Glassy Arrest Behind the Apparent Second Liquid in Water
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arXiv
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| Auteurs principaux: | , |
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| Format: | Preprint |
| Publié: |
2026
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| _version_ | 1866915905517125632 |
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| author | Pabst, Florian Hassanali, Ali |
| author_facet | Pabst, Florian Hassanali, Ali |
| contents | The origin of water's anomalous behavior remains a central open problem in the physical sciences and is often attributed to a liquid-liquid transition (LLT) between high- and low-density liquid states deep in the supercooled regime. Experimental access to this region has been challenging due to rapid crystallization, leaving atomistic simulations as a major source of supporting evidence. Using extensive machine-learning-accelerated first-principles simulations in direct comparison with spectroscopic, structural, and dynamical experimental measurements, we show that features commonly interpreted as signatures of two-liquid behavior emerge at the onset of dynamical arrest. Specifically, we find that two-state fluctuations previously associated with an LLT reflect a transformation from a high-density liquid to a kinetically arrested low-density glass. By mapping equilibrium dynamics across pressure and temperature, our results suggest a reassessment of water's metastable landscape, in which apparent two-state behavior may reflect a relatively high glass-transition temperature of ambient-pressure low-density water, 189$\pm$8 K -- remarkably close to the temperature previously associated with the LLT. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2604_00794 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Glassy Arrest Behind the Apparent Second Liquid in Water Pabst, Florian Hassanali, Ali Soft Condensed Matter The origin of water's anomalous behavior remains a central open problem in the physical sciences and is often attributed to a liquid-liquid transition (LLT) between high- and low-density liquid states deep in the supercooled regime. Experimental access to this region has been challenging due to rapid crystallization, leaving atomistic simulations as a major source of supporting evidence. Using extensive machine-learning-accelerated first-principles simulations in direct comparison with spectroscopic, structural, and dynamical experimental measurements, we show that features commonly interpreted as signatures of two-liquid behavior emerge at the onset of dynamical arrest. Specifically, we find that two-state fluctuations previously associated with an LLT reflect a transformation from a high-density liquid to a kinetically arrested low-density glass. By mapping equilibrium dynamics across pressure and temperature, our results suggest a reassessment of water's metastable landscape, in which apparent two-state behavior may reflect a relatively high glass-transition temperature of ambient-pressure low-density water, 189$\pm$8 K -- remarkably close to the temperature previously associated with the LLT. |
| title | Glassy Arrest Behind the Apparent Second Liquid in Water |
| topic | Soft Condensed Matter |
| url | https://arxiv.org/abs/2604.00794 |