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Title: Unexpectedly Strong Auger Recombination in Halide Perovskites

Abstract

The emergence of halide perovskites for photovoltaic applications has triggered great interest in these materials for solid-state light emission. Higher order electron–hole recombination processes can critically affect the efficiency of such devices. In the present work, the Auger recombination coefficients are computed in the prototypical halide perovskite, CH 3NH 3PbI 3 (MAPbI 3), using first-principles calculations. It is demonstrated that Auger recombination is responsible for the exceptionally high third-order recombination coefficient observed in experiment. The large Auger coefficient is attributed to a coincidental resonance between the bandgap and interband transitions to a complex of higher-lying conduction bands. It is also found that the distortions of PbI 6 octahedra contribute significantly to the high Auger coefficient, offering potential avenues for materials design.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [2]
  1. Univ. of California, Santa Barbara, CA (United States). Dept. of Physics
  2. Univ. of California, Santa Barbara, CA (United States). Materials Dept.
  3. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States); Univ. of California, Santa Barbara, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1543467
Alternate Identifier(s):
OSTI ID: 1472176
Grant/Contract Number:  
AC02-05CH11231; SC0010689; AC0205CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 30; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; chemistry; energy & fuels; materials science; physics; Auger recombination; DFT calculations; halide perovskite; light-emitting diode

Citation Formats

Shen, Jimmy-Xuan, Zhang, Xie, Das, Suvadip, Kioupakis, Emmanouil, and Van de Walle, Chris G. Unexpectedly Strong Auger Recombination in Halide Perovskites. United States: N. p., 2018. Web. doi:10.1002/aenm.201801027.
Shen, Jimmy-Xuan, Zhang, Xie, Das, Suvadip, Kioupakis, Emmanouil, & Van de Walle, Chris G. Unexpectedly Strong Auger Recombination in Halide Perovskites. United States. doi:10.1002/aenm.201801027.
Shen, Jimmy-Xuan, Zhang, Xie, Das, Suvadip, Kioupakis, Emmanouil, and Van de Walle, Chris G. Wed . "Unexpectedly Strong Auger Recombination in Halide Perovskites". United States. doi:10.1002/aenm.201801027. https://www.osti.gov/servlets/purl/1543467.
@article{osti_1543467,
title = {Unexpectedly Strong Auger Recombination in Halide Perovskites},
author = {Shen, Jimmy-Xuan and Zhang, Xie and Das, Suvadip and Kioupakis, Emmanouil and Van de Walle, Chris G.},
abstractNote = {The emergence of halide perovskites for photovoltaic applications has triggered great interest in these materials for solid-state light emission. Higher order electron–hole recombination processes can critically affect the efficiency of such devices. In the present work, the Auger recombination coefficients are computed in the prototypical halide perovskite, CH3NH3PbI3 (MAPbI3), using first-principles calculations. It is demonstrated that Auger recombination is responsible for the exceptionally high third-order recombination coefficient observed in experiment. The large Auger coefficient is attributed to a coincidental resonance between the bandgap and interband transitions to a complex of higher-lying conduction bands. It is also found that the distortions of PbI6 octahedra contribute significantly to the high Auger coefficient, offering potential avenues for materials design.},
doi = {10.1002/aenm.201801027},
journal = {Advanced Energy Materials},
number = 30,
volume = 8,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

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Cited by: 60 works
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Figures / Tables:

Figure 1 Figure 1: 12-atom unit cell of MAPbI3 where the I atoms are at the ideal face-center positions. The arrows indicate displacement of the I atoms upon relaxation within a cubic cell shape. For clarity the length of the displacement vector is enhanced by a factor of five.

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.