Multi-configuration electron–nuclear dynamics: An open-shell approach

Abstract

The multi-configuration electron–nuclear dynamics for open shell systems with a spin-unrestricted formalism is described. The mean fields are evaluated using second-order reduced density matrices for electronic and nuclear degrees of freedom. Applications to light-element diatomics including equilibrium geometries, electronic energies, dipole moments, and absorption spectra are presented. The von Neumann entropies for different spin states of a LiH molecule are compared.