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Overtone Vibrational Dephasing in Liquids Studied by Femtosecond Fifth-Order Nonlinear Spectroscopy

1996; American Physical Society; Volume: 76; Issue: 6 Linguagem: Inglês

10.1103/physrevlett.76.987

1092-0145

Keisuke Tominaga, Keitaro Yoshihara,

Photosynthetic Processes and Mechanisms

We have directly observed vibrational dephasing of the first overtone bands in liquids by femtosecond fifth-order nonlinear spectroscopy for the first time to our knowledge. The overtone and fundamental dephasing processes have been studied for the C-D stretching of CDC${\mathrm{l}}_{3}$ and the sym-methyl stretching of C${\mathrm{D}}_{3}$I in neat liquid and in its binary mixture with CHC${\mathrm{l}}_{3}$. Simulations based on simple stochastic theory or perturbation theory for a harmonic oscillator do not explain both the overtone and fundamental dephasing simultaneously.