Memory Control of Ice Growth During Non-Equilibrium Freezing of Water

Abstract

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.

References in corpus (11)

• Canonical sampling through velocity-rescaling
• Exponentially faster cooling in a colloidal system
• Microscopic Mechanism and Kinetics of Ice Formation at Complex Interfaces: Zooming in on Kaolinite
• Observation of quantum strong Mpemba effect
• Unravelling the contribution of local structures to the anomalies of water: the synergistic action of several factors
• On the "generalized Generalized Langevin Equation"
• Should a hotter paramagnet transform quicker to a ferromagnet? Monte Carlo simulation results for Ising model
• Mpemba effect in a Langevin system: population statistics, metastability and other exact results
• Mpemba meets Newton: Exploring the Mpemba and Kovacs effects in the time-delayed cooling law
• Non-equilibrium memory effects: granular fluids and beyond
• Comments on the validity of the non-stationary Generalized Langevin Equation as a coarse-grained evolution equation for microscopic stochastic dynamics