发表机构
Indian Institute of Science（印度科学学院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
通过分子动力学模拟发现，水的初始温度通过结构记忆影响冻结动力学，呈现非单调依赖，五元环作为动力学陷阱，揭示了记忆驱动的非平衡相变机制。
AI 中文摘要
过冷水冻结是一个经典的非平衡问题，然而热历史对结晶的影响仍不清楚。使用TIP4P/Ice模型的分子动力学模拟，我们研究了初始温度$T_i$如何影响快速淬火至250 K后的冻结过程。通过监测氢键环结构的演化，我们发现冻结时间$t_F$对$T_i$呈非单调依赖，最慢结晶发生在约300 K附近。值得注意的是，这意味着初始较热的水可以比初始较冷的水冻结得更快，这是Mpemba效应的分子尺度类似物。非平稳广义Langevin方程框架表明，双时记忆核保留了系统热历史的信息，直接影响结晶动力学。结构分析进一步揭示，五元环充当动力学陷阱，而环类型之间的相关性调节类冰构型的可及性。这些结果揭示了记忆驱动冻结的分子起源，并确立了结构记忆作为非平衡相变的关键驱动因素。
英文摘要
Freezing of supercooled water is a classic non-equilibrium problem, yet the influence of thermal history on crystallization remains unclear. Using molecular dynamics simulations with the TIP4P/Ice model, we investigate how the initial temperature $T_i$ shapes freezing following rapid quenching to 250 K. By monitoring the evolution of hydrogen-bonded ring structures, we find a non-monotonic dependence of the freezing time $t_F$ on $T_i$, with the slowest crystallization occurring near 300 K. Remarkably, this means that initially hotter water can freeze faster than cooler water, a molecular-scale analogue of the Mpemba effect. A non-stationary generalized Langevin equation framework shows that two-time memory kernels retain information about the system's thermal past, directly influencing crystallization dynamics. Structural analysis further reveals that five-membered rings act as kinetic traps, while correlations among ring types regulate the accessibility of ice-like motifs. These results uncover a molecular origin of memory-driven freezing and establish structural memory as a key driver of non-equilibrium phase transitions.
Journal refAbhigyan Hazarika, Sudeep N. Punnathanam, Biman Bagchi, Prabal K. Maiti; Memory control of ice growth during non-equilibrium freezing of water. J. Chem. Phys. 7 June 2026; 164 (21): 214302
