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过冷液体中低重叠相与高重叠相共存:积分方程研究。

Coexistence of low and high overlap phases in a supercooled liquid: An integral equation investigation.

机构信息

LCP-A2MC, EA3469, Université de Lorraine, 1 Bd. François Arago, Metz F-57078, France.

Dipartimento di Fisica, Università di Trieste, Strada Costiera 11, 34151 Trieste, Grignano, Italy.

出版信息

J Chem Phys. 2017 Mar 21;146(11):114504. doi: 10.1063/1.4978499.

Abstract

The pair structure, free energy, and configurational overlap order parameter Q of an annealed system of two weakly coupled replicas of a supercooled "soft sphere" fluid are determined by solving the hypernetted-chain (HNC) and self-consistent Rogers-Young (RY) integral equations over a wide range of thermodynamic conditions ρ (number-density), T (temperature), and inter-replicas couplings ε. Analysis of the resulting effective (or Landau) potential W(ρ,T; Q) and of its derivative with respect to Q confirms the existence of a "precursor transition" between weak and strong overlap phases below a critical temperature T well above the temperature T of the "ideal glass" transition observed in the limit ε→0. The precursor transition is signalled by a loss of convexity of the potential W(Q) and by a concomitant discontinuity of the order parameter Q just below T, which crosses over to a mean-field-like van der Waals loop at lower temperatures. The HNC and RY equations lead to the same phase transition scenario, with quantitative differences in the predicted temperatures T and T.

摘要

通过求解超冷“软球”流体的两个弱耦合副本的退火系统的超网链(HNC)和自洽罗杰斯 - 杨(RY)积分方程,确定了对一对结构,自由能和构型重叠有序参数 Q,该系统在很宽的热力学条件 ρ(密度),T(温度)和副本之间的耦合 ε范围内。对所得有效(或朗道)势 W(ρ,T;Q)及其对 Q 的导数的分析证实了在低于临界温度 T 的情况下,在弱和强重叠相之间存在“前体转变”,该温度远高于 ε→0 时观察到的“理想玻璃”转变温度 T。前体转变的信号是势 W(Q)失去凸度,以及有序参数 Q 刚好低于 T 时出现的不连续性,这在较低温度下转变为类似平均场的范德华环。HNC 和 RY 方程导致相同的相变情况,预测温度 T 和 T 存在定量差异。

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