Abstract
Femtosecond IR and Raman techniques are compared with respect to their abilities to monitor vibrational relaxation following ultrafast internal conversion. The study was performed on para-nitroaniline which undergoes sub-picosecond internal conversion to the ground state populating a variety of vibrational modes. The NO 2 stretch vibration at 1315 cm −1 responds to the excitation by a strong red shift, visible in transient IR and Raman experiments. It is due to the off-diagonal anharmonic coupling with other modes. The population of the NO 2 stretch mode itself can only be observed in the (anti-Stokes) Raman spectrum, whereas IR spectroscopy is superior in detecting the coupling induced shift.
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