Classical blended quantum formulation of the parallel TDDVR method to the dynamics on furan

Abstract

A major portion (∼98%) of the quantum-classical molecular dynamics approach, namely, Time-Dependent Discrete Variable Representation (TDDVR) method, is recently parallelized using shared-memory parallelization scheme with the aim of performing dynamics on relatively large molecular systems. Therefore, we have chosen the furan as a model system for dynamical simulation. Four lowest singlet excited electronic states 1A2(3s), 1B2(V), 1A1(V*), and 1B1(3p) of furan are vibronically coupled through several conical intersections in the vicinity of Frank-Condon region. The major focus of the present paper is to explore the efficiency of our newly implemented parallelized TDDVR algorithm to perform dynamics on large dimensional quantum systems in vibronically coupled electronic manifold. The present version of parallelized TDDVR algorithm show closely linear speed up with increasing number of computing processors. As a significant speed up is achieved by cycling in the correct way over arrays, all dynamical simulations are performed within a reasonable wall clock time. The photoelectron spectra calculated by the TDDVR method show peak by peak correspondence with the experimental spectra. The TDDVR calculated quantum-classical dynamical outcomes, viz., population and photoelectron spectra, etc. show good agreement with the findings of the well-established quantum dynamical method, i.e. Multi Configuration Time-Dependent Hartree (MCTDH) approach.