Dipartimento di Matematica e Fisica, Università degli Studi Roma Tre, Via della Vasca Navale 84, 00146, Roma, Italy.
Institute of Physical Chemistry, University of Innsbruck, Innrain 52c, A-6020, Innsbruck, Austria.
Eur Phys J E Soft Matter. 2021 Nov 26;44(11):143. doi: 10.1140/epje/s10189-021-00139-1.
In this review, we report recent progress in the field of supercooled water. Due to its uniqueness, water presents numerous anomalies with respect to most simple liquids, showing polyamorphism both in the liquid and in the glassy state. We first describe the thermodynamic scenarios hypothesized for the supercooled region and in particular among them the liquid-liquid critical point scenario that has so far received more experimental evidence. We then review the most recent structural indicators, the two-state model picture of water, and the importance of cooperative effects related to the fact that water is a hydrogen-bonded network liquid. We show throughout the review that water's peculiar properties come into play also when water is in solution, confined, and close to biological molecules. Concerning dynamics, upon mild supercooling water behaves as a fragile glass former following the mode coupling theory, and it turns into a strong glass former upon further cooling. Connections between the slow dynamics and the thermodynamics are discussed. The translational relaxation times of density fluctuations show in fact the fragile-to-strong crossover connected to the thermodynamics arising from the existence of two liquids. When considering also rotations, additional crossovers come to play. Mobility-viscosity decoupling is also discussed in supercooled water and aqueous solutions. Finally, the polyamorphism of glassy water is considered through experimental and simulation results both in bulk and in salty aqueous solutions. Grains and grain boundaries are also discussed.
在这篇综述中,我们报告了过冷水领域的最新进展。由于其独特性,水相对于大多数简单液体表现出许多异常现象,在液态和玻璃态都表现出多晶型性。我们首先描述了过冷区假设的热力学情景,特别是迄今为止得到更多实验证据的液相-液相临界点情景。然后我们回顾了最近的结构指标、水的两态模型图景以及与水是氢键网络液体这一事实相关的协同效应的重要性。我们在整个综述中表明,当水处于溶液中、被限制和接近生物分子时,水的特殊性质也会发挥作用。关于动力学,在轻度过冷时,水遵循模式耦合理论表现为脆性玻璃形成体,而在进一步冷却时则变为强玻璃形成体。讨论了慢动力学和热力学之间的联系。密度涨落的平移弛豫时间实际上显示了与由于两种液体存在而产生的热力学相关的脆性到强的交叉。当考虑到旋转时,会出现额外的交叉。在过冷水中也讨论了流动性-粘度解耦。最后,通过实验和模拟结果考虑了玻璃态水的多晶型性,包括在本体和含盐水溶液中。还讨论了晶粒和晶界。