Longitudinal and transverse excitations: How nominally forbidden signals can be detected in autocorrelation functions relevant to liquids dynamics.

IF 3.1 2区 化学 Q3 CHEMISTRY, PHYSICAL
Eleonora Guarini, Ubaldo Bafile, Daniele Colognesi, Alessandro Cunsolo, Alessio De Francesco, Ferdinando Formisano
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Abstract

This work provides evidence for the crucial role played by the self-part of functions as important as the dynamic structure factor S(Q, ω) and the spectrum of the transverse current autocorrelation CT(Q, ω) in studies of liquid dynamics. By using ab initio molecular dynamics simulations of liquid Ag, we show that a multimode representation also accounts very well for the simulated self-dynamic structure factor Sself(Q, ω), which provides insight on the single-particle dynamics. In particular, we provide a convincing proof that Sself(Q, ω) is responsible for the observation of transverse-like contributions in a longitudinal quantity such as S(Q, ω). It is particularly significant that an analogous situation was found when considering the transverse current. In fact, its self-part, CT,self(Q, ω), was shown to be accountable for the presence of longitudinal-like modes in a transverse quantity, such as CT(Q, ω). Due to the single-particle origin of the transverse signal in the dynamic structure factor, we also show that the apparent Q-dependence of transverse-like frequencies, as inferred from S(Q, ω), differs from the true dispersion of transverse excitations appropriately derived from CT(Q, ω).

纵向和横向激励:如何在与液体动力学相关的自相关函数中检测名义上禁止的信号。
这项工作为与动态结构因子S(Q, ω)和横向电流自相关CT(Q, ω)谱同样重要的函数自部分在液体动力学研究中所起的关键作用提供了证据。通过从头算液体银的分子动力学模拟,我们发现多模表示也很好地解释了模拟的自动态结构因子self(Q, ω),这提供了对单粒子动力学的见解。特别是,我们提供了一个令人信服的证据,证明self(Q, ω)负责观察纵向量(如S(Q, ω))中的横向贡献。特别重要的是,在考虑横向电流时发现了类似的情况。事实上,它的自部分,CT,自(Q, ω),被证明是在横向量中存在纵向模态的原因,如CT(Q, ω)。由于动态结构因子中横向信号的单粒子起源,我们还表明,从S(Q, ω)推断出的类横向频率的表观Q依赖性与从CT(Q, ω)适当推导出的横向激励的真实色散不同。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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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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