Ming Guan

Mössbauer spectroscopy is widely used in chemistry, geology, and solid-state physics to probe the local physical and chemical environment of nuclei in materials. Here, we extended this technique into the optical range using a vacuum ultraviolet laser to probe the low-energy nuclear transitions of thorium-229 ( ²²⁹ Th) doped in calcium fluoride (CaF ₂ ) crystals. We discovered four distinct doping sites for the thorium ions, determined the characteristic electric field gradients emerging from the interaction with the host crystal, and identified the microscopic structure of the two dominant configurations. Site-selective laser excitation enabled the study of the isomeric state lifetime and laser-induced quenching for all sites. This technique provides a powerful probe of the nuclear environment, yielding foundational data for designing future solid-state nuclear clocks.

Recent studies have shown that the lifetime of the isomeric ^{229}Th doped in crystals can be shortened by x-ray or laser irradiation, a phenomenon referred to as isomer quenching. We investigate the temperature dependence of x-ray-induced quenching in ^{229}Th:CaF_{2} and identify a correlation with the afterglow of the host crystal. These results suggest a mechanism in which x-ray-induced electrons migrate through the lattice and are captured at Th sites, enabling isomer deexcitation via internal conversion through electron-nucleus coupling. This mechanism links nuclear decay to charge carrier dynamics in the host crystal, providing a new interface between nuclear and solid-state physics. The findings offer a pathway to optimize the performance of solid-state nuclear clocks.

The radioisotope thorium-229 (²²⁹Th) is renowned for its extraordinarily low-energy, long-lived nuclear first-excited state. This isomeric state can be excited by vacuum ultraviolet (VUV) lasers and ²²⁹Th has been proposed as a reference transition for ultra-precise nuclear clocks. To assess the feasibility and performance of the nuclear clock concept, time-controlled excitation and depopulation of the ²²⁹Th isomer are imperative. Here we report the population of the ²²⁹Th isomeric state through resonant X-ray pumping and detection of the radiative decay in a VUV transparent ²²⁹Th-doped CaF₂ crystal. The decay half-life is measured to 447(25) s, with a transition wavelength of 148.18(42) nm and a radiative decay fraction consistent with unity. Furthermore, we report a new “X-ray quenching” effect which allows to de-populate the isomer on demand and effectively reduce the half-life. Such controlled quenching can be used to significantly speed up the interrogation cycle in future nuclear clock schemes.