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The success of the emerging field of solid-state optical quantum informationprocessing (QIP) critically depends on the access to resonant opticalmaterials. Rare-earth ions (REIs) are suitable candidates for QIP protocols dueto their extraordinary photo-physical and magnetic quantum properties such aslong optical and spin coherence lifetimes ($T_2$). However, moleculesincorporating REIs, despite having advantageous properties such as atomicallyexact quantum tunability, inherent scalability, and large portability, have notyet been studied for QIP applications. As a first testimony of the usefulnessof REI molecules for optical QIP applications, we demonstrate in this studythat narrow spectral holes can be burned in the inhomogeneously broadened$^5$D$_0\to^7$F$_0$ optical transition of a binuclear Eu(III) complex,rendering a homogeneous linewidth ($\Gamma_h$) = 22 $\pm$ 1 MHz, whichtranslates as $T_2 = 14.5$ $\pm$ 0.7 ns at 1.4 K. Moreover, long-lived spectralholes are observed, demonstrating efficient polarization of Eu(III) groundstate nuclear spins, a fundamental requirement for all-optical spininitialization and addressing. These results elucidate the usefulness ofREI-based molecular complexes as versatile coherent light-spin interfaces forapplications in quantum communications and processing.

Molecule-based coherent light-spin interfaces for quantum information processing -- optical spin state polarization in a binuclear Europium complex