Time-dependent approach to electronically excited states of molecules with the multiconfiguration time-dependent Hartree-Fock method

Abstract

In this paper the authors show how the multiconfiguration time-dependent Hartree-Fock (MCTDHF) method can be used for the calculation of electronic properties of molecules associated with the population of excited states. In contrast to other methods for correlated electron dynamics, such as configuration interaction, MCTDHF does not rely on a solution of the electronic Schrodinger equation prior to the propagation. The authors apply this approach to the calculation of vertical excitation energies, transition dipole moments, and oscillator strengths for two test molecules, lithium hydride and methane.