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Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting
Oxysulfide semiconductor, Y(2)Ti(2)O(5)S(2), has recently discovered its exciting potential for visible-light-induced overall water splitting, and therefore, imperatively requires the probing of unknown fundamental charge loss pathways to engineer the photoactivity enhancement. Herein, transient dif...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2021
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8651740/ https://www.ncbi.nlm.nih.gov/pubmed/34876590 http://dx.doi.org/10.1038/s41467-021-27199-3 |
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author | Nandal, Vikas Shoji, Ryota Matsuzaki, Hiroyuki Furube, Akihiro Lin, Lihua Hisatomi, Takashi Kaneko, Masanori Yamashita, Koichi Domen, Kazunari Seki, Kazuhiko |
author_facet | Nandal, Vikas Shoji, Ryota Matsuzaki, Hiroyuki Furube, Akihiro Lin, Lihua Hisatomi, Takashi Kaneko, Masanori Yamashita, Koichi Domen, Kazunari Seki, Kazuhiko |
author_sort | Nandal, Vikas |
collection | PubMed |
description | Oxysulfide semiconductor, Y(2)Ti(2)O(5)S(2), has recently discovered its exciting potential for visible-light-induced overall water splitting, and therefore, imperatively requires the probing of unknown fundamental charge loss pathways to engineer the photoactivity enhancement. Herein, transient diffuse reflectance spectroscopy measurements are coupled with theoretical calculations to unveil the nanosecond to microsecond time range dynamics of the photogenerated charge carriers. In early nanosecond range, the pump-fluence-dependent decay dynamics of the absorption signal is originated from the bimolecular recombination of mobile charge carriers, in contrast, the power-law decay kinetics in late microsecond range is dominated by hole detrapping from exponential tail trap states of valence band. A well-calibrated theoretical model estimates various efficiency limiting material parameters like recombination rate constant, n-type doping density and tail-states parameters. Compared to metal oxides, longer effective carrier lifetime ~6 ns is demonstrated. Different design routes are proposed to realize efficiency beyond 10% for commercial solar-to-hydrogen production from oxysulfide photocatalysts. |
format | Online Article Text |
id | pubmed-8651740 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-86517402021-12-27 Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting Nandal, Vikas Shoji, Ryota Matsuzaki, Hiroyuki Furube, Akihiro Lin, Lihua Hisatomi, Takashi Kaneko, Masanori Yamashita, Koichi Domen, Kazunari Seki, Kazuhiko Nat Commun Article Oxysulfide semiconductor, Y(2)Ti(2)O(5)S(2), has recently discovered its exciting potential for visible-light-induced overall water splitting, and therefore, imperatively requires the probing of unknown fundamental charge loss pathways to engineer the photoactivity enhancement. Herein, transient diffuse reflectance spectroscopy measurements are coupled with theoretical calculations to unveil the nanosecond to microsecond time range dynamics of the photogenerated charge carriers. In early nanosecond range, the pump-fluence-dependent decay dynamics of the absorption signal is originated from the bimolecular recombination of mobile charge carriers, in contrast, the power-law decay kinetics in late microsecond range is dominated by hole detrapping from exponential tail trap states of valence band. A well-calibrated theoretical model estimates various efficiency limiting material parameters like recombination rate constant, n-type doping density and tail-states parameters. Compared to metal oxides, longer effective carrier lifetime ~6 ns is demonstrated. Different design routes are proposed to realize efficiency beyond 10% for commercial solar-to-hydrogen production from oxysulfide photocatalysts. Nature Publishing Group UK 2021-12-07 /pmc/articles/PMC8651740/ /pubmed/34876590 http://dx.doi.org/10.1038/s41467-021-27199-3 Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Nandal, Vikas Shoji, Ryota Matsuzaki, Hiroyuki Furube, Akihiro Lin, Lihua Hisatomi, Takashi Kaneko, Masanori Yamashita, Koichi Domen, Kazunari Seki, Kazuhiko Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
title | Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
title_full | Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
title_fullStr | Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
title_full_unstemmed | Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
title_short | Unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
title_sort | unveiling charge dynamics of visible light absorbing oxysulfide for efficient overall water splitting |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8651740/ https://www.ncbi.nlm.nih.gov/pubmed/34876590 http://dx.doi.org/10.1038/s41467-021-27199-3 |
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