Collision-induced light scattering from fluids composed of tetrahedral molecules. I

The collision-induced polarized and depolarized light scattered from fluids composed of tetrahedral molecules is examined. The correlation functions for the first-order term of the collision-induced rotational Raman effect proposed by Buckingham and Tabisz [21] are derived in the limit of binary interactions. They involve rotational correlation functions of the dipole-quadrupole polarizability, which for tetrahedral molecules is an irreducible third-rank tensor, and third-rank tensor correlation functions for relative translational motion. From a comparison of the frequency-dependent depolarization ratio of liquid carbon tetrachloride with the theoretical prediction it is concluded that also in liquids the collision-induced rotational Raman effect may contribute significantly to the depolarized spectrum for large frequency shifts.