Higher-Order Split Operator Schemes for Solving Tetratomic Reactions Using the Time-Dependent Wave Packet Method.

ABSTRACT

In this work, using the time-dependent quantum wave packet method, quite a few typical higher-order split operators (HOSOs) were for the first time applied to calculate the tetratomic reactive scattering processes in the hyperspherical coordinate. It was found that the HOSOs were hardly efficient for a tetratomic reaction calculation, unlike those for a triatomic reactive scattering calculation. We proposed an efficient HOSO with a force gradient (denoted as 2G1 in the main text) for efficiently and accurately calculating a tetratomic reaction using the quantum wave packet method. Several typical tetratomic reactions, such as H2 + OH, HF + OH, and H2 + OH+, are calculated for demonstrating the effectiveness of the proposed 2G1 in terms of (product state-resolved) reaction probability and inelastic probability, by comparing with the performance of the previously reported various HOSOs. We suggest that the 2G1 propagator could be applied to efficiently calculate a general tetratomic reaction.