Prediction of Nuclear Clock Transitions Frequency Difference between $^{229}$Th$^{3+}$ and $^{229}$Th$^{4+}$ via \textit{ab-initio} Self-Consistent Field Theory

Abstract: The $^{229}\text{Th}$ isotope is a promising candidate for nuclear clocks, with its transition frequency influenced by electron-induced nuclear frequency shifts. This effect is comparatively small and requires high-precision theoretical calculations. In this work, we employed a non-perturbative multi-configuration Dirac-Hartree-Fock (MCDHF) method, in contrast to the perturbation theory used previously, to resolve the field shift effect. This method accounts for subtle differences in the nuclear potential while considering the $^{229}\text{Th}$ isotope in both its ground and isomeric states. Consequently, the nuclear transition frequency difference of between $^{229}\text{Th}^{3+}$ and $^{229}\text{Th}^{4+}$ was determined to be $-639$~MHz with computational convergency down to 1~MHz. Given recent precision measured transition frequency of $^{229}\text{Th}^{4+}$in $^{229}\text{Th}$-doped CaF$2$ [Nature 633, 63 (2024)], the transition frequency of isolated $^{229}\text{Th}^{3+}$ is predicted to be $2,020,406,745 (1)\text{comp.}(77){\delta \langle r^2 \rangle} (100)\text{ext.}$~MHz, with brackets indicating uncertainties stemming from our atomic structure computations, the input nuclear charge radii from nuclear data tables, and the influence of the crystal environment as reported in the literature. This provides valuable guidance for direct laser excitation of isolated $^{229}\text{Th}^{3+}$ based on ion traps experiments.