RESONANCE-ENHANCED PHOTOASSOCIATIVE FORMATION OF GROUND-STATE Rb$_2$ AND SPECTROSCOPY OF MIXED-CHARACTER EXCITED STATES

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We describe experimental and theoretical studies of the effects of resonant electronic state coupling on the formation of ultracold ground-state 85Rb2. The molecules are formed by photoassociation of ultracold atoms in a MOT into the 0u+ state converging to the 5S+5P1/2 limit, followed by radiative decay into high vibrational levels of the ground electronic state, X 1Σg+. The populations of these high-v ground-state levels are monitored by resonance-enhanced two-photon ionization (R2PI) through the 2 1Σu+ state. We find that the populations of vibrational levels v=112-116 are far larger than can be accounted for by the Franck-Condon factors for 0u+←X 1Σg+ transitions. Further, the total number of ground-state molecules formed by this process exhibits oscillatory behavior as the PA laser is tuned through a succession of 0u+ state vibrational levels. Both of these effects are explained by a new calculation of transition amplitudes that includes the resonant character of the spin-orbit coupling between the two 0u+ states converging to the 5P1/2 and 5P3/2 limits. The resulting enhancement of more deeply bound ground-state molecule formation will be useful for future experiments on ultracold molecules. \vspace{12 pt} We also describe evidence from our R2PI spectra for extensive singlet-triplet mixing between excited states of Rb2 at intermediate internuclear separations, apparently also induced by spin-orbit interactions. In particular, the 3 1Σg+ and 1 1Δg states converging to 5s+4d have been observed in excitation from the a 3Σu+ state,}, 261 (2006).} and the 2 3Πu state has been observed in excitation from the X 1Σg+ state.

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Author Institution: Physics Department, University of Connecticut, Storrs, CT 06269; Institut fur Theoretische Physik, Freie Universitat Berlin, 14195 Berlin, Germany

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