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The ionization potential (IP) of radium monofluoride (RaF) was measured to be 4.969(2)[10] eV, revealing a relativistic enhancement in the series of alkaline earth monofluorides. The results are in agreement with a relativistic coupled-cluster prediction of 4.969[7] eV, incorporating up to quantum electrodynamics corrections. Using the same computational methodology, an improved calculation for the dissociation energy ($D_{e}$) of 5.56[5] eV is presented. This confirms that radium monofluoride joins the small group of diatomic molecules for which $D_{e}>\mathrm{IP}$, paving the way for precision control and interrogation of its Rydberg states.

We report on the design and characterization of an antiproton deceleration beamline, based on a pulsed drift tube, for the PUMA experiment at the Antimatter Factory at CERN. The design has been tailored to high-voltage (100 kV) and ultra-high vacuum (below $10^{-10}$ mbar) conditions. A first operation achieved decelerating antiprotons from an initial energy of 100 keV down to ($3898\pm 3$) eV, marking the initial stage in trapping antiprotons for the PUMA experiment. Employing a high-voltage ramping scheme, the pressure remains below $2\cdot 10^{-10}$ mbar upstream of the pulsed drift tube for 75% of the cycle time. The beamline reached a transmission of ($55 \pm 3$)% for antiprotons decelerated to 4 keV. The beam is focused on a position sensitive detector to a spot with horizontal and vertical standard deviations of ${\sigma}_\mathrm{horiz}$ = ($3.0 \pm 0.1$) mm and ${\sigma}_\mathrm{vert}$ = ($3.8 \pm 0.2$) mm, respectively. This spot size is within the acceptance of the PUMA Penning trap.

The excitation energy of the 1/2$^-$ isomer in $^{99}$In at ${N=50}$ is measured to be 671(37) keV and the mass uncertainty of the 9/2$^+$ ground state is significantly reduced using the ISOLTRAP mass spectrometer at ISOLDE/CERN. The measurements exploit a major improvement in the resolution of the multi-reflection time-of-flight mass spectrometer. The results reveal an intriguing constancy of the $1/2^-$ isomer excitation energies in neutron-deficient indium that persists down to the $N = 50$ shell closure, even when all neutrons are removed from the valence shell. This trend is used to test large-scale shell model, \textit{ab initio}, and density functional theory calculations. The models have difficulties describing both the isomer excitation energies and ground-state electromagnetic moments along the indium chain., Comment: 13 pages, 4 figures

The use of radioactive molecules for fundamental physics research is a developing interdisciplinary field limited dominantly by their scarce availability. In this work, radioactive molecular ion beams containing actinide nuclei extracted from uranium carbide targets are produced via the Isotope Separation On-Line technique at the CERN-ISOLDE facility. Two methods of molecular beam production are studied: extraction of molecular ion beams from the ion source, and formation of molecular ions from the mass-separated ion beam in a gas-filled radio-frequency quadrupole ion trap. Ion currents of U$^+$, UO$_{1-3}^+$, UC$_{1-3}^+$, UF$_{1-4}^+$, UF$_{1,2}$O$_{1,2}^+$ are reported. Metastable tantalum and uranium fluoride molecular ions are identified. Formation of UO$_{1-3}^+$, U(OH)$_{1-3}^+$, UC$_{1-3}^+$, UF$_{1,2}$O$_{1,2}^+$ from mass-separated beams of U$^+$, UF$_{1,2}^+$ with residual gas is observed in the ion trap. The effect of trapping time on molecular formation is presented., Comment: 6 pages, 7 figures

STRASSE (Silicon Tracker for RAdioactive nuclei Studies at SAMURAI Experiments) is a new detection system under construction for quasi-free scattering (QFS) measurements at 200-250 MeV/nucleon at the RIBF facility of the RIKEN Nishina Center. It consists of a charged-particle silicon tracker coupled with a dedicated thick liquid hydrogen target (up to 150-mm long) in a compact geometry to fit inside large scintillator or germanium arrays. Its design was optimized for two types of studies using QFS: missing-mass measurements and in-flight prompt $\gamma$-ray spectroscopy. This article describes (i) the resolution requirements needed to go beyond the sensitivity of existing systems for these two types of measurements, (ii) the conceptual design of the system using detailed simulations of the setup and (iii) its complete technical implementation and challenges. The final tracker aims at a sub-mm reaction vertex resolution and is expected to reach a missing-mass resolution below 2 MeV in $\sigma$ for $(p,2p)$ reactions when combined with the CsI(Na) CATANA array., Comment: 25 pages, 29 figures

Combining laser spectroscopy in a Versatile Arc Discharge and Laser Ion Source, with Penning-trap mass spectrometry at the CERN-ISOLDE facility, this work reports on mean-square charge radii of neutron-rich mercury isotopes across the $N = 126$ shell closure, the electromagnetic moments of $^{207}$Hg and more precise mass values of $^{206-208}$Hg. The odd-even staggering (OES) of the mean square charge radii and the kink at $N = 126$ are analyzed within the framework of covariant density functional theory (CDFT), with comparisons between different functionals to investigate the dependence of the results on the underlying single-particle structure. The observed features are defined predominantly in the particle-hole channel in CDFT, since both are present in the calculations without pairing. However, the magnitude of the kink is still affected by the occupation of the $1i_{11/2}$ and $2g_{9/2}$ orbitals with a dependence on the relative energies as well as pairing., Comment: 20 pages, 12 figures, Phys. Rev. C in press

100Sn is of singular interest for nuclear structure. Its closed-shell proton and neutron configuration exhibit exceptional binding and 100Sn is the heaviest nucleus comprising protons and neutrons in equal number, a feature that enhances the contribution of the short-range, proton-neutron pairing interaction and strongly influences its decay via the weak interaction. Decays studies in the region of 100Sn have attempted to prove its doubly magic character but few have studied it from the ab initio theoretical perspective and none have addressed the odd-proton nuclear forces. Here we present, the first direct measurement of the exotic odd-proton nuclide 100In - the beta-decay daughter of 100Sn - and 99In, only one proton below 100Sn. The most advanced mass spectrometry techniques were used to measure 99In, produced at a rate of only a few ions per second, and to resolve the ground and isomeric states in 101In. The experimental results are confronted with new ab initio many-body approaches. The 100-fold improvement in precision of the 100In mass value exarcebates a striking discrepancy in the atomic mass values of 100Sn deduced from recent beta-decay results., Comment: 12 pages, 4 figures, 1 Table

Isotope shifts of $^{223-226,228}$Ra$^{19}$F were measured for different vibrational levels in the electronic transition $A^{2}{}{\Pi}_{1/2}\leftarrow X^{2}{}{\Sigma}^{+}$. The observed isotope shifts demonstrate the particularly high sensitivity of radium monofluoride to nuclear size effects, offering a stringent test of models describing the electronic density within the radium nucleus. Ab initio quantum chemical calculations are in excellent agreement with experimental observations. These results highlight some of the unique opportunities that short-lived molecules could offer in nuclear structure and in fundamental symmetry studies., Comment: The paper was accepted for publication as a Letter in Physical Review Letters

The mean-square charge radii of $^{207,208}$Hg ($Z=80, N=127,128$) have been studied for the first time and those of $^{202,203,206}$Hg ($N=122,123,126$) remeasured by the application of in-source resonance-ionization laser spectroscopy at ISOLDE (CERN). The characteristic \textit{kink} in the charge radii at the $N=126$ neutron shell closure has been revealed, providing the first information on its behavior below the $Z=82$ proton shell closure. A theoretical analysis has been performed within relativistic Hartree-Bogoliubov and non-relativistic Hartree-Fock-Bogoliubov approaches, considering both the new mercury results and existing lead data. Contrary to previous interpretations, it is demonstrated that both the kink at $N=126$ and the odd-even staggering (OES) in its vicinity can be described predominately at the mean-field level, and that pairing does not need to play a crucial role in their origin. A new OES mechanism is suggested, related to the staggering in the occupation of the different neutron orbitals in odd- and even-$A$ nuclei, facilitated by particle-vibration coupling for odd-$A$ nuclei., Comment: 7 pages, 5 figures, Physical Review C, in press

Mass measurements of $^{49,50}$Sc, $^{70}$As, $^{73}$Br and $^{196}$Hg nuclides produced at CERN's radioactive-ion beam facility ISOLDE are presented. The measurements were performed at the ISOLTRAP mass spectrometer by use of the multi-reflection time-of-flight and the Penning-trap mass spectrometry techniques. The new results agree well with previously known literature values. The mass accuracy for all cases has been improved.

We determine for the first time the magnetic dipole moment of a short-lived nucleus with part-per-million (ppm) accuracy. To achieve this two orders of magnitude improvement over previous studies, we implement a number of innovations into our $\beta$-detected Nuclear Magnetic Resonance ($\beta$-NMR) setup at ISOLDE/CERN. Using liquid samples as hosts we obtain narrow, sub-kHz linewidth, resonances, while a simultaneous in-situ $^1$H NMR measurement allows us to calibrate and stabilize the magnetic field to ppm precision, thus eliminating the need for additional $\beta$-NMR reference measurements. Furthermore, we use ab initio calculations of NMR shielding constants to improve the accuracy of the reference magnetic moment, thus removing a large systematic error. We demonstrate the potential of this combined approach with the 1.1 s half-life radioactive nucleus $^{26}$Na, which is relevant for biochemical studies. Our technique can be readily extended to other isotopic chains, providing accurate magnetic moments for many short-lived nuclei. Furthermore, we discuss how our approach can open the path towards a wide range of applications of the ultra-sensitive $\beta$-NMR in physics, chemistry, and biology., Comment: re-submitted

We probe the $N=82$ nuclear shell closure by mass measurements of neutron-rich cadmium isotopes with the ISOLTRAP spectrometer at ISOLDE-CERN. The new mass of $^{132}$Cd offers the first value of the $N=82$, two-neutron shell gap below $Z=50$ and confirms the phenomenon of mutually enhanced magicity at $^{132}$Sn. Using the recently implemented phase-imaging ion-cyclotron-resonance method, the ordering of the low-lying isomers in $^{129}$Cd and their energies are determined. The new experimental findings are used to test large-scale shell-model, mean-field and beyond-mean-field calculations, as well as the ab initio valence-space in-medium similarity renormalization group., Comment: 7 pages, 5 figures; reference added, minor editorial corrections

The study of molecular systems provides exceptional opportunities for the exploration of the fundamental laws of nature and for the search for physics beyond the Standard Model of particle physics. Measurements of molecules composed of naturally occurring nuclei have provided the most stringent upper bounds to the electron electric dipole moment to date, and offer a route to investigate the violation of fundamental symmetries with unprecedented sensitivity. Radioactive molecules - where one or more of their atoms possesses a radioactive nucleus - can contain heavy and deformed nuclei, offering superior sensitivity for EDM measurements as well as for other symmetry-violating effects. Radium monofluoride, RaF, is of particular interest as it is predicted to have an appropriate electronic structure for direct laser cooling. Furthermore, some Ra isotopes are known to be octupole deformed, thereby resulting in a large enhancement of their symmetry-violating nuclear moments. Until now,however, no experimental measurements of RaF have been performed, and their study is impeded by major experimental challenges, as no stable isotopes of radium exist. Here, we present a novel experimental approach to study short-lived radioactive molecules using the highly sensitive collinear resonance ionisation method. With this technique we have measured, for the first time, the energetically low-lying electronic states for each of the isotopically pure RaF molecules at the ISOLDE-CERN. Our results provide strong evidence of the existence of a suitable laser-cooling scheme for these molecules and constitute a pivotal step towards high-precision studies in these systems. Our findings open up new opportunities in the synthesis, manipulation and study of short-lived radioactive molecules, which will have a direct impact in many-body physics, astrophysics, nuclear structure, and fundamental physics research., Comment: Submitted

Neutron-deficient $^{177-185}$Hg isotopes were studied using in-source laser resonance-ionization spectroscopy at the CERN-ISOLDE radioactive ion-beam facility, in an experiment combining different detection methods tailored to the studied isotopes. These include either alpha-decay tagging or Multi-reflection Time-of-Flight gating to identify the isotopes of interest. The endpoint of the odd-even nuclear shape staggering in mercury was observed directly by measuring for the first time the isotope shifts and hyperfine structures of $^{177-180}$Hg. Changes in the mean-square charge radii for all mentioned isotopes, magnetic dipole and electric quadrupole moments of the odd-A isotopes and arguments in favor of $I = 7/2$ spin assignment for $^{177,179}$Hg were deduced. Experimental results are compared with Density Functional Theory (DFT) and Monte-Carlo Shell Model (MCSM) calculations. DFT calculations with several Skyrme parameterizations predict a large jump in the charge radius around the neutron $N = 104$ mid shell, with an odd-even staggering pattern related to the coexistence of nearly-degenerate oblate and prolate minima. This near-degeneracy is highly sensitive to many aspects of the effective interaction, a fact that renders perfect agreement with experiment out of reach for current functionals. Despite this inherent diffculty, the SLy5s1 and a modified UNEDF1^{SO} parameterization predict a qualitatively correct staggering that is off by two neutron numbers. MCSM calculations of states with the experimental spins and parities show good agreement for both electromagnetic moments and the observed charge radii. A clear mechanism for the origin of shape staggering within this context is identified: a substantial change in occupancy of the proton $\pi h_{9/2}$ and neutron $\nu i_{13/2}$ orbitals., Comment: 19 pages, 18 figures

A beamline dedicated to the production of laser-polarized radioactive beams has been constructed at ISOLDE, CERN. We present here different simulations leading to the design and construction of the setup, as well as technical details of the full setup and examples of the achieved polarizations for several radioisotopes. Beamline simulations show a good transmission through the entire line, in agreement with observations. Simulations of the induced nuclear spin-polarization as a function of atom-laser interaction length are presented for $^{26,28}$Na, [1] and for $^{35}$Ar, which is studied in this work. Adiabatic spin rotation of the spin-polarized ensemble of atoms, and how this influences the observed nuclear ensemble polarization, are also performed for the same nuclei. For $^{35}$Ar, we show that multiple-frequency pumping enhances the ensemble polarization by a factor 1.85, in agreement with predictions from a rate equations model. [1] J. Phys. G: Nucl. Part. Phys./1744084005

Direct mass measurements of the low-spin $3/2^{(-)}$ and high-spin $13/2^{(+)}$ states in the neutron-deficient isotopes $^{195}$Po, $^{197}$Po, and high-spin $13/2^{(+)}$ state in $^{199}$Po were performed with the Penning-trap mass spectrometer ISOLTRAP at ISOLDE-CERN. These measurements allow the determination of the excitation energy of the isomeric state arising from the $\nu$i$_{13/2}$ orbital in $^{195,197}$Po. Additionally, the excitation energy of isomeric states of lead, radon, and radium isotopes in this region were obtained from $\alpha$-decay chains. The new excitation energies complete the knowledge of the energy systematics in the region and confirm for the first time that the $13/2^{(+)}$ states remain isomeric, independent of the number of valence neutrons.

Masses adjacent to the classical waiting-point nuclide 130Cd have been measured by using the Penning- trap spectrometer ISOLTRAP at ISOLDE/CERN. We find a significant deviation of over 400 keV from earlier values evaluated by using nuclear beta-decay data. The new measurements show the reduction of the N = 82 shell gap below the doubly magic 132Sn. The nucleosynthesis associated with the ejected wind from type-II supernovae as well as from compact object binary mergers is studied, by using state-of-the-art hydrodynamic simulations. We find a consistent and direct impact of the newly measured masses on the calculated abundances in the A = 128 - 132 region and a reduction of the uncertainties from the precision mass input data.

The recently confirmed neutron-shell closure at N = 32 has been investigated for the first time below the magic proton number Z = 20 with mass measurements of the exotic isotopes 52,53K, the latter being the shortest-lived nuclide investigated at the online mass spectrometer ISOLTRAP. The resulting two-neutron separation energies reveal a 3 MeV shell gap at N = 32, slightly lower than for 52Ca, highlighting the doubly-magic nature of this nuclide. Skyrme-Hartree-Fock-Boguliubov and ab initio Gorkov-Green function calculations are challenged by the new measurements but reproduce qualitatively the observed shell effect., Comment: 5 pages, 5 figures