Microwave photo-association of fine-structure-induced Rydberg $(n+2)D_{5\mathrm{/}2}n{F}_J$ macro-dimer molecules of cesium

Long-range $(n+2)D_{5\mathrm{/}2}n{F}_J$ Rydberg macro-dimers are observed in an ultracold cesium Rydberg gas for $39\le n\le 48$. Strong dipolar “flip” ($⟨D_{5\mathrm{/}2}{F}_{5\mathrm{/}2}\mathrm{\mid }{\widehat{V}}_{dd}\mathrm{\mid }{F}_{5\mathrm{/}2}{D}_{5\mathrm{/}2}⟩$, $⟨D_{5\mathrm{/}2}{F}_{7\mathrm{/}2}\mathrm{\mid }{\widehat{V}}_{dd}\mathrm{\mid }{F}_{7\mathrm{/}2}{D}_{5\mathrm{/}2}⟩$) and “cross” ($⟨D_{5\mathrm{/}2}{F}_{7\mathrm{/}2}\mathrm{\mid }{\widehat{V}}_{dd}\mathrm{\mid }{F}_{5\mathrm{/}2}{D}_{5\mathrm{/}2}⟩$) couplings lead to bound, fine-structure-mixed $(n+2)D_{5\mathrm{/}2}n{F}_J$ macro-dimers at energies between the $F_J$ fine-structure levels. The $DF$ macro-dimers are measured by microwave photo-association from optically prepared $[(n+2)D_{5\mathrm{/}2}{]}_2$ Rydberg pair states. Calculated adiabatic potential curves are used to elucidate the underlying physics and to model the $DF$ macro-dimer spectra, with good overall agreement. Microwave photo-association allows Franck-Condon tuning, which we have studied by varying the detuning of a Rydberg-atom excitation laser. Further, in Stark spectroscopy we have measured molecular DC electric polarizabilities that are considerably larger than those of the atomic states. The large molecular polarizabilities may be caused by high-$\mathrm{\ell }$ mixing. The observed linewidths of the Stark-shifted molecular lines provide initial evidence for intra-molecular induced-dipole-dipole interaction.