Abstract
A femtosecond optical Kerr gate is used for first time to experimentally study the temporal behavior of the molecular interactions of carbon disulfide (CS2) vapor in comparison to its liquid state. This Kerr effect is observed due to the optical birefringence induced in a CS2 sample. Results show that the Kerr relaxation time in the vapor state is faster than in the liquid state, with an overall exponential fit of 0.8 ps molecular relaxation time versus 1.7 ps, respectively. A faster relaxation decay time is observed for the first time in free CS2 molecules, this is attributed to fewer neighboring intermolecular interactions, which results in a lower local viscosity in the vapor compared to the liquid state. Fitting the temporal response of the Kerr vapor signal to individual components of n2 arising from the ultrafast and fast components yields two main decay times: τultrfast = 126 fs and τfast = 530 fs molecular relaxation times, one which agrees with the Debye equation for the air viscosity (associated to the free rotation in air) giving 126 fs and the other is approximately close to the translational diffusion equation producing 530 fs, respectively. In the liquid state, fitting yields three main components: τultrfast = 50 as, τfast = 500 fs, and τslow = 1.5 ps, overall, the tail fits the 1.7 ps molecular relaxation time.
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