Pabst Florian, Baroni Stefano
SISSA─Scuola Internazionale Superiore di Studi Avanzati, 34136 Trieste, Italy.
CNR-IOM, Istituto dell'Officina dei Materiali, SISSA Unit, 34136 Trieste, Italy.
J Phys Chem Lett. 2025 Aug 7;16(31):7915-7920. doi: 10.1021/acs.jpclett.5c01401. Epub 2025 Jul 28.
Water inherently contains trace amounts of various salts, yet the microscopic processes by which salts influence some of its physical properties remain elusive. Notably, the mechanisms that reduce the dielectric constant of water upon salt addition are still debated. The primary absorption peak for electromagnetic radiation─commonly used in microwave heating─shifts toward higher frequencies in saline solutions, suggesting faster water molecular dynamics. This observation, however, contrasts with the simultaneous increase in viscosity and experimental reports that ionic solutes would slow down water molecular motion. In this work, we use molecular dynamics (MD) simulations with deep-neural-network models trained on high-quality quantum mechanical data to mimic interatomic forces and molecular dipoles, to compute the dielectric spectra of perchlorate water saline solution, which may be relevant to the recent discovery of liquid water beneath the thick ice crust at Mars's south pole. Our results reveal that both the reduction in the dielectric constant and the absorption peak shift can be attributed to ion-induced changes in the orientational ordering of water molecules. Additionally, we demonstrate that the self-part of the molecular dipole-dipole correlation function reveals clear signatures of the slowing dynamics within the first cationic solvation shell, consistent with the experimentally observed increase in viscosity.
水本身含有微量的各种盐类,然而盐影响其某些物理性质的微观过程仍然难以捉摸。值得注意的是,加盐后降低水的介电常数的机制仍存在争议。电磁辐射的主要吸收峰(常用于微波加热)在盐溶液中向更高频率移动,这表明水分子动力学更快。然而,这一观察结果与粘度同时增加以及离子溶质会减缓水分子运动的实验报告形成对比。在这项工作中,我们使用分子动力学(MD)模拟,并结合在高质量量子力学数据上训练的深度神经网络模型来模拟原子间力和分子偶极,以计算高氯酸盐水溶液的介电谱,这可能与最近在火星南极厚冰壳下发现液态水有关。我们的结果表明,介电常数的降低和吸收峰的移动都可归因于离子引起的水分子取向有序性的变化。此外,我们证明分子偶极 - 偶极相关函数的自部分揭示了第一阳离子溶剂化壳内动力学减慢的清晰特征,这与实验观察到的粘度增加一致。