Theory of Chemistry beyond the Born-Oppenheimer Concept

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We have proposed and established a quantum chemical theory beyond the Born-Oppenheimer paradigm ; a simultaneous quantum theory of nonadiabatically coupled electronic and nuclear wavepacket dynamics on-the-fly scheme. All the electronic wavefunctions to be treated are necessarily time-dependent and thereby beyond stationary state quantum chemistry based on the Born-Oppenheimer framework. Nonadiabatic electronic-state mixing is realized along branching non-Born-Oppenheimer paths, through which their bifurcations, strong quantum entanglement between nuclear electronic motions, and coherence and decoherence among the phases associated with them are properly represented. Chemical theory and its applications of dynamical electrons in molecules under intense electromagnetic fields have been developed, in which real-time tracking of electronic states is performed in the ultimate aim of control of chemical reactions.