Exploiting SU(N ) dynamical symmetry for rovibronic stabilization of a weakly bound diatomic molecule

We propose a multilevel scheme to coherently transfer the population of a diatomic molecule from a rovibrational level to a target rovibrational level of the same electronic state or another. It involves a linear chain of N rovibrational levels alternating between the initial electronic state and a second electronic state, conveniently selected according to the dipole couplings between consecutive levels. A set of N - 1 simultaneous weak laser π pulses, with simple analytical shapes, each in resonance between two neighbors of the chain, transfers the population from the initial rovibronic state gradually and consecutively through the chain, until at the end of the process it resides in the target rovibronic state, as in a kind of ping-pong game between the two electronic states. Using the partial-wave expansion of the molecular wave function, vibrational bases within the J manifolds of each electronic state, and the rotating-wave approximation (RWA), we map the radial Hamiltonian to the one of a spin s = (N - 1)/2 under a static magnetic field, providing an analytical formula for the populations of the linked states. As an illustration, we apply the scheme to the stabilization into the absolute ground state of a KRb molecule initially in the high-lying upsilon = 75, J = 6 level of the ground electronic state X¹Σ⁺. With a chain of seven rovibronic states, three of them belonging to the excited A¹Σ⁺ electronic state, and pulses of 0.4 ns of duration, the population is fully transferred into the target state in about 1 ns.