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Thorium-229, with its exceptionally low-energy nuclear excited state, is a key candidate for developing nuclear clocks. $^{229}$Th-doped CaF$_2$ crystals, benefiting from calcium fluoride's wide band gap, show great promise as solid-state nuclear clock materials. These crystals are excited by vacuum ultraviolet (VUV) lasers, which over time cause radiation damage. Cooling the crystals can mitigate this damage but introduces a challenge: photoabsorption. This occurs when residual gas molecules condense on the crystal surface, absorbing VUV photons and deteriorating detection efficiency. To solve this, we developed a cooling technique using a copper shield to surround the crystal, acting as a cold trap. This prevents ice-layer formation, even at temperatures below $-100\,^\circ$C, preserving high VUV photon detection efficiency. Our study detailed the experimental cooling setup and demonstrated the effectiveness of the copper shield in maintaining crystal performance, a critical improvement for future solid-state nuclear clocks operating at cryogenic temperatures., Comment: 5 figures

State-resolved laser spectroscopy at the 10$^{-12}$ precision level recently reported in $arXiv$:2406.18719 determined the fractional change in nuclear quadrupole moment between the ground and isomeric state of $^{229}\rm{Th}$, $\Delta Q_0/Q_0$=1.791(2) %. Assuming a prolate spheroid nucleus, this allows to quantify the sensitivity of the nuclear transition frequency to variations of the fine-structure constant $\alpha$ to $K=5900(2300)$, with the uncertainty dominated by the experimentally measured charge radius difference $\Delta \langle r^2 \rangle$ between the ground and isomeric state. This result indicates a three orders of magnitude enhancement over atomic clock schemes based on electron shell transitions. We find that $\Delta Q_0$ is highly sensitive to tiny changes in the nuclear volume, thus the constant volume approximation cannot be used to accurately relate changes in $\langle r^2 \rangle$ and $Q_0$. The difference between the experimental and estimated values in $\Delta Q_0/Q_0$ raises a further question on the octupole contribution to the alpha-sensitivity., Comment: 10 pages, 2 figures

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 $^{229}$Th isomer together with time-resolved monitoring of the radiative decay are imperative. Here we report the population of the $^{229}$Th isomeric state through resonant X-ray pumping and detection of the radiative decay in a VUV transparent $^{229}$Th-doped CaF$_2$ crystal. The decay half-life is measured to $447\pm 25$ s, with a transition wavelength of $148.18 \pm 0.42$ 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 $^{229}$Th 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., Comment: 14 pages with 8 figures and 2 tables

The 8 eV first nuclear excited state in $^{229}$Th is a candidate for implementing an nuclear clock. Doping $^{229}$Th into ionic crystals such as CaF$_2$ is expected to suppress non-radiative decay, enabling nuclear spectroscopy and the realization of a solid-state optical clock. Yet, the inherent radioactivity of $^{229}$Th prohibits the growth of high-quality single crystals with high $^{229}$Th concentration; radiolysis causes fluoride loss, increasing absorption at 8 eV. We overcome this roadblock by annealing $^{229}$Th doped CaF$_2$ at 1250$\unicode{x2103}$ in CF$_4$. The technique presented here allows to adjust the fluoride content without crystal melting, preserving its single-crystal structure. Superionic state annealing ensures rapid fluoride distribution, creating fully transparent and radiation-hard crystals. This approach enables control over the charge state of dopants which can be used in deep UV optics, laser crystals, scintillators, and nuclear clocks., Comment: 5 pages, 5 figures

We have grown $^{232}$Th:CaF$_2$ and $^{229}$Th:CaF$_2$ single crystals for investigations on the VUV laser-accessible first nuclear excited state of $^{229}$Th. To reach high doping concentrations despite the extreme scarcity (and radioactivity) of $^{229}$Th, we have scaled down the crystal volume by a factor 100 compared to established commercial or scientific growth processes. We use the vertical gradient freeze method on 3.2 mm diameter seed single crystals with a 2 mm drilled pocket, filled with a co-precipitated CaF$_2$:ThF$_4$:PbF$_2$ powder in order to grow single crystals. Concentrations of $4\cdot10^{19}$ cm$^{-3}$ have been realized with $^{232}$Th with good ($>$10%) VUV transmission. However, the intrinsic radioactivity of $^{229}$Th drives radio-induced dissociation during growth and radiation damage after solidification. Both lead to a degradation of VUV transmission, limiting the $^{229}$Th concentration to $<5\cdot10^{17}$ cm$^{-3}$., Comment: 12 pages, 18 figures