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This paper reports on the measurement of the ground-state spin and nuclear magnetic dipole moment of $^{61}$Cr. The radioactive ion beam was produced at the CERN-ISOLDE facility and was probed using high-resolution resonance ionization laser spectroscopy with the CRIS apparatus. The present ground-state spin measurement $I = \frac{1}{2}$, differing from the previously adopted $I =(\frac{5}{2})$, has significant consequences on the interpretation of existing beta decay data and nuclear structure in the region. The structure and shape of $^{61}$Cr is interpreted with state-of-the-art Large-Scale Shell Model and Discrete-Non-Orthogonal Shell Model calculations. From the measured magnetic dipole moment $\mu(^{61}$Cr$)=+0.539(7)~\mu_N$ and the theoretical findings, its configuration is understood to be driven by 2 particle - 2 hole neutron excitations with an unpaired $1p_{1/2}$ neutron. This establishes the western border of the $N=40$ Island Of Inversion (IoI), characterized by 4 particle - 4 hole neutron components. We discuss the shape evolution along the Cr isotopic chain as a quantum phase transition at the entrance of the $N=40$ IoI.

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 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 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)

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

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

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

This work reports on the application of a novel electric field-ionization setup for high-resolution laser spectroscopy measurements on bunched fast atomic beams in a collinear geometry. In combination with multi-step resonant excitation to Rydberg states using pulsed lasers, the field ionization technique demonstrates increased sensitivity for isotope separation and measurement of atomic parameters over non-resonant laser ionization methods. The setup was tested at the Collinear Resonance Ionization Spectroscopy experiment at ISOLDE-CERN to perform high-resolution measurements of transitions in the indium atom from the 5s$^2$5d~$^2$D$_{5/2}$ and 5s$^2$5d~$^2$D$_{3/2}$ states to 5s$^2$($n$)p~$^2$P and 5s$^2$($n$)f~$^2$F Rydberg states, up to a principal quantum number of $n$ = 72. The extracted Rydberg level energies were used to re-evaluate the ionization potential of the indium atom to be 46670.1055(21) cm$^{-1}$. The nuclear magnetic dipole and nuclear electric quadrupole hyperfine structure constants and level isotope shifts of the 5s$^2$5d~$^2$D$_{5/2}$ and 5s$^2$5d~$^2$D$_{3/2}$ states were determined for $^{113,115}$In. The results are compared to calculations using relativistic coupled-cluster theory. A good agreement is found with the ionization potential and isotope shifts, while disagreement of hyperfine structure constants indicates an increased importance of electron correlations in these excited atomic states. With the aim of further increasing the detection sensitivity for measurements on exotic isotopes, a systematic study of the field-ionization arrangement implemented in the work was performed and an improved design was simulated and is presented. The improved design offers increased background suppression independent of the distance from field ionization to ion detection.

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

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

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.

Laser spectroscopic studies on minute samples of exotic radioactive nuclei require very efficient experimental techniques. In addition, high resolving powers are required to allow extraction of nu- clear structure information. Here we demonstrate that by using weak atomic transitions, resonance laser ionization spectroscopy is achieved with the required high efficiency (1-10%) and precision (linewidths of tens of MHz). We illustrate experimentally and through the use of simulations how the narrow experimental linewidths are achieved and how distorted resonance ionization spec- troscopy lineshapes can be avoided. The role of the delay of the ionization laser pulse with respect to the excitation laser pulse is crucial: the use of a delayed ionization step permits the best resolving powers and lineshapes. A high efficiency is maintained if the intermediate level has a lifetime that is at least of the order of the excitation laser pulse width. A model that describes this process re- produces well the observed features and will help to optimize the conditions for future experiments., Comment: 11 pages, 11 figures

Collinear laser spectroscopy has been performed on the $^{79}_{30}$Zn$_{49}$ isotope at ISOLDE-CERN. The existence of a long-lived isomer with a few hundred milliseconds half-life was confirmed, and the nuclear spins and moments of the ground and isomeric states in $^{79}$Zn as well as the isomer shift were measured. From the observed hyperfine structures, spins $I = 9/2$ and $I = 1/2$ are firmly assigned to the ground and isomeric states. The magnetic moment $\mu$ ($^{79}$Zn) = $-$1.1866(10) $\mu_{\rm{N}}$, confirms the spin-parity $9/2^{+}$ with a $\nu g_{9/2}^{-1}$ shell-model configuration, in excellent agreement with the prediction from large scale shell-model theories. The magnetic moment $\mu$ ($^{79m}$Zn) = $-$1.0180(12) $\mu_{\rm{N}}$ supports a positive parity for the isomer, with a wave function dominated by a 2h-1p neutron excitation across the $N = 50$ shell gap. The large isomer shift reveals an increase of the intruder isomer mean square charge radius with respect to that of the ground state: $\delta \langle r^{2}_{c}\rangle^{79,79m}$ = +0.204(6) fm$^{2}$, providing first evidence of shape coexistence., Comment: 5 pages, 4 figures, 1 table, Accepeted by Phys. Rev. Lett. (2016)

The magnetic dipole moments and changes in mean-square charge radii of the neutron-rich $^{218m,219,229,231}\text{Fr}$ isotopes were measured with the newly-installed Collinear Resonance Ionization Spectroscopy (CRIS) beam line at ISOLDE, CERN, probing the $7s~^{2}S_{1/2}$ to $8p~^{2}P_{3/2}$ atomic transition. The $\delta\langle r^{2}\rangle^{A,221}$ values for $^{218m,219}\text{Fr}$ and $^{229,231}\text{Fr}$ follow the observed increasing slope of the charge radii beyond $N~=~126$. The charge radii odd-even staggering in this neutron-rich region is discussed, showing that $^{220}\text{Fr}$ has a weakly inverted odd-even staggering while $^{228}\text{Fr}$ has normal staggering. This suggests that both isotopes reside at the borders of a region of inverted staggering, which has been associated with reflection-asymmetric shapes. The $g(^{219}\text{Fr}) = +0.69(1)$ value supports a $\pi 1h_{9/2}$ shell model configuration for the ground state. The $g(^{229,231}\text{Fr})$ values support the tentative $I^{\pi}(^{229,231}\text{Fr}) = (1/2^{+})$ spin, and point to a $\pi s_{1/2}^{-1}$ intruder ground state configuration., Comment: Accepted for publication with Physical Review C

This paper reports on the hyperfine-structure and radioactive-decay studies of the neutron-deficient francium isotopes $^{202-206}$Fr performed with the Collinear Resonance Ionization Spectroscopy (CRIS) experiment at the ISOLDE facility, CERN. The high resolution innate to collinear laser spectroscopy is combined with the high efficiency of ion detection to provide a highly-sensitive technique to probe the hyperfine structure of exotic isotopes. The technique of decay-assisted laser spectroscopy is presented, whereby the isomeric ion beam is deflected to a decay spectroscopy station for alpha-decay tagging of the hyperfine components. Here, we present the first hyperfine-structure measurements of the neutron-deficient francium isotopes $^{202-206}$Fr, in addition to the identification of the low-lying states of $^{202,204}$Fr performed at the CRIS experiment., Comment: Accepted for publication with Physical Review X

Measurements of the ground-state nuclear spins, magnetic and quadrupole moments of the copper isotopes from 61Cu up to 75Cu are reported. The experiments were performed at the ISOLDE facility, using the technique of collinear laser spectroscopy. The trend in the magnetic moments between the N=28 and N=50 shell closures is reasonably reproduced by large-scale shell-model calculations starting from a 56Ni core. The quadrupole moments reveal a strong polarization of the underlying Ni core when the neutron shell is opened, which is however strongly reduced at N=40 due to the parity change between the $pf$ and $g$ orbits. No enhanced core polarization is seen beyond N=40. Deviations between measured and calculated moments are attributed to the softness of the 56Ni core and weakening of the Z=28 and N=28 shell gaps., Comment: 13 pagers, 19 figures, accepted by Physical Review C

In-source resonant ionization laser spectroscopy of the even-$A$ polonium isotopes $^{192-210,216,218}$Po has been performed using the $6p^37s$ $^5S_2$ to $6p^37p$ $^5P_2$ ($\lambda=843.38$ nm) transition in the polonium atom (Po-I) at the CERN ISOLDE facility. The comparison of the measured isotope shifts in $^{200-210}$Po with a previous data set allows to test for the first time recent large-scale atomic calculations that are essential to extract the changes in the mean-square charge radius of the atomic nucleus. When going to lighter masses, a surprisingly large and early departure from sphericity is observed, which is only partly reproduced by Beyond Mean Field calculations., Comment: As submitted to PRL