Liquid Polyamorphism: Some Unsolved Puzzles of Water in Bulk, Nanoconfined, and Biological Environments

IF 0.5 Q4 MATHEMATICS, INTERDISCIPLINARY APPLICATIONS
Complex Systems Pub Date : 2008-02-27 DOI:10.1063/1.2897798
H. Stanley, Pradeep Kumar, G. Franzese, Limei Xu, Zhen-Wei Yan, M. Mazza, S. H. Chen, F. Mallamace, S. Buldyrev
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引用次数: 9

Abstract

We investigate the relation between changes in dynamic and thermodynamic anomalies arising from the presence of the liquid‐liquid critical point in (i) Two models of water, TIP5P and ST2, which display a first order liquid‐liquid phase transition at low temperatures; (ii) the Jagla model, a spherically symmetric two‐scale potential known to possess a liquid‐liquid critical point, in which the competition between two liquid structures is generated by repulsive and attractive ramp interactions; and (iii) A Hamiltonian model of water where the idea of two length/energy scales is built in; this model also displays a first order liquid‐liquid phase transition at low temperatures besides the first order liquid‐gas phase transition at high temperatures. We find a correlation between the dynamic fragility crossover and the locus of specific heat maxima CPmax (“Widom line”) emanating from the critical point. Our findings are consistent with a possible relation between the previously hypothesized liquid‐liquid phase transition and the transition in the dynamics recently observed in neutron scattering experiments on confined water. More generally, we argue that this connection between CPmax and the dynamic crossover is not limited to the case of water, a hydrogen bonded network liquid, but is a more general feature of crossing the Widom line, an extension of the first‐order coexistence line in the supercritical region. We present evidence from experiments and computer simulations supporting the hypothesis that water displays polyamorphism, i.e., water separates into two distinct liquid phases. This concept of a new liquid‐liquid phase transition is finding application to other liquids as well as water, such as silicon and silica. We also discuss related puzzles, such as the mysterious behavior of confined water and the “skin” of hydration water near a biomolecule. Specifically, using molecular dynamics simulations, we also investigate the relation between the dynamic transitions of biomolecules (lysozyme and DNA) and the dynamic and thermodynamic properties of hydration water. We find that the dynamic transition of the macromolecules, sometimes called a “protein glass transition”, occurs at the temperature of dynamic crossover in the diffusivity of hydration water, and also coincides with the maxima of the isobaric specific heat CP and the temperature derivative of the orientational order parameter. We relate these findings to the hypothesis of a liquid‐liquid critical point in water. Our simulations are consistent with the possibility that the protein glass transition results from a change in the behavior of hydration water, specifically from crossing the Widom line.We investigate the relation between changes in dynamic and thermodynamic anomalies arising from the presence of the liquid‐liquid critical point in (i) Two models of water, TIP5P and ST2, which display a first order liquid‐liquid phase transition at low temperatures; (ii) the Jagla model, a spherically symmetric two‐scale potential known to possess a liquid‐liquid critical point, in which the competition between two liquid structures is generated by repulsive and attractive ramp interactions; and (iii) A Hamiltonian model of water where the idea of two length/energy scales is built in; this model also displays a first order liquid‐liquid phase transition at low temperatures besides the first order liquid‐gas phase transition at high temperatures. We find a correlation between the dynamic fragility crossover and the locus of specific heat maxima CPmax (“Widom line”) emanating from the critical point. Our findings are consistent with a possible relation between the previously hypothesized liquid‐liquid phas...
液体多变性:水在体积、纳米和生物环境中的一些未解之谜
我们研究了(i)两种水模型TIP5P和ST2中由于液-液临界点的存在而引起的动力学和热力学异常变化之间的关系,这两种模型在低温下表现为一级液-液相变;(ii) Jagla模型,一个已知具有液-液临界点的球对称二尺度势,其中两种液体结构之间的竞争是由排斥和吸引斜坡相互作用产生的;(iii)水的哈密顿模型,其中建立了两个长度/能量尺度的概念;除了高温下的一阶液相-气相转变外,该模型还显示了低温下的一阶液相-液相相变。我们发现动态脆性交叉与从临界点出发的比热最大值CPmax(“智慧线”)轨迹之间存在相关性。我们的发现与之前假设的液-液相变与最近在承压水中中子散射实验中观察到的动力学转变之间的可能关系一致。更一般地说,我们认为CPmax和动态交叉之间的这种联系并不局限于水(氢键网络液体)的情况,而是跨越Widom线(超临界区域一阶共存线的延伸)的更普遍的特征。我们从实验和计算机模拟中提出证据,支持水表现出多相性的假设,即水分成两个不同的液相。这种新的液-液相变的概念正在寻找其他液体以及水的应用,如硅和二氧化硅。我们还讨论了相关的难题,如封闭水的神秘行为和水合水在生物分子附近的“皮肤”。具体来说,通过分子动力学模拟,我们还研究了生物分子(溶菌酶和DNA)的动态转变与水合水的动力学和热力学性质之间的关系。我们发现大分子的动态转变,有时被称为“蛋白质玻璃化转变”,发生在水化水扩散率的动态交叉温度,也与等压比热CP的最大值和取向顺序参数的温度导数一致。我们将这些发现与水存在液-液临界点的假设联系起来。我们的模拟结果与蛋白质玻璃化转变的可能性是一致的,这是由于水合水的行为发生了变化,特别是由于越过了“智慧线”。我们研究了(i)两种水模型TIP5P和ST2中由于液-液临界点的存在而引起的动力学和热力学异常变化之间的关系,这两种模型在低温下表现为一级液-液相变;(ii) Jagla模型,一个已知具有液-液临界点的球对称二尺度势,其中两种液体结构之间的竞争是由排斥和吸引斜坡相互作用产生的;(iii)水的哈密顿模型,其中建立了两个长度/能量尺度的概念;除了高温下的一阶液相-气相转变外,该模型还显示了低温下的一阶液相-液相相变。我们发现动态脆性交叉与从临界点出发的比热最大值CPmax(“智慧线”)轨迹之间存在相关性。我们的发现与之前假设的液-液相之间的可能关系是一致的。
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
Complex Systems
Complex Systems MATHEMATICS, INTERDISCIPLINARY APPLICATIONS-
CiteScore
1.80
自引率
25.00%
发文量
18
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