Defect Engineering for Quantum Grade Rare-Earth Nanocrystals

Nanostructured systems that combine optical and spin transitions offer new functionalities for quantum technologies by providing efficient quantum light-matter interfaces. Rare-earth (RE) ion-doped nanoparticles are promising in this field as they show long-lived optical and spin quantum states. However, further development of their use in highly demanding applications, such as scalable single-ion-based quantum processors, requires controlling defects that currently limit coherence lifetimes. In this work, we show that a post-treatment process that includes multistep high-temperature annealing followed by high-power microwave oxygen plasma processing advantageously improves key properties for quantum technologies. We obtain single crystalline Eu3+:Y2O3 nanoparticles (NPs) of 100 nm diameter, presenting bulk-like inhomogeneous line widths (Γinh) and population lifetimes (T1). Furthermore, a significant coherence lifetime (T2) extension, up to a factor of 5, is successfully achieved by modifying the oxygen-related point defects in the NPs by the oxygen plasma treatment. These promising results confirm the potential of engineered RE NPs to integrate devices such as cavity-based single-photon sources, quantum memories, and processors. In addition, our strategy could be applied to a large variety of oxides to obtain outstanding crystalline quality NPs for a broad range of applications.