Quantum-classical Liouville approach to molecular dynamics: Surface hopping Gaussian phase-space packets

Abstract

A mixed quantum-clasical model for the dynamics of large molecular systems was worked out allowing for a quantum treatment of the most important degrees of freedom. In particular, it was shown how the surface hopping trajectory procedure can be derived from the QCLE essentially relying on two additional assumptions. The limitations of this approach can be overcome in the SHG approach using sets of surface hopping Gaussian phase-space packets to represent densities and coherences in phase space. The possibility to evaluate the action of nonlocal operators in phase space allows to perform simulations beyond the momentum jump approximation.