Beyond Local Structures in Critical Supercooled Water through Unsupervised Learning

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(15), С. 3996 - 4005

Опубликована: Апрель 4, 2024

The presence of a second critical point in water has been topic intense investigation for the last few decades. molecular origins underlying this phenomenon are typically rationalized terms competition between local high-density (HD) and low-density (LD) structures. Their identification often requires designing parameters that subject to human intervention. Herein, we use unsupervised learning discover structures atomistic simulations close liquid-liquid (LLCP). Encoding information on environment using descriptors, do not find evidence two distinct thermodynamic In contrast, when deploy

Язык: Английский

Structural Origin of Dynamic Heterogeneity in Supercooled Liquids

The Journal of Physical Chemistry B, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

As a liquid is supercooled toward the glass transition point, its dynamics slow significantly, provided that crystallization avoided. With increased supercooling, particle become more spatially heterogeneous, phenomenon known as dynamic heterogeneity. Since discovery, this characteristic of metastable liquids has garnered considerable attention in science. However, precise physical origins heterogeneity remain elusive and widely debated. In perspective, we examine relationship between structural order, based on numerical simulations fragile with isotropic potentials strong directional interactions. We demonstrate angular ordering, arising from many-body steric interactions, plays crucial role cooperativity liquids. Additionally, explore how growth static order correlates slower dynamics. exhibiting super-Arrhenius behavior, spatial extent regions high grows upon cooling, sequential propagation rearrangements within these ordered increases activation energy for motion. contrast, constrained local ordering display distinct "two-state" characteristic, marked by two Arrhenius-type behaviors. argue heterogeneity, irrespective liquid's fragility, arises underlying determined ordering. This perspective aims to deepen our understanding interplay properties

Язык: Английский

Two state model for the ML-BOP potential

Molecular Physics, Год журнала: 2024, Номер unknown

Опубликована: Сен. 26, 2024

Язык: Английский