Abstract
The authors propose the application of time-resolved nonlinear optical techniques to the selective study of the dynamics of vibrational overtones and two-phonon states in condensed media. They present the first experimental demonstration of picosecond coherent anti-Stokes higher-order Raman scattering on the first overtone and the bound two-phonon state of the ${\ensuremath{\nu}}_{2}$ mode in liquid and crystalline C${\mathrm{S}}_{2}$, respectively, and describe its dynamics and deexcitation channel in terms of a simple effective Hamiltonian.
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