The bright side and dark side of hybrid organic–inorganic perovskites
The previously developed bistable amphoteric native defect (BAND) model is used for a comprehensive explanation of the unique photophysical properties and for understanding the remarkable performance of perovskites as photovoltaic materials. It is shown that the amphoteric defects in donor (acceptor...
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sg-ntu-dr.10356-1454402023-02-28T19:30:58Z The bright side and dark side of hybrid organic–inorganic perovskites Walukiewicz, Wladek Wang, Shu Wu, Xinchun Li, Rundong Sherburne, Matthew P. Wu, Bo Sum, Tze Chien Ager, Joel W. Asta, Mark D. School of Physical and Mathematical Sciences Science::Physics::Optics and light Halide Perovskite Defects The previously developed bistable amphoteric native defect (BAND) model is used for a comprehensive explanation of the unique photophysical properties and for understanding the remarkable performance of perovskites as photovoltaic materials. It is shown that the amphoteric defects in donor (acceptor) configuration capture a fraction of photoexcited electrons (holes) dividing them into two groups: higher energy bright and lower energy dark electrons (holes). The spatial separation of the dark electrons and the dark holes and the k-space separation of the bright and the dark charge carriers reduce electron hole recombination rates, emulating the properties of an ideal photovoltaic material with a balanced, spatially separated transport of electrons and holes. The BAND model also offers a straightforward explanation for the exceptional insensitivity of the photovoltaic performance of polycrystalline perovskite films to structural and optical inhomogeneities. The blue-shifted radiative recombination of bright electrons and holes results in a large anti-Stokes effect that provides a quantitative explanation for the spectral dependence of the laser cooling effect measured in perovskite platelets. National Research Foundation (NRF) Accepted version This work (JWA, WW) was supported by the Singapore National Research Foundation through the Intra-CREATE Collaborative Grant NRF2018-ITC001-001. B. W. acknowledges the support from the National Natural Science Foundation of China (NFSC) (grant No. 51802331), Science and Technology Program of Guangzhou (No. 2019050001). T. C. S. acknowledges the support of Nanyang Technological University under its internal grant (M4082480); and the National Research Foundation (NRF) Singapore under its Competitive Research Program (NRF-CRP14-2014-03) and its NRF Investigatorship (NRF-NRFI-2018-04). 2020-12-21T09:17:30Z 2020-12-21T09:17:30Z 2020 Journal Article Walukiewicz, W., Wang, S., Wu, X., Li, R., Sherburne, M. P., Wu, B., ... Asta, M. D. (2020). The bright side and dark side of hybrid organic–inorganic perovskites. The Journal of Physical Chemistry C, 124(50), 27340–27355. doi:10.1021/acs.jpcc.0c08263 1932-7447 https://hdl.handle.net/10356/145440 10.1021/acs.jpcc.0c08263 50 124 27340–27355 27355 en M4082480 NRF-CRP14-2014-03 NRF-NRFI-2018-04 The Journal of Physical Chemistry C 10.21979/N9/9LBMRG This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcc.0c08263 application/pdf application/pdf |
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Science::Physics::Optics and light Halide Perovskite Defects Walukiewicz, Wladek Wang, Shu Wu, Xinchun Li, Rundong Sherburne, Matthew P. Wu, Bo Sum, Tze Chien Ager, Joel W. Asta, Mark D. The bright side and dark side of hybrid organic–inorganic perovskites |
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The previously developed bistable amphoteric native defect (BAND) model is used for a comprehensive explanation of the unique photophysical properties and for understanding the remarkable performance of perovskites as photovoltaic materials. It is shown that the amphoteric defects in donor (acceptor) configuration capture a fraction of photoexcited electrons (holes) dividing them into two groups: higher energy bright and lower energy dark electrons (holes). The spatial separation of the dark electrons and the dark holes and the k-space separation of the bright and the dark charge carriers reduce electron hole recombination rates, emulating the properties of an ideal photovoltaic material with a balanced, spatially separated transport of electrons and holes. The BAND model also offers a straightforward explanation for the exceptional insensitivity of the photovoltaic performance of polycrystalline perovskite films to structural and optical inhomogeneities. The blue-shifted radiative recombination of bright electrons and holes results in a large anti-Stokes effect that provides a quantitative explanation for the spectral dependence of the laser cooling effect measured in perovskite platelets. |
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School of Physical and Mathematical Sciences |
author_facet |
School of Physical and Mathematical Sciences Walukiewicz, Wladek Wang, Shu Wu, Xinchun Li, Rundong Sherburne, Matthew P. Wu, Bo Sum, Tze Chien Ager, Joel W. Asta, Mark D. |
format |
Article |
author |
Walukiewicz, Wladek Wang, Shu Wu, Xinchun Li, Rundong Sherburne, Matthew P. Wu, Bo Sum, Tze Chien Ager, Joel W. Asta, Mark D. |
author_sort |
Walukiewicz, Wladek |
title |
The bright side and dark side of hybrid organic–inorganic perovskites |
title_short |
The bright side and dark side of hybrid organic–inorganic perovskites |
title_full |
The bright side and dark side of hybrid organic–inorganic perovskites |
title_fullStr |
The bright side and dark side of hybrid organic–inorganic perovskites |
title_full_unstemmed |
The bright side and dark side of hybrid organic–inorganic perovskites |
title_sort |
bright side and dark side of hybrid organic–inorganic perovskites |
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2020 |
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https://hdl.handle.net/10356/145440 |
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1759858137898156032 |