Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond

TL;DR

This paper extends the Bethe-Salpeter equation to include phonon-induced dynamical screening, revealing its significant impact on exciton binding energies in halide perovskites and providing a predictive model for phonon screening effects in semiconductors.

Contribution

It introduces a generalized BSE framework incorporating phonon screening and derives a simple predictive expression for its effects based on material parameters.

Findings

Phonon screening significantly reduces exciton binding energies in lead halide perovskites.

A simple model predicts phonon screening effects using four key material parameters.

The approach clarifies the role of phonons in excitonic properties across semiconductors.

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 also 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 the importance of phonon screening effects 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, the static and optical dielectric constants, and the phonon frequency of the most strongly coupled LO phonon mode. This framework helps to elucidate the importance of phonon screening and its relation to excitonic properties in a broad class of semiconductors.