论文标题
杂交QM/mm相互作用的非局部动力学密度的开发
Development of Nonlocal Kinetic-Energy Density Functional for the Hybrid QM/MM Interaction
论文作者
论文摘要
电子动能密度功能的发展是对理论物理和化学的主要兴趣的主题。在这项工作中，非局部动力学功能是根据分子系统的响应函数开发的，以实现在混合QM/MM（量子机械/分子机械）方法中使用的轨道无轨道密度功能理论（DFT）。目前的方法与以前的功能形成了鲜明的对比，在该功能中，同质电子气体作为构建响应函数的参考。作为基准测试，我们将该方法应用于二聚体系统中的QM水分子，并嵌入在冷凝环境中，以与使用Kohn-Sham DFT的QM/MM计算给出的结果进行比较。发现在MM环境的影响下，QM溶质的能量和极化密度可以通过我们的方法充分再现。这项工作表明，基于分子参考系统的响应函数，动力学功能的潜在能力。
Development of the electronic kinetic-energy density functional is a subject of major interest in theoretical physics and chemistry. In this work, the nonlocal kinetic-energy functional is developed in terms of the response function for the molecular system to realize the orbital free density-functional theory(OF-DFT) to be utilized in the hybrid QM/MM(quantum mechanical/molecular mechanical) method. The present approach shows a clear contrast to the previous functionals where the homogeneous electron gas serves as a reference to build the response function. As a benchmark test we apply the method to a QM water molecule in a dimer system and that embedded in a condensed environment to make comparisons with the results given by the QM/MM calculations employing the Kohn-Sham DFT. It was found that the energetics and the polarization density of the QM solute under the influence of the MM environment can be adequately reproduced with our approach. This work suggests the potential ability of the kinetic-energy functional based on the response functions for the molecular reference systems.
