Power dependence of Klyshko's Stokes-anti-Stokes correlation in the inelastic scattering of light

TL;DR

This paper presents a theoretical model describing how the correlation between Stokes and anti-Stokes scattering components varies with excitation power, affecting phonon statistics and temperature measurements in materials like diamond and graphene.

Contribution

It introduces a new effective Hamiltonian model that accounts for Stokes-anti-Stokes correlation dependence on power, extending the understanding of inelastic light scattering beyond traditional Bose-Einstein statistics.

Findings

Correlation effects are significant in low-dimensional systems under resonance.

The model fits experimental data for diamond and graphene.

It predicts phonon conversion into heat or light based on coupling constants.

Abstract

The Stokes and anti-Stokes components in the inelastic scattering of light are related to phonon statistics and have been broadly used to measure temperature and phonon lifetimes in different materials. However, correlation between the components are expected to change the Stokes/anti-Stokes intensity ratio, imposing corrections to the broadly used Bose-Einstein statistics. Here the excitation power dependence of these scattering processes is theoretically described by an effective Hamiltonian that includes correlation between the Stokes and the anti-Stokes events. The model is used to fit available experimental results in three-dimensional diamond and two-dimensional graphene, showing that the phenomenon can significantly increase in the low-dimensional system under specific resonance conditions. By setting the scientific basis for the Stokes-anti-Stokes correlated phenomenon, the use of the Bose-Einstein population function for reasoning the inelastic scattering is generalized, providing a model to predict the conversion of optical phonons into heat or light, according to coupling constants and decay rates. The model applies to inelastic scattering in general.