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一些玻璃形成系统结构动力学的定性变化

Qualitative change in structural dynamics of some glass-forming systems.

作者信息

Novikov V N, Sokolov A P

机构信息

Department of Chemistry and Joint Institute for Neutron Sciences, University of Tennessee, Knoxville, Tennessee 37996, USA.

Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.

出版信息

Phys Rev E Stat Nonlin Soft Matter Phys. 2015 Dec;92(6):062304. doi: 10.1103/PhysRevE.92.062304. Epub 2015 Dec 14.

Abstract

Analysis of the temperature dependence of the structural relaxation time τ(α)(T) in supercooled liquids revealed a qualitatively distinct feature-a sharp, cusplike maximum in the second derivative of logτ(α)(T)at some T(max). It suggests that the super-Arrhenius temperature dependence of τ(α)(T) in glass-forming liquids eventually crosses over to an Arrhenius behavior at T<T(max), and there is no divergence of τ(α)(T) at nonzero T. T(max) can be above or below T(g), depending on the sensitivity of τ(T) to a change in the liquid's density quantified by the exponent γ in the scaling τ(α)(T)∼exp(A/Tρ(-γ)). These results might turn the discussion of the glass transition in a different direction-toward the origin of the limiting activation energy for structural relaxation at low T.

摘要

对过冷液体中结构弛豫时间τ(α)(T)的温度依赖性分析揭示了一个定性上截然不同的特征——在某个T(max)处,logτ(α)(T)的二阶导数出现尖锐的、类似尖点的最大值。这表明玻璃形成液体中τ(α)(T)的超阿伦尼乌斯温度依赖性最终在T<T(max)时转变为阿伦尼乌斯行为,并且在非零温度下τ(α)(T)不会发散。T(max)可以高于或低于T(g),这取决于τ(T)对由标度τ(α)(T)∼exp(A/Tρ(-γ))中的指数γ量化的液体密度变化的敏感性。这些结果可能会使玻璃转变的讨论转向一个不同的方向——朝着低温下结构弛豫的极限活化能的起源。

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