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:
-
- Univ. of California, Santa Barbara, CA (United States). Materials Dept.
- 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. doi: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 = {Wed Sep 05 00:00:00 EDT 2018},
month = {Wed Sep 05 00:00:00 EDT 2018}
}
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