Dissipative quantum dynamics using the stochastic surrogate Hamiltonian approach

Based on the original Stochastic Surrogate Hamiltonian approach for the simulation of open quantum system dynamics, we present a modified algorithm for the swap procedure. The implementation is tested with nuclear relaxation dynamics of model systems known from literature, i.e., the harmonic oscillator and the Morse oscillator. Finally, the stochastic surrogate Hamiltonian is applied to simulate the dynamical electronic excitation and relaxation of a photodesorption process. This is the first application of the stochastic surrogate Hamiltonian in an ab initio context. A comparison to a surrogate Hamiltonian benchmark allows us to evaluate the results obtained. For this purpose, the well-studied laser-induced desorption of NO from NiO(100) is chosen.