Simulation of Chemical Processes in Solution using Hybrid Quantum and Molecular Mechanical Methods

明尼苏达大学双城分校的Jiali Gao获得了理论，模型和计算方法奖的支持，以开发基于混合分子轨道和价键（MOVB）方法的从头计算价键模型，用于描述绝热和非绝热势能面。PI和他的研究小组利用量子力学和分子力学（QM/MM）相结合的方法进行动力学模拟。 他们正在开发一个基于从头算价键理论的QM/MM模型体系，用于研究凝聚相中的化学反应。 他们 采用从头算自洽场价键理论来处理量子力学子系统，以用作指导来制定基于分子轨道理论的定义良好的两态MOVB模型。此外，他们正在开发一种有效的哈密顿MOVB方法，可以方便地校准和实验人员用来研究溶液中的化学反应性和动力学。 最后，他们将MOVB方法扩展到密度泛函理论领域。这项研究的重点是设计计算方法来研究溶液中的化学反应，特别是那些与溶剂本身相互作用起主要作用的系统。 这些研究使我们对凝聚相中的溶剂效应和化学反应性有了更深入的了解。PI和他的同事们已经将他们的方法应用于广泛可用的软件包中，供生物化学，化学，生物物理学，工程学，催化和大气科学等许多领域的非理论家使用。

Jiali Gao of the University of of Minnesota, Twin Cities is supported by an award from the Theory, Models and Computational Methods to develop an ab initio valence bond model based on a mixed molecular orbital and valence bond (MOVB) approach for the description of the adiabatic and diabatic potential energy surfaces. The PI and his research group make use of combined quantum mechanical and molecular mechanical (QM/MM) methods to carry out dynamics simulations. They are developing a hierarchy of QM/MM models based on ab initio valence bond theory for studying chemical reactions in condensed phases. They employ an ab initio self-consistent field valence bond theory to treat the quantum mechanical subsystem for use as a guide to formulate a well-defined, two-state MOVB model based on molecular orbital theory. Additionally they are developing an effective Hamiltonian MOVB method that can be conveniently calibrated and used by experimentalists to study chemical reactivity and dynamics in solution. Finally, they are extending the MOVB method into the realm of density functional theory The focus of this research is to design computational methods to investigate chemical reactions in solution, particularly those systems where interactions with the solvent itself play a major role. These studies lead to a deeper understanding of solvent effects and chemical reactivity in condensed phases. The PI and his coworkers have implemented their methods in widely available software packages for use by non-theorists in many fields of biochemistry, chemistry, biophysics, engineering, catalysis and atmospheric science.