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用于表征软物质中非平衡动力学的输运系数方法。

Transport coefficient approach for characterizing nonequilibrium dynamics in soft matter.

作者信息

He HongRui, Liang Heyi, Chu Miaoqi, Jiang Zhang, de Pablo Juan J, Tirrell Matthew V, Narayanan Suresh, Chen Wei

机构信息

Materials Science Division and Center for Molecular Engineering, Argonne National Laboratory, Lemont, IL 60439.

Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL 60637.

出版信息

Proc Natl Acad Sci U S A. 2024 Jul 30;121(31):e2401162121. doi: 10.1073/pnas.2401162121. Epub 2024 Jul 23.

Abstract

Nonequilibrium states in soft condensed matter require a systematic approach to characterize and model materials, enhancing predictability and applications. Among the tools, X-ray photon correlation spectroscopy (XPCS) provides exceptional temporal and spatial resolution to extract dynamic insight into the properties of the material. However, existing models might overlook intricate details. We introduce an approach for extracting the transport coefficient, denoted as [Formula: see text], from the XPCS studies. This coefficient is a fundamental parameter in nonequilibrium statistical mechanics and is crucial for characterizing transport processes within a system. Our method unifies the Green-Kubo formulas associated with various transport coefficients, including gradient flows, particle-particle interactions, friction matrices, and continuous noise. We achieve this by integrating the collective influence of random and systematic forces acting on the particles within the framework of a Markov chain. We initially validated this method using molecular dynamics simulations of a system subjected to changes in temperatures over time. Subsequently, we conducted further verification using experimental systems reported in the literature and known for their complex nonequilibrium characteristics. The results, including the derived [Formula: see text] and other relevant physical parameters, align with the previous observations and reveal detailed dynamical information in nonequilibrium states. This approach represents an advancement in XPCS analysis, addressing the growing demand to extract intricate nonequilibrium dynamics. Further, the methods presented are agnostic to the nature of the material system and can be potentially expanded to hard condensed matter systems.

摘要

软凝聚态物质中的非平衡态需要一种系统的方法来表征和建模材料,以提高预测能力和应用价值。在这些工具中,X射线光子相关光谱学(XPCS)提供了卓越的时间和空间分辨率,以便深入了解材料特性的动态信息。然而,现有的模型可能会忽略一些复杂的细节。我们引入了一种从XPCS研究中提取传输系数(记为[公式:见正文])的方法。该系数是非平衡统计力学中的一个基本参数,对于表征系统内的传输过程至关重要。我们的方法统一了与各种传输系数相关的格林-久保公式,包括梯度流、粒子-粒子相互作用、摩擦矩阵和连续噪声。我们通过在马尔可夫链框架内整合作用于粒子的随机力和系统力的集体影响来实现这一点。我们最初使用一个随时间变化温度的系统的分子动力学模拟来验证该方法。随后,我们使用文献中报道的具有复杂非平衡特性的实验系统进行了进一步验证。结果,包括推导得到的[公式:见正文]和其他相关物理参数,与先前的观察结果一致,并揭示了非平衡态下的详细动力学信息。这种方法代表了XPCS分析的一个进步,满足了提取复杂非平衡动力学日益增长的需求。此外,所提出的方法与材料系统的性质无关,并且有可能扩展到硬凝聚态物质系统。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c7f/11295068/eb405d4c001b/pnas.2401162121fig01.jpg

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