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甲醇流体中动力学非均匀性的密度依赖性。

Density dependence of dynamical heterogeneity in fluid methanol.

机构信息

IUT Paris Jussieu, Université Paris Diderot, 75205, Paris, France.

出版信息

J Chem Phys. 2013 May 7;138(17):174507. doi: 10.1063/1.4802024.

Abstract

Brillouin and Raman scattering experiments on methanol through its glass transition under pressure are reported. The Brillouin scattering data were analyzed using viscoelastic theory and a fit to the Vinet equation of state. The variation in the linewidth of the longitudinal acoustic mode with pressure shows a broad maximum centered around 3 GPa. The pressure evolution of the relaxation time in the GHz range is obtained, and the Raman data are analyzed in terms of the Boson peak and its associated relaxation time in the THz range. The pressure evolution of these two relaxation processes extends previous determinations of relaxations at lower frequency based on dielectric measurements in supercooled methanol. The relaxation processes in glass-forming methanol have now been investigated over a wide frequency range and their evolution followed over a large variation of density.

摘要

报道了甲醇在压力下通过玻璃化转变的布里渊和拉曼散射实验。使用粘弹性理论和对 Vinet 状态方程的拟合分析了布里渊散射数据。纵声学模式线宽随压力的变化显示出一个在 3 GPa 左右的宽最大值。获得了 GHz 范围内弛豫时间随压力的演化,并根据玻色峰及其在太赫兹范围内的相关弛豫时间分析了拉曼数据。这两个弛豫过程的压力演化扩展了先前基于过冷甲醇介电测量的低频弛豫的确定。现在已经在很宽的频率范围内研究了玻璃形成甲醇中的弛豫过程,并跟踪了其在密度大变化下的演化。

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