Spin eigenstate-dependent Hartree—Fock molecular dynamics

Abstract For the first time we present a fully ab initio molecular dynamics scheme for the treatment of many-electron ground and excited electronic states at the Hartree—Fock level using traditional Gaussian basis sets. The method is designed to simulate dynamics with first principles forces and to find global potential energy minima. Our first test examples concern the dynamics of singlet and triplet Na 4 . We find this cluster to exhibit strongly state-dependent dynamical behaviour that would not be observed in classical simulations.

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