DOE OSTI2025
Rare-earth containing wide band gap oxides, which provide spin-photon interface and narrow linewidth optical emission, are getting significant attention as the most promising candidate materials in advancing quantum transduction and memories. Here, in this work, from ab initio calculations, we identify antiferromagnetic ground states in structurally preferred monoclinic CePO 4 and tetragonal CeVO 4 exhibiting localized occupied and unoccupied Ce 4𝑓 states with 4𝑓−4𝑓 transition characteristics. Interestingly, in CePO 4 , O 2𝑝 and P 3𝑝 states hybridize negligibly with Ce 4𝑓 states, while in CeVO 4 , V 3𝑑 and O 2𝑝 states hybridize and appear as extended states in between the occupied and unoccupied Ce 4𝑓 states. Here, phonon calculations and analysis identify and differentiate Raman active phonon modes along with the spin phonon coupling of Ce in both CePO 4 and CeVO 4 that ultimately lead to different 4𝑓 ground-state crystal-field multiplets, which are critical to accurately describe electronic transitions for foundational quantum transduction and memories. Further, the identified 𝐶 1 site symmetry of Ce, lacking inversion symmetry in CePO 4 , is relevant for quantum memories and 𝐷 2𝑑 site symmetry of Ce exhibiting inversion symmetry in CeVO 4 is relevant for quantum transduction.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗