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关于过冷分子玻璃形成液体在动力学阻滞时的遍历性:邻三联苯的情况。

On the ergodicity of supercooled molecular glass-forming liquids at the dynamical arrest: the o-terphenyl case.

作者信息

Mallamace Francesco, Corsaro Carmelo, Leone Nancy, Villari Valentina, Micali Norberto, Chen Sow-Hsin

机构信息

1] Dipartimento di Fisica e Scienze della Terra, Università di Messina I-98168, Messina, Italy [2] Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge MA 02139.

Dipartimento di Fisica e Scienze della Terra, Università di Messina I-98168, Messina, Italy.

出版信息

Sci Rep. 2014 Jan 17;4:3747. doi: 10.1038/srep03747.

Abstract

The dynamics of supercooled ortho-terphenyl has been studied using photon-correlation spectroscopy (PCS) in the depolarized scattering geometry. The obtained relaxation curves are analyzed according to the mode-coupling theory (MCT) for supercooled liquids. The main results are: i) the observation of the secondary Johari-Goldstein relaxation (β) that has its onset just at the dynamical crossover temperature TB (TM > TB > Tg); ii) the confirmation, of the suggestion of a recent statistical mechanical study, that such a molecular system remains ergodic also below the calorimetric glass-transition temperature Tg. Our experimental data give evidence that the time scales of the primary (α) and this secondary relaxations are correlated. Finally a comparison with recent PCS experiments in a colloidal system confirms the primary role of the dynamical crossover in the physics of the dynamical arrest.

摘要

利用光子相关光谱法(PCS)在去极化散射几何条件下研究了过冷邻三联苯的动力学。根据过冷液体的模式耦合理论(MCT)对所得的弛豫曲线进行了分析。主要结果如下:i)观察到二级乔哈里-戈尔茨坦弛豫(β),其起始点恰好在动力学交叉温度TB(TM > TB > Tg)处;ii)证实了最近一项统计力学研究的建议,即这样的分子体系在量热玻璃化转变温度Tg以下也保持遍历性。我们的实验数据表明一级(α)弛豫和二级弛豫的时间尺度是相关的。最后,与最近在胶体系统中进行的PCS实验的比较证实了动力学交叉在动力学阻滞物理过程中的主要作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/82f1/3894564/82191f27d737/srep03747-f1.jpg

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