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, from ab initio calculations, we identify antiferromagnetic ground states in structurally preferred monoclinic ${\mathrm{CePO}}_4$ and tetragonal ${\mathrm{CeVO}}_4$ exhibiting localized occupied and unoccupied Ce $4f$ states with $4f\text{−}4f$ transition characteristics. Interestingly, in ${\mathrm{CePO}}_4$, O $2p$ and P $3p$ states hybridize negligibly with Ce $4f$ states, while in ${\mathrm{CeVO}}_4$, 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 ${\mathrm{CePO}}_4$ and ${\mathrm{CeVO}}_4$ 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 ${\mathrm{CePO}}_4$, is relevant for quantum memories and $D_{2d}$ site symmetry of Ce exhibiting inversion symmetry in ${\mathrm{CeVO}}_4$ is relevant for quantum transduction.

Close

PrevNext

View figure in article

• Crystal-field excitations
• Electronic structure
• Magnetism
• Spin-phonon coupling
• Rare-earth magnetic materials
• Density functional calculations