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PreprintCC BY-NC-ND 4.0HAL

Electron paramagnetic resonance of Dy3+-doped CaWO4: spin Hamiltonian, crystal-field analysis, and linear electric field effect

  • Achuthan Manoj Kumar
  • Larissa Aboudem-Joumessi
  • Remy Dassonneville
  • Adrien Savoyant
  • Karolina Waszowska
  • Pengrui Jiao
  • Patrice Bertet
  • Philippe Goldner
  • Sylvain Bertaina
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Abstract

We report an electron paramagnetic resonance (EPR) study of Dy3+ in CaWO4 single crystals spanning dopant concentrations from 80~ppb to 247~ppm. The g factors of the ground Kramers doublet at the S4 point-group site, g∥ = 7.22 ± 0.01 and g⊥ = 5.45 ± 0.01, and the hyperfine constants of \ce{^{161}Dy} and 163Dy are determined with an order-of-magnitude improvement in precision over the only previous report. A crystal-field analysis constrained jointly by published optical levels and by the measured g tensor identifies the ground doublet as the lower branch of an anticrossing between the near-degenerate |±11/2> and |∓13/2> states, and explains why optical data alone left the g values unconstrained. \add{The same parameter set, tested on the excited multiplets of the 6H term, reproduces the 6H13/2 crystal-field levels better than the optical parameters themselves.} The angular dependence of the linewidth in the ab plane reveals broadening by random internal electric fields through the linear electric field effect. Calibrating these fields with the residual Er3+ present in the same crystals yields the first electric-field coupling parameters of Dy3+, (B312+B362)1/2 = (34±5)×10−6~cm/V, three times the Er3+ value and the largest reported for a rare-earth ion in this host.The residual linewidth and the concentration-dependent lineshape asymmetry follow the quadratic field scaling expected for a second-order Stark shift, which escapes the inversion-site cancellation constraining the linear effect. Both couplings trace back to the ∼ 20~cm−1 gap to the first opposite-symmetry doublet, a consequence of the dense crystal-field structure of the J=15/2 manifold.

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Cite

BibTeXRIS
BibTeX
@misc{kumar2026electron,
  title = {{Electron paramagnetic resonance of Dy$^3+$-doped CaWO$_4$: spin Hamiltonian, crystal-field analysis, and linear electric field effect}},
  author = {Achuthan Manoj Kumar and Larissa Aboudem-Joumessi and Remy Dassonneville and Adrien Savoyant and Karolina Waszowska and Pengrui Jiao and Patrice Bertet and Philippe Goldner and Sylvain Bertaina},
  howpublished = {HAL},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.31208},
  eprint = {2609.31208},
  archivePrefix = {arXiv},
  url = {https://hal.science/hal-05766616v1},
  note = {CC BY-NC-ND 4.0},
}
RIS
TY  - UNPB
TI  - Electron paramagnetic resonance of Dy^3+-doped CaWO_4: spin Hamiltonian, crystal-field analysis, and linear electric field effect
AU  - Achuthan Manoj Kumar
AU  - Larissa Aboudem-Joumessi
AU  - Remy Dassonneville
AU  - Adrien Savoyant
AU  - Karolina Waszowska
AU  - Pengrui Jiao
AU  - Patrice Bertet
AU  - Philippe Goldner
AU  - Sylvain Bertaina
PY  - 2026
DA  - 2026/09/25
PB  - HAL
DO  - 10.48550/arxiv.2609.31208
UR  - https://hal.science/hal-05766616v1
AB  - We report an electron paramagnetic resonance (EPR) study of Dy^3+ in CaWO_4 single crystals spanning dopant concentrations from 80~ppb to 247~ppm. The g factors of the ground Kramers doublet at the S_4 point-group site, g_∥ = 7.22 ± 0.01 and g_⊥ = 5.45 ± 0.01, and the hyperfine constants of \ce{^{161}Dy} and ^163Dy are determined with an order-of-magnitude improvement in precision over the only previous report. A crystal-field analysis constrained jointly by published optical levels and by the measured g tensor identifies the ground doublet as the lower branch of an anticrossing between the near-degenerate |±11/2> and |∓13/2> states, and explains why optical data alone left the g values unconstrained. \add{The same parameter set, tested on the excited multiplets of the ^6H term, reproduces the ^6H_13/2 crystal-field levels better than the optical parameters themselves.} The angular dependence of the linewidth in the ab plane reveals broadening by random internal electric fields through the linear electric field effect. Calibrating these fields with the residual Er^3+ present in the same crystals yields the first electric-field coupling parameters of Dy^3+, (B_31^2+B_36^2)^1/2 = (34±5)×10^−6~cm/V, three times the Er^3+ value and the largest reported for a rare-earth ion in this host.The residual linewidth and the concentration-dependent lineshape asymmetry follow the quadratic field scaling expected for a second-order Stark shift, which escapes the inversion-site cancellation constraining the linear effect. Both couplings trace back to the ∼ 20~cm^−1 gap to the first opposite-symmetry doublet, a consequence of the dense crystal-field structure of the J=15/2 manifold.
ER  -