Abstract
We continue our previous examination of the fate of individual rotational quantum states in liquids by an analysis of the rotational Raman spectrum of solutions of H2 and D2 in Ar(l). Rewriting the conventional Kubo treatment allows us to show how the character of the spectrum is an immediate consequence of the rotational friction felt by the solutes. On evaluating that friction via classical molecular dynamics we find that the spectra should consist of well-resolved, homogeneously broadened lines, reflecting the picosecond-long dephasing times. We find, in particular, that the rotational states in H2 should relax predominantly by pure dephasing, whereas D2, with its smaller rotational quanta, should exhibit significant energy relaxation as well. The linewidths predicted for H2 are nicely in accord with those computed by more involved nonadiabatic, mixed quantum-classical simulations.
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