Theory of resonant Raman scattering: Toward a comprehensive \textit{ab initio} description

TL;DR

This paper presents a fully quantum mechanical, first-principles theory of Raman scattering that incorporates many-body effects, aiming to enable comprehensive ab initio calculations of Raman spectra including excitonic and non-adiabatic phenomena.

Contribution

It introduces a general, practical framework for calculating Raman scattering rates from first principles using many-body perturbation theory and the Lehmann-Symanzik-Zimmermann reduction formula.

Findings

Derivation of a general expression for Raman scattering rate

Framework that includes excitonic effects

Method to incorporate non-adiabatic effects in Raman calculations

Abstract

We develop a general, fully quantum mechanical theory of Raman scattering from first principles in terms of many-body correlation functions. In order to arrive at expressions that are practically useful in the context of condensed matter physics, we adopt the Lehmann-Symanzik-Zimmermann reduction formula from high-energy physics and formulate in the modern language of many-body perturbation theory. This enables us to derive a general and practically useful expression for the Raman scattering rate in terms of quantities that can be computed \textit{ab initio}. Our work paves the way toward a comprehensive computational approach to the calculation of Raman spectra that goes beyond the current state of the art by capturing both excitonic and non-adiabatic effects.