Light scattering spectroscopy of the liquid-glass transition : comparison with idealized and extended mode coupling theory
Light scattering experiments were performed on several fragile glass-forming materials at temperatures ranging from above the melting temperature T, to below the calorimetric glass transition temperature T, in the frequency range 0.2 GHz to 4000 GHz. The experimental susceptibility spectra x”(o) exhibit both the form and the scaling properties predicted by the idealized mode coupling theory. In particular, the scaling frequency o, was found to obey the power law w, a 1 T T,_jzO for three different materials, confirming the predicted “critical slowing down” as T+ Tc from either above or below. At low frequencies and temperatures the spectra deviate from the predictions due to the neglect of ergodicity-restoring activated transport (hopping) processes. We have therefore reanalyzed the data using the extended version of the theory, including activated transport.
Light scattering spectroscopy of the liquid-glass transition
Supercooled liquids approaching the liquid-glass transition exhibit unusual properties associated with structural relaxation. The mode-coupling theory (MCT) of supercooled liquid dynamics shows that non-linear interactions among density fluctuation modes can produce effects resembling these observations. MCT produces detailed predictions for the dynamics of density fluctuations in supercooled liquids, including a crossover from liquid to glassy dynamics at a critical temperature Tc. Recent light scattering studies of supercooled CaKNO3 are described that have provided detailed tests of MCT both above and below Tc, including a cusp in the scaling time at Tc=105+or-5 degrees C. These experiments are reviewed, and comparisons with both the idealized and extended versions of MCT are described.
Observation of Scaling Behaviour of Dynamic Correlations near Liquid-Glass Transition
A time-of-flight inelastic neutron scattering study of Ca0.4K0.6(NO3)1.4 of the temperature dependence of the dynamic structure factor revealed a clear frequency-independent signature of the glass transition at the conventional transition temperature Tg. Above Tg the data combined with our previous neutron spin echo results display two relaxation processes at well-separated frequencies. The faster process was now found to be consistent with a scaling behaviour corresponding to a critical-type slowing-down when approaching a certain temperature T0, as predicted by recent mode coupling theories. The variation of various properties consistently points to a critical temperature T0 of about 30 K above Tg = 333 K.