Experimental validation of correlation peak universality in classical fluids

IF 5.2 2区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Molecular Liquids Pub Date : 2025-05-15 Epub Date: 2025-03-07 DOI:10.1016/j.molliq.2025.127241
Artur D. Nasyrov, Egor V. Yakovlev, Ivan A. Kushnir, Alina R. Karimova, Stanislav O. Yurchenko, Nikita P. Kryuchkov
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Abstract

The radial distribution function (RDF) in condensed matter provides a key link between structural and thermodynamic properties. A recently developed fluid interpolation method allows the reconstruction of the RDF over a wide temperature range in fluids. This method is based on the observed “universality” of the correlation peaks in the pair correlation function g(r), which holds despite variations in density, temperature, interparticle potentials and system types - from ideal gases to complex biological fluid-like systems. However, so far this universality has only been identified by computer simulations for two-dimensional systems and has not been experimentally validated. This work is dedicated to a more comprehensive analysis of this ‘universality’, including experiments on colloidal suspensions with tunable interactions in external rotating electric fields and 3D systems such Lennard-Jones fluid, and fluid state of Hg and Fe. In particular, we found that the peak norms, their mean values and dispersion show identical behaviour, while differences between peaks are mainly due to non-Gaussian parameters. Furthermore, the obtained dependencies reveal a clear transition between the crystal- and gas-like correlation regimes at close and far distances, suggesting that our approach may provide a new way to analyse fluids of different nature, from atomic and molecular to protein and colloidal systems.
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经典流体相关峰普适性的实验验证
凝聚态物质的径向分布函数(RDF)提供了结构和热力学性质之间的关键联系。最近开发的流体插值方法允许在流体的宽温度范围内重建RDF。该方法基于对相关函数g(r)中相关峰的“通用性”,无论密度、温度、粒子间势和系统类型(从理想气体到复杂的生物流体类系统)如何变化,该方法都保持不变。然而,到目前为止,这种普遍性只是通过二维系统的计算机模拟来确定的,尚未得到实验验证。这项工作致力于对这种“普遍性”进行更全面的分析,包括在外部旋转电场和三维系统(如Lennard-Jones流体)中具有可调相互作用的胶体悬浮液的实验,以及Hg和Fe的流体状态。特别是,我们发现峰规范,它们的平均值和离散度表现出相同的行为,而峰之间的差异主要是由于非高斯参数。此外,所获得的依赖关系揭示了晶体和气体样相关制度在近距离和远距离之间的明显转变,表明我们的方法可能提供一种新的方法来分析不同性质的流体,从原子和分子到蛋白质和胶体系统。
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来源期刊
Journal of Molecular Liquids
Journal of Molecular Liquids 化学-物理:原子、分子和化学物理
CiteScore
10.30
自引率
16.70%
发文量
2597
审稿时长
78 days
期刊介绍: The journal includes papers in the following areas: – Simple organic liquids and mixtures – Ionic liquids – Surfactant solutions (including micelles and vesicles) and liquid interfaces – Colloidal solutions and nanoparticles – Thermotropic and lyotropic liquid crystals – Ferrofluids – Water, aqueous solutions and other hydrogen-bonded liquids – Lubricants, polymer solutions and melts – Molten metals and salts – Phase transitions and critical phenomena in liquids and confined fluids – Self assembly in complex liquids.– Biomolecules in solution The emphasis is on the molecular (or microscopic) understanding of particular liquids or liquid systems, especially concerning structure, dynamics and intermolecular forces. The experimental techniques used may include: – Conventional spectroscopy (mid-IR and far-IR, Raman, NMR, etc.) – Non-linear optics and time resolved spectroscopy (psec, fsec, asec, ISRS, etc.) – Light scattering (Rayleigh, Brillouin, PCS, etc.) – Dielectric relaxation – X-ray and neutron scattering and diffraction. Experimental studies, computer simulations (MD or MC) and analytical theory will be considered for publication; papers just reporting experimental results that do not contribute to the understanding of the fundamentals of molecular and ionic liquids will not be accepted. Only papers of a non-routine nature and advancing the field will be considered for publication.
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