Investigation into thorium sulfate as a spinless crystal for a high-performance solid-state ${}^{229}Th$ nuclear clock

Abstract

The ${}^{229}Th$ isotope has a laser-accessible nuclear transition allowing the construction of a solid-state nuclear clock. Solid-state ${}^{229}Th$ nuclear clock development has focused on ${}^{229}Th$-doped $Ca{F}_2$ and other metal fluorides as the solid material. However, the accuracy of any fluoride-based clock will be reduced by nuclear magnetic dipole coupling to ${}^{19}F$ and by inhomogeneities in the thorium defect environments. Here we explore thorium sulfate, $Th(S{O}_4{)}_2$, as a solution to both problems. Strong bonding and charge delocalization in the $S{O}_4^{2-}$ anion may give $Th(S{O}_4{)}_2$ the wide band gap needed for a good clock. In this work we synthesize $Th(S{O}_4{)}_2$ and probe it as a nuclear clock material spectroscopically, finding that it is opaque to the 148 nm radiation that excites the ${}^{229}Th$ nucleus. Theoretical analysis of the optical spectra shows that charge transfer excitons are responsible for the absorption. We give guidelines for future material development and assess the prospects for $Th(S{O}_4{)}_2$ as a clock material.

20 pages of main text and references, 4 pages of supporting information. v2 expands on v1 by adding experimental results (synthesis and spectroscopy) and additional theoretical results