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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Published inNature communications Vol. 9; no. 1; pp. 293 - 9
Main Authors 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
Format Journal Article
LanguageEnglish
Published England Nature Publishing Group 18.01.2018
Nature Publishing Group UK
Nature Portfolio
Subjects
Absorption
Absorption spectra
Carrier recombination
Current carriers
Distribution functions
Electrons
Excitons
Hole distribution
Lead
Perovskites
Photovoltaic cells
Photovoltaics
Rate constants
Recombination
Sharpening
Solar cells
Spectroscopy
Spectrum analysis
Stoichiometry
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Summary: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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ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-017-02670-2