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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 ($D_{0}$) of 5.54[5] eV is presented. This confirms that radium monofluoride joins the small group of diatomic molecules for which $D_{0}>\mathrm{IP}$, paving the way for precision control and interrogation of its Rydberg states.

The radiative lifetime of the $A$ $^2 \Pi_{1/2}$ (v=0) state in radium monofluoride (RaF) is measured to be 35(1) ns. The lifetime of this state and the related decay rate $\Gamma = 2.86(8) \times 10^7$ $s^{-1}$ are of relevance to the laser cooling of RaF via the optically closed $A$ $^2 \Pi_{1/2} \leftarrow X$ $^2\Sigma_{1/2}$ transition, which makes the molecule a promising probe to search for new physics. RaF is found to have a comparable photon-scattering rate to homoelectronic laser-coolable molecules. Thanks to its highly diagonal Franck-Condon matrix, it is expected to scatter an order of magnitude more photons than other molecules when using just 3 cooling lasers, before it decays to a dark state. The lifetime measurement in RaF is benchmarked by measuring the lifetime of the $8P_{3/2}$ state in Fr to be 83(3) ns, in agreement with literature., Comment: Accepted as a Letter in Physical Review A; 8 pages of main text, 5 pages of supplemental material

Rapid progress in the experimental control and interrogation of molecules, combined with developments in precise calculations of their structure, are enabling new opportunities in the investigation of nuclear and particle physics phenomena. Molecules containing heavy, octupole-deformed nuclei such as radium are of particular interest for such studies, offering an enhanced sensitivity to the properties of fundamental particles and interactions. Here, we report precision laser spectroscopy measurements and theoretical calculations of the structure of the radioactive radium monofluoride molecule, $^{225}$Ra$^{19}$F. Our results allow fine details of the short-range electron-nucleus interaction to be revealed, indicating the high sensitivity of this molecule to the distribution of magnetization, currently a poorly constrained nuclear property, within the radium nucleus. These results provide a direct and stringent test of the description of the electronic wavefunction inside the nuclear volume, highlighting the suitability of these molecules to investigate subatomic phenomena.

Our understanding of nuclear properties in the vicinity of $^{100}$Sn, suggested to be the heaviest doubly magic nucleus with equal numbers of protons (Z=50) and neutrons (N=50), has been a long-standing challenge for experimental and theoretical nuclear physics. Contradictory experimental evidence exists on the role of nuclear collectivity in this region of the nuclear chart. Using precision laser spectroscopy, we measured the ground-state electromagnetic moments of indium (Z=49) isotopes approaching the N=50 neutron number down to 101In, and nuclear charge radii of 101-131In spanning almost the complete range between the two major neutron closed-shells at N=50 and N=82. Our results for both nuclear charge radii and quadrupole moments reveal striking parabolic trends as a function of the neutron number, with a clear reduction toward these two neutron closed-shells, thus supporting a doubly magic character of $^{100}$Sn. Two complementary nuclear many-body frameworks, density functional theory and ab initio methods, elucidate our findings. A detailed comparison with our experimental results exposes deficiencies of nuclear models, establishing a benchmark for future theoretical developments., Comment: 12 pages, 6 figures, 4 tables; text-identical to Nature Physics article (2024)

We present a comprehensive theoretical study of the ionization potentials of the MF (M= Ca, Sr, Ba) molecules using the state-of-the-art relativistic coupled cluster approach with single, double, and perturbative triple excitations (CCSD(T)). We have further corrected our results for the higher order excitations (up to full triples) and the QED self energy and vacuum polarisation contributions. We have performed an extensive investigation of the effect of the various computational parameters on the calculated ionisation potentials, which allowed us to assign realistic uncertainties on our predictions. For CaF and BaF, where precise experiments are available, our predictions are in excellent agreement with the measured values. In case of SrF, we provide a new accurate prediction of the ionisation potential that deviates from the available experimental data, motivating further experimental investigations., Comment: 7 pages, before paper submission (references will be added additionally)

We report the spectroscopy of 11 electronic states in the radioactive molecule radium monofluoride (RaF). The observed excitation energies are compared with state-of-the-art relativistic Fock-space coupled cluster (FS-RCC) calculations, which achieve an agreement of >99.71% (within ~8 meV) for all states. High-order electron correlation and quantum electrodynamics corrections are found to be important at all energies. Establishing the accuracy of calculations is an important step towards high-precision studies of these molecules, which are proposed for sensitive searches of physics beyond the Standard Model., Comment: Submitted for publication

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

Investigation into the properties and structure of unstable nuclei far from stability remains a key avenue of research in modern nuclear physics. These efforts are motivated by the continual observation of unexpected structure phenomena in nuclei with unusual proton-to-neutron ratios. In recent decades, laser spectroscopy techniques have made significant contributions in our understanding of exotic nuclei in different mass regions encompassing almost the entire nuclear chart. This is achieved through determining multiple fundamental properties of nuclear ground and isomeric states, such as nuclear spins, magnetic dipole and electric quadrupole moments and charge radii, via the measurement of hyperfine structures and isotope shifts in the atomic or ionic spectra of the nuclei of interest. These properties, when measured with sufficient precision for a long range of isotopes, offer prominent tests of recently developed state-of-the-art theory and help to stimulate new developments to improve the many-body methods and nucleon-nucleon interactions at the core of these models. With the aim of exploring more exotic short-lived nuclei located ever closer to the proton and neutron driplines, laser spectroscopy techniques, with their continuous technological developments towards higher resolution and higher sensitivity, are extensively employed at current- and next-generation radioactive ion beam facilities worldwide. Ongoing efforts in parallel promise to make even more exotic species available for study at next-generation facilities. Very recently, an innovative application of laser spectroscopy on molecules containing short-lived nuclei has been demonstrated offering additional opportunities for several fields of research, e.g. fundamental symmetry studies and astrophysics., Comment: 129 pages (bibliography 56 pages), 32 figures, invited review for Progress in Particle and Nuclear Physics. Comments and suggestions are welcome

The electric quadrupole moment of $^{49}$Sc was measured by collinear laser spectroscopy at CERN-ISOLDE to be $Q_{\rm s}=-0.159(8)$ $e$b, and a nearly tenfold improvement in precision was reached for the electromagnetic moments of $^{47,49}$Sc. The single-particle behavior and nucleon-nucleon correlations are investigated with the electromagnetic moments of $Z=21$ isotopes and $N=28$ isotones as valence neutrons and protons fill the distinctive $0f_{7/2}$ orbit, respectively, located between magic numbers, 20 and 28. The experimental data are interpreted with shell-model calculations using an effective interaction, and ab-initio valence-space in-medium similarity renormalization group calculations based on chiral interactions. These results highlight the sensitivity of nuclear electromagnetic moments to different types of nucleon-nucleon correlations, and establish an important benchmark for further developments of theoretical calculations., Comment: Accepted by Physics Letters B (2022)

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

We introduce a novel thick-target concept tailored to the extraction of refractory 4d and 5d transition metal radionuclides of molybdenum, technetium, ruthenium and tungsten for radioactive ion beam production. Despite the more than 60-year old history of thick-target ISOL mass-separation facilities like ISOLDE, the extraction of the most refractory elements as radioactive ion beam has so far not been successful. In ordinary thick ISOL targets, their radioisotopes produced in the target are stopped within the condensed target material and have to diffuse through a solid material. Here, we present a concept which overcomes limitations associated with this method. We exploit the recoil momentum of nuclear reaction products for their release from the solid target material. They are thermalized in a carbon monoxide-containing atmosphere, in which volatile carbonyl complexes form readily at ambient temperature and pressure. This compound serves as volatile carrier for transport to the ion source. Excess carbon monoxide is removed by cryogenic gas separation to enable low pressures in the source region, in which the species are ionized and hence made available for radioactive ion beam formation. The setup is operated in batch mode, with the aim to extract isotopes having half-lives of at least several seconds. We report parameter studies of the key processes of the method, which validate this concept and which define the parameters for the setup. This would allow for the first time the extraction of radioactive molybdenum, tungsten and several other transition metals at thick-target ISOL facilities.

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

We perform a combined theoretical and experimental investigation of the superradiance in the quantum coherent system generated by strong laser fields. The semiclassical theory of superradiance that includes the superradiant temporal profile, character duration, time delay, intensity is derived. The experimental data and theoretical predictions of 391-nm forward emission as a function of nitrogen gas pressure are compared and show good agreement. Our results not only demonstrate that the time-delayed optical amplification inside the molecular nitrogen ions is superradiance, but also reveal the quantum optical properties of strong-field physics., Comment: 11 pages, 5 figures

Nuclear charge radii are sensitive probes of different aspects of the nucleon-nucleon interaction and the bulk properties of nuclear matter; thus, they provide a stringent test and challenge for nuclear theory. The calcium region has been of particular interest, as experimental evidence has suggested a new magic number at $N = 32$ [1-3], while the unexpectedly large increases in the charge radii [4,5] open new questions about the evolution of nuclear size in neutron-rich systems. By combining the collinear resonance ionization spectroscopy method with $\beta$-decay detection, we were able to extend the charge radii measurement of potassium ($Z =19$) isotopes up to the exotic $^{52}$K ($t_{1/2}$ = 110 ms), produced in minute quantities. Our work provides the first charge radii measurement beyond $N = 32$ in the region, revealing no signature of the magic character at this neutron number. The results are interpreted with two state-of-the-art nuclear theories. For the first time, a long sequence of isotopes could be calculated with coupled-cluster calculations based on newly developed nuclear interactions. The strong increase in the charge radii beyond $N = 28$ is not well captured by these calculations, but is well reproduced by Fayans nuclear density functional theory, which, however, overestimates the odd-even staggering effect. These findings highlight our limited understanding on the nuclear size of neutron-rich systems, and expose pressing problems that are present in some of the best current models of nuclear theory., Comment: submitted version; revision accepted in Nature Physics

The mesoscopic nature of the atomic nucleus gives rise to a wide array of macroscopic and microscopic phenomena. The size of the nucleus is a window into this duality: while the charge radii globally scale as $A^{1/3}$, their evolution across isotopic chains reveals unanticipated structural phenomena [1-3]. The most ubiquitous of these is perhaps the Odd-Even Staggering (OES) [4]: isotopes with an odd number of neutrons are usually smaller in size than the trend of their even-neutron neighbours suggests. This OES effect varies with the number of protons and neutrons and poses a significant challenge for nuclear theory [5-7]. Here, we examine this problem with new measurements of the charge radii of short-lived copper isotopes up to the very exotic $^{78}$Cu $(Z=29, N=49)$, produced at only 20 ions/s, using the highly-sensitive Collinear Resonance Ionisation Spectroscopy (CRIS) method at ISOLDE-CERN. Due to the presence of a single proton outside of the closed Z=28 shell, these measurements provide crucial insights into the single-particle proton structure and how this affects the charge radii. We observe an unexpected reduction in the OES for isotopes approaching the $N=50$ shell gap. To describe the data, we applied models based on nuclear Density Functional Theory [2,8] (DFT) and ab-initio Valence-Space In-Medium Similarity Renormalization Group (VS-IMSRG) theory [9,10]. Through these comparisons, we demonstrate a relation between the global behavior 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 due to the odd neutron, naturally emerge from the VS-IMSRG calculations.

With increasing demand for accurate calculation of isotope shifts of atomic systems for fundamental and nuclear structure research, an analytic energy derivative approach is presented in the relativistic coupled-cluster theory framework to determine the atomic field shift and mass shift factors. This approach allows the determination of expectation values of atomic operators, overcoming fundamental problems that are present in existing atomic physics methods, i.e. it satisfies the Hellmann-Feynman theorem, does not involve any non-terminating series, and is free from choice of any perturbative parameter. As a proof of concept, the developed analytic response relativistic coupled-cluster theory has been applied to determine mass shift and field shift factors for different atomic states of indium. High-precision isotope-shift measurements of $^{104-127}$In were performed in the 246.8-nm (5p $^2$P$_{3/2}$ $\rightarrow$ 9s $^2$S$_{1/2}$) and 246.0-nm (5p $^2$P$_{1/2}$ $\rightarrow$ 8s $^2$S$_{1/2}$) transitions to test our theoretical results. An excellent agreement between the theoretical and measured values is found, which is known to be challenging in multi-electron atoms. The calculated atomic factors allowed an accurate determination of the nuclear charge radii of the ground and isomeric states of the $^{104-127}$In isotopes, providing an isotone-independent comparison of the absolute charge radii., Comment: Submitted

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

A new approach to observe the radiative decay of the $^{229}$Th nuclear isomer, and to determine its energy and radiative lifetime, is presented. Situated at a uniquely low excitation energy, this nuclear state might be a key ingredient for the development of a nuclear clock, a nuclear laser and the search for time variations of the fundamental constants. The isomer's $\gamma$ decay towards the ground state will be studied with a high-resolution VUV spectrometer after its production by the $\beta$ decay of $^{229}$Ac. The novel production method presents a number of advantages asserting its competitive nature with respect to the commonly used $^{233}$U $\alpha$-decay recoil source. In this paper, a feasibility analysis of this new concept, and an experimental investigation of its key ingredients, using a pure $^{229}$Ac ion beam produced at the ISOLDE radioactive beam facility, is reported., Comment: 11 pages, 5 figures, 2 tables

Nuclear spins and precise values of the magnetic dipole and electric quadrupole moments of the ground-states of neutron-rich $^{76-78}$Cu isotopes were measured using the Collinear Resonance Ionization Spectroscopy (CRIS) experiment at ISOLDE, CERN. The nuclear moments of the less exotic $^{73,75}$Cu isotopes were re-measured with similar precision, yielding values that are consistent with earlier measurements. The moments of the odd-odd isotopes, and $^{78}_{29}$Cu ($N=49$) in particular, are used to investigate excitations of the assumed doubly-magic $^{78}$Ni core through comparisons with large-scale shell-model calculations. Despite the narrowing of the $Z=28$ shell gap between $N\sim45$ and $N=50$, the magicity of $Z=28$ and $N=50$ is restored towards $^{78}$Ni. This is due to weakened dynamical correlations, as clearly probed by the present moment measurements.