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An impurity interacting with an ultracold Fermi gas can form either a polaron state or a dressed molecular state, the molaron, in which the impurity forms a bound state with one gas particle. This molaron state features rich physics, including a negative effective mass around unitarity and a first-order transition to the polaron state. However, these features have remained so far experimentally inaccessible. In this work we show theoretically how the molaron state can be directly prepared experimentally even in its excited states using Raman spectroscopy techniques. Initializing the system in the ultrastrong coupling limit, where the binding energy of the molaron is much larger than the Fermi energy, our protocol maps out the momentum-dependent spectral function of the molecule. Using a diagrammatic approach we furthermore show that the molecular spectral function serves as a direct precursor of the elusive Fulde-Ferell-Larkin-Ovchinnikov phase, which is realized for a finite density of fermionic impurity particles. Our results pave the way to a systematic understanding of how composite particles form in quantum many-body environments and provide a basis to develop new schemes for the observation of exotic phases of quantum many-body systems. Published by the American Physical Society2024