Abstract
Using the polarized and depolarized scattering geometry we studied the concentration dependence of the isotropic and anisotropic Raman spectra of the symmetric stretching mode v 1 of CS2 in liquid mixtures with CCl4 at 25°C. The vibrational relaxation of the v 1 mode can be characterized as a pure dephasing process in the fast modulation regime over the whole concentration range. We discuss orientational correlation functions and correlation times τor indicating a diffusional tumbling motion of the symmetry axis. Testing the most relevant hydrodynamic models we found a strong deviation from linearity of τor against η/T. The orientational diffusion behaviour may be characterized by the transition from the hydrodynamic to the non-hydrodynamic or the so-called sub slip boundary condition.
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