Spin–Orbit Interactions Greatly Accelerate Nonradiative Dynamics in Lead Halide Perovskites
Abstract
In this study, we study the role of spin–orbit coupling (SOC) in nonradiative relaxation of hot electrons and holes in methylammonium lead perovskite, MAPbI3. For this purpose, we have developed the nonadiabatic molecular dynamics method with two-component spinor wave functions that are solutions of the relativistic Kohn–Sham (KS) equations. We find that SOC enhances contributions of Pb(px) and Pb(py) orbitals to the conduction and valence bands. As a result, the KS orbitals become more sensitive to nuclear motions, leading to the increased nonadiabatic couplings. Consequently, SOC greatly speeds up the electron and hole relaxation, making the computed relaxation time scales consistent with available experiments. Furthermore, we suggest that the fast hot carrier relaxation facilitated by the SOC allows rapid transition into the long-lived triplet state that extends charge-carrier lifetime and helps achieve high-efficiency perovskite solar cells.
- Authors:
-
[1];
[2];
[3];
[4]
- Hunan Agricultural Univ., Changsha (People's Republic of China)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of Southern California, Los Angeles, CA (United States)
- Univ. at Buffalo, The State Univ. of New York, Buffalo, NY (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1480032
- Report Number(s):
- LA-UR-18-26702
Journal ID: ISSN 2380-8195
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Energy Letters
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Material Science
Citation Formats
Li, Wei, Zhou, Liujiang, Prezhdo, Oleg V., and Akimov, Alexey V. Spin–Orbit Interactions Greatly Accelerate Nonradiative Dynamics in Lead Halide Perovskites. United States: N. p., 2018.
Web. doi:10.1021/acsenergylett.8b01226.
Li, Wei, Zhou, Liujiang, Prezhdo, Oleg V., & Akimov, Alexey V. Spin–Orbit Interactions Greatly Accelerate Nonradiative Dynamics in Lead Halide Perovskites. United States. https://doi.org/10.1021/acsenergylett.8b01226
Li, Wei, Zhou, Liujiang, Prezhdo, Oleg V., and Akimov, Alexey V. Thu .
"Spin–Orbit Interactions Greatly Accelerate Nonradiative Dynamics in Lead Halide Perovskites". United States. https://doi.org/10.1021/acsenergylett.8b01226. https://www.osti.gov/servlets/purl/1480032.
@article{osti_1480032,
title = {Spin–Orbit Interactions Greatly Accelerate Nonradiative Dynamics in Lead Halide Perovskites},
author = {Li, Wei and Zhou, Liujiang and Prezhdo, Oleg V. and Akimov, Alexey V.},
abstractNote = {In this study, we study the role of spin–orbit coupling (SOC) in nonradiative relaxation of hot electrons and holes in methylammonium lead perovskite, MAPbI3. For this purpose, we have developed the nonadiabatic molecular dynamics method with two-component spinor wave functions that are solutions of the relativistic Kohn–Sham (KS) equations. We find that SOC enhances contributions of Pb(px) and Pb(py) orbitals to the conduction and valence bands. As a result, the KS orbitals become more sensitive to nuclear motions, leading to the increased nonadiabatic couplings. Consequently, SOC greatly speeds up the electron and hole relaxation, making the computed relaxation time scales consistent with available experiments. Furthermore, we suggest that the fast hot carrier relaxation facilitated by the SOC allows rapid transition into the long-lived triplet state that extends charge-carrier lifetime and helps achieve high-efficiency perovskite solar cells.},
doi = {10.1021/acsenergylett.8b01226},
journal = {ACS Energy Letters},
number = 9,
volume = 3,
place = {United States},
year = {Thu Aug 16 00:00:00 EDT 2018},
month = {Thu Aug 16 00:00:00 EDT 2018}
}
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