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Interpretation of the GHz to THz dielectric relaxation dynamics of water in the framework of the Coupling Model
Journal of Molecular Liquids ( IF 5.3 ) Pub Date : 2018-01-08 , DOI: 10.1016/j.molliq.2018.01.039
K.L. Ngai

The microscopic origins of the processes in water observed at temperatures above and below room temperature by dielectric relaxation spectroscopy in the range from GHz to beyond THz are identified by three sequential and interrelated contributions in the framework of the Coupling Model. Appearing after vibration and boson peak is the caged water dynamics. Cage decays with the onset of the primitive relaxation of the Coupling Model (CM), which is practically coincident with the nearly exponential structural α-relaxation. These sequential processes explain the nearly Debye α-loss peak, the high frequency power law (HFPL) associated with it, and the higher frequency dispersion before reaching the vibrational contributions. High frequency and short time experimental data of several glass-formers obtained by different techniques are presented to show the same three processes with the same relationship between them, as proposed for water. Crucial supports of the CM explanation come from neutron scattering experiments on water showing that: (1) caging and decaging indeed occurs in the HFPL regime; (2) the dynamics of the HFPL is independent of the scattering vector Q, in accord with the HFPL is comprised of caged dynamics and decaging; and (3) the terminal process is normal diffusion, justifying the 20 GHz dielectric loss peak originates from the structural α-relaxation, which follows after the completion of decaging, i.e. the end of the HFPL regime.



中文翻译:

耦合模型框架下水的GHz到THz介电弛豫动力学的解释

在耦合模型的框架内,通过三个连续且相互关联的贡献,可以确定在GHz以上至THz以上范围内通过介电弛豫光谱法在高于和低于室温的温度下在水中观察到的过程的微观起源。笼状水动力学在振动和玻色子峰之后出现。笼子随着耦合模型(CM)的原始松弛的开始而衰减,这实际上与几乎指数的结构α松弛相吻合。这些顺序过程说明了接近Debyeα损耗峰,与之相关的高频功率定律(HFPL),以及达到振动贡献之前的较高频率色散。提出了通过不同技术获得的几种玻璃形成器的高频和短时实验数据,以显示针对水的相同的三个过程,它们之间具有相同的关系。CM解释的关键支持来自对水的中子散射实验,结果表明:(1)HFPL机制中确实发生了笼罩和笼罩;(2)HFPL的动力学独立于散射矢量根据HFPL,Q由笼式动力学和减幅组成;(3)最终过程是正态扩散,证明20 GHz介电损耗峰源于结构α松弛,该α松弛在降幅完成后即HFPL制度结束后出现。

更新日期:2018-01-08
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