Atomic lattice clocks have spurred numerous ideas for tests of fundamental physics, detection of general relativistic effects, and studies of interacting many-body systems. On the other hand, molecular structure and dynamics offer rich energy scales that are at the heart of new protocols in precision measurement and quantum information science. Here we demonstrate a fundamentally distinct type of lattice clock that is based on vibrations in diatomic molecules, and present coherent Rabi oscillations between weakly and deeply bound molecules that persist for 10's of milliseconds. This control is made possible by a state-insensitive magic lattice trap that weakly couples to molecular vibronic resonances and enhances the coherence time between molecules and light by several orders of magnitude. The achieved quality factor Q = 8 × 10 11 results from 30-Hz narrow resonances for a 25-THz clock transition in Sr2. Our technique of extended coherent manipulation is applicable to long-term storage of quantum information in qubits based on ultracold polar molecules, while the vibrational clock enables precise probes of interatomic forces, tests of Newtonian gravitation at ultrashort range, and model-independent searches for electron-to-proton mass ratio variations.

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The collective absorption and emission of light by an ensemble of atoms is at the heart of many fundamental quantum optical effects and the basis for numerous applications. However, beyond weak excitation, both experiment and theory become increasingly challenging. Here, we explore the regimes from weak excitation to inversion with ensembles of up to one thousand atoms that are trapped and optically interfaced using the evanescent field surrounding an optical nanofiber. We realize strong inversion, with about 80 % of the atoms being excited, and study their subsequent radiative decay into the guided modes. The data is very well described by a simple model that assumes a cascaded interaction of the guided light with the atoms. Our results contribute to the fundamental understanding of the collective interaction of light and matter and are relevant for applications ranging from quantum memories to sources of nonclassical light to optical frequency standards.