Singly occupied 4⁢𝑓 antiferromagnetic insulators: CePO4 and CeVO4

Paudyal, Hari; Limbu, Yogendra; Flatté, Michael E.; Paudyal, Durga

doi:10.1103/21wz-rcpn

Singly occupied 4⁢𝑓 antiferromagnetic insulators: CePO₄ and CeVO₄

Journal Article · Mon Oct 06 00:00:00 EDT 2025 · Physical Review. B

DOI:https://doi.org/10.1103/21wz-rcpn· OSTI ID:3011348

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Univ. of Iowa, Iowa City, IA (United States)
Univ. of Iowa, Iowa City, IA (United States); Eindhoven Univ. of Technology (Netherlands)

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 CePO₄ and tetragonal CeVO₄ exhibiting localized occupied and unoccupied Ce 4⁢𝑓 states with 4⁢𝑓−4⁢𝑓 transition characteristics. Interestingly, in CePO₄, O 2⁢𝑝 and P 3⁢𝑝 states hybridize negligibly with Ce 4⁢𝑓 states, while in CeVO₄, V 3⁢𝑑 and O 2⁢𝑝 states hybridize and appear as extended states in between the occupied and unoccupied Ce 4⁢𝑓 states. Here, phonon calculations and analysis identify and differentiate Raman active phonon modes along with the spin phonon coupling of Ce in both CePO₄ and CeVO₄ that ultimately lead to different 4⁢𝑓 ground-state crystal-field multiplets, which are critical to accurately describe electronic transitions for foundational quantum transduction and memories. Further, the identified 𝐶₁ site symmetry of Ce, lacking inversion symmetry in CePO₄, is relevant for quantum memories and 𝐷_2⁢𝑑 site symmetry of Ce exhibiting inversion symmetry in CeVO₄ is relevant for quantum transduction.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Iowa, Iowa City, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; SC0023393

OSTI ID:: 3011348

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 15 Vol. 112; ISSN 2469-9969; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Singly occupied 4⁢𝑓 antiferromagnetic insulators: CePO4 and CeVO4

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Singly occupied 4⁢𝑓 antiferromagnetic insulators: CePO₄ and CeVO₄