A quantum solute-solvent interaction using spectral representation technique applied to the electronic structure theory in solution
A quantum solute-solvent interaction using spectral representation technique applied to the electronic structure theory in solution
复制标题
使用光谱表示技术应用于溶液中电子结构理论的量子溶质-溶剂相互作用
DOI：
10.1063/1.1604381
复制
发表时间：
2003
影响因子：
4.4
通讯作者：
F. Hirata
中科院分区：
文献类型：
--
作者：
T. Yamazaki;Hirofumi Sato;F. Hirata
本文提出了一种处理溶液中分子电子结构的新方法。与参考相互作用位点模型自洽场理论等混合型方法不同，新方法不仅描述了溶质的电子结构，而且还描述了基于Hartree-Fock冻结密度公式的溶质-溶剂相互作用的量子化学。在处理中，由于溶剂的量子效应，包括交换排斥，投影到溶质的哈密顿使用光谱表示方法。溶质周围的溶剂分布由液体的积分方程理论处理。作为说明性的应用程序的方法，贵原子，氖和氩，在液体氖的电子和溶剂化结构进行了研究。我们还研究了液氦中过剩电子的电子结构。初步结果表明，由于溶剂分子的溶质的电子和溶剂化结构的量子力学效应是成功的表示的新方法。
In this paper, we present a new approach to treat the electronic structure of a molecule in solution. Unlike the hybrid-type method, such as the reference interaction site model self-consistent-field theory, the new approach describes not only the electronic structure of solute but also solute–solvent interactions in terms of the quantum chemistry based on the Hartree–Fock frozen density formulation. In the treatment, the quantum effect due to solvent, including exchange repulsion, is projected on to the solute Hamiltonian using the spectral representation method. The solvent distribution around the solute is handled by the integral equation theory of liquids. As illustrative applications of the approach, the electronic and solvation structure of noble atoms, neon and argon, in liquid neon are studied. We also investigate the electronic structure of an excess electron in liquid helium. The preliminary results demonstrate that the quantum-mechanical effect on the electronic and solvation structure of the solute due to solvent molecules is successfully represented by the new method.