Dynamically asymmetric binary glass formers studied by dielectric and NMR spectroscopy.

Abstract

We investigate the component dynamics in asymmetric binary glass formers. Focusing on the dielectric spectra of the high-Tg components m-tricresyl phosphate and quinaldine mixed with toluene as low-Tg component, the broadend spectra cannot be described by Kohlrausch or Cole-Davidson (CD) functions. Instead, we apply a generalized CD function which allows to control the width of the susceptibility independently of its high-frequency flank. The spectra show a common broadening and failure of the frequency-temperature superposition with increasing toluene concentration. This is confirmed by stimulated echo experiments showing an increased stretching of the probed orientational correlation function. In analogy to the definition of Tg, we consider "isodynamic points". For each component, a different but linear concentration dependence of 1/Tiso is revealed, indicating different time scales. Qualitativly, we do not find significant differences for the present mixtures with Tg-contrasts of 63-89K compared to those with larger Tg-contrast ( [Formula: see text] K): Whereas the high-Tg component shows relaxation features similar to those of neat glass formers, yet, with "atypical" weak relaxation broadening, the faster low-Tg component displays pronounced dynamic heterogeneities. This is supported by scrutinizing NMR relaxation data of several mixtures investigated previously as a function of concentration. A universal evolution of the dynamics of the high-Tg as well as the low-Tg component is suggested for mixtures with high [Formula: see text]Tg .