一种用于一般态-态反应散射的交互渐近区域分解方法。

An interaction-asymptotic region decomposition method for general state-to-state reactive scatterings.

机构信息

State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People's Republic of China and Center for Advanced Chemical Physics and 2011 Frontier Centre for Quantum Science and Technology, University of Science and Technology of China, 96 Jinzhai Road, Hefei 230026, China.

Institute of Theoretical and Computational Chemistry, Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China.

出版信息

J Chem Phys. 2019 Apr 7;150(13):134105. doi: 10.1063/1.5085651.

DOI:10.1063/1.5085651

PMID:30954049

Abstract

A single set of coordinates, which is optimal for both asymptotic product and reactant, is difficult to find in a state-to-state reactive scattering calculation using the quantum wave packet method. An interaction-asymptotic region decomposition (IARD) method was proposed in this work to solve this "coordinate problem." In the method, the interaction region and asymptotic regions are applied with the local optimal coordinate system, i.e., hyperspherical and corresponding Jacobi coordinates. The IARD method is capable of efficiently and accurately accomplishing a calculation with a grid box for the Jacobi coordinate R extending several hundred bohrs for both reactant and product arrangements. We demonstrate the effectiveness of the IARD method with the reaction of H + HD, which is the simplest direct reaction, and F + HD, which is a typical reaction involving resonances with products of extremely slow translational energy and requires extremely long absorbing potential in all channels.

摘要

使用量子波包方法进行态-态反应散射计算时，很难找到同时对反应物和生成物都最优的一组坐标。本文提出了一种“坐标问题”的交互渐近区域分解（IARD）方法来解决这一问题。在该方法中，交互区域和渐近区域分别采用了局部最优坐标系，即超球坐标和相应的Jacobi 坐标。IARD 方法可以高效、准确地计算 Jacobi 坐标 R 的网格箱，对于反应物和生成物的排列，R 的取值可以延伸到几百个 Bohr。我们用 H + HD 的反应和 F + HD 的反应验证了 IARD 方法的有效性，这两个反应分别是最简单的直接反应和典型的包含共振的反应，生成物的平动能量极低，在所有通道中都需要非常长的吸收势。