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结构弛豫和振动激发在液体和玻璃高频动力学中的作用。

Role of structural relaxations and vibrational excitations in the high-frequency dynamics of liquids and glasses.

作者信息

Chong Song-Ho

机构信息

Institute for Molecular Science, Okazaki 444-8585, Japan.

出版信息

Phys Rev E Stat Nonlin Soft Matter Phys. 2006 Sep;74(3 Pt 1):031205. doi: 10.1103/PhysRevE.74.031205. Epub 2006 Sep 25.

Abstract

We present theoretical investigation on the high-frequency collective dynamics in liquids and glasses at microscopic length scales and in the terahertz frequency region based on the mode-coupling theory for ideal liquid-glass transition. We focus on recently investigated issues from inelastic-x-ray-scattering and computer-simulation studies for dynamic structure factors and longitudinal and transversal current spectra: the anomalous dispersion of the high-frequency sound velocity and the nature of the low-frequency excitation called the boson peak. It will be discussed how the sound mode interferes with other low-lying modes present in the system. Thereby, we provide a systematic explanation of the anomalous sound-velocity dispersion in systems--ranging from high temperature liquid down to deep inside the glass state--in terms of the contributions from the structural-relaxation processes and from vibrational excitations called the anomalous-oscillation peak (AOP). A possibility of observing negative dispersion--the decrease of the sound velocity upon increase of the wave number--is argued when the sound-velocity dispersion is dominated by the contribution from the vibrational dynamics. We also show that the low-frequency excitation, observable in both of the glass-state longitudinal and transversal current spectra at the same resonance frequency, is the manifestation of the AOP. As a consequence of the presence of the AOP in the transversal current spectra, it is predicted that the transversal sound velocity also exhibits the anomalous dispersion. These results of the theory are demonstrated for a model of the Lennard-Jones system.

摘要

基于理想液体 - 玻璃转变的模式耦合理论,我们对微观长度尺度和太赫兹频率区域内液体和玻璃中的高频集体动力学进行了理论研究。我们关注近期非弹性X射线散射和计算机模拟研究中关于动态结构因子以及纵向和横向电流谱的问题:高频声速的反常色散以及被称为玻色子峰的低频激发的本质。将讨论声模式如何与系统中存在的其他低频模式相互干扰。由此,我们从结构弛豫过程和被称为反常振荡峰(AOP)的振动激发的贡献方面,对从高温液体到玻璃态深处的系统中的反常声速色散进行了系统解释。当声速色散由振动动力学的贡献主导时,论证了观察到负色散(即波数增加时声速降低)的可能性。我们还表明,在玻璃态纵向和横向电流谱中以相同共振频率可观察到的低频激发是AOP的表现。由于横向电流谱中存在AOP,预计横向声速也会表现出反常色散。该理论结果在Lennard - Jones系统模型中得到了验证。

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