过冷液体结构弛豫的谱形研究。

IF 3.1 2区 化学 Q3 CHEMISTRY, PHYSICAL
Till Böhmer, Florian Pabst, Jan Philipp Gabriel, Rolf Zeißler, Thomas Blochowicz
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引用次数: 0

摘要

过冷液体中的结构弛豫是非指数的。在磁化率表示χ″(ν)中,观察到结构弛豫的频谱形状为一个不对称的加宽峰,具有ν1低和ν-β高频行为。在这篇展望性的文章中,我们讨论了关于结构弛豫的谱形状的一般概念、最近的结果和开放的问题。特别是,我们着重观察到ν-1/2的高频行为似乎是广泛的过冷液体的一般特征。此外,我们回顾了大量的证据,表明取向互相关的贡献可能导致某些物质的一般光谱形状偏离,特别是在介电损耗光谱中。此外,分子内动力学对含有更复杂和柔性分子的物质的光谱形状有重要影响。最后,我们讨论了关于一般ν-1/2行为的潜在物理起源和光谱形状在高温下的演变的开放性问题。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
On the spectral shape of the structural relaxation in supercooled liquids.

Structural relaxation in supercooled liquids is non-exponential. In susceptibility representation, χ″(ν), the spectral shape of the structural relaxation is observed as an asymmetrically broadened peak with a ν1 low- and ν-β high-frequency behavior. In this perspective article, we discuss common notions, recent results, and open questions regarding the spectral shape of the structural relaxation. In particular, we focus on the observation that a high-frequency behavior of ν-1/2 appears to be a generic feature in a broad range of supercooled liquids. Moreover, we review extensive evidence that contributions from orientational cross-correlations can lead to deviations from the generic spectral shape in certain substances, in particular in dielectric loss spectra. In addition, intramolecular dynamics can contribute significantly to the spectral shape in substances containing more complex and flexible molecules. Finally, we discuss the open questions regarding potential physical origins of the generic ν-1/2 behavior and the evolution of the spectral shape toward higher temperatures.

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来源期刊
Journal of Chemical Physics
Journal of Chemical Physics 物理-物理:原子、分子和化学物理
CiteScore
7.40
自引率
15.90%
发文量
1615
审稿时长
2 months
期刊介绍: The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance. Topical coverage includes: Theoretical Methods and Algorithms Advanced Experimental Techniques Atoms, Molecules, and Clusters Liquids, Glasses, and Crystals Surfaces, Interfaces, and Materials Polymers and Soft Matter Biological Molecules and Networks.
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