Study of intermolecular interactions in liquid nitrobenzene by depolarized hyper-Rayleigh scattering

We employed depolarized hyper-Rayleigh scattering (HRS) to investigate the intermolecular interactions in liquid nitrobenzene. By comparing the depolarization ratios of the second-harmonic scattered light from neat nitrobenzene and mixtures of nitrobenzene and methanol of varying mixing ratios, we demonstrated the existence of a coherent component of HRS in liquid nitrobenzene. The coherent component was found to essentially disappear at a sufficiently high dilution of the nitrobenzene liquid. We also observed that both localized orientational correlation and delocalized libron excitation contribute to coherent HRS in liquid nitrobenzene. The delocalized contribution to coherent HRS was found to diminish much more readily with the introduction of interstitial foreign molecules than the localized contribution.