Lars von der Wense

While laser excitation of the nuclear isomeric transition in $^{229}$Th has been recently achieved for thorium atoms embedded in large-bandgap crystals, laser excitation and characterization of the nuclear transition in trapped $^{229}$Th$^{3+}$ ions has not yet been accomplished. To address these experiments, a cryogenic Paul trap setup has been designed, built, and commissioned at LMU Munich. Here, we present the specifications of the new experimental platform and demonstrate its successful operation, showing the extraction, subsequent ion-guiding, mass-purification, and trapping of $^{229}$Th$^{3+}$ and $^{229\text{m}}$Th$^{3+}$ ions from a newly designed buffer-gas stopping cell as well as of $^{88}$Sr$^{+}$ ions from laser ablation of a solid target. Further, we show sympathetic laser cooling of $^{229\text{(m)}}$Th$^{3+}$ by Doppler-cooled $^{88}$Sr$^{+}$ ions and the formation of mixed-species Coulomb crystals.

Thorium ions and molecules, recognized for their distinctive nuclear and atomic attributes, are central to numerous trapped-ion experiments globally. Our study introduces an effective, compact source of thorium ions produced via laser ablation of microgram-scale, salt-based samples. We thoroughly analyze the variety of ion species and charge states generated at varying laser fluences. Utilizing 10$μ$g of thorium fluoride crystals and laser fluences between $1.00 - 7.00$ J$\cdot$cm$^{-2}$ we produce thorium molecular ions $^{232}$ThF$_x$$^{n+}$ (with $x= 0 - 3$ and charge states up to $n = 3+$), including ThF$^{2+}$ and ThF$^{3+}$. These species are particularly relevant for spectroscopy; ThF$^{3+}$ is valuable for its stable closed-shell configuration, while ThF$^{2+}$, which is isoelectronic to RaF, offers a unique probe for studying nuclear structure and fundamental symmetries due to its simple electronic structure with a single unpaired electron. Density functional theory calculations of the distribution of positive charge in the produced molecular cations and the simplicity of this setup indicate that this method is easily transferable to other actinide systems.

The excitation of the 8 eV $^{229m}$Th isomer through the electronic bridge mechanism in highly charged ions is investigated theoretically. By exploiting the rich level scheme of open $4f$ orbitals and the robustness of highly charged ions against photoionization, a pulsed high-intensity optical laser can be used to efficiently drive the nuclear transition by coupling it to the electronic shell. We show how to implement a promising electronic bridge scheme in an electron beam ion trap starting from a metastable electronic state. This setup would avoid the need for a tunable vacuum ultraviolet laser. Based on our theoretical predictions, determining the isomer energy with an uncertainty of $10^{-5}$ eV could be achieved in one day of measurement time using realistic laser parameters.

A new concept for narrow-band direct nuclear laser spectroscopy of $^{229\text{m}}$Th is proposed, using a single comb mode of a vacuum ultraviolet frequency comb generated from the 7th harmonic of an Yb-doped fiber laser system. In this concept more than $10^{14}$ $^{229}$Th atoms on a surface are irradiated in parallel and a successful nuclear excitation is probed via the internal-conversion (IC) decay channel. A net scanning time of 15 minutes for the most recent 1~$σ$ energy uncertainty interval of 0.34 eV appears to be achievable when searching for the nuclear transition. In case of successful observation, the isomer's energy value would be constrained to an uncertainty of about 100~MHz, which is a factor of $10^6$ of improvement compared to today's knowledge. Further, the comb mode could be stabilized to the nuclear transition using the same detection method, allowing for the development of an IC-based solid-state nuclear clock, which is shown to achieve the same performance as a crystal-lattice nuclear clock, however, with the advantage of a drastically simpler detection scheme. Finally, it is shown that the same laser system could be used to narrow down the isomer's transition energy by further six orders of magnitude during laser excitation of $^{229}$Th$^{3+}$ ions in a Paul trap and to drive nuclear Rabi oscillations, as required for the development of a nuclear clock based on a single $^{229}$Th$^{3+}$ ion.