Coherent states/density functional theory approach to molecular dynamics

We present a combined coherent states (CS)/density functional theory approach to molecular dynamics within the electron nuclear dynamics framework. Nuclei are described by a product of narrow, frozen Gaussian wave packets that is approximately separable into translational, rotational, and vibrational CS parts. Electrons are described by a single-determinantal Thouless CS in a time-dependent Kohn–Sham fashion. This novel approach improves several features of the Car–Parrinello method by providing an ab initio CS Lagrangian, a quasi-classical CS description for the nuclei, and a non-redundant representation of a general electronic single-determinantal state. Preliminary simulations of the H+ + H2 reaction at ELab = 30 eV are also presented.