Controlling ^229Th isomeric state population in a VUV transparent crystal

The radioisotope Th-229 is renowned for its extraordinarily low-energy, long-lived nuclear first-excited state. This isomeric state can be excited by VUV lasers and the transition from the ground state has been proposed as a reference transition for ultra-precise nuclear clocks. Such nuclear clocks will find multiple applications, ranging from fundamental physics studies to practical implementations. Recent investigations extracted valuable constraints on the nuclear transition energy and lifetime, populating the isomer in stochastic nuclear decay of U-233 or Ac-229. However, to assess the feasibility and performance of the (solid-state) nuclear clock concept, time-controlled excitation and depopulation of the ^229Th isomer together with time-resolved monitoring of the radiative decay 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 0. 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 by at least a factor 50. Such controlled quenching can be used to significantly speed up the interrogation cycle in future nuclear clock schemes. Our results show that full control over the ^229Th nuclear isomer population can be achieved in a crystal environment. In particular, non-radiative decay processes that might lead to a broadening of the isomer transition linewidth are negligible, paving the way for the development of a compact and robust solid-state nuclear clock. Further studies are needed to reveal the underlying physical mechanism of the X-ray quenching effect.