All-optical cw quadruple resonance excitation: A coherently driven five-level molecular system

Abstract

We report here a continuous-wave, high-resolution, and all-optical quadruple resonance laser excitation experiment. To demonstrate this excitation technique, we have used an inhomogeneously broadened molecular sample (Na-2). We emphasize the enhanced ability afforded by the technique to reach new ranges of internuclear separation as well as access to a large range of molecular electronic states. Using the Autler-Townes split line shape of a rovibronic transition and the E field amplitude of the corresponding coupling laser, we have measured with high precision the absolute value of the molecular electronic transition dipole moment matrix elements, with more flexibility than the double and the triple resonance based excitation schemes used previously. This technique may also be used in a stimulated Raman adiabatic passage configuration for effective transfer of ultracold molecules, formed at long internuclear distance, to the lowest vibrational level of the ground electronic state. (Less)