Analytical pulse design for controlling the vibrational dynamics of polar diatomic molecules

Based on the idea of reverse engineering, we present an analytical pulse design protocol for controlling the vibrational dynamics of polar diatomics in a given electronic state. Using the appropriately shaped midinfrared laser pulse, the potential energy function is altered via the electric permanent dipole moment such that the molecule is driven along the user-defined quantum pathway. The proposed control is validated by accurately solving the time-dependent Schrodinger equation of the HeH+ molecular ion with two completely different methods. We find that besides smooth transitions, arbitrary Rabi oscillations as well as vibrational ladder climbing can be efficiently controlled with the present scheme. As a result, the molecule is successively excited beyond the potential barrier, leading to enhanced dissociation in the ground electronic state (Phys. Rev. A 106, 043113, 2022).