Marius Müller

State-of-the-art optical clocks achieve fractional precisions of $10^{-18}$ and below using ensembles of atoms in optical lattices or individual ions in radio-frequency traps. Promising candidates for novel clocks are highly charged ions (HCIs) and nuclear transitions, which are largely insensitive to external perturbations and reach wavelengths beyond the optical range, now becoming accessible to frequency combs. However, insufficiently accurate atomic structure calculations still hinder the identification of suitable transitions in HCIs. Here, we report on the discovery of a long-lived metastable electronic state in a HCI by measuring the mass difference of the ground and the excited state in Re, the first non-destructive, direct determination of an electronic excitation energy. This result agrees with our advanced calculations, and we confirmed them with an Os ion with the same electronic configuration. We used the high-precision Penning-trap mass spectrometer PENTATRAP, unique in its synchronous use of five individual traps for simultaneous mass measurements. The cyclotron frequency ratio $R$ of the ion in the ground state to the metastable state could be determined to a precision of $δR=1\cdot 10^{-11}$, unprecedented in the heavy atom regime. With a lifetime of about 130 days, the potential soft x-ray frequency reference at $ν=4.86\cdot 10^{16}\,\text{Hz}$ has a linewidth of only $Δν\approx 5\cdot 10^{-8}\,\text{Hz}$, and one of the highest electronic quality factor ($Q=\fracν{Δν}\approx 10^{24}$) ever seen in an experiment. Our low uncertainty enables searching for more HCI soft x-ray clock transitions, needed for promising precision studies of fundamental physics in a thus far unexplored frontier.

This paper reports on the development and testing of a novel, highly efficient technique for the injection of very rare species into electron beam ion traps (EBITs) for the production of highly charged ions (HCI). It relies on in-trap laser-induced desorption of atoms from a sample brought very close to the electron beam resulting in a very high capture efficiency in the EBIT. We have demonstrated a steady production of HCI of the stable isotope $^{165}\mathrm{Ho}$ from samples of only $10^{12}$ atoms ($\sim$ 300 pg) in charge states up to 45+. HCI of these species can be subsequently extracted for use in other experiments or stored in the trapping volume of the EBIT for spectroscopic measurements. The high efficiency of this technique expands the range of rare isotope HCIs available for high-precision nuclear mass and spectroscopic measurements. A first application of this technique is the production of HCI of the synthetic radioisotope $^{163}\mathrm{Ho}$ for a high-precision measurement of the $Q_{\mathrm{EC}}$-value of the electron capture in $^{163}\mathrm{Ho}$ within the Electron Capture in Holmium experiment (ECHo collaboration) ultimately leading to a measurement of the electron neutrino mass with an uncertainty on the sub-eV level.