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Physical Review E

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Transition from single-molecule to cooperative dynamics in a simple glass former: Raman line-shape analysis

N. V. Surovtsev, S. V. Adichtchev, and V. K. Malinovsky

Institute of Automation and Electrometry, Russian Academy of Sciences, Novosibirsk, 630090, Russia

Phys. Rev. E 76, 021502 – Published 14 August, 2007

DOI: https://doi.org/10.1103/PhysRevE.76.021502

Abstract

Parameters for orientational and inhomogeneous broadening are found from the line shape analysis of the Raman spectrum of the glass former $α$ -picoline during cooling from low-viscous to glassy state. The orientational phase loss time $τ_{OPL}$ , extracted from the analysis, coincides with the $α$ relaxation time at $T > T_{A}$ , where $T_{A}$ is the temperature of transition from an Arrhenius-like to a non-Arrhenius behavior for the $α$ -relaxation time dependence on temperature. At lower temperatures $τ_{OPL} (T)$ continues the Arrhenius behavior, in contrast to the $α$ -relaxation time. The width of inhomogeneous broadening of the Raman line decreases noticeably as temperature increases in the temperature range $T_{g} < T < T_{A}$ , approaching to zero at $T \sim T_{A}$ . The findings evidence the transition of molecular dynamics from individual to cooperative at $T = T_{A}$ .

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