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Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process

Photovoltaic devices based on metal halide perovskites are rapidly improving in efficiency. Once the Shockley–Queisser limit is reached, charge-carrier extraction will be limited only by radiative bimolecular recombination of electrons with holes. Yet, this fundamental process, and its link with mat...

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Autores principales: Davies, Christopher L., Filip, Marina R., Patel, Jay B., Crothers, Timothy W., Verdi, Carla, Wright, Adam D., Milot, Rebecca L., Giustino, Feliciano, Johnston, Michael B., Herz, Laura M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5773627/
https://www.ncbi.nlm.nih.gov/pubmed/29348550
http://dx.doi.org/10.1038/s41467-017-02670-2
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author Davies, Christopher L.
Filip, Marina R.
Patel, Jay B.
Crothers, Timothy W.
Verdi, Carla
Wright, Adam D.
Milot, Rebecca L.
Giustino, Feliciano
Johnston, Michael B.
Herz, Laura M.
author_facet Davies, Christopher L.
Filip, Marina R.
Patel, Jay B.
Crothers, Timothy W.
Verdi, Carla
Wright, Adam D.
Milot, Rebecca L.
Giustino, Feliciano
Johnston, Michael B.
Herz, Laura M.
author_sort Davies, Christopher L.
collection PubMed
description Photovoltaic devices based on metal halide perovskites are rapidly improving in efficiency. Once the Shockley–Queisser limit is reached, charge-carrier extraction will be limited only by radiative bimolecular recombination of electrons with holes. Yet, this fundamental process, and its link with material stoichiometry, is still poorly understood. Here we show that bimolecular charge-carrier recombination in methylammonium lead triiodide perovskite can be fully explained as the inverse process of absorption. By correctly accounting for contributions to the absorption from excitons and electron-hole continuum states, we are able to utilise the van Roosbroeck–Shockley relation to determine bimolecular recombination rate constants from absorption spectra. We show that the sharpening of photon, electron and hole distribution functions significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy. Our findings provide vital understanding of band-to-band recombination processes in this hybrid perovskite, which comprise direct, fully radiative transitions between thermalized electrons and holes.
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spelling pubmed-57736272018-01-23 Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process Davies, Christopher L. Filip, Marina R. Patel, Jay B. Crothers, Timothy W. Verdi, Carla Wright, Adam D. Milot, Rebecca L. Giustino, Feliciano Johnston, Michael B. Herz, Laura M. Nat Commun Article Photovoltaic devices based on metal halide perovskites are rapidly improving in efficiency. Once the Shockley–Queisser limit is reached, charge-carrier extraction will be limited only by radiative bimolecular recombination of electrons with holes. Yet, this fundamental process, and its link with material stoichiometry, is still poorly understood. Here we show that bimolecular charge-carrier recombination in methylammonium lead triiodide perovskite can be fully explained as the inverse process of absorption. By correctly accounting for contributions to the absorption from excitons and electron-hole continuum states, we are able to utilise the van Roosbroeck–Shockley relation to determine bimolecular recombination rate constants from absorption spectra. We show that the sharpening of photon, electron and hole distribution functions significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy. Our findings provide vital understanding of band-to-band recombination processes in this hybrid perovskite, which comprise direct, fully radiative transitions between thermalized electrons and holes. Nature Publishing Group UK 2018-01-18 /pmc/articles/PMC5773627/ /pubmed/29348550 http://dx.doi.org/10.1038/s41467-017-02670-2 Text en © The Author(s) 2018 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/.
spellingShingle Article
Davies, Christopher L.
Filip, Marina R.
Patel, Jay B.
Crothers, Timothy W.
Verdi, Carla
Wright, Adam D.
Milot, Rebecca L.
Giustino, Feliciano
Johnston, Michael B.
Herz, Laura M.
Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
title Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
title_full Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
title_fullStr Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
title_full_unstemmed Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
title_short Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
title_sort bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5773627/
https://www.ncbi.nlm.nih.gov/pubmed/29348550
http://dx.doi.org/10.1038/s41467-017-02670-2
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