Generation of Multiple Phase-Locked Stokes and Anti-Stokes Components in an Impulsively Excited Raman Medium

Abstract

We report on the observation of a highly efficient transformation of laser radiation into higher-order Stokes and anti-Stokes components in impulsively vibrationally excited gaseous S${\mathrm{F}}_{6}$. The specific (Bessel-like) behavior of their intensity with the gas pressure reveals the mutual coherence of the generated frequencies. We propose this new regime of Raman frequency conversion for generation of sub-fs pulses.