We report the engineering of molecular potentials at large interatomic distances. The molecular states are generated by off-resonant optical coupling to a highly excited, long-range Rydberg molecular potential. The coupling produces a potential well in the low-lying molecular potential, which supports a bound state. The depth of the potential well, and thus the binding energy of the molecule, can be tuned by the coupling parameters. We characterize these molecules and find good agreement with a theoretical model based on the coupling of the two involved adiabatic potential energy curves. Our results open numerous possibilities to create long-range molecules between ultracold ground-state atoms and to use them for ultracold chemistry and applications such as Feshbach resonances, Efimov physics, or the study of halo molecules.

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• Cold and ultracold molecules
• Interatomic & molecular potentials
• Long-range interactions
• Photoassociation
• Potential energy surfaces