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...
| Main Authors: | , , , , , , , , , |
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| Format: | Journal article |
| Language: | English |
| Published: |
Springer Nature
2018
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| _version_ | 1797054711426187264 |
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| author | Davies, C Filip, M Patel, J Crothers, T Verdi, C Wright, A Milot, R Giustino, F Johnston, M Herz, L |
| author_facet | Davies, C Filip, M Patel, J Crothers, T Verdi, C Wright, A Milot, R Giustino, F Johnston, M Herz, L |
| author_sort | Davies, C |
| collection | OXFORD |
| 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. |
| first_indexed | 2024-03-06T19:01:03Z |
| format | Journal article |
| id | oxford-uuid:138af7dc-9c0f-432d-b54f-bd35b3c23be6 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T19:01:03Z |
| publishDate | 2018 |
| publisher | Springer Nature |
| record_format | dspace |
| spelling | oxford-uuid:138af7dc-9c0f-432d-b54f-bd35b3c23be62022-03-26T10:14:27ZBimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption processJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:138af7dc-9c0f-432d-b54f-bd35b3c23be6EnglishSymplectic Elements at OxfordSpringer Nature2018Davies, CFilip, MPatel, JCrothers, TVerdi, CWright, AMilot, RGiustino, FJohnston, MHerz, LPhotovoltaic 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. |
| spellingShingle | Davies, C Filip, M Patel, J Crothers, T Verdi, C Wright, A Milot, R Giustino, F Johnston, M Herz, L 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 |
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