Picosecond pump–probe and polarization techniques in supersonic molecular beams: Measurement of ultrafast vibrational-rotational dephasing and coherence

Observation of picosecond transients in supersonic molecular beams of stilbene and aniline is reported. Pump probe and polarization techniques are employed. The pump laser pulse exciting an optically active mode and a delayed pulse probing this population as a function of the delay time. Data on stilbene and aniline at vibrational and rotational temperatures of <10 and <5 K are reported.(AIP)