PBFC-PI量子动力学方法及应用

对多原子体系的量子动力学计算非常重要, 然而, 对含六原子以上的分子体系进行精确量子动力学计算仍具挑战性. 面向过程的基函数定制(PBFC)-并行迭代(PI)方法是一种高效的量子动力学方法, 已应用于对含九原子的丙二醛异构体系的氢迁移速率的精确量子计算. 本综述首先阐明了PBFC的基本思想, 之后重点回顾了PBFC-PI方法的具体内容、 该方法与其它方法的结合及其应用方面的新进展. 应用这些方法实现了对单氢迁移、 协同双氢迁移和分步双氢迁移3种类型基准体系的大规模并行计算, 有助于获得对氢迁移过程的新认识.

The PBFC-PI Quantum Dynamical Method and Its Applications

Quantum dynamics（QD） calculations of polyatomic systems are very important， however， accurate QD calculations for molecular system with more than six atoms remain a challenge nowadays. The process-oriented basis function customization（PBFC）-parallelized iterative（PI） method is an e?cient QD method developed by Bian’s group， which has been applied in accurate QD calculations of H transfer rate in malonaldehyde， a nine-atom isomerization system. In this review， we ?rst present an explanation on the basic idea of PBFC， which may have general importance， and then focus on the details of the PBFC-PI method， its combination with other methods and the recent progresses in its applications. Using these methods， large-scale parallel calculations have been performed for three kinds of benchmark systems， featuring single H transfer， concerted double H transfer， and sequential double H transfer， respectively. These calculations are helpful for acquiring new insights into H transfer processes.