Mixed Quantum/Classical Molecular Dynamics Simulations of Chemical Reactions in Clusters and in Solids

Abstract

Abstract An overview is given of a recent method for dynamical simulations of many‐atom systems, which incorporates also important quantum effects. The method treats a few pertinent degrees of freedom (e.g., a light atom) by time‐dependent wavepackets and all the other coordinates by classical trajectories. The classical and quantum subsystems are coupled in this approach by a hybrid quantum/classical Time‐Dependent Self‐Consistent Field (TDSCF) approximation. The properties, validity, range, and limitations of this method are discussed, and numerical tests of its accuracy are presented for simple model systems. The method is illustrated by applications to photodissociation of HI molecules in solid Xe and in Xe clusters of different sizes. The scope of potential applications, open problems, and possible directions of extending the method are discussed.