Abstract
We combine optimal control theory with the multi-configuration time-dependent Hartree–Fock method to control the dynamics of interacting particles. We use the resulting scheme to optimize state-to-state transitions in a one-dimensional (1D) model of helium and to entangle the external degrees-of-freedom of two rubidium atoms in a 1D optical lattice. Comparisons with optimization results based on the exact solution of the Schrödinger equation show that the scheme can be used to optimize even involved processes in systems consisting of interacting particles in a reliable and efficient way.