Quantum gas systems provide a unique experimental platform to study the crossover between Bose–Einstein condensed molecular pairs and Bardeen–Cooper–Schrieffer superfluidity. The few studies in optical lattices have so far focused on the case when only the lowest Bloch band is populated, thus excluding orbital degrees of freedom. Here we demonstrate the preparation of ultracold Feshbach molecules of fermionic atoms in the second Bloch band of an optical square lattice. We cover a wide range of interaction strengths, including the regime of unitarity in the middle of the crossover. Binding energies and band relaxation dynamics are measured by means of a method resembling mass spectrometry. We find that the longest lifetimes arise for strongly interacting Feshbach molecules at the onset of unitarity. In the case of strong confinement in a deep lattice potential, we observe bound dimers also for negative values of the scattering length, extending previous findings for molecules in the lowest band.
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