Sensitivity of coherent anti-Stokes Raman lineshape to time asymmetry of laser pulses

TL;DR

This paper demonstrates that the lineshape in coherent anti-Stokes Raman scattering is significantly affected by the time asymmetry of laser pulses, leading to potential line narrowing effects not predicted by traditional models.

Contribution

It introduces a new analysis considering laser pulse asymmetry, revealing deviations from known spectral profiles and suggesting a line narrowing phenomenon.

Findings

Lineshape deviations due to pulse asymmetry

Potential line narrowing effect observed

Implications for spectral analysis accuracy

Abstract

We show that coherent anti-Stokes Raman lineshapes do not follow known spectral profiles if the time asymmetry of realistic laser pulses is taken into account. Examples are given for nanosecond and picosecond laser pulses commonly employed in frequency-resolved coherent anti-Stokes Raman scattering. More remarkably, the analysis suggests an effect of line narrowing in comparison to the customary approach, based primarily on the Voigt lineshape.