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

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 ^[3]; Van de Walle, Chris G. ^[3]

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

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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

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

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

OSTI ID:: 1468978

Journal Information:: ACS Energy Letters, Journal Name: 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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