论文标题
通过多碎片密度矩阵嵌入的多站点反应动力学
Multi-site Reaction Dynamics Through Multi-fragment Density Matrix Embedding
论文作者
论文摘要
无序化学反应的实际描述，其中涉及多个位点的多种物种，目前使用相关的电子结构方法挑战。在这里，我们描述了多碎片密度矩阵嵌入理论的梯度理论，该理论有可能提供最小的计算框架，以在相关电子级别对此类过程进行建模。我们介绍了梯度理论的推导和实施，使用密度矩阵嵌入对模型系统的验证以及化学反应的验证，以及在小水群中质子转运的分子动力学模拟中的应用，这是多站点反应动力学的一个简单示例。
The practical description of disordered chemical reactions, where reactions involve multiple species at multiple sites, is presently challenge using correlated electronic structure methods. Here we describe the gradient theory of multi-fragment density matrix embedding theory, which potentially provides a minimal computational framework to model such processes at the correlated electron level. We present the derivation and implementation of the gradient theory, its validation on model systems and chemical reactions using density matrix embedding, and its application to a molecular dynamics simulation of proton transport in a small water cluster, a simple example of multi-site reaction dynamics.
