title: Semiclassical Monte-Carlo approach for modelling non-adiabatic dynamics in extended molecules.
abstract: Modelling of non-adiabatic dynamics in extended molecular systems and solids is a next frontier of atomistic electronic structure theory. The underlying numerical algorithms should operate only with a few quantities (that can be efficiently obtained from quantum chemistry), provide a controlled approximation (which can be systematically improved) and capture important phenomena such as branching (multiple products), detailed balance and evolution of electronic coherences. Here we propose a new algorithm based on Monte-Carlo sampling of classical trajectories, which satisfies the above requirements and provides a general framework for existing surface hopping methods for non-adiabatic dynamics simulations. In particular, our algorithm can be viewed as a post-processing technique for analysing numerical results obtained from the conventional surface hopping approaches. Presented numerical tests for several model problems demonstrate efficiency and accuracy of the new method.
authors.affiliation: Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA.
authors.forename: Vyacheslav N
authors.initials: VN
authors.lastname: Gorshkov
authors.forename: Sergei
authors.initials: S
authors.lastname: Tretiak
authors.forename: Dmitry
authors.initials: D
authors.lastname: Mozyrsky