Depolarized light scattering,flow birefringence and local order in molecular liquids

We propose a generalization of De Gennes' theory of flow birefringence 3] to the case of two distinct local anisotropy variables and also some extensions to the existing three variable theories of light scattering spectra. We show that the application of the theories with one or with two local anisotropy variables to analyse flow birefringence and light scattering spectra give numerically different results. We also show that it is possible to determinewhether the second local anisotropy variable is a primary or a secondary variable.

The VH and HH light scattering spectra of a number of symmetric top molecules are analysed. They show an unambiguous ‘shear mode coupling’ down to very small values of (q ²η/ρΦ). These results are discussed and compared to flow birefringence experiments in the light of our theoretical considerations. The three variable correction is shown to be small and within experimental error for all liquids studied except one (pyridine). The flow birefringence coefficient for CCl₄ is measured and found to be negative as predicted by our theory. Limitations to the formalism of generalized hydrodynamics are also discussed briefly.