Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond

Filip, Marina R.; Haber, Jonah B.; Neaton, Jeffrey B.

doi:10.1103/physrevlett.127.067401

Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond

Journal Article · Thu Aug 05 00:00:00 EDT 2021 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.127.067401· OSTI ID:1821153

Filip, Marina R. ^[1]; Haber, Jonah B. ^[2]; Neaton, Jeffrey B. ^[3]

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1821153

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 6 Vol. 127; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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