Nonadiabatic Dynamics at Metal Surfaces: Fewest Switches Surface Hopping with Electronic Relaxation
Zuxin Jin, Joseph E. Subotnik
Abstract
A new scheme is proposed for modeling molecular nonadiabatic dynamics near metal surfaces. The charge-transfer character of such dynamics is exploited to construct an efficient reduced representation for the electronic structure. In this representation, the fewest switches surface hopping (FSSH) approach can be naturally modified to include electronic relaxation (ER). The resulting FSSH-ER method is valid across a wide range of coupling strengths as supported by tests applied to the Anderson–Holstein model for electron transfer. Future work will combine this scheme with ab initio electronic structure calculations.
Topics & Concepts
Representation (politics)Surface hoppingElectronic structureRelaxation (psychology)Coupling (piping)Charge (physics)Ab initioStatistical physicsChemical physicsElectron transferSurface (topology)PhysicsMolecular dynamicsMaterials scienceComputer scienceChemistryCondensed matter physicsQuantum mechanicsPhysical chemistryPolitical scienceMetallurgyGeometryPsychologyLawMathematicsPoliticsSocial psychologySpectroscopy and Quantum Chemical StudiesElectrochemical Analysis and ApplicationsPhotochemistry and Electron Transfer Studies