溶剂化体系线性响应性质的计算研究
Linear Response Properties of Solvated Systems: A Computational Study
摘要：
我们提出了一个静态和动态线性极化率在溶液中的计算研究。我们使用不同的理论方法来描述溶剂效应，从量子力学/分子力学（QM/MM）的量子嵌入方法。特别是，我们考虑非极化和极化QM/MM方法，后者的基础上的波动电荷（FQ）力场。此外，我们使用的量子嵌入方法的上下文中定义的多级Hartree-Fock（MLHF），其中系统被划分为活动和非活动区域，并结合它与第三层所描述的FQ模型的装置。多尺度的方法，然后用作参考波函数的运动方程耦合团簇（EOM-CC）的响应特性，允许电子相关的帐户。所开发的模型被施加到两个有机部分的线性响应特性的计算-即，对硝基苯胺和苯甲腈-在非水溶剂-1，4-二氧六环，乙腈，和四氢呋喃。计算的极化率，然后讨论的物理化学的溶质-溶剂相互作用所描述的每种方法（静电，极化和泡利排斥），最后与现有的实验参考。
英文摘要：
We present a computational study of static and dynamic linear polarizabilities in solution. We use different theoretical approaches to describe solvent effects, ranging from quantum mechanics/molecular mechanics (QM/MM) to quantum embedding approaches. In particular, we consider non-polarizable and polarizable QM/MM methods, the latter based on the fluctuating charge (FQ) force field. In addition, we use a quantum embedding method defined in the context of multilevel Hartree-Fock (MLHF), where the system is divided into active and inactive regions, and combine it with a third layer described by means of the FQ model. The multiscale approaches are then used as reference wave functions for equation-of-motion coupled cluster (EOM-CC) response properties, allowing for the account of electron correlation. The developed models are applied to the calculation of linear response properties of two organic moieties -- namely, para-nitroaniline and benzonitrile -- in non-aqueous solvents -- 1,4-dioxane, acetonitrile, and tetrahydrofuran. The computed polarizabilities are then discussed in terms of the physico-chemical solute-solvent interactions described by each method (electrostatic, polarization and Pauli repulsion), and finally compared with the available experimental references.
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