Observation of a Low-Lying Metastable Electronic State in Highly Charged Lead by Penning-Trap Mass Spectrometry.

Highly charged ions (HCIs) offer many opportunities for next-generation clock research due to the vast landscape of available electronic transitions in different charge states. The development of extreme ultraviolet frequency combs has enabled the search for clock transitions based on shorter wavelengths in HCIs. However, without initial knowledge of the energy of the clock states, these narrow transitions are difficult to be probed by lasers. In this Letter, we provide experimental observation and theoretical calculation of a long-lived electronic state in Nb-like Pb^{41+} that could be used as a clock state. With the mass spectrometer PENTATRAP, the excitation energy of this metastable state is directly determined as a mass difference at an energy of 31.2(8) eV, corresponding to one of the most precise relative mass determinations to date with a fractional uncertainty of 4×10^{-12}. This experimental result agrees within 1σ with two partially different ab initio multiconfiguration Dirac-Hartree-Fock calculations of 31.68(13) eV and 31.76(35) eV, respectively. With a calculated lifetime of 26.5(5.3) days, the transition from this metastable state to the ground state bears a quality factor of 1.1×10^{23} and allows for the construction of a HCI clock with a fractional frequency instability of <10^{-19}/sqrt[τ].

Fast silicon carbide MOSFET based high-voltage push-pull switch for charge state separation of highly charged ions with a Bradbury-Nielsen gate.

In this paper, we report on the development of a fast high-voltage switch, which is based on two enhancement mode N-channel silicon carbide metal-oxide-semiconductor field-effect transistors in push-pull configuration. The switch is capable of switching high voltages up to 600 V on capacitive loads with rise and fall times on the order of 10 ns and pulse widths ≥20 ns. Using this switch, it was demonstrated that, from the charge state distribution of bunches of highly charged ions ejected from an electron beam ion trap with a specific kinetic energy, single charge states can be separated by fast switching of the high voltage applied to a Bradbury-Nielsen Gate with a resolving power of about 100.

High-precision mass measurement of doubly magic 208 Pb.

The absolute atomic mass of 208 Pb has been determined with a fractional uncertainty of 7 × 10 - 11 by measuring the cyclotron-frequency ratio R of 208 Pb 41 + to 132 Xe 26 + with the high-precision Penning-trap mass spectrometer Pentatrap and computing the binding energies E Pb and E Xe of the missing 41 and 26 atomic electrons, respectively, with the ab initio fully relativistic multi-configuration Dirac-Hartree-Fock (MCDHF) method. R has been measured with a relative precision of 9 × 10 - 12 . E Pb and E Xe have been computed with an uncertainty of 9.1 eV and 2.1 eV, respectively, yielding 207.976 650 571 ( 14 )  u ( u = 9.314 941 024 2 ( 28 ) × 10 8  eV/c 2 ) for the 208 Pb neutral atomic mass. This result agrees within 1.2 σ with that from the Atomic-Mass Evaluation (AME) 2020, while improving the precision by almost two orders of magnitude. The new mass value directly improves the mass precision of 14 nuclides in the region of Z = 81-84 and is the most precise mass value with A > 200 . Thus, the measurement establishes a new region of reference mass values which can be used e.g. for precision mass determination of transuranium nuclides, including the superheavies.

Isochronous mass spectrometry in an electrostatic storage ring.

For sensitive studies of molecular ions in electrostatic storage rings, the exact knowledge of the isobaric composition of stored beams from a variety of ion sources is essential. Conventional mass-filtering techniques are often inefficient to resolve the beam components. Here, we report the first isochronous mass spectrometry in an electrostatic storage ring, which offers a high mass resolution of Δm/m < 1 × 10-5 even for heavy molecular species with m > 100 u and uncooled ion beams. Mass contaminations can be resolved and identified at relative fractions down to 0.02%.

Measurement of the bound-electron g-factor difference in coupled ions.

Quantum electrodynamics (QED) is one of the most fundamental theories of physics and has been shown to be in excellent agreement with experimental results1-5. In particular, measurements of the electron's magnetic moment (or g factor) of highly charged ions in Penning traps provide a stringent probe for QED, which allows testing of the standard model in the strongest electromagnetic fields6. When studying the differences between isotopes, many common QED contributions cancel owing to the identical electron configuration, making it possible to resolve the intricate effects stemming from the nuclear differences. Experimentally, however, this quickly becomes limited, particularly by the precision of the ion masses or the magnetic field stability7. Here we report on a measurement technique that overcomes these limitations by co-trapping two highly charged ions and measuring the difference in their g factors directly. We apply a dual Ramsey-type measurement scheme with the ions locked on a common magnetron orbit8, separated by only a few hundred micrometres, to coherently extract the spin precession frequency difference. We have measured the isotopic shift of the bound-electron g factor of the isotopes 20Ne9+ and 22Ne9+ to 0.56-parts-per-trillion (5.6 × 10-13) precision relative to their g factors, an improvement of about two orders of magnitude compared with state-of-the-art techniques7. This resolves the QED contribution to the nuclear recoil, accurately validates the corresponding theory and offers an alternative approach to set constraints on new physics.

A digital feedback system for advanced ion manipulation techniques in Penning traps.

The possibility of applying active feedback to a single ion in a Penning trap using a fully digital system is demonstrated. Previously realized feedback systems rely on analog circuits that are susceptible to environmental fluctuations and long term drifts, as well as being limited to the specific task they were designed for. The presented system is implemented using a field-programmable gate array (FPGA)-based platform (STEMlab), offering greater flexibility, higher temporal stability, and the possibility for highly dynamic variation of feedback parameters. The system's capabilities were demonstrated by applying feedback to the ion detection system primarily consisting of a resonant circuit. This allowed shifts in its resonance frequency of up to several kHz and free modification of its quality factor within two orders of magnitude, which reduces the temperature of a single ion by a factor of 6. Furthermore, a phase-sensitive detection technique for the axial ion oscillation was implemented, which reduces the current measurement time by two orders of magnitude, while simultaneously eliminating model-related systematic uncertainties. The use of FPGA technology allowed the implementation of a fully-featured data acquisition system, making it possible to realize feedback techniques that require constant monitoring of the ion signal. This was successfully used to implement a single-ion self-excited oscillator.

Constraints on the Coupling between Axionlike Dark Matter and Photons Using an Antiproton Superconducting Tuned Detection Circuit in a Cryogenic Penning Trap.

We constrain the coupling between axionlike particles (ALPs) and photons, measured with the superconducting resonant detection circuit of a cryogenic Penning trap. By searching the noise spectrum of our fixed-frequency resonant circuit for peaks caused by dark matter ALPs converting into photons in the strong magnetic field of the Penning-trap magnet, we are able to constrain the coupling of ALPs with masses around 2.7906-2.7914 neV/c^{2} to g_{aγ}<1×10^{-11} GeV^{-1}. This is more than one order of magnitude lower than the best laboratory haloscope and approximately 5 times lower than the CERN axion solar telescope (CAST), setting limits in a mass and coupling range which is not constrained by astrophysical observations. Our approach can be extended to many other Penning-trap experiments and has the potential to provide broad limits in the low ALP mass range.

Penning trap mass measurements of the deuteron and the HD+ molecular ion.

The masses of the lightest atomic nuclei and the electron mass1 are interlinked, and their values affect observables in atomic2, molecular3-5 and neutrino physics6, as well as metrology. The most precise values for these fundamental parameters come from Penning trap mass spectrometry, which achieves relative mass uncertainties of the order of 10-11. However, redundancy checks using data from different experiments reveal considerable inconsistencies in the masses of the proton, the deuteron and the helion (the nucleus of helium-3), suggesting that the uncertainty of these values may have been underestimated. Here we present results from absolute mass measurements of the deuteron and the HD+ molecular ion using 12C as a mass reference. Our value for the deuteron mass, 2.013553212535(17) atomic mass units, has better precision than the CODATA value7 by a factor of 2.4 and differs from it by 4.8 standard deviations. With a relative uncertainty of eight parts per trillion, this is the most precise mass value measured directly in atomic mass units. Furthermore, our measurement of the mass of the HD+ molecular ion, 3.021378241561(61) atomic mass units, not only allows a rigorous consistency check of our results for the masses of the deuteron (this work) and the proton8, but also establishes an additional link for the masses of tritium9 and helium-3 (ref. 10) to the atomic mass unit. Combined with a recent measurement of the deuteron-to-proton mass ratio11, the uncertainty of the reference value of the proton mass7 can be reduced by a factor of three.

Quantitative Long-Term Monitoring of the Circulating Gases in the KATRIN Experiment Using Raman Spectroscopy.

The Karlsruhe Tritium Neutrino (KATRIN) experiment aims at measuring the effective electron neutrino mass with a sensitivity of 0.2 eV/c2, i.e., improving on previous measurements by an order of magnitude. Neutrino mass data taking with KATRIN commenced in early 2019, and after only a few weeks of data recording, analysis of these data showed the success of KATRIN, improving on the known neutrino mass limit by a factor of about two. This success very much could be ascribed to the fact that most of the system components met, or even surpassed, the required specifications during long-term operation. Here, we report on the performance of the laser Raman (LARA) monitoring system which provides continuous high-precision information on the gas composition injected into the experiment's windowless gaseous tritium source (WGTS), specifically on its isotopic purity of tritium-one of the key parameters required in the derivation of the electron neutrino mass. The concentrations cx for all six hydrogen isotopologues were monitored simultaneously, with a measurement precision for individual components of the order 10-3 or better throughout the complete KATRIN data taking campaigns to date. From these, the tritium purity, εT, is derived with precision of <10-3 and trueness of <3 × 10-3, being within and surpassing the actual requirements for KATRIN, respectively.

Application of the Continuous Stern-Gerlach Effect for Laser Spectroscopy of the

We report on the successful demonstration of a novel scheme for detecting optical transitions in highly charged ions. We applied it to determine the frequency of the dipole-forbidden 2p ^{2}P_{1/2}-^{2}P_{3/2} transition in the fine structure of ^{40}Ar^{13+} using a single ion stored in the harmonic potential of a Penning trap. Our measurement scheme does not require detection of fluorescence, instead it makes use of the continuous Stern-Gerlach effect. Our value of 679.216464(4)_{stat}(5)_{syst} THz is in reasonable agreement with the current best literature values and improves its uncertainty by a factor of 24.

Quantum-state-selective electron recombination studies suggest enhanced abundance of primordial HeH.

The epoch of first star formation in the early Universe was dominated by simple atomic and molecular species consisting mainly of two elements: hydrogen and helium. Gaining insight into this constitutive era requires a thorough understanding of molecular reactivity under primordial conditions. We used a cryogenic ion storage ring combined with a merged electron beam to measure state-specific rate coefficients of dissociative recombination, a process by which electrons destroy molecular ions. We found a pronounced decrease of the electron recombination rates for the lowest rotational states of the helium hydride ion (HeH+), compared with previous measurements at room temperature. The reduced destruction of cold HeH+ translates into an enhanced abundance of this primordial molecule at redshifts of first star and galaxy formation.

Long-Term Monitoring of the Internal Energy Distribution of Isolated Cluster Systems.

A method is presented to monitor the internal energy distribution of cluster anions via delayed electron detachment by pulsed photoexcitation and demonstrated on Co_{4}^{-} in an electrostatic ion beam trap. In a cryogenic operation, we calibrate the detachment delay to internal energy. By laser frequency scans, at room temperature, we reconstruct the time-dependent internal energy distribution of the clusters. The mean energies of ensembles from a cold and a hot ion source both approach thermal equilibrium. Our data yield a radiative emission law and the absorptivity of the cluster for thermal radiation.

Double-trap measurement of the proton magnetic moment at 0.3 parts per billion precision.

Precise knowledge of the fundamental properties of the proton is essential for our understanding of atomic structure as well as for precise tests of fundamental symmetries. We report on a direct high-precision measurement of the magnetic moment µp of the proton in units of the nuclear magneton µN The result, µp = 2.79284734462 (±0.00000000082) µN, has a fractional precision of 0.3 parts per billion, improves the previous best measurement by a factor of 11, and is consistent with the currently accepted value. This was achieved with the use of an optimized double-Penning trap technique. Provided a similar measurement of the antiproton magnetic moment can be performed, this result will enable a test of the fundamental symmetry between matter and antimatter in the baryonic sector at the 10-10 level.

Isotope dependence of the Zeeman effect in lithium-like calcium.

The magnetic moment µ of a bound electron, generally expressed by the g-factor µ=-g µB s h(-1) with µB the Bohr magneton and s the electron's spin, can be calculated by bound-state quantum electrodynamics (BS-QED) to very high precision. The recent ultra-precise experiment on hydrogen-like silicon determined this value to eleven significant digits, and thus allowed to rigorously probe the validity of BS-QED. Yet, the investigation of one of the most interesting contribution to the g-factor, the relativistic interaction between electron and nucleus, is limited by our knowledge of BS-QED effects. By comparing the g-factors of two isotopes, it is possible to cancel most of these contributions and sensitively probe nuclear effects. Here, we present calculations and experiments on the isotope dependence of the Zeeman effect in lithium-like calcium ions. The good agreement between the theoretical predicted recoil contribution and the high-precision g-factor measurements paves the way for a new generation of BS-QED tests.

Precision Test of Many-Body QED in the Be+ 2p Fine Structure Doublet Using Short-Lived Isotopes.

Absolute transition frequencies of the 2s 2S{1/2}→2p2P{1/2,3/2} transitions in Be^{+} were measured for the isotopes ^{7,9-12}Be. The fine structure splitting of the 2p state and its isotope dependence are extracted and compared to results of ab initio calculations using explicitly correlated basis functions, including relativistic and quantum electrodynamics effects at the order of mα(6) and mα(7) ⁢ln α. Accuracy has been improved in both the theory and experiment by 2 orders of magnitude, and good agreement is observed. This represents one of the most accurate tests of quantum electrodynamics for many-electron systems, being insensitive to nuclear uncertainties.

Billion-fold enhancement in sensitivity of nuclear magnetic resonance spectroscopy for magnesium ions in solution.

ß-nuclear magnetic resonance (NMR) spectroscopy is highly sensitive compared to conventional NMR spectroscopy, and may be applied for several elements across the periodic table. ß-NMR has previously been successfully applied in the fields of nuclear and solid-state physics. In this work, ß-NMR is applied, for the first time, to record an NMR spectrum for a species in solution. (31)Mg ß-NMR spectra are measured for as few as 10(7) magnesium ions in ionic liquid (EMIM-Ac) within minutes, as a prototypical test case. Resonances are observed at 3882.9 and 3887.2 kHz in an external field of 0.3 T. The key achievement of the current work is to demonstrate that ß-NMR is applicable for the analysis of species in solution, and thus represents a novel spectroscopic technique for use in general chemistry and potentially in biochemistry.

Phase-sensitive cyclotron frequency measurements at ultralow energies.

A novel technique for a direct and coherent measurement of the modified cyclotron frequency of an ion in a Penning trap at energies close to the thermal cooling limit is presented. This allows a rapid and both precise and accurate determination of the free-space cyclotron frequency in real Penning traps despite the existence of electric and magnetic field imperfections and relativistic shifts. The demonstrated performance paves the way for considerably improved bound-state g-factor measurements on the 10 ppt level and mass measurements in the 1 ppt range and possibly below.

A battery-based, low-noise voltage source.

A highly stable, low-noise voltage source was designed to improve the stability of the electrode bias voltages of a Penning trap. To avoid excess noise and ground loops, the voltage source is completely independent of the public electric network and uses a 12 V car battery to generate output voltages of +/-15 and +/-5 V. First, the dc supply voltage is converted into ac-voltage and gets amplified. Afterwards, the signal is rectified, filtered, and regulated to the desired output value. Each channel can deliver up to 1.5 A. The current as well as the battery voltage and the output voltages can be read out via a universal serial bus (USB) connection for monitoring purposes. With the presented design, a relative voltage stability of 7 x 10(-7) over 6.5 h and a noise level equal or smaller than 30 nV/square root(Hz) is achieved.

Stable voltage source for Penning trap experiments.

A voltage reference has been developed to bias ring electrodes of two Penning traps between -90 and 0 V. For output voltages near -90 V, the Allan deviation of the system's voltage instability is less than 1 part in 10(8) over all time scales shorter than 10(4) s. For averaging times longer than several seconds, the system's stability is determined almost completely by the noise, drift, and aging of the zener diodes in the array of voltage reference integrated circuits. For shorter averaging times, active filters built into the new system significantly reduce the intrinsic noise of the zener diodes. The system makes it possible to continuously adjust the ring voltages for frequency locking the axial motion in the two Penning traps. By keeping electrical noise highly correlated between the two traps, measurement uncertainty should be reduced for precision experiments such as Penning trap mass spectrometry.

Atomic clusters and ion-cyclotron-resonance mass spectrometry: a fruitful combination.

Clusters consisting of a few atoms build the bridge between individual atoms and the condensed phase of matter and they are, thus, of high general interest. Over the last two decades, considerable progress has been made in the study of their properties, and ion storage techniques, in particular the use of ion cyclotron resonance (Penning) traps, are important tools for advanced investigations. Vice versa, cluster ions can serve as probes for the evaluation of ion-trap properties. Furthermore, they are ideally suited for the calibration of mass spectrometers and for consistency checks in high-accuracy mass determinations. Examples from the research areas mentioned, i.e. the investigation of cluster properties and the application of cluster ions for Penning-trap studies and mass calibration, are reported.