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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Main Authors: Walukiewicz, Wladek, Wang, Shu, Wu, Xinchun, Li, Rundong, Sherburne, Matthew P., Wu, Bo, Sum, Tze Chien, Ager, Joel W., Asta, Mark D.
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2020
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Online Access:https://hdl.handle.net/10356/145440
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Institution: Nanyang Technological University
Language: English
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spelling 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
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Physics::Optics and light
Halide Perovskite
Defects
spellingShingle 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
description 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.
author2 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
publishDate 2020
url https://hdl.handle.net/10356/145440
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