Abstract
It is shown that the intramolecular Fermi doublet {${\ensuremath{\nu}}_{1}$,2${\ensuremath{\nu}}_{2}$} in crystalline ${\mathrm{CO}}_{2}$ arising from resonant anharmonic coupling between a single-phonon state and a quasibound two-phonon state can be coherently driven and its dynamics determined by time-resolved nonlinear optical techniques. Coherence relaxation times for both components of the doublet are measured between 9 K and the fusion point (217 K). A mechanism for loss of coherence is proposed which involves modulation by low-lying intermolecular modes.
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