Ab initio study of water. II. Liquid structure, electronic and thermodynamic properties over a wide range of temperature and density
Ab initio study of water. II. Liquid structure, electronic and thermodynamic properties over a wide range of temperature and density
复制标题
水的从头开始研究。
DOI：
10.1063/1.480195
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发表时间：
1999
影响因子：
4.4
通讯作者：
F. Hirata
中科院分区：
文献类型：
--
作者：
Hirofumi Sato;F. Hirata
采用从头算分子轨道理论结合液体积分方程方法，在较宽的温度（0°-600 °C）和密度（0.6- 1.4g/cm ~ 3）范围内，研究了水的电子结构、液体结构及其热力学性质.与通过包括分子模拟的经典统计力学对水的标准处理不同，水分子中氧原子和氢原子上的有效电荷不是“输入参数”，而是在液体中电子结构和密度对相关函数的自洽确定过程中从理论中自然预测的。结果表明，分子的偶极矩和电子极化能随温度和密度的增加而减小。偶极矩的理论计算结果与NMR化学位移结合分子动力学模拟确定的实验数据定量雅阁。松林角若井...
The electronic and liquid structures of water and its thermodynamic properties are studied over a wide range of temperature (0°–600 °C) and density (0.6–1.4 g/cm3) based on the ab initio molecular orbital theory combined with the integral equation method of liquid. Unlike standard treatments of water by means of the classical statistical mechanics including molecular simulations, the effective charges on oxygen and hydrogen atoms in water molecules are not “input parameters,” but naturally predicted from the theory in the course of self-consistent determination of the electronic structure and the density pair correlation functions in liquids. It is found that the molecular dipole moments and electronic polarization energies decrease with increasing temperature and/or density. The theoretical results for dipole moments are in quantitative accord with the experimental data, which has been determined based on the NMR chemical shift coupled with the molecular dynamics simulation [N. Matsubayashi, C. Wakai, an...