system’s optical response to environmental perturbations. Our strategy significantly expands the capabilities of resonant light manipulation through permittivity modulation, opening avenues for on-chip optical devices, advanced sensing, and beyond. © The Author(s) 2024. |
Walther, Luis; Radacki, Krzysztof; Dewhurst, Rian D; Bertermann, Rüdiger; Finze, Maik; Braunschweig, Holger All-Inorganic sp-Chain Ligands: Isoelectronic B/N Analogues of E. O. Fischer's Alkynylcarbynes Journal Article Angewandte Chemie - International Edition, 63 (30), 2024, ISSN: 14337851, (Cited by: 0). Abstract | Links | BibTeX | Tags: azide; boron; halide; ligand; nanowire; tungsten; Alkynylcarbene; Borylation; Cationic complexes; Diazenido complex; Halide abstraction; Inorganics; Isoelectronics; Molecular wires; Sp chains; [3+2]-cycloaddition; article; borylation; case report; cycloaddition; Diels Alder reaction; Ligands @article{Walther2024, title = {All-Inorganic sp-Chain Ligands: Isoelectronic B/N Analogues of E. O. Fischer's Alkynylcarbynes}, author = {Luis Walther and Krzysztof Radacki and Rian D Dewhurst and Rüdiger Bertermann and Maik Finze and Holger Braunschweig}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85196487754&doi=10.1002%2fanie.202404930&partnerID=40&md5=a3b7b1e54e914af660cef048fba965c1}, doi = {10.1002/anie.202404930}, issn = {14337851}, year = {2024}, date = {2024-01-01}, journal = {Angewandte Chemie - International Edition}, volume = {63}, number = {30}, publisher = {John Wiley and Sons Inc}, abstract = {Borylation of a tungsten-bound N2 ligand and halide abstraction provides access to a cationic complex with an unprecedented linear NNBR ligand. This complex undergoes [3+2] cycloaddition with azides, and an unexpected chain-extension reaction with an iminoborane, leading to a complex with a five-atom B/N chain. These two [NNBR]-containing complexes, inorganic analogues of E. O. Fischer's alkynylcarbynes, are very rare examples of molecules containing all-inorganic chains of sp-hybridized atoms. © 2024 Wiley-VCH GmbH.}, note = {Cited by: 0}, keywords = {azide; boron; halide; ligand; nanowire; tungsten; Alkynylcarbene; Borylation; Cationic complexes; Diazenido complex; Halide abstraction; Inorganics; Isoelectronics; Molecular wires; Sp chains; [3+2]-cycloaddition; article; borylation; case report; cycloaddition; Diels Alder reaction; Ligands}, pubstate = {published}, tppubtype = {article} } Borylation of a tungsten-bound N2 ligand and halide abstraction provides access to a cationic complex with an unprecedented linear NNBR ligand. This complex undergoes [3+2] cycloaddition with azides, and an unexpected chain-extension reaction with an iminoborane, leading to a complex with a five-atom B/N chain. These two [NNBR]-containing complexes, inorganic analogues of E. O. Fischer's alkynylcarbynes, are very rare examples of molecules containing all-inorganic chains of sp-hybridized atoms. © 2024 Wiley-VCH GmbH. |
Kahl, Robert T; Erhardt, Andreas; Krauss, Gert; Seibold, Ferdinand; Dolynchuk, Oleksandr; Thelakkat, Mukundan; Thurn-Albrecht, Thomas Effect of Chemical Modification on Molecular Ordering in Polydiketopyrrolopyrrole Copolymers: From Liquid Crystalline to Crystalline Journal Article Macromolecules, 57 (11), pp. 5243 – 5252, 2024, ISSN: 00249297, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Kahl20245243, title = {Effect of Chemical Modification on Molecular Ordering in Polydiketopyrrolopyrrole Copolymers: From Liquid Crystalline to Crystalline}, author = {Robert T Kahl and Andreas Erhardt and Gert Krauss and Ferdinand Seibold and Oleksandr Dolynchuk and Mukundan Thelakkat and Thomas Thurn-Albrecht}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85194953005&doi=10.1021%2facs.macromol.4c00264&partnerID=40&md5=82aa8c2a94c2415ef37525be97f91421}, doi = {10.1021/acs.macromol.4c00264}, issn = {00249297}, year = {2024}, date = {2024-01-01}, journal = {Macromolecules}, volume = {57}, number = {11}, pages = {5243 – 5252}, publisher = {American Chemical Society}, abstract = {The chemical architecture of conjugated polymers is often designed by contemplating and understanding the consequences of structural changes on electronic properties at the molecular level. However, even minor changes to the chemical structure of a polymer can significantly influence the packing arrangement, which also influences the electronic properties of the bulk material. Here, we investigate the molecular arrangement in the ordered state at room temperature of a series of three different polydiketopyrrolopyrroles (PDPPs) in bulk and oriented thin films in detail by wide-angle X-ray scattering and by atomic force microscopy. The changes in the chemical structure of the investigated PDPPs, namely, an additional side chain or a different flanking unit, lead to an increase in long-range order and thereby to a change in the phase state from sanidic ordered via sanidic rectangular or oblique to crystalline. © 2024 The Authors. Published by American Chemical Society.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The chemical architecture of conjugated polymers is often designed by contemplating and understanding the consequences of structural changes on electronic properties at the molecular level. However, even minor changes to the chemical structure of a polymer can significantly influence the packing arrangement, which also influences the electronic properties of the bulk material. Here, we investigate the molecular arrangement in the ordered state at room temperature of a series of three different polydiketopyrrolopyrroles (PDPPs) in bulk and oriented thin films in detail by wide-angle X-ray scattering and by atomic force microscopy. The changes in the chemical structure of the investigated PDPPs, namely, an additional side chain or a different flanking unit, lead to an increase in long-range order and thereby to a change in the phase state from sanidic ordered via sanidic rectangular or oblique to crystalline. © 2024 The Authors. Published by American Chemical Society. |
Li, Chaohui; Zhang, Kaicheng; Maiti, Santanu; Peng, Zijian; Tian, Jingjing; Park, Hyoungwon; Byun, Jiwon; Xie, Zhiqiang; Dong, Lirong; Qiu, Shudi; Bornschlegl, Andreas J; Liu, Chao; Zhang, Jiyun; Osvet, Andres; Heumueller, Thomas; Christiansen, Silke H; Halik, Marcus; Unruh, Tobias; Li, Ning; Lüer, Larry; Brabec, Christoph J Tailoring the Dimensionality of 2D/3D Heterojunctions for Inverted Perovskite Solar Cells Journal Article ACS Energy Letters, 9 (3), pp. 779 – 788, 2024, ISSN: 23808195, (Cited by: 1). Abstract | Links | BibTeX | Tags: @article{Li2024779, title = {Tailoring the Dimensionality of 2D/3D Heterojunctions for Inverted Perovskite Solar Cells}, author = {Chaohui Li and Kaicheng Zhang and Santanu Maiti and Zijian Peng and Jingjing Tian and Hyoungwon Park and Jiwon Byun and Zhiqiang Xie and Lirong Dong and Shudi Qiu and Andreas J Bornschlegl and Chao Liu and Jiyun Zhang and Andres Osvet and Thomas Heumueller and Silke H Christiansen and Marcus Halik and Tobias Unruh and Ning Li and Larry Lüer and Christoph J Brabec}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85184934047&doi=10.1021%2facsenergylett.4c00045&partnerID=40&md5=c38ab972feb0d23e4f5b0a8b69cda29d}, doi = {10.1021/acsenergylett.4c00045}, issn = {23808195}, year = {2024}, date = {2024-01-01}, journal = {ACS Energy Letters}, volume = {9}, number = {3}, pages = {779 – 788}, publisher = {American Chemical Society}, abstract = {Interface engineering is crucial to achieving stable perovskite photovoltaic devices. A versatile approach is developed to tailor interface properties via integrating co-assembled monolayers (co-SAMs) at the p-type buried interface and by capping a two-dimensional (2D) perovskite layer at the n-type upper interface with vacuum quenching. Optimized co-SAMs promote the coverage of the hole transport layer, significantly reducing the incidence of leakage currents. Based on this foundation, we develop damp-heat-stable perovskite solar cells by precisely tailoring the fragments of 2D perovskite layers through vacuum annealing with phenethylammonium iodide. An impressive open-circuit voltage of 1.216 V is achieved, corresponding to 92% of the value determined by the detailed-balance limit, along with a power conversion efficiency of 23.68%. Ultimately, integrating co-SAMs and the vacuum-assisted annealing fabricated devices maintain 96% and 80% of initial efficiencies after 1200 and 500 h of tracking at a maximum power point under 55 and 85 °C, respectively. © 2024 American Chemical Society}, note = {Cited by: 1}, keywords = {}, pubstate = {published}, tppubtype = {article} } Interface engineering is crucial to achieving stable perovskite photovoltaic devices. A versatile approach is developed to tailor interface properties via integrating co-assembled monolayers (co-SAMs) at the p-type buried interface and by capping a two-dimensional (2D) perovskite layer at the n-type upper interface with vacuum quenching. Optimized co-SAMs promote the coverage of the hole transport layer, significantly reducing the incidence of leakage currents. Based on this foundation, we develop damp-heat-stable perovskite solar cells by precisely tailoring the fragments of 2D perovskite layers through vacuum annealing with phenethylammonium iodide. An impressive open-circuit voltage of 1.216 V is achieved, corresponding to 92% of the value determined by the detailed-balance limit, along with a power conversion efficiency of 23.68%. Ultimately, integrating co-SAMs and the vacuum-assisted annealing fabricated devices maintain 96% and 80% of initial efficiencies after 1200 and 500 h of tracking at a maximum power point under 55 and 85 °C, respectively. © 2024 American Chemical Society |
Alam, Shahidul; Aldosari, Haya; Petoukhoff, Christopher E; Váry, Tomáš; Althobaiti, Wejdan; Alqurashi, Maryam; Tang, Hua; Khan, Jafar I; Nádaždy, Vojtech; Müller-Buschbaum, Peter; Welch, Gregory C; Laquai, Frédéric Thermally-Induced Degradation in PM6:Y6-Based Bulk Heterojunction Organic Solar Cells Journal Article Advanced Functional Materials, 34 (6), 2024, ISSN: 1616301X, (Cited by: 5). Abstract | Links | BibTeX | Tags: @article{Alam2024b, title = {Thermally-Induced Degradation in PM6:Y6-Based Bulk Heterojunction Organic Solar Cells}, author = {Shahidul Alam and Haya Aldosari and Christopher E Petoukhoff and Tomáš Váry and Wejdan Althobaiti and Maryam Alqurashi and Hua Tang and Jafar I Khan and Vojtech Nádaždy and Peter Müller-Buschbaum and Gregory C Welch and Frédéric Laquai}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85174907866&doi=10.1002%2fadfm.202308076&partnerID=40&md5=48034adbebe4c83aacea2669a2ffd91b}, doi = {10.1002/adfm.202308076}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, volume = {34}, number = {6}, publisher = {John Wiley and Sons Inc}, abstract = {Thermally induced degradation of organic photovoltaic devices hinders the commercialization of this emerging PV technology. Thus, a precise understanding of the origin of thermal device instability, as well as identifying strategies to circumvent degradation is of utmost importance. Here, it investigates thermally-induced degradation of state-of-the-art PBDB-T-2F (PM6):BTP (Y6) bulk heterojunction solar cells at different temperatures and reveal changes of their optical properties, photophysics, and morphology. The open-circuit voltage and fill factor of thermally degraded devices are limited by dissociation and charge collection efficiency differences, while the short-circuit current density is only slightly affected. Energy-resolved electrochemical impedance spectroscopy measurements reveal that thermally degraded samples exhibit a higher energy barrier for the charge-transfer state to charge-separated state conversion. Furthermore, the field dependence of charge generation, recombination, and extraction are studied by time-delayed collection field and transient photocurrent and photovoltage experiments, indicating significant bimolecular recombination limits device performance. Finally, coupled optical-electrical device simulations are conducted to fit the devices’ current-voltage characteristics, enabling us to find useful correlations between optical and electrical properties of the active layers and device performance parameters. © 2023 Wiley-VCH GmbH.}, note = {Cited by: 5}, keywords = {}, pubstate = {published}, tppubtype = {article} } Thermally induced degradation of organic photovoltaic devices hinders the commercialization of this emerging PV technology. Thus, a precise understanding of the origin of thermal device instability, as well as identifying strategies to circumvent degradation is of utmost importance. Here, it investigates thermally-induced degradation of state-of-the-art PBDB-T-2F (PM6):BTP (Y6) bulk heterojunction solar cells at different temperatures and reveal changes of their optical properties, photophysics, and morphology. The open-circuit voltage and fill factor of thermally degraded devices are limited by dissociation and charge collection efficiency differences, while the short-circuit current density is only slightly affected. Energy-resolved electrochemical impedance spectroscopy measurements reveal that thermally degraded samples exhibit a higher energy barrier for the charge-transfer state to charge-separated state conversion. Furthermore, the field dependence of charge generation, recombination, and extraction are studied by time-delayed collection field and transient photocurrent and photovoltage experiments, indicating significant bimolecular recombination limits device performance. Finally, coupled optical-electrical device simulations are conducted to fit the devices’ current-voltage characteristics, enabling us to find useful correlations between optical and electrical properties of the active layers and device performance parameters. © 2023 Wiley-VCH GmbH. |
Christis, Maximilian; Henning, Alex; Bartl, Johannes D; Zeidler, Andreas; Rieger, Bernhard; Stutzmann, Martin; Sharp, Ian D Annealing-Free Ohmic Contacts to n-Type GaN via Hydrogen Plasma-Assisted Atomic Layer Deposition of Sub-Nanometer AlOx Journal Article Advanced Materials Interfaces, 11 (4), 2024, ISSN: 21967350, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Christis2024, title = {Annealing-Free Ohmic Contacts to n-Type GaN via Hydrogen Plasma-Assisted Atomic Layer Deposition of Sub-Nanometer AlOx}, author = {Maximilian Christis and Alex Henning and Johannes D Bartl and Andreas Zeidler and Bernhard Rieger and Martin Stutzmann and Ian D Sharp}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85178238869&doi=10.1002%2fadmi.202300758&partnerID=40&md5=71aea20b37752d132e7c3d0aa31e097f}, doi = {10.1002/admi.202300758}, issn = {21967350}, year = {2024}, date = {2024-01-01}, journal = {Advanced Materials Interfaces}, volume = {11}, number = {4}, publisher = {John Wiley and Sons Inc}, abstract = {A plasma-assisted atomic layer deposition (PE-ALD) process is reported for creating ohmic contacts to n-type GaN that combines native oxide reduction, near-surface doping, and encapsulation of GaN in a single processing step, thereby eliminating the need for both wet chemical etching of the native oxide before metallization and thermal annealing after contact formation. Repeated ALD cycling of trimethyl aluminum (TMA) and high-intensity hydrogen (H2) plasma results in the deposition of a sub-nanometer-thin (≈8 Å) AlOx layer via the partial transformation of the GaN surface oxide into AlOx. Hydrogen plasma-induced nitrogen vacancies in the near-surface region of GaN serve as shallow donors, promoting efficient out-of-plane electrical transport. Subsequent metallization with a Ti/Al/Ti/Au stack results in low contact resistance, ohmic behavior, and smooth morphology without requiring annealing. This electrical contracting approach thus meets the thermal budget requirements for Si-based complementary metal–oxide–semiconductor structures and can facilitate the design and fabrication of advanced GaN-on-Si heterodevices. © 2023 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } A plasma-assisted atomic layer deposition (PE-ALD) process is reported for creating ohmic contacts to n-type GaN that combines native oxide reduction, near-surface doping, and encapsulation of GaN in a single processing step, thereby eliminating the need for both wet chemical etching of the native oxide before metallization and thermal annealing after contact formation. Repeated ALD cycling of trimethyl aluminum (TMA) and high-intensity hydrogen (H2) plasma results in the deposition of a sub-nanometer-thin (≈8 Å) AlOx layer via the partial transformation of the GaN surface oxide into AlOx. Hydrogen plasma-induced nitrogen vacancies in the near-surface region of GaN serve as shallow donors, promoting efficient out-of-plane electrical transport. Subsequent metallization with a Ti/Al/Ti/Au stack results in low contact resistance, ohmic behavior, and smooth morphology without requiring annealing. This electrical contracting approach thus meets the thermal budget requirements for Si-based complementary metal–oxide–semiconductor structures and can facilitate the design and fabrication of advanced GaN-on-Si heterodevices. © 2023 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH. |
Streibel, Verena; Schönecker, Johanna L; Wagner, Laura I; Sirotti, Elise; Munnik, Frans; Kuhl, Matthias; Jiang, Chang-Ming; Eichhorn, Johanna; Santra, Saswati; Sharp, Ian D Zirconium Oxynitride Thin Films for Photoelectrochemical Water Splitting Journal Article ACS Applied Energy Materials, 7 (9), pp. 4004 – 4015, 2024, ISSN: 25740962, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Streibel20244004, title = {Zirconium Oxynitride Thin Films for Photoelectrochemical Water Splitting}, author = {Verena Streibel and Johanna L Schönecker and Laura I Wagner and Elise Sirotti and Frans Munnik and Matthias Kuhl and Chang-Ming Jiang and Johanna Eichhorn and Saswati Santra and Ian D Sharp}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85192135302&doi=10.1021%2facsaem.4c00303&partnerID=40&md5=d80c2a5898a81af879366dbf20e5afda}, doi = {10.1021/acsaem.4c00303}, issn = {25740962}, year = {2024}, date = {2024-01-01}, journal = {ACS Applied Energy Materials}, volume = {7}, number = {9}, pages = {4004 – 4015}, publisher = {American Chemical Society}, abstract = {Transition metal oxynitrides are a promising class of functional materials for photoelectrochemical (PEC) applications. Although these compounds are most commonly synthesized via ammonolysis of oxide precursors, such synthetic routes often lead to poorly controlled oxygen-to-nitrogen anion ratios, and the harsh nitridation conditions are incompatible with many substrates, including transparent conductive oxides. Here, we report direct reactive sputter deposition of a family of zirconium oxynitride thin films and the comprehensive characterization of their tunable structural, optical, and functional PEC properties. Systematic increases of the oxygen content in the reactive sputter gas mixture enable access to different crystalline structures within the zirconium oxynitride family. Increasing oxygen contents lead to a transition from metallic to semiconducting to insulating phases. In particular, crystalline Zr2ON2-like films have band gaps in the UV-visible range and are n-type semiconductors. These properties, together with a valence band maximum position located favorably relative to the water oxidation potential, make them viable photoanode candidates. Using chopped linear sweep voltammetry, we indeed confirm that our Zr2ON2 films are PEC-active for the oxygen evolution reaction in alkaline electrolytes. We further show that high-vacuum annealing boosts their PEC performance characteristics. Although the observed photocurrents are low compared to state-of-the-art photoanodes, these dense and planar thin films can offer a valuable platform for studying oxynitride photoelectrodes, as well as for future nanostructuring, band gap engineering, and defect engineering efforts. © 2024 The Authors. Published by American Chemical Society.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Transition metal oxynitrides are a promising class of functional materials for photoelectrochemical (PEC) applications. Although these compounds are most commonly synthesized via ammonolysis of oxide precursors, such synthetic routes often lead to poorly controlled oxygen-to-nitrogen anion ratios, and the harsh nitridation conditions are incompatible with many substrates, including transparent conductive oxides. Here, we report direct reactive sputter deposition of a family of zirconium oxynitride thin films and the comprehensive characterization of their tunable structural, optical, and functional PEC properties. Systematic increases of the oxygen content in the reactive sputter gas mixture enable access to different crystalline structures within the zirconium oxynitride family. Increasing oxygen contents lead to a transition from metallic to semiconducting to insulating phases. In particular, crystalline Zr2ON2-like films have band gaps in the UV-visible range and are n-type semiconductors. These properties, together with a valence band maximum position located favorably relative to the water oxidation potential, make them viable photoanode candidates. Using chopped linear sweep voltammetry, we indeed confirm that our Zr2ON2 films are PEC-active for the oxygen evolution reaction in alkaline electrolytes. We further show that high-vacuum annealing boosts their PEC performance characteristics. Although the observed photocurrents are low compared to state-of-the-art photoanodes, these dense and planar thin films can offer a valuable platform for studying oxynitride photoelectrodes, as well as for future nanostructuring, band gap engineering, and defect engineering efforts. © 2024 The Authors. Published by American Chemical Society. |
Boggiano, Hilario D; Nan, Lin; Grinblat, Gustavo; Maier, Stefan A; Cortés, Emiliano; Bragas, Andrea V Focusing Surface Acoustic Waves with a Plasmonic Hypersonic Lens Journal Article Nano Letters, 24 (21), pp. 6362 – 6368, 2024, ISSN: 15306984, (Cited by: 1; All Open Access, Green Open Access). Abstract | Links | BibTeX | Tags: @article{Boggiano20246362, title = {Focusing Surface Acoustic Waves with a Plasmonic Hypersonic Lens}, author = {Hilario D Boggiano and Lin Nan and Gustavo Grinblat and Stefan A Maier and Emiliano Cortés and Andrea V Bragas}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85193514427&doi=10.1021%2facs.nanolett.4c01251&partnerID=40&md5=3ea1994a8774267df4aee72565ffc413}, doi = {10.1021/acs.nanolett.4c01251}, issn = {15306984}, year = {2024}, date = {2024-01-01}, journal = {Nano Letters}, volume = {24}, number = {21}, pages = {6362 – 6368}, publisher = {American Chemical Society}, abstract = {Plasmonic nanoantennas have proven to be efficient transducers of electromagnetic to mechanical energy and vice versa. The sudden thermal expansion of these structures after an ultrafast optical pulsed excitation leads to the emission of hypersonic acoustic waves to the supporting substrate, which can be detected by another antenna that acts as a high-sensitivity mechanical probe due to the strong modulation of its optical response. Here, we propose and experimentally demonstrate a nanoscale acoustic lens comprised of 11 gold nanodisks whose collective oscillation at gigahertz frequencies gives rise to an interference pattern that results in a diffraction-limited surface acoustic beam of about 340 nm width, with an amplitude contrast of 60%. Via spatially decoupled pump-probe experiments, we were able to map the radiated acoustic energy in the proximity of the focal area, obtaining a very good agreement with the continuum elastic theory. © 2024 American Chemical Society.}, note = {Cited by: 1; All Open Access, Green Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Plasmonic nanoantennas have proven to be efficient transducers of electromagnetic to mechanical energy and vice versa. The sudden thermal expansion of these structures after an ultrafast optical pulsed excitation leads to the emission of hypersonic acoustic waves to the supporting substrate, which can be detected by another antenna that acts as a high-sensitivity mechanical probe due to the strong modulation of its optical response. Here, we propose and experimentally demonstrate a nanoscale acoustic lens comprised of 11 gold nanodisks whose collective oscillation at gigahertz frequencies gives rise to an interference pattern that results in a diffraction-limited surface acoustic beam of about 340 nm width, with an amplitude contrast of 60%. Via spatially decoupled pump-probe experiments, we were able to map the radiated acoustic energy in the proximity of the focal area, obtaining a very good agreement with the continuum elastic theory. © 2024 American Chemical Society. |
Guo, Renjun; Xiong, Qiu; Ulatowski, Aleksander; Li, Saisai; Ding, Zijin; Xiao, Tianxiao; Liang, Suzhe; Heger, Julian E; Guan, Tianfu; Jiang, Xinyu; Sun, Kun; Reb, Lennart K; Reus, Manuel A; Chumakov, Andrei; Schwartzkopf, Matthias; Yuan, Minjian; Hou, Yi; Roth, Stephan V; Herz, Laura M; Gao, Peng; Müller-Buschbaum, Peter Trace Water in Lead Iodide Affecting Perovskite Crystal Nucleation Limits the Performance of Perovskite Solar Cells Journal Article Advanced Materials, 36 (7), 2024, ISSN: 09359648, (Cited by: 15; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Guo2024, title = {Trace Water in Lead Iodide Affecting Perovskite Crystal Nucleation Limits the Performance of Perovskite Solar Cells}, author = {Renjun Guo and Qiu Xiong and Aleksander Ulatowski and Saisai Li and Zijin Ding and Tianxiao Xiao and Suzhe Liang and Julian E Heger and Tianfu Guan and Xinyu Jiang and Kun Sun and Lennart K Reb and Manuel A Reus and Andrei Chumakov and Matthias Schwartzkopf and Minjian Yuan and Yi Hou and Stephan V Roth and Laura M Herz and Peng Gao and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85178892866&doi=10.1002%2fadma.202310237&partnerID=40&md5=e15f49722f921e4ced782115980d3dab}, doi = {10.1002/adma.202310237}, issn = {09359648}, year = {2024}, date = {2024-01-01}, journal = {Advanced Materials}, volume = {36}, number = {7}, publisher = {John Wiley and Sons Inc}, abstract = {The experimental replicability of highly efficient perovskite solar cells (PSCs) is a persistent challenge faced by laboratories worldwide. Although trace impurities in raw materials can impact the experimental reproducibility of high-performance PSCs, the in situ study of how trace impurities affect perovskite film growth is never investigated. Here, light is shed on the impact of inevitable water contamination in lead iodide (PbI2) on the replicability of device performance, mainly depending on the synthesis methods of PbI2. Through synchrotron-based structure characterization, it is uncovered that even slight additions of water to PbI2 accelerate the crystallization process in the perovskite layer during annealing. However, this accelerated crystallization also results in an imbalance of charge-carrier mobilities, leading to a degradation in device performance and reduced longevity of the solar cells. It is also found that anhydrous PbI2 promotes a homogenous nucleation process and improves perovskite film growth. Finally, the PSCs achieve a remarkable certified power conversion efficiency of 24.3%. This breakthrough demonstrates the significance of understanding and precisely managing the water content in PbI2 to ensure the experimental replicability of high-efficiency PSCs. © 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.}, note = {Cited by: 15; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The experimental replicability of highly efficient perovskite solar cells (PSCs) is a persistent challenge faced by laboratories worldwide. Although trace impurities in raw materials can impact the experimental reproducibility of high-performance PSCs, the in situ study of how trace impurities affect perovskite film growth is never investigated. Here, light is shed on the impact of inevitable water contamination in lead iodide (PbI2) on the replicability of device performance, mainly depending on the synthesis methods of PbI2. Through synchrotron-based structure characterization, it is uncovered that even slight additions of water to PbI2 accelerate the crystallization process in the perovskite layer during annealing. However, this accelerated crystallization also results in an imbalance of charge-carrier mobilities, leading to a degradation in device performance and reduced longevity of the solar cells. It is also found that anhydrous PbI2 promotes a homogenous nucleation process and improves perovskite film growth. Finally, the PSCs achieve a remarkable certified power conversion efficiency of 24.3%. This breakthrough demonstrates the significance of understanding and precisely managing the water content in PbI2 to ensure the experimental replicability of high-efficiency PSCs. © 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH. |
Schneider, Tilman; Seebauer, Florian; Beuerle, Florian; Würthner, Frank A Monodisperse, End-Capped Ru(bda) Oligomer with Outstanding Performance in Heterogeneous Electrochemical Water Oxidation Journal Article Advanced Materials Technologies, 9 (11), 2024, ISSN: 2365709X, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Schneider2024, title = {A Monodisperse, End-Capped Ru(bda) Oligomer with Outstanding Performance in Heterogeneous Electrochemical Water Oxidation}, author = {Tilman Schneider and Florian Seebauer and Florian Beuerle and Frank Würthner}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85181252987&doi=10.1002%2fadmt.202301721&partnerID=40&md5=9c7edafdf201526afcd83f0d7a6d5410}, doi = {10.1002/admt.202301721}, issn = {2365709X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Materials Technologies}, volume = {9}, number = {11}, publisher = {John Wiley and Sons Inc}, abstract = {Water oxidation catalysis is a key step for sustainable fuel production by water splitting into hydrogen and oxygen. The synthesis of a novel coordination oligomer based on four Ru(bda) (bda = 2,2′-bipyridine-6,6′-dicarboxylate) centers, three 4,4′-bipyridine (4,4′-bpy) linkers, and two 4-picoline (4-pic) end caps is reported. The monodispersity of this tetranuclear compound is characterized by NMR techniques. Heterogeneous electrochemical water oxidation after immobilization on multi-walled carbon nanotubes (MWCNTs) shows catalytic performance unprecedented for this compound class, with a turnover frequency (TOF) of 133 s−1 and a turnover number (TON) of 4.89 × 106, at a current density of 43.8 mA cm−2 and a potential of 1.45 V versus normal hydrogen electrode (NHE). © 2024 The Authors. Advanced Materials Technologies published by Wiley-VCH GmbH.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Water oxidation catalysis is a key step for sustainable fuel production by water splitting into hydrogen and oxygen. The synthesis of a novel coordination oligomer based on four Ru(bda) (bda = 2,2′-bipyridine-6,6′-dicarboxylate) centers, three 4,4′-bipyridine (4,4′-bpy) linkers, and two 4-picoline (4-pic) end caps is reported. The monodispersity of this tetranuclear compound is characterized by NMR techniques. Heterogeneous electrochemical water oxidation after immobilization on multi-walled carbon nanotubes (MWCNTs) shows catalytic performance unprecedented for this compound class, with a turnover frequency (TOF) of 133 s−1 and a turnover number (TON) of 4.89 × 106, at a current density of 43.8 mA cm−2 and a potential of 1.45 V versus normal hydrogen electrode (NHE). © 2024 The Authors. Advanced Materials Technologies published by Wiley-VCH GmbH. |
Bartolomei, Beatrice; Sbacchi, Maria; Rosso, Cristian; Günay-Gürer, Ayse; Zdražil, Lukáš; Cadranel, Alejandro; Kralj, Slavko; Guldi, Dirk M; Prato, Maurizio Synthetic Strategies for the Selective Functionalization of Carbon Nanodots Allow Optically Communicating Suprastructures Journal Article Angewandte Chemie - International Edition, 63 (5), 2024, ISSN: 14337851, (Cited by: 3; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Bartolomei2024, title = {Synthetic Strategies for the Selective Functionalization of Carbon Nanodots Allow Optically Communicating Suprastructures}, author = {Beatrice Bartolomei and Maria Sbacchi and Cristian Rosso and Ayse Günay-Gürer and Lukáš Zdražil and Alejandro Cadranel and Slavko Kralj and Dirk M Guldi and Maurizio Prato}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85180731101&doi=10.1002%2fanie.202316915&partnerID=40&md5=9010c5533b14b0b5dd1e65363c1a5a4a}, doi = {10.1002/anie.202316915}, issn = {14337851}, year = {2024}, date = {2024-01-01}, journal = {Angewandte Chemie - International Edition}, volume = {63}, number = {5}, publisher = {John Wiley and Sons Inc}, abstract = {The surface of Carbon Nanodots (CNDs) stands as a rich chemical platform, able to regulate the interactions between particles and external species. Performing selective functionalization of these nanoscale entities is of practical importance, however, it still represents a considerable challenge. In this work, we exploited the organic chemistry toolbox to install target functionalities on the CND surface, while monitoring the chemical changes on the material's outer shell through nuclear magnetic resonance spectroscopy. Following this, we investigated the use of click chemistry to covalently connect CNDs of different nature en-route towards covalent suprastructures with unprecedent molecular control. The different photophysical properties of the connected particles allowed their optical communication in the excited state. This work paves the way for the development of selective and addressable CND building blocks which can act as modular nanoscale synthons that mirror the long-established reactivity of molecular organic synthesis. © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.}, note = {Cited by: 3; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The surface of Carbon Nanodots (CNDs) stands as a rich chemical platform, able to regulate the interactions between particles and external species. Performing selective functionalization of these nanoscale entities is of practical importance, however, it still represents a considerable challenge. In this work, we exploited the organic chemistry toolbox to install target functionalities on the CND surface, while monitoring the chemical changes on the material's outer shell through nuclear magnetic resonance spectroscopy. Following this, we investigated the use of click chemistry to covalently connect CNDs of different nature en-route towards covalent suprastructures with unprecedent molecular control. The different photophysical properties of the connected particles allowed their optical communication in the excited state. This work paves the way for the development of selective and addressable CND building blocks which can act as modular nanoscale synthons that mirror the long-established reactivity of molecular organic synthesis. © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. |
Qu, Wenqiang; Xu, Zixiang; Gruber, Christoph G; Li, Hongmei; Hu, Xiaonan; Zhou, Limin; Duan, Haiyan; Zhang, Jin; Liu, Min; Cortés, Emiliano; Zhang, Dengsong Environmental Science and Technology, 58 (36), pp. 16215 – 16224, 2024, ISSN: 0013936X, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Qu202416215, title = {Accelerating Toluene Oxidation over Boron-Titanium-Oxygen Interface: Steric Hindrance of the Methyl Group Induced by the Plane-Adsorption Configuration}, author = {Wenqiang Qu and Zixiang Xu and Christoph G Gruber and Hongmei Li and Xiaonan Hu and Limin Zhou and Haiyan Duan and Jin Zhang and Min Liu and Emiliano Cortés and Dengsong Zhang}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85202652526&doi=10.1021%2facs.est.4c06079&partnerID=40&md5=cec430551f771a82af143f79e06bf386}, doi = {10.1021/acs.est.4c06079}, issn = {0013936X}, year = {2024}, date = {2024-01-01}, journal = {Environmental Science and Technology}, volume = {58}, number = {36}, pages = {16215 – 16224}, publisher = {American Chemical Society}, abstract = {Elimination of dilute gaseous toluene is one of the critical concerns within the field of indoor air remediation. The typical degradation route on titanium-based catalysts, “toluene-benzaldehyde-carbon dioxide”, necessitates the oxidation of the methyl group as a prerequisite for photocatalytic toluene oxidation. However, the inherent planar adsorption configuration of toluene molecules, dominated by the benzene rings, leads to significant steric hindrance for the methyl group. This steric hindrance prevents the methyl group from contacting the active species on the catalyst surface, thereby limiting the removal of toluene under indoor conditions. To date, no effective strategy to control the steric hindrance of the methyl group has been identified. Herein, we showed a B-Ti-O interface that exhibits significantly enhanced toluene removal efficiency under indoor conditions. In-depth investigations revealed that, compared to typical Ti-based photocatalysts, the steric hindrance between the methyl group and the catalyst surface decreased from 3.42 to 3.03 Å on the designed interface. This reduction originates from the matching of orbital energy levels between Ti 3dz2 and C 2pz of the benzene ring. The decreased steric hindrance improved the efficiency of toluene being attacked by surface active species, allowing for rapid conversion into benzaldehyde and benzoic acid species for subsequent reactions. Our work provides novel insights into the steric hindrance effect in the elimination of aromatic volatile organic compounds. © 2024 American Chemical Society.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Elimination of dilute gaseous toluene is one of the critical concerns within the field of indoor air remediation. The typical degradation route on titanium-based catalysts, “toluene-benzaldehyde-carbon dioxide”, necessitates the oxidation of the methyl group as a prerequisite for photocatalytic toluene oxidation. However, the inherent planar adsorption configuration of toluene molecules, dominated by the benzene rings, leads to significant steric hindrance for the methyl group. This steric hindrance prevents the methyl group from contacting the active species on the catalyst surface, thereby limiting the removal of toluene under indoor conditions. To date, no effective strategy to control the steric hindrance of the methyl group has been identified. Herein, we showed a B-Ti-O interface that exhibits significantly enhanced toluene removal efficiency under indoor conditions. In-depth investigations revealed that, compared to typical Ti-based photocatalysts, the steric hindrance between the methyl group and the catalyst surface decreased from 3.42 to 3.03 Å on the designed interface. This reduction originates from the matching of orbital energy levels between Ti 3dz2 and C 2pz of the benzene ring. The decreased steric hindrance improved the efficiency of toluene being attacked by surface active species, allowing for rapid conversion into benzaldehyde and benzoic acid species for subsequent reactions. Our work provides novel insights into the steric hindrance effect in the elimination of aromatic volatile organic compounds. © 2024 American Chemical Society. |
Sortino, Luca; Gale, Angus; Kühner, Lucca; Li, Chi; Biechteler, Jonas; Wendisch, Fedja J; Kianinia, Mehran; Ren, Haoran; Toth, Milos; Maier, Stefan A; Aharonovich, Igor; Tittl, Andreas Optically addressable spin defects coupled to bound states in the continuum metasurfaces Journal Article Nature Communications, 15 (1), 2024, ISSN: 20411723, (Cited by: 3; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Sortino2024, title = {Optically addressable spin defects coupled to bound states in the continuum metasurfaces}, author = {Luca Sortino and Angus Gale and Lucca Kühner and Chi Li and Jonas Biechteler and Fedja J Wendisch and Mehran Kianinia and Haoran Ren and Milos Toth and Stefan A Maier and Igor Aharonovich and Andreas Tittl}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85186906047&doi=10.1038%2fs41467-024-46272-1&partnerID=40&md5=c9383a9c9df645054bd4c72a4bdc7041}, doi = {10.1038/s41467-024-46272-1}, issn = {20411723}, year = {2024}, date = {2024-01-01}, journal = {Nature Communications}, volume = {15}, number = {1}, publisher = {Nature Research}, abstract = {Van der Waals (vdW) materials, including hexagonal boron nitride (hBN), are layered crystalline solids with appealing properties for investigating light-matter interactions at the nanoscale. hBN has emerged as a versatile building block for nanophotonic structures, and the recent identification of native optically addressable spin defects has opened up exciting possibilities in quantum technologies. However, these defects exhibit relatively low quantum efficiencies and a broad emission spectrum, limiting potential applications. Optical metasurfaces present a novel approach to boost light emission efficiency, offering remarkable control over light-matter coupling at the sub-wavelength regime. Here, we propose and realise a monolithic scalable integration between intrinsic spin defects in hBN metasurfaces and high quality (Q) factor resonances, exceeding 102, leveraging quasi-bound states in the continuum (qBICs). Coupling between defect ensembles and qBIC resonances delivers a 25-fold increase in photoluminescence intensity, accompanied by spectral narrowing to below 4 nm linewidth and increased narrowband spin-readout efficiency. Our findings demonstrate a new class of metasurfaces for spin-defect-based technologies and pave the way towards vdW-based nanophotonic devices with enhanced efficiency and sensitivity for quantum applications in imaging, sensing, and light emission. © The Author(s) 2024.}, note = {Cited by: 3; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Van der Waals (vdW) materials, including hexagonal boron nitride (hBN), are layered crystalline solids with appealing properties for investigating light-matter interactions at the nanoscale. hBN has emerged as a versatile building block for nanophotonic structures, and the recent identification of native optically addressable spin defects has opened up exciting possibilities in quantum technologies. However, these defects exhibit relatively low quantum efficiencies and a broad emission spectrum, limiting potential applications. Optical metasurfaces present a novel approach to boost light emission efficiency, offering remarkable control over light-matter coupling at the sub-wavelength regime. Here, we propose and realise a monolithic scalable integration between intrinsic spin defects in hBN metasurfaces and high quality (Q) factor resonances, exceeding 102, leveraging quasi-bound states in the continuum (qBICs). Coupling between defect ensembles and qBIC resonances delivers a 25-fold increase in photoluminescence intensity, accompanied by spectral narrowing to below 4 nm linewidth and increased narrowband spin-readout efficiency. Our findings demonstrate a new class of metasurfaces for spin-defect-based technologies and pave the way towards vdW-based nanophotonic devices with enhanced efficiency and sensitivity for quantum applications in imaging, sensing, and light emission. © The Author(s) 2024. |
Bienek, Oliver; Rieth, Tim; Kühne, Julius; Fuchs, Benedikt; Kuhl, Matthias; Wagner, Laura I; Todenhagen, Lina M; Wolz, Lukas; Henning, Alex; Sharp, Ian D Suppressing substrate oxidation during plasma-enhanced atomic layer deposition on semiconductor surfaces Journal Article Applied Physics Letters, 124 (7), 2024, ISSN: 00036951, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Bienek2024, title = {Suppressing substrate oxidation during plasma-enhanced atomic layer deposition on semiconductor surfaces}, author = {Oliver Bienek and Tim Rieth and Julius Kühne and Benedikt Fuchs and Matthias Kuhl and Laura I Wagner and Lina M Todenhagen and Lukas Wolz and Alex Henning and Ian D Sharp}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85184995453&doi=10.1063%2f5.0182200&partnerID=40&md5=935ed758a1718e8963b335cb7d8ccae6}, doi = {10.1063/5.0182200}, issn = {00036951}, year = {2024}, date = {2024-01-01}, journal = {Applied Physics Letters}, volume = {124}, number = {7}, publisher = {American Institute of Physics Inc.}, abstract = {Plasma-enhanced atomic layer deposition (PE-ALD) is widely employed in microelectronics, energy, and sensing applications. Typically, PE-ALD processes for metal oxides utilize remote inductively coupled plasmas operated at powers of >200 W, ensuring a sufficient flux of oxygen radicals to the growth surface. However, this approach often leads to significant oxidation of chemically sensitive substrates, including most technological semiconductors. Here, we demonstrate that plasma powers as low as 5 W can effectively suppress substrate oxidation while maintaining the structural, optical, and electronic quality of the films. Specifically, we investigate the growth of titanium oxide (TiOx) using two commonly used metalorganic precursors, titanium isopropoxide and tetrakis(dimethylamino)titanium. Films deposited with 5 and 300 W oxygen plasma power are nearly indiscernible from one another, exhibiting significantly lower defect concentrations than those obtained from thermal ALD with H2O. The low plasma power process preserves desired physical characteristics of PE-ALD films, including large optical constants (n > 2.45 at 589 nm), negligible defect-induced sub-bandgap optical absorption (α < 102 cm−1), and high electrical resistivity (>105 Ω cm). Similar behavior, including suppressed interface oxidation and low defect content, is observed on both Si and InP substrates. As an example application of this approach, the assessment of InP/TiOx photocathodes and Si/TiOx photoanodes reveals a significant improvement in the photocurrent onset potential in both cases, enabled by suppressed substrate oxidation during low power PE-ALD. Overall, low power PE-ALD represents a generally applicable strategy for producing high quality metal oxide thin films while minimizing detrimental substrate reactions. © 2024 Author(s).}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Plasma-enhanced atomic layer deposition (PE-ALD) is widely employed in microelectronics, energy, and sensing applications. Typically, PE-ALD processes for metal oxides utilize remote inductively coupled plasmas operated at powers of >200 W, ensuring a sufficient flux of oxygen radicals to the growth surface. However, this approach often leads to significant oxidation of chemically sensitive substrates, including most technological semiconductors. Here, we demonstrate that plasma powers as low as 5 W can effectively suppress substrate oxidation while maintaining the structural, optical, and electronic quality of the films. Specifically, we investigate the growth of titanium oxide (TiOx) using two commonly used metalorganic precursors, titanium isopropoxide and tetrakis(dimethylamino)titanium. Films deposited with 5 and 300 W oxygen plasma power are nearly indiscernible from one another, exhibiting significantly lower defect concentrations than those obtained from thermal ALD with H2O. The low plasma power process preserves desired physical characteristics of PE-ALD films, including large optical constants (n > 2.45 at 589 nm), negligible defect-induced sub-bandgap optical absorption (α < 102 cm−1), and high electrical resistivity (>105 Ω cm). Similar behavior, including suppressed interface oxidation and low defect content, is observed on both Si and InP substrates. As an example application of this approach, the assessment of InP/TiOx photocathodes and Si/TiOx photoanodes reveals a significant improvement in the photocurrent onset potential in both cases, enabled by suppressed substrate oxidation during low power PE-ALD. Overall, low power PE-ALD represents a generally applicable strategy for producing high quality metal oxide thin films while minimizing detrimental substrate reactions. © 2024 Author(s). |
Kang, Yicui; João, Simão M; Lin, Rui; Liu, Kang; Zhu, Li; Fu, Junwei; Cheong, Weng-Chon; Lee, Seunghoon; Frank, Kilian; Nickel, Bert; Liu, Min; Lischner, Johannes; Cortés, Emiliano Effect of crystal facets in plasmonic catalysis Journal Article Nature Communications, 15 (1), 2024, ISSN: 20411723, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Kang2024, title = {Effect of crystal facets in plasmonic catalysis}, author = {Yicui Kang and Simão M João and Rui Lin and Kang Liu and Li Zhu and Junwei Fu and Weng-Chon Cheong and Seunghoon Lee and Kilian Frank and Bert Nickel and Min Liu and Johannes Lischner and Emiliano Cortés}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85192576803&doi=10.1038%2fs41467-024-47994-y&partnerID=40&md5=275dab6aa6f84f710ec1d1afe78e1679}, doi = {10.1038/s41467-024-47994-y}, issn = {20411723}, year = {2024}, date = {2024-01-01}, journal = {Nature Communications}, volume = {15}, number = {1}, publisher = {Nature Research}, abstract = {While the role of crystal facets is well known in traditional heterogeneous catalysis, this effect has not yet been thoroughly studied in plasmon-assisted catalysis, where attention has primarily focused on plasmon-derived mechanisms. Here, we investigate plasmon-assisted electrocatalytic CO2 reduction using different shapes of plasmonic Au nanoparticles - nanocube (NC), rhombic dodecahedron (RD), and octahedron (OC) - exposing 100, 110, and 111 facets, respectively. Upon plasmon excitation, Au OCs doubled CO Faradaic efficiency (FECO) and tripled CO partial current density (jCO) compared to a dark condition, with NCs also improving under illumination. In contrast, Au RDs maintained consistent performance irrespective of light exposure, suggesting minimal influence of light on the reaction. Temperature experiments ruled out heat as the main factor to explain such differences. Atomistic simulations and electromagnetic modeling revealed higher hot carrier abundance and electric field enhancement on Au OCs and NCs than RDs. These effects now dominate the reaction landscape over the crystal facets, thus shifting the reaction sites when comparing dark and plasmon-activated processes. Plasmon-assisted H2 evolution reaction experiments also support these findings. The dominance of low-coordinated sites over facets in plasmonic catalysis suggests key insights for designing efficient photocatalysts for energy conversion and carbon neutralization. © The Author(s) 2024.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } While the role of crystal facets is well known in traditional heterogeneous catalysis, this effect has not yet been thoroughly studied in plasmon-assisted catalysis, where attention has primarily focused on plasmon-derived mechanisms. Here, we investigate plasmon-assisted electrocatalytic CO2 reduction using different shapes of plasmonic Au nanoparticles - nanocube (NC), rhombic dodecahedron (RD), and octahedron (OC) - exposing 100, 110, and 111 facets, respectively. Upon plasmon excitation, Au OCs doubled CO Faradaic efficiency (FECO) and tripled CO partial current density (jCO) compared to a dark condition, with NCs also improving under illumination. In contrast, Au RDs maintained consistent performance irrespective of light exposure, suggesting minimal influence of light on the reaction. Temperature experiments ruled out heat as the main factor to explain such differences. Atomistic simulations and electromagnetic modeling revealed higher hot carrier abundance and electric field enhancement on Au OCs and NCs than RDs. These effects now dominate the reaction landscape over the crystal facets, thus shifting the reaction sites when comparing dark and plasmon-activated processes. Plasmon-assisted H2 evolution reaction experiments also support these findings. The dominance of low-coordinated sites over facets in plasmonic catalysis suggests key insights for designing efficient photocatalysts for energy conversion and carbon neutralization. © The Author(s) 2024. |
Guan, Tianfu; Liang, Suzhe; Kang, Yicui; Pensa, Evangelina; Li, Dong; Liang, Wenkai; Liang, Zhiqiang; Bulut, Yusuf; Reck, Kristian A; Xiao, Tianxiao; Guo, Renjun; Drewes, Jonas; Strunskus, Thomas; Schwartzkopf, Matthias; Faupel, Franz; Roth, Stephan V; Cortés, Emiliano; Jiang, Lin; Müller-Buschbaum, Peter High-Power Impulse Magnetron Sputter Deposition of Ag on Self-Assembled Au Nanoparticle Arrays at Low-Temperature Dewetting Conditions Journal Article ACS Applied Materials and Interfaces, 16 (30), pp. 40286 – 40296, 2024, ISSN: 19448244, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Guan202440286, title = {High-Power Impulse Magnetron Sputter Deposition of Ag on Self-Assembled Au Nanoparticle Arrays at Low-Temperature Dewetting Conditions}, author = {Tianfu Guan and Suzhe Liang and Yicui Kang and Evangelina Pensa and Dong Li and Wenkai Liang and Zhiqiang Liang and Yusuf Bulut and Kristian A Reck and Tianxiao Xiao and Renjun Guo and Jonas Drewes and Thomas Strunskus and Matthias Schwartzkopf and Franz Faupel and Stephan V Roth and Emiliano Cortés and Lin Jiang and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85199009897&doi=10.1021%2facsami.4c10726&partnerID=40&md5=a7ca86aa0f5e6d9bc9de02d23f1dee67}, doi = {10.1021/acsami.4c10726}, issn = {19448244}, year = {2024}, date = {2024-01-01}, journal = {ACS Applied Materials and Interfaces}, volume = {16}, number = {30}, pages = {40286 – 40296}, publisher = {American Chemical Society}, abstract = {Plasmons have facilitated diverse analytical applications due to the boosting signal detectability by hot spots. In practical applications, it is crucial to fabricate straightforward, large-scale, and reproducible plasmonic substrates. Dewetting treatment, via applying direct thermal annealing of metal films, has been used as a straightforward method in the fabrication of such plasmonic nanostructures. However, tailoring the evolution of the dewetting process of metal films poses considerable experimental complexities, mainly due to nanoscale structure formation. Here, we use grazing-incidence small- and wide-angle X-ray scattering for the in situ investigation of the high-power impulse magnetron sputter deposition of Ag on self-assembled Au nanoparticle arrays at low-temperature dewetting conditions. This approach allows us to examine both the direct formation of binary Au/Ag nanostructure and the consequential impact of the dewetting process on the spatial arrangement of the bimetallic nanoparticles. It is observed that the dewetting at 100 °C is sufficient to favor the establishment of a homogenized structural configuration of bimetallic nanostructures, which is beneficial for localized surface plasmon resonances (LSPRs). The fabricated metal nanostructures show potential application for the surface-enhanced Raman scattering (SERS) detection of rhodamine 6G molecules. As SERS platform, bimetallic nanostructures formed with dewetting conditions turn out to be superior to those without dewetting conditions. The method in this work is envisioned as a facile strategy for the fabrication of plasmonic nanostructures. © 2024 The Authors. Published by American Chemical Society.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Plasmons have facilitated diverse analytical applications due to the boosting signal detectability by hot spots. In practical applications, it is crucial to fabricate straightforward, large-scale, and reproducible plasmonic substrates. Dewetting treatment, via applying direct thermal annealing of metal films, has been used as a straightforward method in the fabrication of such plasmonic nanostructures. However, tailoring the evolution of the dewetting process of metal films poses considerable experimental complexities, mainly due to nanoscale structure formation. Here, we use grazing-incidence small- and wide-angle X-ray scattering for the in situ investigation of the high-power impulse magnetron sputter deposition of Ag on self-assembled Au nanoparticle arrays at low-temperature dewetting conditions. This approach allows us to examine both the direct formation of binary Au/Ag nanostructure and the consequential impact of the dewetting process on the spatial arrangement of the bimetallic nanoparticles. It is observed that the dewetting at 100 °C is sufficient to favor the establishment of a homogenized structural configuration of bimetallic nanostructures, which is beneficial for localized surface plasmon resonances (LSPRs). The fabricated metal nanostructures show potential application for the surface-enhanced Raman scattering (SERS) detection of rhodamine 6G molecules. As SERS platform, bimetallic nanostructures formed with dewetting conditions turn out to be superior to those without dewetting conditions. The method in this work is envisioned as a facile strategy for the fabrication of plasmonic nanostructures. © 2024 The Authors. Published by American Chemical Society. |
Wang, Qiyou; Gong, Yujie; Zi, Xin; Gan, Lei; Pensa, Evangelina; Liu, Yuxiang; Xiao, Yusen; Li, Hongmei; Liu, Kang; Fu, Junwei; Liu, Jun; Stefancu, Andrei; Cai, Chao; Chen, Shanyong; Zhang, Shiguo; Lu, Ying-Rui; Chan, Ting-Shan; Ma, Chao; Cao, Xueying; Cortés, Emiliano; Liu, Min Coupling Nano and Atomic Electric Field Confinement for Robust Alkaline Oxygen Evolution Journal Article Angewandte Chemie - International Edition, 63 (28), 2024, ISSN: 14337851, (Cited by: 8; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Wang2024b, title = {Coupling Nano and Atomic Electric Field Confinement for Robust Alkaline Oxygen Evolution}, author = {Qiyou Wang and Yujie Gong and Xin Zi and Lei Gan and Evangelina Pensa and Yuxiang Liu and Yusen Xiao and Hongmei Li and Kang Liu and Junwei Fu and Jun Liu and Andrei Stefancu and Chao Cai and Shanyong Chen and Shiguo Zhang and Ying-Rui Lu and Ting-Shan Chan and Chao Ma and Xueying Cao and Emiliano Cortés and Min Liu}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85195690153&doi=10.1002%2fanie.202405438&partnerID=40&md5=4185ba4411edd789080ce5e3183b09b5}, doi = {10.1002/anie.202405438}, issn = {14337851}, year = {2024}, date = {2024-01-01}, journal = {Angewandte Chemie - International Edition}, volume = {63}, number = {28}, publisher = {John Wiley and Sons Inc}, abstract = {The alkaline oxygen evolution reaction (OER) is a promising avenue for producing clean fuels and storing intermittent energy. However, challenges such as excessive OH− consumption and strong adsorption of oxygen-containing intermediates hinder the development of alkaline OER. In this study, we propose a cooperative strategy by leveraging both nano-scale and atomically local electric fields for alkaline OER, demonstrated through the synthesis of Mn single atom doped CoP nanoneedles (Mn SA-CoP NNs). Finite element method simulations and density functional theory calculations predict that the nano-scale local electric field enriches OH− around the catalyst surface, while the atomically local electric field improves *O desorption. Experimental validation using in situ attenuated total reflection infrared and Raman spectroscopy confirms the effectiveness of the nano-scale and atomically electric fields. Mn SA-CoP NNs exhibit an ultra-low overpotential of 189 mV at 10 mA cm−2 and stable operation over 100 hours at ~100 mA cm−2 during alkaline OER. This innovative strategy provides new insights for enhancing catalyst performance in energy conversion reactions. © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.}, note = {Cited by: 8; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The alkaline oxygen evolution reaction (OER) is a promising avenue for producing clean fuels and storing intermittent energy. However, challenges such as excessive OH− consumption and strong adsorption of oxygen-containing intermediates hinder the development of alkaline OER. In this study, we propose a cooperative strategy by leveraging both nano-scale and atomically local electric fields for alkaline OER, demonstrated through the synthesis of Mn single atom doped CoP nanoneedles (Mn SA-CoP NNs). Finite element method simulations and density functional theory calculations predict that the nano-scale local electric field enriches OH− around the catalyst surface, while the atomically local electric field improves *O desorption. Experimental validation using in situ attenuated total reflection infrared and Raman spectroscopy confirms the effectiveness of the nano-scale and atomically electric fields. Mn SA-CoP NNs exhibit an ultra-low overpotential of 189 mV at 10 mA cm−2 and stable operation over 100 hours at ~100 mA cm−2 during alkaline OER. This innovative strategy provides new insights for enhancing catalyst performance in energy conversion reactions. © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. |
de Kam, Lucas B T; Maier, Thomas L; Krischer, Katharina Electrolyte effects on the alkaline hydrogen evolution reaction: A mean-field approach Journal Article Electrochimica Acta, 497 , 2024, ISSN: 00134686, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{deKam2024, title = {Electrolyte effects on the alkaline hydrogen evolution reaction: A mean-field approach}, author = {Lucas B T de Kam and Thomas L Maier and Katharina Krischer}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85195863948&doi=10.1016%2fj.electacta.2024.144530&partnerID=40&md5=568a9ec1f88599475525bd6d1a5f6cee}, doi = {10.1016/j.electacta.2024.144530}, issn = {00134686}, year = {2024}, date = {2024-01-01}, journal = {Electrochimica Acta}, volume = {497}, publisher = {Elsevier Ltd}, abstract = {This paper introduces the combination of an advanced double-layer model with electrochemical kinetics to explain electrolyte effects on the alkaline hydrogen evolution reaction. It is known from experimental studies that the alkaline hydrogen evolution current shows a strong dependence on the concentration and identity of cations in the electrolyte, but is independent of pH. To explain these effects, we formulate the faradaic current in terms of the electric potential in the double layer, which is calculated using a mean-field model that takes into account the cation and anion sizes as well as the electric dipole moment of water molecules. We propose that the Volmer step consists of two activated processes: a water reduction sub-step, and a sub-step in which OH− is transferred away from the reaction plane through the double layer. Either of these sub-steps may limit the rate. The proposed models for these sub-steps qualitatively explain experimental observations, including cation effects, pH-independence, and the trend reversal between gold and platinum electrodes. We also assess the quantitative accuracy of the water-reduction-limited current model; we suggest that the predicted functional relationship is valid as long as the hydrogen bonding structure of water near the electrode is sufficiently maintained. © 2024 The Author(s)}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } This paper introduces the combination of an advanced double-layer model with electrochemical kinetics to explain electrolyte effects on the alkaline hydrogen evolution reaction. It is known from experimental studies that the alkaline hydrogen evolution current shows a strong dependence on the concentration and identity of cations in the electrolyte, but is independent of pH. To explain these effects, we formulate the faradaic current in terms of the electric potential in the double layer, which is calculated using a mean-field model that takes into account the cation and anion sizes as well as the electric dipole moment of water molecules. We propose that the Volmer step consists of two activated processes: a water reduction sub-step, and a sub-step in which OH− is transferred away from the reaction plane through the double layer. Either of these sub-steps may limit the rate. The proposed models for these sub-steps qualitatively explain experimental observations, including cation effects, pH-independence, and the trend reversal between gold and platinum electrodes. We also assess the quantitative accuracy of the water-reduction-limited current model; we suggest that the predicted functional relationship is valid as long as the hydrogen bonding structure of water near the electrode is sufficiently maintained. © 2024 The Author(s) |
Mentzel, Paul; Holzapfel, Marco; Schmiedel, Alexander; Günther, Johanna; Michel, Maximilian; Krummenacher, Ivo; Wodyński, Artur; Kaupp, Martin; Braunschweig, Holger; Lambert, Christoph Structure and Photophysics of N-Tolanyl-phenochalcogenazines and their Radical Cations Journal Article Chemistry - A European Journal, 30 (19), 2024, ISSN: 09476539, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Mentzel2024, title = {Structure and Photophysics of N-Tolanyl-phenochalcogenazines and their Radical Cations}, author = {Paul Mentzel and Marco Holzapfel and Alexander Schmiedel and Johanna Günther and Maximilian Michel and Ivo Krummenacher and Artur Wodyński and Martin Kaupp and Holger Braunschweig and Christoph Lambert}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85185108520&doi=10.1002%2fchem.202303782&partnerID=40&md5=b86f6d73ed4a41c13fbe919d29156c99}, doi = {10.1002/chem.202303782}, issn = {09476539}, year = {2024}, date = {2024-01-01}, journal = {Chemistry - A European Journal}, volume = {30}, number = {19}, publisher = {John Wiley and Sons Inc}, abstract = {The study focuses on the structural and photophysical characteristics of neutral and oxidized forms of N-tolanyl-phenochalcogenazines PZX-tolan with X=O, S, Se, and Te. X-ray crystal structure analyses show a pseudo-equatorial (pe) structure of the tolan substituent in the O, S, and Se dyads, while the Te dyad possesses a pseudo-axial (pa) structure. DFT calculations suggest the pe structure for O and S, and the pa structure for Se and Te as stable forms. Steady-state and femtosecond-time resolved optical spectroscopy in toluene solution indicate that the O and S dyads emit from a CT state, whereas the Se and Te dyads emit from a tolan-localized state. The T1 state is tolan-localized in all cases, showing phosphorescence at 77 K. The heavy atom effect of chalcogens induces intersystem crossing from S1 to Tx, resulting in a decreasing S1 lifetime from 2.1 ns to 0.42 ps. The T1 states possess potential for singlet oxygen sensitization with a high quantum yield (ca. 40 %) for the O, S, and Se dyads. Radical cations exhibit spin density primarily localized at the heterocycle. EPR measurements and quasirelativistic DFT calculations reveal a very strong g-tensor anisotropy, supporting the pe structure for the S and Se derivatives. © 2024 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The study focuses on the structural and photophysical characteristics of neutral and oxidized forms of N-tolanyl-phenochalcogenazines PZX-tolan with X=O, S, Se, and Te. X-ray crystal structure analyses show a pseudo-equatorial (pe) structure of the tolan substituent in the O, S, and Se dyads, while the Te dyad possesses a pseudo-axial (pa) structure. DFT calculations suggest the pe structure for O and S, and the pa structure for Se and Te as stable forms. Steady-state and femtosecond-time resolved optical spectroscopy in toluene solution indicate that the O and S dyads emit from a CT state, whereas the Se and Te dyads emit from a tolan-localized state. The T1 state is tolan-localized in all cases, showing phosphorescence at 77 K. The heavy atom effect of chalcogens induces intersystem crossing from S1 to Tx, resulting in a decreasing S1 lifetime from 2.1 ns to 0.42 ps. The T1 states possess potential for singlet oxygen sensitization with a high quantum yield (ca. 40 %) for the O, S, and Se dyads. Radical cations exhibit spin density primarily localized at the heterocycle. EPR measurements and quasirelativistic DFT calculations reveal a very strong g-tensor anisotropy, supporting the pe structure for the S and Se derivatives. © 2024 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH. |
Posnjak, Gregor; Yin, Xin; Butler, Paul; Bienek, Oliver; Dass, Mihir; Lee, Seungwoo; Sharp, Ian D; Liedl, Tim Diamond-lattice photonic crystals assembled from DNA origami Journal Article Science, 384 (6697), pp. 781 – 785, 2024, ISSN: 00368075, (Cited by: 6; All Open Access, Green Open Access). Abstract | Links | BibTeX | Tags: @article{Posnjak2024781, title = {Diamond-lattice photonic crystals assembled from DNA origami}, author = {Gregor Posnjak and Xin Yin and Paul Butler and Oliver Bienek and Mihir Dass and Seungwoo Lee and Ian D Sharp and Tim Liedl}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85193516157&doi=10.1126%2fscience.adl2733&partnerID=40&md5=6d4f8061bc1a63794487b181922a88ed}, doi = {10.1126/science.adl2733}, issn = {00368075}, year = {2024}, date = {2024-01-01}, journal = {Science}, volume = {384}, number = {6697}, pages = {781 – 785}, publisher = {American Association for the Advancement of Science}, abstract = {Colloidal self-assembly allows rational design of structures on the micrometer and submicrometer scale. One architecture that can generate complete three-dimensional photonic bandgaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable with the wavelength of visible or ultraviolet light. In this work, we demonstrate three-dimensional photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nanometers. This structure serves as a scaffold for atomic-layer deposition of high–refractive index materials such as titanium dioxide, yielding a tunable photonic bandgap in the near-ultraviolet. © 2024 American Association for the Advancement of Science. All rights reserved.}, note = {Cited by: 6; All Open Access, Green Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Colloidal self-assembly allows rational design of structures on the micrometer and submicrometer scale. One architecture that can generate complete three-dimensional photonic bandgaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable with the wavelength of visible or ultraviolet light. In this work, we demonstrate three-dimensional photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nanometers. This structure serves as a scaffold for atomic-layer deposition of high–refractive index materials such as titanium dioxide, yielding a tunable photonic bandgap in the near-ultraviolet. © 2024 American Association for the Advancement of Science. All rights reserved. |
Hegner, Franziska S; Cohen, Adi; Rudel, Stefan S; Kronawitter, Silva M; Grumet, Manuel; Zhu, Xiangzhou; Korobko, Roman; Houben, Lothar; Jiang, Chang-Ming; Schnick, Wolfgang; Kieslich, Gregor; Yaffe, Omer; Sharp, Ian D; Egger, David A The Critical Role of Anharmonic Lattice Dynamics for Macroscopic Properties of the Visible Light Absorbing Nitride Semiconductor CuTaN2 Journal Article Advanced Energy Materials, 14 (19), 2024, ISSN: 16146832, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Hegner2024, title = {The Critical Role of Anharmonic Lattice Dynamics for Macroscopic Properties of the Visible Light Absorbing Nitride Semiconductor CuTaN2}, author = {Franziska S Hegner and Adi Cohen and Stefan S Rudel and Silva M Kronawitter and Manuel Grumet and Xiangzhou Zhu and Roman Korobko and Lothar Houben and Chang-Ming Jiang and Wolfgang Schnick and Gregor Kieslich and Omer Yaffe and Ian D Sharp and David A Egger}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85188909385&doi=10.1002%2faenm.202303059&partnerID=40&md5=8d45614f8e878ca4ff40bda022a028f0}, doi = {10.1002/aenm.202303059}, issn = {16146832}, year = {2024}, date = {2024-01-01}, journal = {Advanced Energy Materials}, volume = {14}, number = {19}, publisher = {John Wiley and Sons Inc}, abstract = {Ternary nitride semiconductors are rapidly emerging as a promising class of materials for energy conversion applications, offering an appealing combination of strong light absorption in the visible range, desirable charge transport characteristics, and good chemical stability. In this work, it is shown that finite-temperature lattice dynamics in CuTaN2 – a prototypical ternary nitride displaying particularly strong visible light absorption – exhibit a pronounced anharmonic character that plays an essential role in defining its macroscopic optoelectronic and thermal properties. Low-frequency vibrational modes that are Raman-inactive from symmetry considerations of the average crystal structure and unstable in harmonic phonon calculations are found to appear as intensive Raman features near room temperature. The atomic contributions to the anharmonic vibrations are characterized by combining Raman measurements with molecular dynamics and density functional theory calculations. This analysis reveals that anharmonic lattice dynamics have large ramifications on the fundamental properties of this compound, resulting in uniaxial negative thermal expansion and the opening of its bandgap to a near-optimal value for solar energy harvesting. The atomic-level understanding of anharmonic lattice dynamics, as well as the finding that they strongly influence key properties of this semiconductor at room temperature, have important implications for design of new functional materials, especially within the emerging class of ternary nitride semiconductors. © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Ternary nitride semiconductors are rapidly emerging as a promising class of materials for energy conversion applications, offering an appealing combination of strong light absorption in the visible range, desirable charge transport characteristics, and good chemical stability. In this work, it is shown that finite-temperature lattice dynamics in CuTaN2 – a prototypical ternary nitride displaying particularly strong visible light absorption – exhibit a pronounced anharmonic character that plays an essential role in defining its macroscopic optoelectronic and thermal properties. Low-frequency vibrational modes that are Raman-inactive from symmetry considerations of the average crystal structure and unstable in harmonic phonon calculations are found to appear as intensive Raman features near room temperature. The atomic contributions to the anharmonic vibrations are characterized by combining Raman measurements with molecular dynamics and density functional theory calculations. This analysis reveals that anharmonic lattice dynamics have large ramifications on the fundamental properties of this compound, resulting in uniaxial negative thermal expansion and the opening of its bandgap to a near-optimal value for solar energy harvesting. The atomic-level understanding of anharmonic lattice dynamics, as well as the finding that they strongly influence key properties of this semiconductor at room temperature, have important implications for design of new functional materials, especially within the emerging class of ternary nitride semiconductors. © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. |
Tu, Suo; Tian, Ting; Xiao, Tianxiao; Yao, Xiangtong; Shen, Sicong; Wu, Yansong; Liu, Yinlong; Bing, Zhenshan; Huang, Kai; Knoll, Alois; Yin, Shanshan; Liang, Suzhe; Heger, Julian E; Pan, Guangjiu; Schwartzkopf, Matthias; Roth, Stephan V; Müller-Buschbaum, Peter Humidity Stable Thermoelectric Hybrid Materials Toward a Self-Powered Triple Sensing System Journal Article Advanced Functional Materials, 34 (25), 2024, ISSN: 1616301X, (Cited by: 4; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Tu2024, title = {Humidity Stable Thermoelectric Hybrid Materials Toward a Self-Powered Triple Sensing System}, author = {Suo Tu and Ting Tian and Tianxiao Xiao and Xiangtong Yao and Sicong Shen and Yansong Wu and Yinlong Liu and Zhenshan Bing and Kai Huang and Alois Knoll and Shanshan Yin and Suzhe Liang and Julian E Heger and Guangjiu Pan and Matthias Schwartzkopf and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85184738841&doi=10.1002%2fadfm.202316088&partnerID=40&md5=287dd8d98d9b38231d5a939bd31c8f2c}, doi = {10.1002/adfm.202316088}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, volume = {34}, number = {25}, publisher = {John Wiley and Sons Inc}, abstract = {Highly sensitive and humidity-resistive detection of the most common physical stimuli is of primary importance for practical application in real-time monitoring. Here, a simple yet effective strategy is reported to achieve a highly humidity-stable hybrid composite that enables simultaneous and accurate pressure and temperature sensing in a single sensor. The improved electronic performance is due to the enhanced planarity of poly (3,-4ethylenedioxythiophene) (PEDOT) and charge transfer between PEDOT:polystyrene sulfonate (PEDOT:PSS) and multi-walled carbon nanotubes (CNTs) by strong π–π interaction. The preferred electronic pathway induced by a robust morphology in the hybrid composite is responsible for the high humidity stability. This study also demonstrates that the sensor has tremendous potential for intelligent object identification with a high level of 97.78% accuracy. Together with the position-detection capability of a triboelectric nanogenerator (TENG), advantages for potential industrial applications of the triple sensing system in terms of intelligent classification without seeing are foreseen. © 2024 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.}, note = {Cited by: 4; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Highly sensitive and humidity-resistive detection of the most common physical stimuli is of primary importance for practical application in real-time monitoring. Here, a simple yet effective strategy is reported to achieve a highly humidity-stable hybrid composite that enables simultaneous and accurate pressure and temperature sensing in a single sensor. The improved electronic performance is due to the enhanced planarity of poly (3,-4ethylenedioxythiophene) (PEDOT) and charge transfer between PEDOT:polystyrene sulfonate (PEDOT:PSS) and multi-walled carbon nanotubes (CNTs) by strong π–π interaction. The preferred electronic pathway induced by a robust morphology in the hybrid composite is responsible for the high humidity stability. This study also demonstrates that the sensor has tremendous potential for intelligent object identification with a high level of 97.78% accuracy. Together with the position-detection capability of a triboelectric nanogenerator (TENG), advantages for potential industrial applications of the triple sensing system in terms of intelligent classification without seeing are foreseen. © 2024 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. |
Xiao, Tianxiao; Tu, Suo; Tian, Ting; Chen, Wei; Cao, Wei; Liang, Suzhe; Guo, Renjun; Liu, Liangzhen; Li, Yanan; Guan, Tianfu; Liu, Haochen; Wang, Kai; Schwartzkopf, Matthias; Fischer, Roland A; Roth, Stephan V; Müller-Buschbaum, Peter Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell Journal Article Nano Energy, 125 , 2024, ISSN: 22112855, (Cited by: 3; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Xiao2024b, title = {Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell}, author = {Tianxiao Xiao and Suo Tu and Ting Tian and Wei Chen and Wei Cao and Suzhe Liang and Renjun Guo and Liangzhen Liu and Yanan Li and Tianfu Guan and Haochen Liu and Kai Wang and Matthias Schwartzkopf and Roland A Fischer and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189558263&doi=10.1016%2fj.nanoen.2024.109555&partnerID=40&md5=fe94f06e4335e9dfe56b1d138c4a15ec}, doi = {10.1016/j.nanoen.2024.109555}, issn = {22112855}, year = {2024}, date = {2024-01-01}, journal = {Nano Energy}, volume = {125}, publisher = {Elsevier Ltd}, abstract = {Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems. © 2024 The Authors}, note = {Cited by: 3; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems. © 2024 The Authors |
Kumar, Labeesh; Nandan, Bhanu; Sarkar, Swagato; König, Tobias A F; Pohl, Darius; Tsuda, Takuya; Zainuddin, Muhammad S B; Humenik, Martin; Scheibel, Thomas; Horechyy, Andriy Enhanced photocatalytic performance of coaxially electrospun titania nanofibers comprising yolk-shell particles Journal Article Journal of Colloid and Interface Science, 674 , pp. 560 – 575, 2024, ISSN: 00219797, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Kumar2024560, title = {Enhanced photocatalytic performance of coaxially electrospun titania nanofibers comprising yolk-shell particles}, author = {Labeesh Kumar and Bhanu Nandan and Swagato Sarkar and Tobias A F König and Darius Pohl and Takuya Tsuda and Muhammad S B Zainuddin and Martin Humenik and Thomas Scheibel and Andriy Horechyy}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85197361436&doi=10.1016%2fj.jcis.2024.06.133&partnerID=40&md5=80e88d019a726da6fa5ed4a36d48cc7f}, doi = {10.1016/j.jcis.2024.06.133}, issn = {00219797}, year = {2024}, date = {2024-01-01}, journal = {Journal of Colloid and Interface Science}, volume = {674}, pages = {560 – 575}, publisher = {Academic Press Inc.}, abstract = {The present paper reports the fabrication of novel types of hybrid fibrous photocatalysts by combining block copolymer (BCP) templating, sol–gel processing, and coaxial electrospinning techniques. Coaxial electrospinning produces core–shell nanofibers (NFs), which are converted into hollow porous TiO2 NFs using an oxidative calcination step. Hybrid BCP micelles comprising a single plasmonic nanoparticle (NP) in their core and thereof derived silica-coated core–shell particles are utilized as precursors to generate yolk-shell type particulate inclusions in photocatalytically active NFs. The catalytic and photocatalytic activity of calcined NFs comprising different types of yolk-shell particles is systematically investigated and compared. Interestingly, calcined NFs comprising silica-coated yolk-shells demonstrate enhanced catalytic and photocatalytic performance despite the presence of silica shell separating plasmonic NP from the TiO2 matrix. Electromagnetic simulations indicate that this enhancement is caused by a localized surface plasmon resonance and a confinement effect in silica-coated yolk-shells embedded in porous TiO2 NFs. Utilization of the coaxially electrospun TiO2 NFs in combination with yolk-shells comprising plasmonic NPs reveals to be a potent method for the photocatalytic decomposition of numerous pollutants. It is worth noting that this study stands as the first occurrence of combining yolk-shells (Au@void@SiO2) with porous electrospun NFs (TiO2) for photocatalytic purposes and gaining an understanding of plasmon and confinement effects for photocatalytic performance. This approach represents a promising route for fabricating highly active and up-scalable fibrous photocatalytic systems. © 2024 The Authors}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The present paper reports the fabrication of novel types of hybrid fibrous photocatalysts by combining block copolymer (BCP) templating, sol–gel processing, and coaxial electrospinning techniques. Coaxial electrospinning produces core–shell nanofibers (NFs), which are converted into hollow porous TiO2 NFs using an oxidative calcination step. Hybrid BCP micelles comprising a single plasmonic nanoparticle (NP) in their core and thereof derived silica-coated core–shell particles are utilized as precursors to generate yolk-shell type particulate inclusions in photocatalytically active NFs. The catalytic and photocatalytic activity of calcined NFs comprising different types of yolk-shell particles is systematically investigated and compared. Interestingly, calcined NFs comprising silica-coated yolk-shells demonstrate enhanced catalytic and photocatalytic performance despite the presence of silica shell separating plasmonic NP from the TiO2 matrix. Electromagnetic simulations indicate that this enhancement is caused by a localized surface plasmon resonance and a confinement effect in silica-coated yolk-shells embedded in porous TiO2 NFs. Utilization of the coaxially electrospun TiO2 NFs in combination with yolk-shells comprising plasmonic NPs reveals to be a potent method for the photocatalytic decomposition of numerous pollutants. It is worth noting that this study stands as the first occurrence of combining yolk-shells (Au@void@SiO2) with porous electrospun NFs (TiO2) for photocatalytic purposes and gaining an understanding of plasmon and confinement effects for photocatalytic performance. This approach represents a promising route for fabricating highly active and up-scalable fibrous photocatalytic systems. © 2024 The Authors |
Tian, Ting; Tu, Suo; Xu, Ang; Yin, Shanshan; Oechsle, Anna Lena; Xiao, Tianxiao; Vagias, Apostolos; Eichhorn, Johanna; Suo, Jinping; Yang, Zhangcan; Bernstorff, Sigrid; Müller-Buschbaum, Peter Unraveling the Morphology-Function Correlation of Mesoporous ZnO Films upon Water Exposure Journal Article Advanced Functional Materials, 34 (8), 2024, ISSN: 1616301X, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Tian2024, title = {Unraveling the Morphology-Function Correlation of Mesoporous ZnO Films upon Water Exposure}, author = {Ting Tian and Suo Tu and Ang Xu and Shanshan Yin and Anna Lena Oechsle and Tianxiao Xiao and Apostolos Vagias and Johanna Eichhorn and Jinping Suo and Zhangcan Yang and Sigrid Bernstorff and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85175527704&doi=10.1002%2fadfm.202311793&partnerID=40&md5=c31a4f3b28afc46702547814c531584e}, doi = {10.1002/adfm.202311793}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, volume = {34}, number = {8}, publisher = {John Wiley and Sons Inc}, abstract = {Ubiquitous moisture in synthetic conditions and ambient environments can strongly influence the conductivity of ZnO semiconductors via the chemisorption and physisorption of water molecules on the ZnO surface. Such an intrinsically water-sensitive nature will become more evident in mesoporous ZnO films where a large surface area and active sites are created simultaneously. However, fundamental insights underlying water-mediated ZnO surface chemistry and electrical conductivity and the factors affecting them remain ambiguous due to the complexity of ZnO surfaces and the difficulties of in situ characterizations at multi-dimensions. Here, self-assembling diblock copolymers are exploited as structure-directing agents to achieve mesoporous ZnO thin films with highly tailorable structural characteristics ranging from nanomorphologies, over crystalline levels, to defect contents. As verified by theoretical calculations, the presence of oxygen vacancy will facilitate favorable water adsorption and subsequent dissociation on the polar ZnO surfaces. Upon humidity exposure with progressively increased levels, mesoporous ZnO films are revealed to follow an almost positive relationship between adsorption and electrical conductivity but show superior morphological stability. This work not only elucidates the water-governed ZnO surface chemistry but may also promote a comprehensive understanding of the morphology-function relationship on ZnO-based electronics. © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Ubiquitous moisture in synthetic conditions and ambient environments can strongly influence the conductivity of ZnO semiconductors via the chemisorption and physisorption of water molecules on the ZnO surface. Such an intrinsically water-sensitive nature will become more evident in mesoporous ZnO films where a large surface area and active sites are created simultaneously. However, fundamental insights underlying water-mediated ZnO surface chemistry and electrical conductivity and the factors affecting them remain ambiguous due to the complexity of ZnO surfaces and the difficulties of in situ characterizations at multi-dimensions. Here, self-assembling diblock copolymers are exploited as structure-directing agents to achieve mesoporous ZnO thin films with highly tailorable structural characteristics ranging from nanomorphologies, over crystalline levels, to defect contents. As verified by theoretical calculations, the presence of oxygen vacancy will facilitate favorable water adsorption and subsequent dissociation on the polar ZnO surfaces. Upon humidity exposure with progressively increased levels, mesoporous ZnO films are revealed to follow an almost positive relationship between adsorption and electrical conductivity but show superior morphological stability. This work not only elucidates the water-governed ZnO surface chemistry but may also promote a comprehensive understanding of the morphology-function relationship on ZnO-based electronics. © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. |
Rasouli, Azam; Kudyba, Artur; Bruzda, Grzegorz; Safarian, Jafar; Tranell, Gabriella High-Temperature Reactive Wetting of Natural Quartz by Liquid Magnesium Journal Article Materials, 17 (6), 2024, ISSN: 19961944, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Rasouli2024, title = {High-Temperature Reactive Wetting of Natural Quartz by Liquid Magnesium}, author = {Azam Rasouli and Artur Kudyba and Grzegorz Bruzda and Jafar Safarian and Gabriella Tranell}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189066882&doi=10.3390%2fma17061302&partnerID=40&md5=9c63350502cd6144c155f86b3c7474f5}, doi = {10.3390/ma17061302}, issn = {19961944}, year = {2024}, date = {2024-01-01}, journal = {Materials}, volume = {17}, number = {6}, publisher = {Multidisciplinary Digital Publishing Institute (MDPI)}, abstract = {High-temperature wetting of natural, high-purity quartz (SiO2) and liquid magnesium (Mg) was investigated at temperatures between 973 and 1273 K. Sessile drop experiments using the capillary purification (CP) procedure were carried out under an Ar gas atmosphere (N6.0), eliminating the native oxide layer on the surface of Mg melt. The results showed that the wetting behavior was strongly dependent on temperature. At 973 and 1073 K, the wetting system displayed relatively large contact angles of 90° and 65°, respectively, demonstrating modest wetting. The wetting increased to some extent by increasing the temperature to 1123 K with a wetting angle of 22°. However, the SiO2/Mg system demonstrated complete wetting at temperatures of 1173 K and above. Furthermore, interface microstructure examination showed different reaction product phases/microstructures, depending on the wetting experiment temperature. © 2024 by the authors.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } High-temperature wetting of natural, high-purity quartz (SiO2) and liquid magnesium (Mg) was investigated at temperatures between 973 and 1273 K. Sessile drop experiments using the capillary purification (CP) procedure were carried out under an Ar gas atmosphere (N6.0), eliminating the native oxide layer on the surface of Mg melt. The results showed that the wetting behavior was strongly dependent on temperature. At 973 and 1073 K, the wetting system displayed relatively large contact angles of 90° and 65°, respectively, demonstrating modest wetting. The wetting increased to some extent by increasing the temperature to 1123 K with a wetting angle of 22°. However, the SiO2/Mg system demonstrated complete wetting at temperatures of 1173 K and above. Furthermore, interface microstructure examination showed different reaction product phases/microstructures, depending on the wetting experiment temperature. © 2024 by the authors. |
Maier, Thomas L; de Kam, Lucas B T; Golibrzuch, Matthias; Angerer, Tina; Becherer, Markus; Krischer, Katharina How Metal/Insulator Interfaces Enable an Enhancement of the Hydrogen Evolution Reaction Kinetics Journal Article ChemElectroChem, 11 (11), 2024, ISSN: 21960216, (Cited by: 0; All Open Access, Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Maier2024, title = {How Metal/Insulator Interfaces Enable an Enhancement of the Hydrogen Evolution Reaction Kinetics}, author = {Thomas L Maier and Lucas B T. de Kam and Matthias Golibrzuch and Tina Angerer and Markus Becherer and Katharina Krischer}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85193040302&doi=10.1002%2fcelc.202400109&partnerID=40&md5=fd23b3506d9f1ab0592cb211f1de3759}, doi = {10.1002/celc.202400109}, issn = {21960216}, year = {2024}, date = {2024-01-01}, journal = {ChemElectroChem}, volume = {11}, number = {11}, publisher = {John Wiley and Sons Inc}, abstract = {The nanostructuring of electrodes is a common way of increasing electrocatalytic activity. Yet, the fact that the presence of insulating material in nanostructured composites can have a positive effect on efficiency was an unexpected recent finding. The rate enhancement has been linked to different electric fields at the insulator and metal interfaces, facilitating enhanced transport of reaction products into the bulk electrolyte. In this article, we further uncover the origin of the rate enhancement with parameter studies and simulations. We experimentally investigate various parameter dependencies of the alkaline Hydrogen Evolution Reaction (HER) on well-defined nanometer-sized Au arrays embedded in a silicon nitride insulating layer. We find a significant enhancement of the HER for all experimental conditions and opposite activity trends with pH, electrolyte concentration and the cationic species compared to a continuous Au electrode. Using a mean field model, we quantify the electrostatic interfacial pressure above the Au and the insulator patches. Combining the double layer simulations with rate equations, we demonstrate that all parameter variations can be consistently explained by the fact that the double layer structure above the insulator patches is much less rigid than above the metal islands and is independent of the applied potential. © 2024 The Authors. ChemElectroChem published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } The nanostructuring of electrodes is a common way of increasing electrocatalytic activity. Yet, the fact that the presence of insulating material in nanostructured composites can have a positive effect on efficiency was an unexpected recent finding. The rate enhancement has been linked to different electric fields at the insulator and metal interfaces, facilitating enhanced transport of reaction products into the bulk electrolyte. In this article, we further uncover the origin of the rate enhancement with parameter studies and simulations. We experimentally investigate various parameter dependencies of the alkaline Hydrogen Evolution Reaction (HER) on well-defined nanometer-sized Au arrays embedded in a silicon nitride insulating layer. We find a significant enhancement of the HER for all experimental conditions and opposite activity trends with pH, electrolyte concentration and the cationic species compared to a continuous Au electrode. Using a mean field model, we quantify the electrostatic interfacial pressure above the Au and the insulator patches. Combining the double layer simulations with rate equations, we demonstrate that all parameter variations can be consistently explained by the fact that the double layer structure above the insulator patches is much less rigid than above the metal islands and is independent of the applied potential. © 2024 The Authors. ChemElectroChem published by Wiley-VCH GmbH. |
Huang, Tzu-Yen; Brun, Anton Le P; Sochor, Benedikt; Wu, Chun-Ming; Bulut, Yusuf; Müller-Buschbaum, Peter; Roth, Stephan V; Yang, Yan-Ling Nanometer-Thick ITIC Bulk Heterojunction Films as Non-Fullerene Acceptors in Organic Solar Cells Journal Article ACS Applied Nano Materials, 7 (15), pp. 17588 – 17595, 2024, ISSN: 25740970, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Huang202417588, title = {Nanometer-Thick ITIC Bulk Heterojunction Films as Non-Fullerene Acceptors in Organic Solar Cells}, author = {Tzu-Yen Huang and Anton P Le Brun and Benedikt Sochor and Chun-Ming Wu and Yusuf Bulut and Peter Müller-Buschbaum and Stephan V Roth and Yan-Ling Yang}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85199690359&doi=10.1021%2facsanm.4c02865&partnerID=40&md5=3a48422082eab27e5ae5e7ac9c337dcd}, doi = {10.1021/acsanm.4c02865}, issn = {25740970}, year = {2024}, date = {2024-01-01}, journal = {ACS Applied Nano Materials}, volume = {7}, number = {15}, pages = {17588 – 17595}, publisher = {American Chemical Society}, abstract = {The nanomorphology of bulk heterojunctions (BHJs) plays a critical role in determining the performance of non-fullerene organic solar cells (OSCs). Thermal annealing is commonly used to reorganize the donor and acceptor phases within the BHJs. In this study, we investigate the vertical morphology of BHJ blend films incorporating the poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3‴-di(2-octyldodecyl)-2,2′;5′,2″;5″,2‴-quaterthiophen-5,5‴-diyl)] (PffBT4T-2OD) polymer as the donor and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC) as the acceptor. Neutron reflectivity patterns and scattering length density profiles reveal that the surface of the BHJ films became diffuse when the annealing temperature was above 150 °C. We further find that mitigated agglomeration of PffBT4T-2OD side chains exhibits minimal impact on morphology post-annealing. Instead, ITIC molecules trigger aggregations, accompanied by interface diffusion and increased film roughness. X-ray scattering confirms a 5-fold increase in aggregated ITIC nanodomains after annealing. Our findings highlight that unstable ITIC phases dominate the BHJ morphology of thin films, leading to the thermal instability of OSCs. This study enhances our understanding of the BHJ morphology and offers insights into improving the performance of energy conversion devices. © 2024 American Chemical Society.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } The nanomorphology of bulk heterojunctions (BHJs) plays a critical role in determining the performance of non-fullerene organic solar cells (OSCs). Thermal annealing is commonly used to reorganize the donor and acceptor phases within the BHJs. In this study, we investigate the vertical morphology of BHJ blend films incorporating the poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3‴-di(2-octyldodecyl)-2,2′;5′,2″;5″,2‴-quaterthiophen-5,5‴-diyl)] (PffBT4T-2OD) polymer as the donor and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC) as the acceptor. Neutron reflectivity patterns and scattering length density profiles reveal that the surface of the BHJ films became diffuse when the annealing temperature was above 150 °C. We further find that mitigated agglomeration of PffBT4T-2OD side chains exhibits minimal impact on morphology post-annealing. Instead, ITIC molecules trigger aggregations, accompanied by interface diffusion and increased film roughness. X-ray scattering confirms a 5-fold increase in aggregated ITIC nanodomains after annealing. Our findings highlight that unstable ITIC phases dominate the BHJ morphology of thin films, leading to the thermal instability of OSCs. This study enhances our understanding of the BHJ morphology and offers insights into improving the performance of energy conversion devices. © 2024 American Chemical Society. |
Reus, Manuel A; Baier, Thomas; Lindenmeir, Christoph G; Weinzierl, Alexander F; Buyan-Arivjikh, Altantulga; Wegener, Simon A; Kosbahn, David P; Reb, Lennart K; Rubeck, Jan; Schwartzkopf, Matthias; Roth, Stephan V; Müller-Buschbaum, Peter Modular slot-die coater for in situ grazing-incidence x-ray scattering experiments on thin films Journal Article Review of Scientific Instruments, 95 (4), 2024, ISSN: 00346748, (Cited by: 1; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Reus2024b, title = {Modular slot-die coater for in situ grazing-incidence x-ray scattering experiments on thin films}, author = {Manuel A Reus and Thomas Baier and Christoph G Lindenmeir and Alexander F Weinzierl and Altantulga Buyan-Arivjikh and Simon A Wegener and David P Kosbahn and Lennart K Reb and Jan Rubeck and Matthias Schwartzkopf and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85191250978&doi=10.1063%2f5.0204673&partnerID=40&md5=2368b6fa4cd1af9516bc308d5b33c7a5}, doi = {10.1063/5.0204673}, issn = {00346748}, year = {2024}, date = {2024-01-01}, journal = {Review of Scientific Instruments}, volume = {95}, number = {4}, publisher = {American Institute of Physics}, abstract = {Multimodal in situ experiments during slot-die coating of thin films pioneer the way to kinetic studies on thin-film formation. They establish a powerful tool to understand and optimize the formation and properties of thin-film devices, e.g., solar cells, sensors, or LED films. Thin-film research benefits from time-resolved grazing-incidence wide- and small-angle x-ray scattering (GIWAXS/GISAXS) with a sub-second resolution to reveal the evolution of crystal structure, texture, and morphology during the deposition process. Simultaneously investigating optical properties by in situ photoluminescence measurements complements in-depth kinetic studies focusing on a comprehensive understanding of the triangular interdependency of processing, structure, and function for a roll-to-roll compatible, scalable thin-film deposition process. Here, we introduce a modular slot-die coater specially designed for in situ GIWAXS/GISAXS measurements and applicable to various ink systems. With a design for quick assembly, the slot-die coater permits the reproducible and comparable fabrication of thin films in the lab and at the synchrotron using the very same hardware components, as demonstrated in this work by experiments performed at Deutsches Elektronen-Synchrotron (DESY). Simultaneous to GIWAXS/GISAXS, photoluminescence measurements probe optoelectronic properties in situ during thin-film formation. An environmental chamber allows to control the atmosphere inside the coater. Modular construction and lightweight design make the coater mobile, easy to transport, quickly extendable, and adaptable to new beamline environments. © 2024 Author(s).}, note = {Cited by: 1; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Multimodal in situ experiments during slot-die coating of thin films pioneer the way to kinetic studies on thin-film formation. They establish a powerful tool to understand and optimize the formation and properties of thin-film devices, e.g., solar cells, sensors, or LED films. Thin-film research benefits from time-resolved grazing-incidence wide- and small-angle x-ray scattering (GIWAXS/GISAXS) with a sub-second resolution to reveal the evolution of crystal structure, texture, and morphology during the deposition process. Simultaneously investigating optical properties by in situ photoluminescence measurements complements in-depth kinetic studies focusing on a comprehensive understanding of the triangular interdependency of processing, structure, and function for a roll-to-roll compatible, scalable thin-film deposition process. Here, we introduce a modular slot-die coater specially designed for in situ GIWAXS/GISAXS measurements and applicable to various ink systems. With a design for quick assembly, the slot-die coater permits the reproducible and comparable fabrication of thin films in the lab and at the synchrotron using the very same hardware components, as demonstrated in this work by experiments performed at Deutsches Elektronen-Synchrotron (DESY). Simultaneous to GIWAXS/GISAXS, photoluminescence measurements probe optoelectronic properties in situ during thin-film formation. An environmental chamber allows to control the atmosphere inside the coater. Modular construction and lightweight design make the coater mobile, easy to transport, quickly extendable, and adaptable to new beamline environments. © 2024 Author(s). |
Almora, Osbel; Cabrera, Carlos I; Erten-Ela, Sule; Forberich, Karen; Fukuda, Kenjiro; Guo, Fei; Hauch, Jens; Ho-Baillie, Anita W Y; Jacobsson, Jesper T; Janssen, Rene A J; Kirchartz, Thomas; Loi, Maria A; Mathew, Xavier; Mitzi, David B; Nazeeruddin, Mohammad K; Paetzold, Ulrich W; Rand, Barry P; Rau, Uwe; Someya, Takao; Unger, Eva; Vaillant-Roca, Lídice; Brabec, Christoph J Device Performance of Emerging Photovoltaic Materials (Version 4) Journal Article Advanced Energy Materials, 14 (4), 2024, ISSN: 16146832, (Cited by: 8; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Almora2024, title = {Device Performance of Emerging Photovoltaic Materials (Version 4)}, author = {Osbel Almora and Carlos I Cabrera and Sule Erten-Ela and Karen Forberich and Kenjiro Fukuda and Fei Guo and Jens Hauch and Anita W Y Ho-Baillie and Jesper T Jacobsson and Rene A J Janssen and Thomas Kirchartz and Maria A Loi and Xavier Mathew and David B Mitzi and Mohammad K Nazeeruddin and Ulrich W Paetzold and Barry P Rand and Uwe Rau and Takao Someya and Eva Unger and Lídice Vaillant-Roca and Christoph J Brabec}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85179733522&doi=10.1002%2faenm.202303173&partnerID=40&md5=1c0215d482802ecd01505122d7519361}, doi = {10.1002/aenm.202303173}, issn = {16146832}, year = {2024}, date = {2024-01-01}, journal = {Advanced Energy Materials}, volume = {14}, number = {4}, publisher = {John Wiley and Sons Inc}, abstract = {Following the 3rd release of the “Emerging PV reports”, the best achievements in the performance of emerging photovoltaic (e-PV) devices in diverse e-PV research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2022. Updated graphs, tables, and analyses are provided with several performance parameters, such as power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, for example, the detailed balance efficiency limit. The 4th installment of the “Emerging PV reports” discusses the “PV emergence” classification with respect to the “PV technology generations” and “PV research waves” and highlights the latest device performance progress in multijunction and flexible photovoltaics. Additionally, Dale-Scarpulla's plots of efficiency-effort in terms of cumulative academic publication count are also introduced. © 2023 Wiley-VCH GmbH.}, note = {Cited by: 8; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Following the 3rd release of the “Emerging PV reports”, the best achievements in the performance of emerging photovoltaic (e-PV) devices in diverse e-PV research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2022. Updated graphs, tables, and analyses are provided with several performance parameters, such as power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, for example, the detailed balance efficiency limit. The 4th installment of the “Emerging PV reports” discusses the “PV emergence” classification with respect to the “PV technology generations” and “PV research waves” and highlights the latest device performance progress in multijunction and flexible photovoltaics. Additionally, Dale-Scarpulla's plots of efficiency-effort in terms of cumulative academic publication count are also introduced. © 2023 Wiley-VCH GmbH. |
Reus, Manuel A; Reb, Lennart K; Kosbahn, David P; Roth, Stephan V; Müller-Buschbaum, Peter INSIGHT: in situ heuristic tool for the efficient reduction of grazing-incidence X-ray scattering data Journal Article Journal of Applied Crystallography, 57 , pp. 509 – 528, 2024, ISSN: 00218898, (Cited by: 5; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Reus2024509, title = {INSIGHT: in situ heuristic tool for the efficient reduction of grazing-incidence X-ray scattering data}, author = {Manuel A Reus and Lennart K Reb and David P Kosbahn and Stephan V Roth and Peter Müller-Buschbaum}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85189931954&doi=10.1107%2fS1600576723011159&partnerID=40&md5=a928626dbb33d73f92d7880e27a75d81}, doi = {10.1107/S1600576723011159}, issn = {00218898}, year = {2024}, date = {2024-01-01}, journal = {Journal of Applied Crystallography}, volume = {57}, pages = {509 – 528}, publisher = {International Union of Crystallography}, abstract = {INSIGHT is a Python-based software tool for processing and reducing 2D grazing-incidence wide- and small-angle X-ray scattering (GIWAXS/GISAXS) data. It offers the geometric transformation of the 2D GIWAXS/GISAXS detector image to reciprocal space, including vectorized and parallelized pixelwise intensity correction calculations. An explicit focus on efficient data management and batch processing enables full control of large time-resolved synchrotron and laboratory data sets for a detailed analysis of kinetic GIWAXS/ GISAXS studies of thin films. It processes data acquired with arbitrarily rotated detectors and performs vertical, horizontal, azimuthal and radial cuts in reciprocal space. It further allows crystallographic indexing and GIWAXS pattern simulation, and provides various plotting and export functionalities. Customized scripting offers a one-step solution to reduce, process, analyze and export findings of large in situ and operando data sets. © 2024 International Union of Crystallography. All rights reserved.}, note = {Cited by: 5; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } INSIGHT is a Python-based software tool for processing and reducing 2D grazing-incidence wide- and small-angle X-ray scattering (GIWAXS/GISAXS) data. It offers the geometric transformation of the 2D GIWAXS/GISAXS detector image to reciprocal space, including vectorized and parallelized pixelwise intensity correction calculations. An explicit focus on efficient data management and batch processing enables full control of large time-resolved synchrotron and laboratory data sets for a detailed analysis of kinetic GIWAXS/ GISAXS studies of thin films. It processes data acquired with arbitrarily rotated detectors and performs vertical, horizontal, azimuthal and radial cuts in reciprocal space. It further allows crystallographic indexing and GIWAXS pattern simulation, and provides various plotting and export functionalities. Customized scripting offers a one-step solution to reduce, process, analyze and export findings of large in situ and operando data sets. © 2024 International Union of Crystallography. All rights reserved. |
Jan, Pei-En; Liang, Hao-Chi; Cheng, Ren-Wei; Greve, Christopher R; Chuang, Yung-Tang; Chiu, Yung-Ling; Tan, Guang-Hsun; Elsenety, Mohamed M; Chang, Chih-Li; Dorrah, Dalia M; Lai, Hoong-Lien; Chiu, Po-Wei; Sun, Sheng-Yuan; Li, Yun-Li; Herzig, Eva M; Chou, Ho-Hsiu; Lin, Hao-Wu Advanced Functional Materials, 2024, ISSN: 1616301X, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Jan2024, title = {Molecular Design Strategy for Meta-Substituted Aromatic Organic Halides in Zero-Lead-Release Halide Perovskites with Efficient Waterproof Light Emission}, author = {Pei-En Jan and Hao-Chi Liang and Ren-Wei Cheng and Christopher R Greve and Yung-Tang Chuang and Yung-Ling Chiu and Guang-Hsun Tan and Mohamed M Elsenety and Chih-Li Chang and Dalia M Dorrah and Hoong-Lien Lai and Po-Wei Chiu and Sheng-Yuan Sun and Yun-Li Li and Eva M Herzig and Ho-Hsiu Chou and Hao-Wu Lin}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85203043862&doi=10.1002%2fadfm.202408323&partnerID=40&md5=a4d8aa1813df5d142bfe44e08872c17a}, doi = {10.1002/adfm.202408323}, issn = {1616301X}, year = {2024}, date = {2024-01-01}, journal = {Advanced Functional Materials}, publisher = {John Wiley and Sons Inc}, abstract = {Halide perovskites have received an immense attention in the field of optoelectronics due to their outstanding photophysical properties. But so far, lead-based halide perovskites still account for most of the research, which raises concerns due to lead toxicity. Herein, a new design strategy is proposed utilizing a super large, energetically higher singlet and triplet energy levels aromatic organic cation to incorporate into the perovskite structure, forming ultra-stable high-performance 2D/3D (quasi-2D) perovskite. The judicious molecular design of connecting all the phenyl groups at their meta sites ensures the simultaneous achievement of a large molecular weight and high singlet and triplet energy levels. The resulting quasi-2D perovskite thin films not only exhibits excellent emission properties but also, surprisingly, show long-term waterproof-level stability. The robustness of these perovskites is confirmed by their extraordinary emission stability upon direct water immersion and almost undetectable lead release in water. Proof-of-concept of a water-resistant color conversion-type perovskite near-infrared (NIR) light-emitting diode (LED) is demonstrated, showing high external quantum efficiency (EQE) and power conversion efficiency (PCE) of 20.5% and 13.3%, respectively. It is believed these results and strategy pave a new way for realizing environmentally friendly lead halide materials and devices. © 2024 Wiley-VCH GmbH.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Halide perovskites have received an immense attention in the field of optoelectronics due to their outstanding photophysical properties. But so far, lead-based halide perovskites still account for most of the research, which raises concerns due to lead toxicity. Herein, a new design strategy is proposed utilizing a super large, energetically higher singlet and triplet energy levels aromatic organic cation to incorporate into the perovskite structure, forming ultra-stable high-performance 2D/3D (quasi-2D) perovskite. The judicious molecular design of connecting all the phenyl groups at their meta sites ensures the simultaneous achievement of a large molecular weight and high singlet and triplet energy levels. The resulting quasi-2D perovskite thin films not only exhibits excellent emission properties but also, surprisingly, show long-term waterproof-level stability. The robustness of these perovskites is confirmed by their extraordinary emission stability upon direct water immersion and almost undetectable lead release in water. Proof-of-concept of a water-resistant color conversion-type perovskite near-infrared (NIR) light-emitting diode (LED) is demonstrated, showing high external quantum efficiency (EQE) and power conversion efficiency (PCE) of 20.5% and 13.3%, respectively. It is believed these results and strategy pave a new way for realizing environmentally friendly lead halide materials and devices. © 2024 Wiley-VCH GmbH. |
Derelli, Davide; Frank, Kilian; Grote, Lukas; Mancini, Federica; Dippel, Ann-Christin; Gutowski, Olof; Nickel, Bert; Koziej, Dorota Direct Synthesis of CuPd Icosahedra Supercrystals Studied by In Situ X-Ray Scattering Journal Article Small, 20 (32), 2024, ISSN: 16136810, (Cited by: 0; All Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: @article{Derelli2024, title = {Direct Synthesis of CuPd Icosahedra Supercrystals Studied by In Situ X-Ray Scattering}, author = {Davide Derelli and Kilian Frank and Lukas Grote and Federica Mancini and Ann-Christin Dippel and Olof Gutowski and Bert Nickel and Dorota Koziej}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85188518964&doi=10.1002%2fsmll.202311714&partnerID=40&md5=95bcc8e6ed98322bfb411c2169f05879}, doi = {10.1002/smll.202311714}, issn = {16136810}, year = {2024}, date = {2024-01-01}, journal = {Small}, volume = {20}, number = {32}, publisher = {John Wiley and Sons Inc}, abstract = {Nanocrystal self-assembly into supercrystals provides a versatile platform for creating novel materials and devices with tailored properties. While common self-assembly strategies imply the use of purified nanoparticles after synthesis, conversion of chemical precursors directly into nanocrystals and then supercrystals in simple procedures has been rarely reported. Here, the nucleation and growth of CuPd icosahedra and their consecutive assembly into large closed-packed face-centered cubic (fcc) supercrystals are studied. To this end, the study simultaneously and in situ measures X-ray total scattering with pair distribution function analysis (TS-PDF) and small-angle X-ray scattering (SAXS). It is found that the supercrystals' formation is preceded by an intermediate dense phase of nanocrystals displaying short-range order (SRO). It is further shown that the organization of oleic acid/oleylamine surfactants into lamellar structures likely drives the emergence of the SRO phase and later of the supercrystals by reducing the volume accessible to particle diffusion. The supercrystals' formation as well as their disassembly are triggered by temperature. The study demonstrates that ordering of solvent molecules can be crucial in the direct synthesis of supercrystals. The study also provides a general approach to investigate novel preparation routes of supercrystals in situ and across several length scales via X-ray scattering. © 2024 The Authors. Small published by Wiley-VCH GmbH.}, note = {Cited by: 0; All Open Access, Hybrid Gold Open Access}, keywords = {}, pubstate = {published}, tppubtype = {article} } Nanocrystal self-assembly into supercrystals provides a versatile platform for creating novel materials and devices with tailored properties. While common self-assembly strategies imply the use of purified nanoparticles after synthesis, conversion of chemical precursors directly into nanocrystals and then supercrystals in simple procedures has been rarely reported. Here, the nucleation and growth of CuPd icosahedra and their consecutive assembly into large closed-packed face-centered cubic (fcc) supercrystals are studied. To this end, the study simultaneously and in situ measures X-ray total scattering with pair distribution function analysis (TS-PDF) and small-angle X-ray scattering (SAXS). It is found that the supercrystals' formation is preceded by an intermediate dense phase of nanocrystals displaying short-range order (SRO). It is further shown that the organization of oleic acid/oleylamine surfactants into lamellar structures likely drives the emergence of the SRO phase and later of the supercrystals by reducing the volume accessible to particle diffusion. The supercrystals' formation as well as their disassembly are triggered by temperature. The study demonstrates that ordering of solvent molecules can be crucial in the direct synthesis of supercrystals. The study also provides a general approach to investigate novel preparation routes of supercrystals in situ and across several length scales via X-ray scattering. © 2024 The Authors. Small published by Wiley-VCH GmbH. |
Berger, Luca M; Barkey, Martin; Maier, Stefan A; Tittl, Andreas Metallic and All-Dielectric Metasurfaces Sustaining Displacement-Mediated Bound States in the Continuum Journal Article Advanced Optical Materials, 12 (5), 2024, ISSN: 21951071, (Cited by: 6; All Open Access, Green Open Access, Hybrid Gold Open Access). Abstract | Links | BibTeX | Tags: Nanophotonics; Photonic devices; Angular-robust; Bound state in the continuum; Bound-states; Metallics; Metasurface; Microscope objective; Mid-IR spectroscopy; Reflective microscope objective; Reflective microscopes; Superlattice; Incident light @article{Berger2024, title = {Metallic and All-Dielectric Metasurfaces Sustaining Displacement-Mediated Bound States in the Continuum}, author = {Luca M Berger and Martin Barkey and Stefan A Maier and Andreas Tittl}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85169339120&doi=10.1002%2fadom.202301269&partnerID=40&md5=e2109c06d6b9ff2112970d07bbc33976}, doi = {10.1002/adom.202301269}, issn = {21951071}, year = {2024}, date = {2024-01-01}, journal = {Advanced Optical Materials}, volume = {12}, number = {5}, publisher = {John Wiley and Sons Inc}, abstract = {Bound states in the continuum (BICs) are localized electromagnetic modes within the continuous spectrum of radiating waves. Due to their infinite lifetimes without radiation losses, BICs are driving research directions in lasing, non-linear optical processes, and sensing. However, conventional methods for converting BICs into leaky resonances, or quasi-BICs, with high-quality factors typically rely on breaking the in-plane inversion symmetry of the metasurface and often result in resonances that are strongly dependent on the angle of the incident light, making them unsuitable for many practical applications. Here, an emerging class of BIC-driven metasurfaces is numerically analyzed and experimentally demonstrated, where the coupling to the far field is controlled by the displacement of individual resonators. In particular, both all-dielectric and metallic as well as positive and inverse displacement-mediated metasurfaces sustaining angular-robust quasi-BICs are investigated in the mid-infrared spectral region. Their optical behavior with regard to changes in the angle of incidence is investigated and experimentally shows their superior performance compared to two conventional alternatives: silicon-based tilted ellipses and cylindrical nanoholes in gold. These findings are anticipated to open exciting perspectives for bio-sensing, conformal optical devices, and photonic devices using focused light. © 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH.}, note = {Cited by: 6; All Open Access, Green Open Access, Hybrid Gold Open Access}, keywords = {Nanophotonics; Photonic devices; Angular-robust; Bound state in the continuum; Bound-states; Metallics; Metasurface; Microscope objective; Mid-IR spectroscopy; Reflective microscope objective; Reflective microscopes; Superlattice; Incident light}, pubstate = {published}, tppubtype = {article} } Bound states in the continuum (BICs) are localized electromagnetic modes within the continuous spectrum of radiating waves. Due to their infinite lifetimes without radiation losses, BICs are driving research directions in lasing, non-linear optical processes, and sensing. However, conventional methods for converting BICs into leaky resonances, or quasi-BICs, with high-quality factors typically rely on breaking the in-plane inversion symmetry of the metasurface and often result in resonances that are strongly dependent on the angle of the incident light, making them unsuitable for many practical applications. Here, an emerging class of BIC-driven metasurfaces is numerically analyzed and experimentally demonstrated, where the coupling to the far field is controlled by the displacement of individual resonators. In particular, both all-dielectric and metallic as well as positive and inverse displacement-mediated metasurfaces sustaining angular-robust quasi-BICs are investigated in the mid-infrared spectral region. Their optical behavior with regard to changes in the angle of incidence is investigated and experimentally shows their superior performance compared to two conventional alternatives: silicon-based tilted ellipses and cylindrical nanoholes in gold. These findings are anticipated to open exciting perspectives for bio-sensing, conformal optical devices, and photonic devices using focused light. © 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH. |
Sirotti, Elise; Böhm, Stefan; Sharp, Ian D Ultrastable Zn3N2 Thin Films via Integration of Amorphous GaN Protection Layers Journal Article Advanced Materials Interfaces, 11 (22), 2024, ISSN: 21967350, (Cited by: 0). Abstract | Links | BibTeX | Tags: @article{Sirotti2024, title = {Ultrastable Zn3N2 Thin Films via Integration of Amorphous GaN Protection Layers}, author = {Elise Sirotti and Stefan Böhm and Ian D Sharp}, url = {https://www.scopus.com/inward/record.uri?eid=2-s2.0-85196511694&doi=10.1002%2fadmi.202400214&partnerID=40&md5=dc119cc28d4f1c2ccb3c5d6edda495f7}, doi = {10.1002/admi.202400214}, issn = {21967350}, year = {2024}, date = {2024-01-01}, journal = {Advanced Materials Interfaces}, volume = {11}, number = {22}, publisher = {John Wiley and Sons Inc}, abstract = {Zinc nitride (Zn3N2) is a promising semiconductor for a range of optoelectronic and energy conversion applications, offering a direct bandgap of 1.0 eV, large carrier mobilities, and abundant constituent elements. However, the material is prone to bulk oxidation in ambient environments, which has thus far impeded its practical deployment. While previous approaches have focused on stabilizing the material via integration of ZnO surface layers, these strategies introduce additional challenges regarding elevated processing temperatures and limited control of interface properties. In this study, it is shown that amorphous GaN thin films can serve as highly stable protection layers on Zn3N2 surfaces and can be deposited at the same growth temperature and in the same deposition system as the underlying semiconductor. The GaN-capped Zn3N2 structures exhibit long-term stability, surviving over 3 years of exposure to ambient conditions with no discernible alterations in composition, structure, or electrical properties. Notably, the amorphous GaN coatings can even impede Zn3N2 oxidation under prolonged aqueous exposure. Thus, this study offers a solution to stabilize Zn3N2 in ambient conditions, providing a viable pathway to its utilization in robust and high-performance electronic devices, such as thin film transistors and solar energy conversion systems. © 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH.}, note = {Cited by: 0}, keywords = {}, pubstate = {published}, tppubtype = {article} } Zinc nitride (Zn3N2) is a promising semiconductor for a range of optoelectronic and energy conversion applications, offering a direct bandgap of 1.0 eV, large carrier mobilities, and abundant constituent elements. However, the material is prone to bulk oxidation in ambient environments, which has thus far impeded its practical deployment. While previous approaches have focused on stabilizing the material via integration of ZnO surface layers, these strategies introduce additional challenges regarding elevated processing temperatures and limited control of interface properties. In this study, it is shown that amorphous GaN thin films can serve as highly stable protection layers on Zn3N2 surfaces and can be deposited at the same growth temperature and in the same deposition system as the underlying semiconductor. The GaN-capped Zn3N2 structures exhibit long-term stability, surviving over 3 years of exposure to ambient conditions with no discernible alterations in composition, structure, or electrical properties. Notably, the amorphous GaN coatings can even impede Zn3N2 oxidation under prolonged aqueous exposure. Thus, this study offers a solution to stabilize Zn3N2 in ambient conditions, providing a viable pathway to its utilization in robust and high-performance electronic devices, such as thin film transistors and solar energy conversion systems. © 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH. |