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

Abstract

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.

Authors:
 [1];  [2];  [1];  [1]
  1. Univ. of California, Santa Barbara, CA (United States). Materials Dept.
  2. Univ. of California, Santa Barbara, CA (United States). Dept. of Physics
Publication Date:
Research Org.:
Univ. of California, Santa Barbara, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Contributing Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
OSTI Identifier:
1468978
Grant/Contract Number:  
SC0010689; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; radiative recombination; hybrid perovskites; solar cells; first-principles calculations

Citation Formats

Zhang, Xie, Shen, Jimmy-Xuan, Wang, Wennie, and Van de Walle, Chris G. First-Principles Analysis of Radiative Recombination in Lead-Halide Perovskites. United States: N. p., 2018. Web. https://doi.org/10.1021/acsenergylett.8b01297.
Zhang, Xie, Shen, Jimmy-Xuan, Wang, Wennie, & Van de Walle, Chris G. First-Principles Analysis of Radiative Recombination in Lead-Halide Perovskites. United States. https://doi.org/10.1021/acsenergylett.8b01297
Zhang, Xie, Shen, Jimmy-Xuan, Wang, Wennie, and Van de Walle, Chris G. Wed . "First-Principles Analysis of Radiative Recombination in Lead-Halide Perovskites". United States. https://doi.org/10.1021/acsenergylett.8b01297. https://www.osti.gov/servlets/purl/1468978.
@article{osti_1468978,
title = {First-Principles Analysis of Radiative Recombination in Lead-Halide Perovskites},
author = {Zhang, Xie and Shen, Jimmy-Xuan and Wang, Wennie and Van de Walle, Chris G.},
abstractNote = {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.},
doi = {10.1021/acsenergylett.8b01297},
journal = {ACS Energy Letters},
number = ,
volume = 3,
place = {United States},
year = {2018},
month = {9}
}

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Cited by: 13 works
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