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Embedded cluster approach for accurate electronic structure calculations of 229Th :CaF2

Nalikowski, Kamil LU ; Veryazov, Valera LU orcid ; Beeks, Kjeld ; Schumm, Thorsten and Krośnicki, Marek (2025) In Physical Review B 111(11).
Abstract

Building on recent advances of the embedded cluster approach combined with multiconfigurational theory, this work investigates the electronic states in thorium-doped CaF2 crystals. Th:CaF2 is established as a promising material for solid-state nuclear clocks, which utilize the laser-Accessible isomeric state in thorium-229. By comparing simulated absorption spectra of a library of defect configurations with experimental data, we demonstrate the impact of fluorine vacancies and calcium vacancies on the Th:CaF2 electronic structure. Our results indicate that fluorine-deficient sites can introduce local electronic states within the band gap, resonant with the isomer energy, potentially contributing to... (More)

Building on recent advances of the embedded cluster approach combined with multiconfigurational theory, this work investigates the electronic states in thorium-doped CaF2 crystals. Th:CaF2 is established as a promising material for solid-state nuclear clocks, which utilize the laser-Accessible isomeric state in thorium-229. By comparing simulated absorption spectra of a library of defect configurations with experimental data, we demonstrate the impact of fluorine vacancies and calcium vacancies on the Th:CaF2 electronic structure. Our results indicate that fluorine-deficient sites can introduce local electronic states within the band gap, resonant with the isomer energy, potentially contributing to nonradiative decay or quenching of the Th-229 isomer. We also explore the potential of electron-nuclear-bridge mechanisms to enhance nuclear excitation or deexcitation, offering a pathway for more efficient control over the nuclear clock. This study provides key insights for optimizing the crystal environment for nuclear metrology applications and opens new avenues for further experimental and theoretical exploration of thorium-doped ionic crystals.

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author
; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review B
volume
111
issue
11
article number
115103
publisher
American Physical Society
external identifiers
  • scopus:86000140124
ISSN
2469-9950
DOI
10.1103/PhysRevB.111.115103
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2025 American Physical Society.
id
86687a5c-3bc7-4e77-9d36-bcee83f78413
date added to LUP
2025-03-23 11:35:06
date last changed
2025-04-04 14:29:45
@article{86687a5c-3bc7-4e77-9d36-bcee83f78413,
  abstract     = {{<p>Building on recent advances of the embedded cluster approach combined with multiconfigurational theory, this work investigates the electronic states in thorium-doped CaF<sub>2</sub> crystals. Th:CaF<sub>2</sub> is established as a promising material for solid-state nuclear clocks, which utilize the laser-Accessible isomeric state in thorium-229. By comparing simulated absorption spectra of a library of defect configurations with experimental data, we demonstrate the impact of fluorine vacancies and calcium vacancies on the Th:CaF<sub>2</sub> electronic structure. Our results indicate that fluorine-deficient sites can introduce local electronic states within the band gap, resonant with the isomer energy, potentially contributing to nonradiative decay or quenching of the Th-229 isomer. We also explore the potential of electron-nuclear-bridge mechanisms to enhance nuclear excitation or deexcitation, offering a pathway for more efficient control over the nuclear clock. This study provides key insights for optimizing the crystal environment for nuclear metrology applications and opens new avenues for further experimental and theoretical exploration of thorium-doped ionic crystals.</p>}},
  author       = {{Nalikowski, Kamil and Veryazov, Valera and Beeks, Kjeld and Schumm, Thorsten and Krośnicki, Marek}},
  issn         = {{2469-9950}},
  language     = {{eng}},
  month        = {{03}},
  number       = {{11}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review B}},
  title        = {{Embedded cluster approach for accurate electronic structure calculations of <sup>229</sup>Th :CaF<sub>2</sub>}},
  url          = {{http://dx.doi.org/10.1103/PhysRevB.111.115103}},
  doi          = {{10.1103/PhysRevB.111.115103}},
  volume       = {{111}},
  year         = {{2025}},
}