Better models of solvation in quantum chemistry

目前，模拟化学过程溶剂化的主要竞争技术是QM/MM，其中溶质的量子力学处理是在溶剂的分子力学模型中处理的；连续介质溶剂化模型，其中考虑了溶剂的介电响应。两者都有各自的优点，但前者的主要缺点是需要大量的热力学采样；后者的主要缺点是缺乏对介电屏蔽以外的任何影响的处理。在这个项目中，我们的目标是为溶剂化建立更好的理论模型，提高重要物理效应的覆盖范围，同时仍然避免需要昂贵的模拟。三个关键要素是：(1)包括电介质屏蔽以外的效应，如泡利排斥和色散；(2)建立正确解释溶剂对溶质分子结构影响的模型，包括解释形成空腔的能量消耗的术语；(3)在过渡金属均相催化剂的严格测试和化学应用领域的优化

Presently the key competing techniques for modelling solvation of chemical processes are QM/MM, in which the quantum mechanical treatment of the solute is treated in a molecular mechanical model of the solvent; and continuum solvation models, in which the dielectric response of the solvent is considered. Both have their strengths, but the key disadvantage of the former is the need for extensive thermodynamic sampling; and the key disadvantage of the latter is lack of treatment of any effect beyond dielectric screening. In the project we aim to build better theoretical models for solvation, improving the coverage of important physical effects whilst still avoiding the need for expensive simulations. The three key elements are: (1) inclusion of effects other than dielectric screening, such as Pauli repulsion and dispersion; (2) construction of models that correctly account for the effect of the solvent on molecular structure of the solute, by including terms to account for the energetic const of forming the cavity; and (3) rigorous testing and chemical applications in the field of optimization of transition metal homogeneous catalysts