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| Main Authors: | , , , , , |
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| Format: | Preprint |
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2026
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2605.25457 |
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| _version_ | 1866913161250078720 |
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| author | Jiang, Xinyue Shang, Yating Li, Jianhui Zou, Zhaoyong Zuo, Yanxia Xie, Yuqun |
| author_facet | Jiang, Xinyue Shang, Yating Li, Jianhui Zou, Zhaoyong Zuo, Yanxia Xie, Yuqun |
| contents | Ethanol-water mixtures are a classic example of thermodynamic non-ideality, yet the structural origin of their pronounced anomalies, such as volume contraction and a large negative excess entropy, has remained a long-standing puzzle. Here, we demonstrate these anomalies are not equilibrium properties but calorimetric fingerprint of an arrested phase transition. By imposing periodic thermal oscillations, we drive a 50% (v/v) ethanol-water system along a complete hierarchical self-assembly pathway that progressed from ethanol clusters to water-containing droplets, then to acicular flakes, and finally to micron-scale ordered ethanol aggregates. Fluorescence spectroscopy, two-dimensional correlation analysis and nuclear magnetic resonance revealed the underlying non-equilibrium molecular mechanism: a periodic perturbation of the water-dominated hydrogen-bond network initiates a ethanol-water coexistence intermediate, ultimately leading to the stable ordered assembly of an ethanol-rich phase. Our finding demonstrated that periodic physical perturbations capable drive spontaneous ordering across multiple length scales in a simple binary mixture, providing a kinetic perspective on the structural origin of solution non-ideality, and carry general implications for self-assembly strategies in soft matter. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2605_25457 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Non-equilibrium pathway to mesoscale ordering in ethanol-water binary liquid Jiang, Xinyue Shang, Yating Li, Jianhui Zou, Zhaoyong Zuo, Yanxia Xie, Yuqun Soft Condensed Matter Atomic Physics Ethanol-water mixtures are a classic example of thermodynamic non-ideality, yet the structural origin of their pronounced anomalies, such as volume contraction and a large negative excess entropy, has remained a long-standing puzzle. Here, we demonstrate these anomalies are not equilibrium properties but calorimetric fingerprint of an arrested phase transition. By imposing periodic thermal oscillations, we drive a 50% (v/v) ethanol-water system along a complete hierarchical self-assembly pathway that progressed from ethanol clusters to water-containing droplets, then to acicular flakes, and finally to micron-scale ordered ethanol aggregates. Fluorescence spectroscopy, two-dimensional correlation analysis and nuclear magnetic resonance revealed the underlying non-equilibrium molecular mechanism: a periodic perturbation of the water-dominated hydrogen-bond network initiates a ethanol-water coexistence intermediate, ultimately leading to the stable ordered assembly of an ethanol-rich phase. Our finding demonstrated that periodic physical perturbations capable drive spontaneous ordering across multiple length scales in a simple binary mixture, providing a kinetic perspective on the structural origin of solution non-ideality, and carry general implications for self-assembly strategies in soft matter. |
| title | Non-equilibrium pathway to mesoscale ordering in ethanol-water binary liquid |
| topic | Soft Condensed Matter Atomic Physics |
| url | https://arxiv.org/abs/2605.25457 |