Abstract
Polarization-selective pump-probe and echo experiments on the OH vibration of HOD in ${\mathrm{D}}_{2}\mathrm{O}$ with $45\text{\ensuremath{-}}\text{femtosecond}$ (fs) infrared pulses are analyzed self-consistently to reveal the time scales for vibrational relaxation, dephasing, and molecular reorientation. Librational motion and hydrogen bond fluctuations on 50- and $180\text{\ensuremath{-}}\mathrm{fs}$ time scales precede picosecond collective reorganization.
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