Crossover between Solid-like and Liquid-like Behavior in Supercooled Liquids
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| Main Authors: | , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866918059825954816 |
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| author | Tian, X. R. Zhang, D. M. Zhang, B. Sun, D. Y. Gong, X. G. |
| author_facet | Tian, X. R. Zhang, D. M. Zhang, B. Sun, D. Y. Gong, X. G. |
| contents | In supercooled liquids, at a temperature between the glass transition temperature Tg and the melting point Tm, thermodynamic properties remain continuous, while dynamic behavior exhibits anomalies. The origin of such thermodynamics-dynamic decoupling has long been a puzzle in the field of glass researches. In this study, we show that the ratio of the alpha-relaxation time associated with the relative and center-of-mass coordinate of nearest-neighbor atomic pairs can effectively characterize the dynamic features of supercooled liquids. With this approach, supercooled liquids can be categorized into two distinct 'states' based on their dynamics: solid-like and liquid-like behaviors. We further propose four possible paths from the liquid to the final glass state, each exhibiting unique thermodynamic and dynamic behaviors. Two of these paths predict a characteristic temperature Tx between Tm and Tg, where a crossover between solid-like and liquid-like behaviors occurs in supercooled liquids. The molecular dynamics simulations of several supercooled liquids reveal that the actual path followed by all these systems undergo the crossover between solid-like and liquid-like behaviors. Tx is found to reside in a similar temperature range as the critical temperature Tc in the mode-coupling theory and the breakdown temperature Tb of the Stokes-Einstein relation. This crossover provides a new microscopic perspective for explaining macroscopic dynamic anomalies, and the absence of a typical thermodynamic phase transition at Tg. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2506_06957 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Crossover between Solid-like and Liquid-like Behavior in Supercooled Liquids Tian, X. R. Zhang, D. M. Zhang, B. Sun, D. Y. Gong, X. G. Soft Condensed Matter Disordered Systems and Neural Networks In supercooled liquids, at a temperature between the glass transition temperature Tg and the melting point Tm, thermodynamic properties remain continuous, while dynamic behavior exhibits anomalies. The origin of such thermodynamics-dynamic decoupling has long been a puzzle in the field of glass researches. In this study, we show that the ratio of the alpha-relaxation time associated with the relative and center-of-mass coordinate of nearest-neighbor atomic pairs can effectively characterize the dynamic features of supercooled liquids. With this approach, supercooled liquids can be categorized into two distinct 'states' based on their dynamics: solid-like and liquid-like behaviors. We further propose four possible paths from the liquid to the final glass state, each exhibiting unique thermodynamic and dynamic behaviors. Two of these paths predict a characteristic temperature Tx between Tm and Tg, where a crossover between solid-like and liquid-like behaviors occurs in supercooled liquids. The molecular dynamics simulations of several supercooled liquids reveal that the actual path followed by all these systems undergo the crossover between solid-like and liquid-like behaviors. Tx is found to reside in a similar temperature range as the critical temperature Tc in the mode-coupling theory and the breakdown temperature Tb of the Stokes-Einstein relation. This crossover provides a new microscopic perspective for explaining macroscopic dynamic anomalies, and the absence of a typical thermodynamic phase transition at Tg. |
| title | Crossover between Solid-like and Liquid-like Behavior in Supercooled Liquids |
| topic | Soft Condensed Matter Disordered Systems and Neural Networks |
| url | https://arxiv.org/abs/2506.06957 |