Observation of blue-shifted ultralong-range Cs₂ Rydberg molecules

We observe ultralong-range blue-shifted Cs$_{2}$ molecular states near $ns_{1/2}$ Rydberg states in an optical dipole trap, where $31\leq n\leq34$. The accidental near degeneracy of $(n-4)l$ and $ns$ Rydberg states for $l>2$ in Cs, due to the small fractional $ns$ quantum defect, leads to non-adiabatic coupling among these states, producing potential wells above the $ns$ thresholds. Two important consequences of admixing high angular momentum states with $ns$ states are the formation of large permanent dipole moments, $\sim 15-100\,$Debye, and accessibility of these states via two-photon association. The observed states are in excellent agreement with theory. Both projections of the total angular momentum on the internuclear axis are visible in the experiment.