Research Group Ions

Molecules have proven to be sensitive tools for studying physics beyond the standard model, with heavy and deformed nuclei offering decisive sensitivity to parity- and time-reversal-violating effects. However, almost all elements beyond lead, occupying the 6p~to~5f atomic orbitals, lack stable isotopes, hence molecules containing them are referred to as radioactive molecules. Among those, radium monofluoride has seen particular interest, but to date, research on radioactive molecules has mainly been limited to large-scale nuclear facilities. Here, we present a scheme that allows efficient and fast harvest of radioactive ions (including short-lived Ra), and show ion gas-phase reaction studies of singly and doubly charged Ra, Po, and Pb ions with SF$_6$ gas inside an ion trap. Our results show that the chemical reaction rate of Ra$^+$ is in line with trends of other alkaline earth elements, further support by quantum chemical computations. The reaction Ra$^{2+}$ + SF$_6$ $\rightarrow$ RaF${^+}$ + SF$_5^{+}$ achieves an almost unity conversion efficiency, making it particularly suitable for the application for studies in physics beyond the standard model. The scheme enables future decentralized research avenues with short-lived radioactive molecules for fundamental physics research at laboratories without the need for local nuclear reactors or accelerators.

We present a novel technique to probe electroweak nuclear properties by measuring parity violation (PV) in single molecular ions in a Penning trap. The trap's strong magnetic field Zeeman shifts opposite-parity rotational and hyperfine molecular states into near degeneracy. The weak interaction-induced mixing between these degenerate states can be larger than in atoms by more than twelve orders of magnitude, thereby vastly amplifying PV effects. The single molecule sensitivity would be suitable for applications to nuclei across the nuclear chart, including rare and unstable nuclei.

Parity non-conservation (PNC) due to the weak interaction is predicted to give rise to enantiomer dependent vibrational constants in chiral molecules, but the phenomenon has so far eluded experimental observation. The enhanced sensitivity of molecules to physics beyond the Standard Model (BSM), has led to substantial advances in molecular precision spectroscopy, and these may be applied to PNC searches as well. Specifically, trapped molecular ion experiments leverage the universality of trapping charged particles to optimize the molecular ion species studied toward BSM searches, but in searches for PNC only a few chiral molecular ion candidates have been proposed so far. Importantly, viable candidates need to be internally cold and their internal state populations should be detectable with high quantum efficiency. To this end, we focus on molecular ions that can be created by near threshold resonant two-photon ionization and detected via state-selective photo-dissociation. Such candidates need to be stable in both charged and neutral chiral versions to be amenable to these methods. Here, we present a collection of suitable chiral molecular ion candidates we have found, including CHDBrI$^+$ and CHCaBrI$^+$, that fulfill these conditions according to our \textit{ab initio} calculations. We find that organo-metallic species have a low ionization energy as neutrals and relatively high dissociation thresholds. Finally, we compute the magnitude of the PNC values for vibrational transitions for some of these candidates. An experimental demonstration of state preparation and readout for these candidates will be an important milestone toward measuring PNC in chiral molecules for the first time.

Recent theoretical works have proposed atomic clocks based on narrow optical transitions in highly charged ions. The most interesting candidates for searches of new physics are those which occur at rare orbital crossings where the shell structure of the periodic table is reordered. There are only three such crossings expected to be accessible in highly charged ions, and hitherto none have been observed as both experiment and theory have proven difficult. In this work we observe an orbital crossing in highly charged ions for the first time, in a system chosen to be tractable from both sides: Pr$^{9+}$. We present electron beam ion trap measurements of its spectra, including the inter-configuration lines that reveal the sought-after crossing. The proposed nHz-wide clock line, found to be at 452.334(1) nm, proceeds through hyperfine admixture of its upper state with an E2-decaying level. With state-of-the-art calculations we show that it has a very high sensitivity to new physics and extremely low sensitivity to external perturbations, making it a unique candidate for proposed precision studies.

We present experimental data on H2 formation processes on gas-phase polycyclic aromatic hydrocarbon (PAH) cations. This process was studied by exposing coronene radical cations, confined in a radio-frequency ion trap, to gas phase H atoms. Sequential attachment of up to 23 hydrogen atoms has been observed. Exposure to atomic D instead of H allows one to distinguish attachment from competing abstraction reactions, as the latter now leave a unique fingerprint in the measured mass spectra. Modeling of the experimental results using realistic cross sections and barriers for attachment and abstraction yield a 1:2 ratio of abstraction to attachment cross sections. The strong contribution of abstraction indicates that H2 formation on interstellar PAH cations is an order of magnitude more relevant than previously thought.

We analyze the complex level structure of ions with many-valence-electron open [Kr] 4$d^\textrm{m}$ sub-shells ($\textrm{m}$=7-4) with ab initio calculations based on configuration-interaction many-body perturbation theory (CI+MBPT). Charge-state-resolved optical and extreme ultraviolet (EUV) spectra of Sn$^{7+}$-Sn$^{10+}$ ions were obtained using an electron beam ion trap. Semi-empirical spectral fits carried out with the orthogonal parameters technique and Cowan code calculations lead to 90 identifications of magnetic-dipole transitions and the determination of 79 energy ground-configuration levels, questioning some earlier EUV-line assignments. Our results, the most complete data set available to date for these ground configurations, confirm the ab initio predictive power of CI+MBPT calculations for the these complex electronic systems.

We experimentally re-evaluate the fine structure of Sn$^{11+...14+}$ ions. These ions are essential in bright extreme-ultraviolet (EUV) plasma-light sources for next-generation nanolithography, but their complex electronic structure is an open challenge for both theory and experiment. We combine optical spectroscopy of magnetic dipole $M1$ transitions, in a wavelength range covering 260\,nm to 780\,nm, with charge-state selective ionization in an electron beam ion trap. Our measurements confirm the predictive power of \emph{ab initio} calculations based on Fock space coupled cluster theory. We validate our line identification using semi-empirical Cowan calculations with adjustable wavefunction parameters. Available Ritz combinations further strengthen our analysis. Comparison with previous work suggests that line identifications in the EUV need to be revisited.

Transition frequencies between low-lying energy levels in a single trapped $^{138}$Ba$^{+}$ ion have been measured with laser spectroscopy referenced to an optical frequency comb. By extracting the frequencies of one-photon and two-photon components of the line shape using an eight-level optical Bloch model, we achieved 0.1 MHz accuracy for the 5d $^{2}$D$_{3/2}$ - 6p $^{2}$P$_{1/2}$ and 6s $^{2}$S$_{1/2}$ - 5d $^{2}$D$_{3/2}$ transition frequencies, and 0.2 MHz for the 6s $^{2}$S$_{1/2}$ - 6p $^{2}$P$_{1/2}$ transition frequency.

As an important step towards an atomic parity violation experiment in one single trapped Ra$^+$ ion, laser spectroscopy experiments were performed with on-line produced short-lived $^{212,213,214}$Ra$^+$ ions. The isotope shift of the $6\,^2$D$_{3/2}$\,-\,$7\,^2$P$_{1/2}$ and $6\,^2$D$_{3/2}$\,-\,$7\,^2$P$_{3/2}$ transitions and the hyperfine structure constant of the $7\,^2$S$_{1/2}$ and $6\,^2$D$_{3/2}$ states in $^{213}$Ra$^+$ were measured. These values provide a benchmark for the required atomic theory. A lower limit of $232(4)$ ms for the lifetime of the metastable $6\,^2$D$_{5/2}$ state was measured by optical shelving.

The structures for the TRI$μ$P facility have been completed and commissioned. At the facility radioactive nuclides are produced to study fundamental interactions and symmetries. An important feature is the possibility to trap radioactive atoms in order to obtain and hold a pure substrate-free sample for precision measurements. In the TRI$μ$P facility a production target is followed by a magnetic separator, where radioactive isotopes are produced in inverse reaction kinematics. Separation up to 99.95% could be achieved for $^{21}$Na. A novel transmitting thermal ionizing device was developed to stop the energetic isotopes. Some 50% of stopped $^{21}$Na could be extracted and transported as low energy singly charged ions into a radio frequency quadrupole cooler and buncher with 35% transmission efficiency. The ions are transported lossless via a drift tube and a low energy electrostatic beam line into the experimental setup. Such ions can be neutralized on hot metal foils and the resulting atoms can be stored in a magneto-optical trap. The functioning of that principle was demonstrated with stable Na extracted from the thermal ionizer, radioactive beams will follow next.

The general conclusion of Seevinck and Larsson is that our model exploits the so-called coincidence-time loophole and produces sinusoidal (quantum-like) correlations but does not model the singlet state because it does not violate the relevant Bell inequality derived by Larsson and Gill, since in order to obtain the sinusoidal correlations the probability of coincidences in our model goes to zero. In this reply, we refute their arguments that lead to this conclusion and demonstrate that our model can reproduce results of photon and ion-trap experiments with frequencies of coincidences that are not in conflict with the observations.