Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond
Abstract
The ab initio Bethe-Salpeter equation (BSE) approach, an established method for the study of excitons in materials, is typically solved in a limit where only static screening from electrons is captured. Here, we generalize this framework to include dynamical screening from phonons at lowest order in the electron-phonon interaction. We apply this generalized BSE approach to a series of inorganic lead halide perovskites, CsPbX3, with X=Cl, Br, and I. We find that inclusion of screening from phonons significantly reduces the computed exciton binding energies of these systems. By deriving a simple expression for phonon screening effects, we reveal general trends for their importance in semiconductors and insulators, based on a hydrogenic exciton model. We demonstrate that the magnitude of the phonon screening correction in isotropic materials can be reliably predicted using four material specific parameters: the reduced effective mass, static and optical dielectric constants, and frequency of the most strongly coupled longitudinal-optical phonon mode. Finally, this framework helps to elucidate the importance of phonon screening and its relation to excitonic properties in a broad class of semiconductors.
- Authors:
-
- Univ. of Oxford (United Kingdom); Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC)
- OSTI Identifier:
- 1821153
- Grant/Contract Number:
- AC02-05CH11231; TG-DMR190070; V010840/1
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 127; Journal Issue: 6; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; dielectric properties; excitons; optical phonons; spin-orbit coupling; semiconductor compounds; ab initio calculations; density functional calculations
Citation Formats
Filip, Marina R., Haber, Jonah B., and Neaton, Jeffrey B. Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond. United States: N. p., 2021.
Web. doi:10.1103/physrevlett.127.067401.
Filip, Marina R., Haber, Jonah B., & Neaton, Jeffrey B. Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond. United States. https://doi.org/10.1103/physrevlett.127.067401
Filip, Marina R., Haber, Jonah B., and Neaton, Jeffrey B. Thu .
"Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond". United States. https://doi.org/10.1103/physrevlett.127.067401. https://www.osti.gov/servlets/purl/1821153.
@article{osti_1821153,
title = {Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond},
author = {Filip, Marina R. and Haber, Jonah B. and Neaton, Jeffrey B.},
abstractNote = {The ab initio Bethe-Salpeter equation (BSE) approach, an established method for the study of excitons in materials, is typically solved in a limit where only static screening from electrons is captured. Here, we generalize this framework to include dynamical screening from phonons at lowest order in the electron-phonon interaction. We apply this generalized BSE approach to a series of inorganic lead halide perovskites, CsPbX3, with X=Cl, Br, and I. We find that inclusion of screening from phonons significantly reduces the computed exciton binding energies of these systems. By deriving a simple expression for phonon screening effects, we reveal general trends for their importance in semiconductors and insulators, based on a hydrogenic exciton model. We demonstrate that the magnitude of the phonon screening correction in isotropic materials can be reliably predicted using four material specific parameters: the reduced effective mass, static and optical dielectric constants, and frequency of the most strongly coupled longitudinal-optical phonon mode. Finally, this framework helps to elucidate the importance of phonon screening and its relation to excitonic properties in a broad class of semiconductors.},
doi = {10.1103/physrevlett.127.067401},
journal = {Physical Review Letters},
number = 6,
volume = 127,
place = {United States},
year = {Thu Aug 05 00:00:00 EDT 2021},
month = {Thu Aug 05 00:00:00 EDT 2021}
}
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