Implementation of a time-dependent multiconfiguration self-consistent-field method for coupled electron-nuclear dynamics in diatomic molecules driven by intense laser pulses

We present an implementation of a time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method [R. Anzaki et al., Phys. Chem. 19, 22008 (2017)] with the full configuration interaction expansion for coupled electron-nuclear dynamics in diatomic molecules subject to strong laser field. In this method, total wave function is expressed as superposition different configurations constructed from electronic Slater determinants and orthonormal nuclear basis functions. The primitive functions nuclei electrons are strictly independent each other without invoking Born-Oppenheimer approximation. Our treats motion its dimensionality on curvilinear coordinates, while propagated one-dimensional stretching coordinate rotational neglected. apply high-harmonic generation dissociative ionization hydrogen molecule discuss role correlation.