基于杂化泛函的第一性原理模拟研究液态水和冰的密度与压缩性
Density and Compressibility of Liquid Water and Ice from First-Principles Simulations with Hybrid Functionals.
作者信息
Gaiduk Alex P, Gygi François, Galli Giulia
机构信息
†Institute for Molecular Engineering, The University of Chicago, 5747 South Ellis Avenue, Chicago, Illinois 60637, United States.
‡Department of Computer Science, University of California, Davis, One Shields Avenue, Davis, California 95616, United States.
出版信息
J Phys Chem Lett. 2015 Aug 6;6(15):2902-8. doi: 10.1021/acs.jpclett.5b00901. Epub 2015 Jul 13.
We determined the equilibrium density and compressibility of water and ice from first-principles molecular dynamics simulations using gradient-corrected (PBE) and hybrid (PBE0) functionals. Both functionals predicted the density of ice to be larger than that of water, by 15 (PBE) and 35% (PBE0). The PBE0 functional yielded a lower density of both ice and water with respect to PBE, leading to better agreement with experiment for ice but not for liquid water. Approximate inclusion of dispersion interactions on computed molecular-dynamics trajectories led to a substantial improvement of the PBE0 results for the density of liquid water, which, however, resulted to be slightly lower than that of ice.
我们通过使用梯度校正（PBE）和杂化（PBE0）泛函的第一性原理分子动力学模拟，确定了水和冰的平衡密度及压缩性。两种泛函均预测冰的密度比水的密度大，PBE预测大15%，PBE0预测大35%。相对于PBE，PBE0泛函得出的冰和水的密度更低，这使得其对冰密度的预测与实验结果更吻合，但对液态水密度的预测并非如此。在计算的分子动力学轨迹上近似包含色散相互作用，使得PBE0对液态水密度的预测结果有了显著改善，然而，结果显示其略低于冰的密度。
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