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Nuclear charge radii globally scale with atomic mass number A as A 1∕3 , and isotopes with an odd number of neutrons are usually slightly smaller in size than their even-neutron neighbours. This odd–even staggering, ubiquitous throughout the nuclear landscape 1 , varies with the number of protons and neutrons, and poses a substantial challenge for nuclear theory 2 – 4 . Here, we report measurements of the charge radii of short-lived copper isotopes up to the very exotic 78 Cu (with proton number Z = 29 and neutron number N = 49), produced at only 20 ions s –1 , using the collinear resonance ionization spectroscopy method at the Isotope Mass Separator On-Line Device facility (ISOLDE) at CERN. We observe an unexpected reduction in the odd–even staggering for isotopes approaching the N = 50 shell gap. To describe the data, we applied models based on nuclear density functional theory 5 , 6 and A -body valence-space in-medium similarity renormalization group theory 7 , 8 . Through these comparisons, we demonstrate a relation between the global behaviour of charge radii and the saturation density of nuclear matter, and show that the local charge radii variations, which reflect the many-body polarization effects, naturally emerge from A -body calculations fitted to properties of A ≤ 4 nuclei. Isotopes with an odd number of neutrons are usually slightly smaller in size than their even-neutron neighbours. In charge radii of short-lived copper isotopes, a reduction of this effect is observed when the neutron number approaches fifty.

Molecular spectroscopy offers opportunities for the exploration of the fundamental laws of nature and the search for new particle physics beyond the standard model 1 – 4 . Radioactive molecules—in which one or more of the atoms possesses a radioactive nucleus—can contain heavy and deformed nuclei, offering high sensitivity for investigating parity- and time-reversal-violation effects 5 , 6 . Radium monofluoride, RaF, is of particular interest because it is predicted to have an electronic structure appropriate for laser cooling 6 , thus paving the way for its use in high-precision spectroscopic studies. Furthermore, the effects of symmetry-violating nuclear moments are strongly enhanced 5 , 7 – 9 in molecules containing octupole-deformed radium isotopes 10 , 11 . However, the study of RaF has been impeded by the lack of stable isotopes of radium. Here we present an experimental approach to studying short-lived radioactive molecules, which allows us to measure molecules with lifetimes of just tens of milliseconds. Energetically low-lying electronic states were measured for different isotopically pure RaF molecules using collinear resonance ionisation at the ISOLDE ion-beam facility at CERN. Our results provide evidence of the existence of a suitable laser-cooling scheme for these molecules and represent a key step towards high-precision studies in these systems. Our findings will enable further studies of short-lived radioactive molecules for fundamental physics research. Measurements of low-energy electronic states of radium monofluoride validate predictions of the use of this short-lived radioactive molecule in exploring fundamental physics and provide evidence of its suitability for laser cooling.

In rare cases, the removal of a single proton (Z) or neutron (N) from an atomic nucleus leads to a dramatic shape change. These instances are crucial for understanding the components of the nuclear interactions that drive deformation. The mercury isotopes (Z = 80) are a striking example1,2: their close neighbours, the lead isotopes (Z = 82), are spherical and steadily shrink with decreasing N. The even-mass (A = N + Z) mercury isotopes follow this trend. The odd-mass mercury isotopes 181,183,185Hg, however, exhibit noticeably larger charge radii. Due to the experimental difficulties of probing extremely neutron-deficient systems, and the computational complexity of modelling such heavy nuclides, the microscopic origin of this unique shape staggering has remained unclear. Here, by applying resonance ionization spectroscopy, mass spectrometry and nuclear spectroscopy as far as 177Hg, we determine 181Hg as the shape-staggering endpoint. By combining our experimental measurements with Monte Carlo shell model calculations, we conclude that this phenomenon results from the interplay between monopole and quadrupole interactions driving a quantum phase transition, for which we identify the participating orbitals. Although shape staggering in the mercury isotopes is a unique and localized feature in the nuclear chart, it nicely illustrates the concurrence of single-particle and collective degrees of freedom at play in atomic nuclei.

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.

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.

The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements. Measuring the electron affinity, a fundamental chemical property, has been challenging for rare elements due to sensitivity limitations. Here, the authors present a novel ion-trap technique capable of performing high-precision affinity measurements with orders of magnitude fewer samples.

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.

The presented paper discusses the production of radioactive ion beams of francium, radium, and actinium from thick uranium carbide (UC x ) targets at ISOLDE, CERN. This study focuses on the release curves and extractable yields of francium, radium and actinium isotopes. The ion source temperature was varied in order to study the relative contributions of surface and laser ionization to the production of the actinium ion beams. The experimental results are presented in the form of release parameters. Representative extractable yields per μ C are presented for 222 - 231 Ac, several Ra and Fr isotopes in the mass ranges 214 ≤ A ≤ 233 and 205 ≤ A ≤ 231 respectively. The release efficiency for several isotopes of each of the studied elements was calculated by comparing their yields to the estimated in-target production rates modeled by CERN-FLUKA. The maximal extraction efficiency of actinium was calculated to be 2.1(6)% for a combination of surface ionization using a Ta ion source and resonant laser ionization using the two-step 438.58 nm, and 424.69 nm scheme.

The radioactive element astatine exists only in trace amounts in nature. Its properties can therefore only be explored by study of the minute quantities of artificially produced isotopes or by performing theoretical calculations. One of the most important properties influencing the chemical behaviour is the energy required to remove one electron from the valence shell, referred to as the ionization potential. Here we use laser spectroscopy to probe the optical spectrum of astatine near the ionization threshold. The observed series of Rydberg states enabled the first determination of the ionization potential of the astatine atom, 9.31751(8) eV. New ab initio calculations are performed to support the experimental result. The measured value serves as a benchmark for quantum chemistry calculations of the properties of astatine as well as for the theoretical prediction of the ionization potential of superheavy element 117, the heaviest homologue of astatine. The application of astatine, one of the rarest elements on the earth, in the treatment of cancer requires a better understanding of its chemistry. Rothe et al . report the first measurement of the ionization potential of astatine, against which high-level quantum calculations are benchmarked.

There is a large body of evidence that atomic nuclei can undergo octupole distortion and assume the shape of a pear. This phenomenon is important for measurements of electric-dipole moments of atoms, which would indicate CP violation and hence probe physics beyond the Standard Model of particle physics. Isotopes of both radon and radium have been identified as candidates for such measurements. Here, we observed the low-lying quantum states in 224 Rn and 226 Rn by accelerating beams of these radioactive nuclei. We show that radon isotopes undergo octupole vibrations but do not possess static pear-shapes in their ground states. We conclude that radon atoms provide less favourable conditions for the enhancement of a measurable atomic electric-dipole moment. Octupole deformation in nuclei is important to understand nuclear structure and electric dipole moments of heavy atoms. Here the authors measure energies of excited quantum states in radon isotopes and find that these isotopes do not provide favourable conditions in the search for CP-violation.