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, 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.
- Authors:
-
[1];
[2];
[3];
[3];
[2]
- Univ. of California, Santa Barbara, CA (United States). Dept. of Physics
- Univ. of California, Santa Barbara, CA (United States). Materials Dept.
- Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (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). Scientific User Facilities Division
- OSTI Identifier:
- 1543467
- Alternate Identifier(s):
- OSTI ID: 1472176
- Grant/Contract Number:
- AC02-05CH11231; SC0010689; DE‐SC0010689; DE‐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. https://doi.org/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. https://doi.org/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. https://doi.org/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}
}
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Figures / Tables:
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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Works referencing / citing this record:
First‐Principles Simulation of Carrier Recombination Mechanisms in Halide Perovskites
journal, April 2020
- Zhang, Xie; Shen, Jimmy‐Xuan; Van de Walle, Chris G.
- Advanced Energy Materials, Vol. 10, Issue 13
Phase control of quasi-2D perovskites and improved light-emitting performance by excess organic cations and nanoparticle intercalation
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Highly stable enhanced near-infrared amplified spontaneous emission in solution-processed perovskite films by employing polymer and gold nanorods
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.