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

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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)

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.

Suggested Citation

  • 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 & Laura M. Herz, 2018. "Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-017-02670-2
    DOI: 10.1038/s41467-017-02670-2
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    Cited by:

    1. Mingcong Wang & Yajun Gao & Kai Wang & Jiang Liu & Stefaan De Wolf & Frédéric Laquai, 2022. "Photo-induced enhancement of lattice fluctuations in metal-halide perovskites," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Jongchul Lim & Manuel Kober-Czerny & Yen-Hung Lin & James M. Ball & Nobuya Sakai & Elisabeth A. Duijnstee & Min Ji Hong & John G. Labram & Bernard Wenger & Henry J. Snaith, 2022. "Long-range charge carrier mobility in metal halide perovskite thin-films and single crystals via transient photo-conductivity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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