Theoretical Development of Predicted Iteration Method for Considering Electron Dynamics in Quantum Molecular Dynamics

In the present study, a theoretical principle of molecular dynamics methods is developed, in which electron transfers are taken into account effectively based on quantum mechanics. In chemical reaction systems, electrodynamics should be considered in the molecular dynamics simulation because electron transfers play an important role. In this study, an effective procedure is proposed to treat time evolutions of electronic wavefunctions. In the procedure, electronic wavefunctions can be transformed to other spaces such as Mulliken atomic charges or electrostatic potentials, and then their time evolutions are coupled with the motions of ionic cores. The present method is applied to some chemical reaction systems, and charge transfer effects can be treated successfully in molecular dynamics simulations. The importance of a coupling method of molecular dynamics and electrodynamics is described.