Genuine Johari–Goldstein β-relaxations in glass-forming binary mixtures |
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Institution: | 1. Dipartimento di Fisica and INFM, Università di Pisa, Largo Pontecorvo 3, I-56127, Pisa, Italy;2. CNR-INFM, CRS SOFT, Piazzale Aldo Moro 2, I-00185 Roma, Italy;3. Naval Research Laboratory, Washington, DC 20375-5320, USA;4. Poly Lab-CNR, Largo B. Pontecorvo 3, 56127 Pisa, Italy;1. Université Lille 1, Villeneuve d’Ascq, France;2. Naval Research Laboratory, Washington, DC 20375-5320, USA |
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Abstract: | Broadband dielectric spectroscopy measurements were performed on glass-forming binary mixtures, composed of rigid polar molecules dissolved at low concentration in apolar viscous solvent (tristyrene). Dielectric spectra were dominated by the polar molecule contribution, so enabling the study of its dynamic behavior. A well resolved secondary relaxation, not attributable to internal degrees of freedom, was visible in both the liquid and glassy states: for its intermolecular nature, it can be called a ‘genuine’ Johari–Goldstein (JG) relaxation, in the sense that it is a local and non-cooperative process but entailing the motion of the molecule as a whole. Among our results, the following ones are noteworthy: (a) polar systems in the neat state showed an excess wing that became a well resolved JG-peak on mixing with the apolar solvent; (b) the time-scale distance between structural and JG loss peak increased with the apolar solvent fraction; (c) broader the structural loss peak was, larger was the separation in the frequency scale between structural and JG peak; (d) the JG relaxation time showed a non-Arrhenius temperature behavior above Tg, paralleling that of the structural relaxation time. All the results can be rationalized in the framework of Coupling Model. |
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