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

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.