A size-consistent multi-state mapping approach to surface hopping
Joseph E. Lawrence, Jonathan R. Mannouch, Jeremy O. Richardson
Abstract
We develop a multi-state generalization of the recently proposed mapping approach to surface hopping (MASH) for the simulation of electronically nonadiabatic dynamics. This new approach extends the original MASH method to be able to treat systems with more than two electronic states. It differs from previous approaches in that it is size consistent and rigorously recovers the original two-state MASH in the appropriate limits. We demonstrate the accuracy of the method by applying it to a series of model systems for which exact benchmark results are available, and we find that the method is well suited to the simulation of photochemical relaxation processes.
Topics & Concepts
Benchmark (surveying)Surface hoppingGeneralizationState (computer science)Surface (topology)Statistical physicsComputer scienceSeries (stratigraphy)Relaxation (psychology)AlgorithmMathematicsPhysicsMolecular dynamicsQuantum mechanicsGeometryCartographyMathematical analysisBiologyGeographySocial psychologyPsychologyPaleontologySpectroscopy and Quantum Chemical StudiesAdvanced Chemical Physics StudiesQuantum, superfluid, helium dynamics