Abstract

Coherent Raman scattering of delayed probing pulses after stimulated Raman excitation of molecular transitions is applied for a novel spectroscopy. Measuring the signal transient over long delay time intervals ≳ 10 -8 s numerical Fourier transformation yields precise spectroscopic information with a resolution ≲ 10 -3 cm -1. Experimental data are presented for the Q-band of the ν 1 vibration of CH 4 in the supersonic expansion. The potential of our Fourier transform Raman spectroscopy is demonstrated resolving the tensor splitting of the J = 2 transitions.

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