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Ultracold molecules have experienced increasing attention in recent years. Compared to ultracold atoms, they possess several unique properties that make them perfect candidates for the implementation of new quantum-technological applications in several fields, from quantum simulation to quantum sensing and metrology. In particular, ultracold molecules of two-electron atoms (such as strontium or ytterbium) also inherit the peculiar properties of these atomic species, above all, the possibility to access metastable electronic states via direct excitation on optical clock transitions with ultimate sensitivity and accuracy. We report on the production and coherent manipulation of molecular bound states of two fermionic 173Yb atoms in different electronic (orbital) states 1S0 and eP0 in the proximity of a scattering resonance involving atoms in different spin and electronic states, called orbital Feshbach resonance. We demonstrate that orbital molecules can be coherently photoassociated starting from a gas of ground-state atoms in a three-dimensional optical lattice by observing several photoassociation and photodissociation cycles. We also show the possibility to coherently control the molecular internal state by using Raman-assisted transfer to swap the nuclear spin of one of the atoms forming the molecule, thus demonstrating a powerful manipulation and detection tool of these molecular bound states. Finally, by exploiting this peculiar detection technique we provide the first information on the lifetime of the molecular states in a many-body setting, paving the way towards future investigations of strongly interacting Fermi gases in a still unexplored regime. G. Cappellini, et al. |