Polarization effects in time resolved incoherent anti‐Stokes Raman spectroscopy

Recently the anti‐Stokes spectroscopy after strong vibrational excitation via resonant absorption was rediscovered, for the study of population relaxation dynamics. A closer theoretical inspection of this experimental approach reveals that properly chosen polarization conditions allow the study of molecular reorientational motion. Furthermore the sign of a/γ (the invariants of the Raman polarizability tensor) can be determined. Experimental data for chlorinated alkanes will be presented.