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Rare-earth ions are promising solid state systems to build light-matterinterfaces at the quantum level. This relies on their potential to show narrowoptical homogeneous linewidths or, equivalently, long-lived optical quantumstates. In this letter, we report on europium molecular crystals that exhibitlinewidths in the 10s of kHz range, orders of magnitude narrower than othermolecular centers. We harness this property to demonstrate efficient opticalspin initialization, coherent storage of light using an atomic frequency comb,and optical control of ion-ion interactions towards implementation of quantumgates. These results illustrate the utility of rare-earth molecular crystals asa new platform for photonic quantum technologies that combines highly coherentemitters with the unmatched versatility in composition, structure, andintegration capability of molecular materials.

Rare-Earth Molecular Crystals with Ultra-narrow Optical Linewidths for Photonic Quantum Technologies