Abstract:
: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.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Davies CL,Filip MR,Patel JB,Crothers TW,Verdi C,Wright AD,Milot RL,Giustino F,Johnston MB,Herz LMdoi
10.1038/s41467-017-02670-2subject
Has Abstractpub_date
2018-01-18 00:00:00pages
293issue
1issn
2041-1723pii
10.1038/s41467-017-02670-2journal_volume
9pub_type
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