Dynamically asymmetric binary glass formers studied by dielectric and NMR spectroscopy

2019 
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/T iso 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 ( 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 T g .
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