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

Christopher L. Davies, Marina R. Filip, Jay B. Patel, Timothy W. Crothers, Carla Verdi, Adam D. Wright, Rebecca L. Milot, Feliciano Giustino, Michael B. Johnston and Laura M. Herz ()
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Christopher L. Davies: University of Oxford, Clarendon Laboratory
Marina R. Filip: University of Oxford
Jay B. Patel: University of Oxford, Clarendon Laboratory
Timothy W. Crothers: University of Oxford, Clarendon Laboratory
Carla Verdi: University of Oxford
Adam D. Wright: University of Oxford, Clarendon Laboratory
Rebecca L. Milot: University of Oxford, Clarendon Laboratory
Feliciano Giustino: University of Oxford
Michael B. Johnston: University of Oxford, Clarendon Laboratory
Laura M. Herz: University of Oxford, Clarendon Laboratory

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-017-02670-2

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