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<p>Supercooled liquids display sluggish dynamics, often attributed to their structural characteristics, yet the underlying mechanism remains elusive. Here we conduct numerical investigations into the structure–dynamics relationship in model glass-forming liquids, with a specific focus on an elementary particle rearrangement mode known as the ‘T1 process’. We discover that the ability of a T1 process to preserve glassy structural order before and after is pivotal towards determining a liquid’s fragility—whether it exhibits super-Arrhenius-like or Arrhenius-like behaviour. If a T1 process disrupts local structural order, it must occur independently without cooperativity, resulting in Arrhenius-like behaviour. By contrast, if it can maintain order, it sequentially propagates from disordered peripheries to the middle of high-structural-order regions, leading to cooperativity and super-Arrhenius-like behaviour. Our study establishes a microscopic link between liquid-structure ordering, dynamic cooperativity and super-Arrhenius-like dynamics, extending the understanding of the structure–dynamics relationships in supercooled liquids.</p>

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Microscopic structural origin of slow dynamics in glass-forming liquids

  • 期刊论文

  • 发表日期：

    2025年1月8日

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  • Seiichiro Ishino,
  • Yuan-Chao Hu,
  • Hajime Tanaka

摘要

Supercooled liquids display sluggish dynamics, often attributed to their structural characteristics, yet the underlying mechanism remains elusive. Here we conduct numerical investigations into the structure–dynamics relationship in model glass-forming liquids, with a specific focus on an elementary particle rearrangement mode known as the ‘T1 process’. We discover that the ability of a T1 process to preserve glassy structural order before and after is pivotal towards determining a liquid’s fragility—whether it exhibits super-Arrhenius-like or Arrhenius-like behaviour. If a T1 process disrupts local structural order, it must occur independently without cooperativity, resulting in Arrhenius-like behaviour. By contrast, if it can maintain order, it sequentially propagates from disordered peripheries to the middle of high-structural-order regions, leading to cooperativity and super-Arrhenius-like behaviour. Our study establishes a microscopic link between liquid-structure ordering, dynamic cooperativity and super-Arrhenius-like dynamics, extending the understanding of the structure–dynamics relationships in supercooled liquids.