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In spite of the high-density and strongly correlated nature of the atomic nucleus, experimental and theoretical evidence suggests that around particular ‘magic’ numbers of nucleons, nuclear properties are governed by a single unpaired nucleon 1 , 2 . A microscopic understanding of the extent of this behaviour and its evolution in neutron-rich nuclei remains an open question in nuclear physics 3 – 5 . The indium isotopes are considered a textbook example of this phenomenon 6 , in which the constancy of their electromagnetic properties indicated that a single unpaired proton hole can provide the identity of a complex many-nucleon system 6 , 7 . Here we present precision laser spectroscopy measurements performed to investigate the validity of this simple single-particle picture. Observation of an abrupt change in the dipole moment at N  = 82 indicates that, whereas the single-particle picture indeed dominates at neutron magic number N  = 82 (refs.  2 , 8 ), it does not for previously studied isotopes. To investigate the microscopic origin of these observations, our work provides a combined effort with developments in two complementary nuclear many-body methods: ab initio valence-space in-medium similarity renormalization group and density functional theory (DFT). We find that the inclusion of time-symmetry-breaking mean fields is essential for a correct description of nuclear magnetic properties, which were previously poorly constrained. These experimental and theoretical findings are key to understanding how seemingly simple single-particle phenomena naturally emerge from complex interactions among protons and neutrons. Precision laser spectroscopy measurements of neutron-rich indium isotopes were performed to investigate the validity and identify limitations of theoretical descriptions of nuclei based on simple single-particle approaches.

Resonant laser ionization and spectroscopy are widely used techniques at radioactive ion beam facilities to produce pure beams of exotic nuclei and measure the shape, size, spin and electromagnetic multipole moments of these nuclei. However, in such measurements it is difficult to combine a high efficiency with a high spectral resolution. Here we demonstrate the on-line application of atomic laser ionization spectroscopy in a supersonic gas jet, a technique suited for high-precision studies of the ground- and isomeric-state properties of nuclei located at the extremes of stability. The technique is characterized in a measurement on actinium isotopes around the N =126 neutron shell closure. A significant improvement in the spectral resolution by more than one order of magnitude is achieved in these experiments without loss in efficiency. It is challenging to explore properties of heavy elements as they can only be produced artificially. Here, the authors demonstrate a high resolution spectroscopy method, studying the properties of actinium, which can be extended to the study of other elements located at the end of the periodic table.

Molecules containing heavy radioactive nuclei are predicted to be extremely sensitive to violations of the fundamental symmetries of nature. The nuclear octupole deformation of certain radium isotopes massively boosts the sensitivity of radium monofluoride molecules to symmetry-violating nuclear properties. Moreover, these molecules are predicted to be laser coolable. Here we report measurements of the rovibronic structure of radium monofluoride molecules, which allow the determination of their laser cooling scheme. We demonstrate an improvement in resolution of more than two orders of magnitude compared to the state of the art. Our developments allowed measurements of minuscule amounts of hot molecules, with only a few hundred per second produced in a particular rotational state. The combined precision and sensitivity achieved in this work offer opportunities for studies of radioactive molecules of interest in fundamental physics, chemistry and astrophysics. Measurements of the rovibronic structure of radium monofluoride molecules allow the identification of a laser cooling scheme. This will enable precise tests of fundamental physics, such as searches for parity or time-reversal symmetry violation.

A two-step resonance photo-ionization scheme has been used to ionize samarium atoms in the SPES tantalum hot-cavity ion source. The effect of the ion load on the ion beam time structure and the laser enhancement of the ion yield has been studied at different ion source temperatures. Generally, the introduction of more positive ions (ion load) affects negatively the overall confinement of the laser ions inside the volume of the ion source. Possible enhancement of the laser ion confinement through the introduction of neutrals is observed as well. The ion load is also observed to affect the confinement in the transfer line much more than in the hot cavity. Measurement of the time structure with inverted polarity of the cavity DC heating supply confirmed the significance of the longitudinal potential for ion extraction. The laser enhancements of the ion yield are found to be sensitive to the ion load at low operating temperature of the ion source i.e. 1800°C, whereas at 2050°C and 2200°C, they are relatively stable till an ion load value of 1.2 µA.

CERN-MEDICIS is an isotope mass separation facility dedicated to biomedical research located in a type A work sector, receiving on average 50% of the 1.4 GeV protons delivered by the Proton Synchrotron Booster (PSB). It was commissioned with Radioactive Ion Beams (RIB’s) in 2017. MEDICIS has operated for the past 5 years in batch mode, with targets irradiated in a station located at the HRS beam dump, and with external sources provided by MEDICIS cyclotrons and nuclear reactors partners, notably during the Long Shutdown (LS2). Additional features of the facility include the MELISSA laser ion source, radiochemistry on implanted radionuclides and an online gamma-ray spectroscopy implantation monitoring. In 2022, we introduced Key Performance Indicators (KPI’s) to monitor the operation of the facility for collected efficiencies, the optimisation of the radiological risks and evaluate impact of possible modifications of the station, paralleling for instance LHC’s integrated luminosity. Defined KPI’s cover aspects in the operation cycle, e.g. planning in CERN schedule, target irradiations, duration of the process, radiological risk mitigation, facility up-time, developments and maintenance. MEDICIS KPI’s can help distinguish which of the operation and infrastructure life cycle requires immediate intervention, developments or consolidation. Those are related to the irradiation stations and irradiation possibilities, the beamlines (parallel collections), target and ion sources (reliability), robot handling and infrastructure, or the separation process itself.

Highly accurate and precise electronic structure calculations of heavy radioactive atoms and their molecules are important for several research areas, including chemical, nuclear, and particle physics. Ab initio quantum chemistry can elucidate structural details in these systems that emerge from the interplay of relativistic and electron correlation effects, but the large number of electrons complicates the calculations, and the scarcity of experiments prevents insightful theory-experiment comparisons. Here we report the spectroscopy of the 14 lowest excited electronic states in the radioactive molecule radium monofluoride (RaF), which is proposed as a sensitive probe for searches of new physics. The observed excitation energies are compared with state-of-the-art relativistic Fock-space coupled cluster calculations, which achieve an agreement of ≥99.64% (within  ~12 meV) with experiment for all states. Guided by theory, a firm assignment of the angular momentum and term symbol is made for 10 states and a tentative assignment for 4 states. The role of high-order electron correlation and quantum electrodynamics effects in the excitation energies is studied and found to be important for all states. Heavy-atom molecules can possess complicated electronic structures due to pronounced electron correlation and relativistic effects. Here, the authors describe electronic states of RaF in detail by combining accurate spectroscopy and theory approaches.

Accelerator-based techniques are one of the leading ways to produce radioactive nuclei. In this work, the Isotope Separation On-Line method was employed at the CERN-ISOLDE facility to produce neptunium and plutonium from a uranium carbide target material using 1.4-GeV protons. Neptunium and plutonium were laser-ionized and extracted as 30-keV ion beams. A Multi-Reflection Time-of-Flight mass spectrometer was used for ion identification by means of time-of-flight measurements as well as for isobaric separation. Isotope shifts were investigated for the 395.6-nm ground state transition in \\(^{236,237,239}\\)Np and the 413.4-nm ground state transition in \\(^{236,239,240}\\)Pu. Rates of \\(^{235-241}\\)Np and \\(^{234-241}\\)Pu ions were measured and compared with predictions of in-target production mechanisms simulated with GEANT4 and FLUKA to elucidate the processes by which these nuclei, which contain more protons than the target nucleus, are formed. \\(^{241}\\)Pu is the heaviest nuclide produced and identified at a proton-accelerator-driven facility to date. We report the availability of neptunium and plutonium as two additional elements at CERN-ISOLDE and discuss the limit of accelerator-based isotope production at high-energy proton accelerator facilities for nuclides in the actinide region.

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.

The thick-target ISOL (Isotope mass Separation OnLine) method provides beams of more than 1000 radionuclides of 74 elements. The method is well established for elements with sufficiently high volatility at ca. 2000 {\\deg}C. To extract non-volatile elements the formation of a volatile molecule is required. While successful in some cases (e.g. carbon or boron), most of these elements are not yet available as ISOL beam. A variety of volatile carrier molecules has been proposed for all elements produced in the target material, but their probability of survival during the extraction and ionization process is often limited by the high temperatures required for isotope diffusion in the thick targets and for ion source operation. While cold target concepts have already been proposed, the normal mode of operation of the typically used Versatile Arc Discharge Ion Source (VADIS) with a hot cathode is not well suited. Here, we report about first measurements with an electron-impact ion source operated at ambient temperature using electrons that were liberated via the photo-electric effect from a copper cathode.