We report on the observation of a Raman frequency conversion mechanism different from the usual Stokes (anti-Stokes) stimulated process. A continuous down-shift of laser pulse frequency was measured for sufficiently short (≤40fs) pulses propagating in gaseous SF₆. We attribute this behavior to the extremely nonstationary nuclear response of SF₆ molecules to the light field with a duration shorter than the period of the Raman-active vibration.
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Korn et al. (1998) studied this question.
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