Spectral model of time-domain coherent anti-Stokes Raman scattering

TL;DR

This paper presents a spectral model for time-domain coherent anti-Stokes Raman scattering (CARS), linking it to the Yuratich equation and highlighting the influence of the probe laser's spectral envelope on CARS signals.

Contribution

It introduces a spectral model for time-domain CARS based on the Yuratich equation, providing analytical insights into probe spectral effects.

Findings

CARS time traces depend strongly on the probe laser spectral envelope.

Analytical expressions for CARS lineshapes are derived.

The model aligns with experimental results previously analyzed numerically.

Abstract

We show that the increasingly popular nonlinear optical technique of time-domain coherent anti-Stokes Raman scattering (CARS), which is usually understood in terms of the semiclassical time-dependent third-order polarization, can be equally explained in terms of the time-delayed version of the Yuratich equation so popular in traditional frequency-domain CARS. The method brings out the strong dependence of CARS time traces and time-delayed CARS lineshapes on the spectral envelope of the probe laser electric field. Examples are analytically shown for experimental results that are otherwise treated by means of numerical methods only.