First-Principles Analysis of Radiative Recombination in Lead-Halide Perovskites

Zhang, Xie; Shen, Jimmy-Xuan; Wang, Wennie; Van de Walle, Chris G.

doi:10.1021/acsenergylett.8b01297

Title: First-Principles Analysis of Radiative Recombination in Lead-Halide Perovskites

Journal Article · Wed Sep 05 00:00:00 EDT 2018 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.8b01297· OSTI ID:1468978

Zhang, Xie ^[1]; Shen, Jimmy-Xuan ^[2]; Wang, Wennie ^[1]; Van de Walle, Chris G. ^[1]

Univ. of California, Santa Barbara, CA (United States). Materials Dept.
Univ. of California, Santa Barbara, CA (United States). Dept. of Physics

Slow radiative recombination due to a slightly indirect band gap has been proposed to explain the high efficiency of lead-halide perovskite solar cells. In this work, we calculate the radiative recombination rate from first principles for the prototypical lead-halide perovskite, MAPbI₃ (MA=CH₃NH₃). Since the structure is dynamic, with the MA molecule rotating even at room temperature, we determine the momentum mismatch between the band edges as a function of the orientation of the MA molecule. Our results demonstrate that the indirect nature of the band gap suppresses the radiative recombination rate by less than a factor of two, and that the radiative recombination coefficient is as high as in traditional direct-gap semiconductors. Our study provides a rigorous assessment of the radiative recombination mechanisms and their relation to the high efficiency of lead-halide perovskite solar cells, and will provide a sound basis for accurate modeling.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Grant/Contract Number:: SC0010689; AC02-05CH11231

OSTI ID:: 1468978

Journal Information:: ACS Energy Letters, Vol. 3; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 56 works

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