Journal of Chemical Physics, Vol.106, No.20, 8401-8408, 1997
Depolarized Dynamic Light-Scattering from 3 Low-Molecular-Weight Glass-Forming Liquids - A Test of the Scattering Mechanism
Depolarized dynamic light scattering (DDLS) experiments are performed on the glass forming materials ortho terphenyl (OTP), bis-methyl-methoxy-phenyl-cyclohexane (BMMPC), and bis-methyl-phenyl-cyclohexane (BMPC). Depolarized spectra are obtained for the bulk liquids and for solutions of varying concentration in CCl4. Effective optical anisotropies of the molecules are obtained from the solution spectra. A detailed analysis of the DDLS spectra, as well asa comparison with the results of quasielastic neutron scattering (QENS) experiments, indicates that the DDLS spectra in the bulk liquids result from at least two physical mechanisms : (i) The low frequency part of the spectrum, in the frequency range of the ct peak, arises mainly from the molecular reorientation mechanism. The integrated intensity of this contribution is proportional to the square of the effective molecular anisotropy. (ii) At higher frequencies (but still below the Boson peak), the predominant contribution to the DDLS spectrum arises from interaction-induced scattering. The intensity of this contribution increases with increasing temperature (decreasing density) in the way expected for the cancellation effect. The implications of these results for the comparison of DDLS and QENS experiments and for the comparison of the data to the predictions of mode coupling theories of glass forming liquids are discussed.
Keywords:RAYLEIGH-SCATTERING;STRUCTURAL RELAXATION;SUPERCOOLED LIQUIDS;RAMAN-SCATTERING;ALPHA-RELAXATION;SCALING BEHAVIOR;BETA-RELAXATION;ORTHO-TERPHENYL;TRANSITION;NEUTRON