超冷水中的动态异质性及其光谱指纹
Cesare Malosso1,2, Edward Danquah Donkor3,4, Stefano Baroni2,5
1Laboratory of Computational Science and Modeling, IMX, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland.
The Journal of chemical physics
|October 10, 2025
概括
研究人员探索了其第二个液体-液体临界点 (LLCP) 附近超冷水的动态. 他们发现了高密度液体 (HDL) 和低密度液体 (LDL) 阶段的明显分子运动和振动光谱.
科学领域:
- 物理化学 物理化学
- 计算材料科学科学 计算材料科学
- 软物质物理学 软物质物理学
背景情况:
- 理论和实验证据表明,超冷水中存在第二个液体-液体临界点 (LLCP).
- 这种LLCP与高密度液体 (HDL) 和低密度液体 (LDL) 水相的共存有关.
- 虽然LLCP的热力学已知,但临界点附近的HDL和LDL的动态性质尚不清楚.
研究的目的:
- 研究在假定LLCP附近的HDL和LDL相的动态和光谱特征.
- 描述深度超冷水中的分子移动性和振动行为.
- 提供动态指纹,以帮助实验检测液体-液体过渡.
主要方法:
- 用机器学习的原子间潜力来模拟超冷水.
- 利用范霍夫相关函数进行动态分析.
- 计算了红外吸收 (IR) 光谱,以探测振动特性.
主要成果:
- 低密度液体 (LDL) 表现出缓慢和异质的分子运动.
- 高密度液体 (HDL) 显示更快,更均的动态.
- 在LDL和HDL之间观察到明显的振动光谱,特别是在远IR区域 (4001000厘米-1).
结论:
- 这项研究为LLCP附近超冷水的行为提供了新的动态和光谱见解.
- 这些发现区分了HDL和LDL阶段的微观动态.
- 为探测水中难以捉摸的液体-液体过渡的实验努力提供指导.
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