• Accepted Paper

Defect assignment of the clock site in 229Th:CaF2

Daniel A. Rehn, Harry W. T. Morgan, Harris E. Mason, H. B. Tran Tan, Ricky Elwell, Igor M. Savukov, Michael J. Martin, Andrei Derevianko, and Eric R. Hudson

Phys. Rev. Lett. - Accepted 13 November, 2026

DOI: https://doi.org/10.1103/1z49-m1tn

Abstract

The performance of solid-state 229Th nuclear clocks depends sensitively on the microscopic environment of the thorium nucleus in the host crystal. Here we reassess the dominant quadrupole-split thorium site in 229Th:CaF_2$, which has been assigned to a thorium dimer in recent spectroscopic work. Thermodynamic estimates, density functional theory calculations, and electric-field-gradient comparisons instead favor an isolated $\text{Th}^{4+}}$ substitution on a $^{2+}} site charge-compensated by two nearby fluoride interstitials in a 90∘ configuration, consistent with earlier literature. The same calculation identifies another defect, also with fluoride interstitials but in a different spatial arrangement, that matches weaker observed spectral lines. The defect responsible for the clock transition therefore features a single $^{229}} nucleus with nearby fluoride ions, rather than thorium aggregation. This defect assignment has implications for achievable linewidths and provides a microscopic basis for reducing broadening in solid-state nuclear clocks.

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