Cavity-free continuum solvation: implementation and parametrization in a multiwavelet framework

Weighted-density functionals for cavity formation and dispersion energies in continuum solvation models

Continuum solvation models enable efficient first principles calculations of chemical reactions in solution, but require extensive parametrization and fitting for each solvent and class of solute systems. Here, we examine the assumptions of continuum solvation models in detail and replace empirical terms with physical models in order to construct a minimally-empirical solvation model. Specifically, we derive solvent radii from the nonlocal dielectric response of the solvent from ab initio calculations, construct a closed-form and parameter-free weighted-density approximation for the free energ…

隐式溶剂模型的自动参数化用于盲法预测溶解自由能

Automatic parametrization of implicit solvent models for the blind prediction of solvation free energies

本文提出系统协议自动参数化隐式溶剂模型，结合极性和非极性组件，通过分子相似性开发评分算法，利用668组实验数据验证，实现溶解自由能预测的高精度。

基于微分几何的溶剂化模型中的参数优化

Parameter optimization in differential geometry based solvation models

本文提出基于微分几何的溶剂化模型参数优化方法，通过扰动和凸优化理论稳定数值解，提升模型对极性和非极性分子的溶剂化自由能预测精度。

The charge-asymmetric nonlocally-determined local-electric (CANDLE) solvation model

Many important applications of electronic structure methods involve molecules or solid surfaces in a solvent medium. Since explicit treatment of the solvent in such methods is usually not practical, calculations often employ continuum solvation models to approximate the effect of the solvent. Previous solvation models either involve a parametrization based on atomic radii, which limits the class of applicable solutes, or based on solute electron density, which is more general but less accurate, especially for charged systems. We develop an accurate and general solvation model that includes a c…

Competitive Solvation of (Bis)(trifluoromethanesulfonyl)imide Anion by Acetonitrile and Water

Competitive solvation of an ion by two or more solvents is one of the key phenomena determining the identity of our world. Solvation in polar solvents frequently originates from non-additive non-covalent interactions. Pre-parametrized potentials poorly capture these interactions, unless the force field derivation is repeated for every new system. Development cost increases drastically as new chemical species are supplied. This work represents an alternative simulation approach, PM7-MD, by coupling the latest semiempirical parametrization, PM7, with equation-of-motion propagation scheme and tem…

利用量子化学模拟和隐式溶剂模型研究电化学双电层

Investigating the Electrochemical Double Layer with Quantum-Chemical Simulations and Implicit Solvation Models

本文通过量子化学模拟和隐式溶剂模型评估DRISM在电化学双电层建模中的表现，对比了Poisson-Boltzmann模型和显式分子动力学结果，发现Lennard-Jones参数对金属离子与金属水相互作用敏感，采用配对特定参数可提高模型准确性。