Towards Time-Dependent Density-Functional Theory for Molecules in Strong Laser Pulses

To describe the dynamical interplay of electronic and nuclear degrees of freedom in molecules exposed to strong laser pulses, we present two different variational approaches based on the statonary-action principle: A mean-field treatment of the electron-nuclear interaction and an explicitly correlated ansatz. The two methods are tested on a one-dimensional model of H 2 + which can be solved exactly. The correlated approach significantly improves upon the mean-field treatment, especially in the case of laser fields strong enough to cause substantial dissociation.