Search

We report on the masses and hyperfine structure of ground and isomeric states in $^{114,116,118,120}$Ag isotopes, measured with the phase-imaging ion-cyclotron-resonance technique (PI-ICR) with the JYFLTRAP mass spectrometer and the collinear laser spectroscopy beamline at the Ion Guide Isotope Separator On-Line (IGISOL) facility, Jyv\"askyl\"a, Finland. We measured the masses and excitation energies, electromagnetic moments, and charge radii, and firmly established the nuclear spins of the long-lived states. A new isomer was discovered in $^{118}$Ag and the half-lives of $^{118}$Ag long-lived states were reevaluated. We unambiguously pinned down the level ordering of all long-lived states, placing the inversion of the $I = 0^-$ and $I = 4^+$ states at $A = 118$ $(N = 71)$. Lastly, we compared the electromagnetic moments of each state to empirical single-particle moments to identify the dominant configuration where possible., Comment: 11 pages paper (excl. references) + 3 pages of supplementary material

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 development of atomic many-body methods, capable of incorporating electron correlation effects accurately, is required for isotope shift (IS) studies. In combination with precise measurements, such calculations help to extract nuclear charge radii differences, and to probe for signatures of physics beyond the Standard Model of particle physics. We review here a few recently-developed methods in the relativistic many-body perturbation theory (RMBPT) and relativistic coupled-cluster (RCC) theory frameworks for calculations of IS factors in the highly charged ions (HCIs), and neutral or singly-charged ions, respectively. The results are presented for a wide range of atomic systems in order to demonstrate the interplay between quantum electrodynamics (QED) and electron correlation effects. In view of this, we start our discussions with the RMBPT calculations for a few HCIs by rigorously treating QED effects; then we outline methods to calculate IS factors in the one-valence atomic systems using two formulations of the RCC approach. Then we present calculations for two valence atomic systems, by employing the Fock-space RCC methods. For completeness, we briefly discuss theoretical input required for the upcoming experiments, their possibilities to probe nuclear properties and implications to fundamental physics studies., Comment: Topical Review Preprint for J. Phys. B, Comments and Suggestions are welcome!

The magnetic dipole and the spectroscopic quadrupole moments of the nuclear ground states in the odd-mass nickel isotopes $^{59-67}$Ni have been determined using collinear laser spectroscopy at the CERN-ISOLDE facility. They are compared to ab initio valence-space in-medium similarity renormalization group (VS-IMSRG) calculations including contributions of two-body currents as well as to shell-model calculations. The two-body-current contributions significantly improve the agreement with experimental data, reducing the mean-square deviation from the experimental moments by a factor of 3 to 5, depending on the employed interaction. For all interactions, the largest contributions are obtained for the $5/2^-$ ($7/2^-$) isotopes $^{65}$Ni ($^{55}$Ni), which is ascribed to the high angular momentum of the $f$ orbitals. Our results demonstrate that the inclusion of two-body-current contributions to the magnetic moment in an isotopic chain of complex nuclei can be handled by the VS-IMSRG and can outperform phenomenological shell-model calculations using effective $g$-factors in the nickel region., Comment: Published in Physics Letters B, 10 pages, 3 figures

Collinear laser spectroscopy measurements were performed on $^{68-74}$Ge isotopes ($Z = 32$) at ISOLDE-CERN, by probing the $4s^2 4p^2 \, ^3\!P_1 \rightarrow 4s^2 4p 5s \, ^3\!P_1^o$ atomic transition (269~nm) of germanium. Nuclear charge radii are determined via the measured isotope shifts, revealing a larger local variation than the neighboring isotopic chains. Nuclear density functional theory with the Fayans functionals Fy($\Delta r$,HFB) and Fy(IVP), and the SV-min Skyrme describes the experimental data for the differential charge radii $\delta\langle r^{2} \rangle$ and charge radii $R_{\rm c}$ within the theoretical uncertainties. The observed large variation in the charge radii of germanium isotopes is better accounted for by theoretical models incorporating ground state quadrupole correlations. This suggests that the polarization effects due to pairing and deformation contribute to the observed large odd-even staggering in the charge radii of the Ge isotopic chain., Comment: 6 pages,5 figures

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

We investigate the effects of two-body currents on magnetic dipole moments of medium-mass and heavy nuclei using the valence-space in-medium similarity renormalization group with chiral effective field theory interactions and currents. Focusing on near doubly magic nuclei from oxygen to bismuth, we have found that the leading two-body currents globally improve the agreement with experimental magnetic moments. Moreover, our results show the importance of multi-shell effects for $^{41}$Ca, which suggest that the $Z=N=20$ gap in $^{40}$Ca is not as robust as in $^{48}$Ca. The increasing contribution of two-body currents in heavier systems is explained by the operator structure of the center-of-mass dependent Sachs term., Comment: 6 pages, 4 figures, supplemental material included

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.

Nuclear moments of the antimony isotopes $^{113-133}$Sb are measured by collinear laser spectroscopy and used to benchmark phenomenological shell-model and \textit{ab initio} calculations in the valence-space in-medium similarity renormalization group (VS-IMSRG). The shell-model calculations reproduce the electromagnetic moments over all Sb isotopes when suitable effective $g$-factors and charges are employed. Good agreement is achieved by VS-IMSRG for magnetic moments on the neutron-deficient side for both odd-even and odd-odd Sb isotopes while its results deviate from experiment on the neutron-rich side. When the same effective $g$-factors are used, VS-IMSRG agrees with experiment nearly as well as the shell model. Hence, the wave functions are very similar in both approaches and missing contributions to the M1 operator are identified as the cause of the discrepancy of VS-IMSRG with experiment. Electric quadrupole moments remain more challenging for VS-IMSRG.

Collinear laser spectroscopy was performed on the isomer of the aluminium isotope $^{26m}$Al. The measured isotope shift to $^{27}$Al in the $3s^{2}3p\;^{2}\!P^\circ_{3/2} \rightarrow 3s^{2}4s\;^{2}\!S_{1/2}$ atomic transition enabled the first experimental determination of the nuclear charge radius of $^{26m}$Al, resulting in $R_c$=\qty{3.130\pm.015}{\femto\meter}. This differs by 4.5 standard deviations from the extrapolated value used to calculate the isospin-symmetry breaking corrections in the superallowed $\beta$ decay of $^{26m}$Al. Its corrected $\mathcal{F}t$ value, important for the estimation of $V_{ud}$ in the CKM matrix, is thus shifted by one standard deviation to \qty{3071.4\pm1.0}{\second}., Comment: 5 pages, 2 figures, submitted to Phys. Rev. Lett

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 the 14 lowest excited electronic states in the radioactive molecule radium monofluoride (RaF). The observed excitation energies are compared with fully relativistic state-of-the-art Fock-space coupled cluster (FS-RCC) 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 energy of excited states is studied, found to be important for all states. Establishing the simultaneous accuracy and precision of calculations is an important step for research at the intersection of particle, nuclear, and chemical physics, including searches of physics beyond the Standard Model, for which RaF is a promising probe., Comment: Significant changes compared to previous version with additional experimental data. Accepted for publication under a different title

This whitepaper presents the research priorities decided on by attendees of the 2022 Town Meeting for Fundamental Symmetries, Neutrons and Neutrinos, which took place December 13-15, 2022 in Chapel Hill, NC, as part of the Nuclear Science Advisory Committee (NSAC) 2023 Long Range Planning process. A total of 275 scientists registered for the meeting. The whitepaper makes a number of explicit recommendations and justifies them in detail.

Precise theoretical calculations of open-shell atomic systems are critical for extracting fundamental physics parameters from precision experiments. Here we present proof-of-principle calculations illustrating the effectiveness of the valence-space formulation of the ab initio in-medium similarity renormalization group, widely used in nuclear theory, as a new ab initio method for atomic systems. We adapt this approach to study properties of closed- and open-shell many-electron systems from helium to calcium. Ground-state energies, excitation spectra, and ionization energies are obtained for selected atoms, and reasonable agreement is found with benchmark coupled-cluster and many-body perturbation theory calculations, where available., Comment: 6 pages, 8 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)

Static electric dipole moments of nondegenerate systems probe mass scales for physics beyond the Standard Model well beyond those reached directly at high energy colliders. Discrimination between different physics models, however, requires complementary searches in atomic-molecular-and-optical, nuclear and particle physics. In this report, we discuss the current status and prospects in the near future for a compelling suite of such experiments, along with developments needed in the encompassing theoretical framework., Comment: Contribution to Snowmass 2021; updated with community edits and endorsements

A wide range of quantum sensing technologies are rapidly being integrated into the experimental portfolio of the high energy physics community. Here we focus on sensing with atomic interferometers; mechanical devices read out with optical or microwave fields; precision spectroscopic methods with atomic, nuclear, and molecular systems; and trapped atoms and ions. We give a variety of detection targets relevant to particle physics for which these systems are uniquely poised to contribute. This includes experiments at the precision frontier like measurements of the electron dipole moment and electromagnetic fine structure constant and searches for fifth forces and modifications of Newton's law of gravity at micron-to-millimeter scales. It also includes experiments relevant to the cosmic frontier, especially searches for gravitional waves and a wide variety of dark matter candidates spanning heavy, WIMP-scale, light, and ultra-light mass ranges. We emphasize here the need for more developments both in sensor technology and integration into the broader particle physics community., Comment: contribution to Snowmass 2021 18 pages, 3 figures; updated author list and references, fixed typos

The structure of nuclei around the neutron-rich nucleus 132Sn is of particular interest due to the vicinity of the Z = 50 and N = 82 shell closures and the r-process nucleosynthetic path. Four states in 131Sn with a strong single-particle-like component have previously been studied via the (d,p) reaction, with limited excitation energy resolution. The 130Sn(9Be,8Be)131Sn and 130Sn(13C,12C)131Sn single-neutron transfer reactions were performed in inverse kinematics at the Holifield Radioactive Ion Beam Facility using particle-gamma coincidence spectroscopy. The uncertainties in the energies of the single-particle-like states have been reduced by more than an order of magnitude using the energies of gamma rays. The previous tentative Jpi values have been confirmed. Decays from high-spin states in 131Sn have been observed following transfer on the isomeric component of the 130Sn beam. The improved energies and confirmed spin-parities of the p-wave states important to the r-process lead to direct-semidirect cross-sections for neutron capture on the ground state of 130Sn at 30 keV that are in agreement with previous analyses. A similar assessment of the impact of neutron-transfer on the isomer would require significant nuclear structure and reaction theory input. There are few measurements of transfer reaction on isomers, and this is the first on an isomer in the 132Sn region., Comment: 7 pages, 4 figures

Collinear laser spectroscopy is performed on the nickel isotopes $^{58-68,70}$Ni, using a time-resolved photon counting system. From the measured isotope shifts, nuclear charge radii $R_c$ are extracted and compared to theoretical results. Three ab initio approaches all employ, among others, the chiral interaction NNLO$_{\rm sat}$, which allows an assessment of their accuracy. We find agreement with experiment in differential radii $\delta \left\langle r_\mathrm{c}^2 \right\rangle$ for all employed ab initio methods and interactions, while the absolute radii are consistent with data only for NNLO$_{\rm sat}$. Within nuclear density functional theory, the Skyrme functional SV-min matches experiment more closely than the Fayans functional Fy($\Delta r$,HFB).

We use the nuclear density functional theory to determine nuclear electric quadrupole and magnetic dipole moments in all one-particle and one-hole neighbours of eight doubly magic nuclei. We align angular momenta along the intrinsic axial-symmetry axis with broken time-reversal symmetry, which allows us to explore fully the self-consistent charge, spin, and current polarisation. Spectroscopic moments are determined for symmetry-restored wave functions and compared with available experimental data. We find that the obtained polarisations do not call for using quadrupole- or dipole-moment operators with effective charges or effective g-factors., Comment: 16 LaTeX pages, 6 figures, extended version, accepted as a Letter in Journal of Physics G

The accuracy of atomic theory calculations limits the extraction of nuclear charge radii from isotope shift measurements of odd-proton nuclei. For Na isotopes, though precise spectroscopic measurements have existed since more than half a century, calculations by different methods offer a wide range of values. Here, we present accurate atomic calculations to reliably extract the Na charge radii. By combining experimental matter radii with nuclear coupled-cluster calculations based on nucleon-nucleon and three-nucleon forces, we constrain the parameters obtained from the atomic calculations. Therefore, this study guides atomic theory and highlights the importance of using accurate atomic and nuclear computations in our understanding of the size of light nuclei.

Molecules containing superheavy atoms can be artificially created to serve as sensitive probes for study of symmetry-violating phenomena. Here, we provide a detailed theoretical study for diatomic molecules containing the superheavy lawrencium nuclei. The sensitivity to time-reversal violating properties was studied for different neutral and ionic molecules. The effective electric fields in these systems were found to be about 3-4 times larger than other known molecules on which electron electric dipole moment experiments are being performed. Similarly, these superheavy molecules exhibit an enhancement of more than 5 times for parity- and time-reversal-violating scalar-pseudoscalar nucleus-electron interactions. We also briefly comment on some experimental aspects by discussing the production of these systems., Comment: 7 pages, 2 figures, 2 tables

The occupancies and vacancies of the valence neutron orbitals across the stable tin isotopic chain from $112\leq A\leq 124$ have been determined. These were inferred from the cross sections of neutron-adding and -removing reactions. In each case, the reactions were chosen to have good angular-momentum matching for transfer to the low- and high-$\ell$ orbitals present in this valence space. These new data are compared to older systematic studies. The effective single-neutron energies are determined by combining information from energy centroids determined from the adding and removing reactions. Two of the five orbitals are nearly degenerate, below $N=64$, and approximately two MeV more bound than the other three, which are also degenerate., Comment: 11 pages, 10 figures

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

Radium compounds have attracted recently considerable attention due to both development of experimental techniques for high-precision laser spectroscopy of molecules with short-lived nuclei and amenability of certain radium compounds for direct cooling with lasers. Currently, radium monofluoride (RaF) is one of the most studied molecules among the radium compounds, both theoretically and recently also experimentally. Complementary studies of further diatomic radium derivatives are highly desired to assess the influence of chemical substitution on diverse molecular parameters, especially on those connected with laser cooling, such as vibronic transition probabilities, and those related to violations of fundamental symmetries. In this article high-precision \emph{ab initio} studies of electronic and vibronic levels of diatomic radium monochloride (RaCl) are presented. Recently developed approaches for treating electronic correlation with Fock-space coupled cluster methods are applied for this purpose. Theoretical results are compared to an early experimental investigation by Lagerqvist and used to partially reassign the experimentally observed transitions and molecular electronic levels of RaCl. Effective constants of $\mathcal{P}$-odd hyperfine interaction $W_{\rm{a}}$ and $\mathcal{P,T}$-odd scalar-pseudoscalar nucleus-electron interaction $W_{\rm{s}}$ in the ground electronic state of RaCl are estimated within the framework of a quasirelativistic Zeroth-Order Regular Approximation approach and compared to parameters in RaF and RaOH., Comment: 18 pages, 2 figures, 5 tables

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

Collinear laser spectroscopy measurements were performed on $^{69,71,73}$Ge isotopes ($Z = 32$) at ISOLDE-CERN. The hyperfine structure of the $4s^2 4p^2 \, ^3P_1 \rightarrow 4s^2 4p 5s \, ^3P_1^o$ transition of the germanium atom was probed with laser light of 269 nm, produced by combining the frequency-mixing and frequency-doubling techniques. The hyperfine fields for both atomic levels were calculated using state-of-the-art atomic relativistic Fock-space coupled-cluster calculations. A new $^{73}$Ge quadrupole moment was determined from these calculations and previously measured precision hyperfine parameters, yielding $Q_{\rm s}$ = $-$0.198(4) b, in excellent agreement with the literature value from molecular calculations. The moments of $^{69}$Ge have been revised: $\mu$ = +0.920(5) $\mu_{N}$ and $Q_{\rm s}$= +0.114(8) b, and those of $^{71}$Ge have been confirmed. The experimental moments around $N = 40$ are interpreted with large-scale shell-model calculations using the JUN45 interaction, revealing rather mixed wave function configurations, although their $g$-factors are lying close to the effective single-particle values. Through a comparison with neighboring isotones, the structural change from the single-particle nature of nickel to deformation in germanium is further investigated around $N = 40$., Comment: accepted in Phys. Rev. C., in production

We discuss how molecule-based searches offer complementary probes to study the violation of fundamental symmetries. These experiments have the potential to probe not only the electron EDM, but also hadronic CPV phenomena. Future experimental developments will offer generic sensitivity to probe flavor neutral sources of both leptonic and hadronic CPV at scales of $\geq$ 100 TeV, and flavor changing CPV at scales of $\geq$ 1000 TeV.

Hyperfine spectra of $^\text{27-32}$Al ($Z=13$) have been measured at the ISOLDE-CERN facility via collinear laser spectroscopy using the $3s^23p\ ^2\text{P}^\text{o} _{3/2}\rightarrow 3s^24s\ ^2\text{S}_{1/2}$ atomic transition. For the first time, mean-square charge radii of radioactive aluminum isotopes have been determined alongside the previously unknown magnetic dipole moment of $^{29}$Al and electric quadrupole moments of $^{29,30}$Al. A potentially reduced charge radius at $N=19$ may suggest an effect of the $N=20$ shell closure, which is visible in the Al chain, contrary to other isotopic chains in the $sd$ shell. The experimental results are compared to theoretical calculations in the framework of the valence-space in-medium similarity renormalization group using multiple sets of two and three-nucleon forces from chiral effective field theory. While the trend of experimental magnetic dipole and electric quadrupole moments is well reproduced, the absolute values are underestimated by theory, consistent with earlier studies. Moreover, both the scale and trend of the charge radii appear to be very sensitive to the chosen interaction.

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.

We present the first laser spectroscopic measurement of the neutron-rich nucleus $^{68}$Ni at the \mbox{$N=40$} subshell closure and extract its nuclear charge radius. Since this is the only short-lived isotope for which the dipole polarizability $\alpha_{\rm D}$ has been measured, the combination of these observables provides a benchmark for nuclear structure theory. We compare them to novel coupled-cluster calculations based on different chiral two- and three-nucleon interactions, for which a strong correlation between the charge radius and dipole polarizability is observed, similar to the stable nucleus $^{48}$Ca. Three-particle--three-hole correlations in coupled-cluster theory substantially improve the description of the experimental data, which allows to constrain the neutron radius and neutron skin of $^{68}$Ni., Comment: 6 pages, 3 figures

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.

Strongly correlated many-body systems often display the emergence of simple patterns and regular behaviour of their global properties. Phenomena such as clusterization, collective motion and appearance of shell structures are commonly observed across different size, time, and energy scales in our universe. Although at the microscopic level their individual parts are described by complex interactions, the collective behaviour of these systems can exhibit strikingly regular patterns. This contribution provides an overview of the experimental signatures that are commonly used to identify the emergence of shell structures and collective phenomena in distinct physical systems. Examples in macroscopic systems are presented alongside features observed in atomic nuclei. The discussion is focused on the experimental trends observed for exotic nuclei in the vicinity of nuclear closed-shells, and the new challenges that recent experiments have posed in our understanding of emergent phenomena in nuclei., Comment: Invited contribution prepared for the special issue of "The tower of effective (field) theories and the emergence of nuclear phenomena

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

Measurements of atomic transitions in different isotopes offer key information on the nuclear charge radius. The anticipated high-precision experimental techniques, augmented by atomic calculations, will soon enable extraction of the higher-order radial moments of the charge density distribution. To assess the value of such measurements for nuclear structure research, we study the information content of the fourth radial moment $\rf$ by means of nuclear density functional theory and a multiple correlation analysis. We show that $\rf$ can be directly related to the surface thickness of nuclear density, a fundamental property of the atomic nucleus that is difficult to obtain for radioactive systems. Precise knowledge of these radial moments is essential to establish reliable constraints on the existence of new forces from precision isotope shift measurements ., Comment: 5 pages, 4 figures

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 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

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.

The hyperfine spectra of $^{51,53-64}$Mn were measured in two experimental runs using collinear laser spectroscopy at ISOLDE, CERN. Laser spectroscopy was performed on the atomic $3d^5\ 4s^2\ ^{6}\text{S}_{5/2}\rightarrow 3d^5\ 4s4p\ ^{6}\text{P}_{3/2}$ and ionic $3d^5\ 4s\ ^{5}\text{S}_2 \rightarrow 3d^5\ 4p\ ^{5}\text{P}_3$ transitions, yielding two sets of isotope shifts. The mass and field shift factors for both transitions have been calculated in the multiconfiguration Dirac-Fock framework and were combined with a King plot analysis in order to obtain a consistent set of mean-square charge radii which, together with earlier work on neutron-deficient Mn, allow the study of nuclear structure changes from $N=25$ across $N=28$ up to $N=39$. A clear development of deformation is observed towards $N=40$, confirming the conclusions of the nuclear moments studies. From a Monte Carlo Shell Model study of the shape in the Mn isotopic chain, it is suggested that the observed development of deformation is not only due to an increase in static prolate deformation but also due to shape fluctuations and triaxiality. The changes in mean-square charge radii are well reproduced using the Duflo-Zuker formula except in the case of large deformation., Comment: 9 figures, submitted to PRC

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)

Despite being a complex many-body system, the atomic nucleus exhibits simple structures for certain "magic" numbers of protons and neutrons. The calcium chain in particular is both unique and puzzling: evidence of doubly-magic features are known in 40,48Ca, and recently suggested in two radioactive isotopes, 52,54Ca. Although many properties of experimentally known Ca isotopes have been successfully described by nuclear theory, it is still a challenge to predict their charge radii evolution. Here we present the first measurements of the charge radii of 49,51,52Ca, obtained from laser spectroscopy experiments at ISOLDE, CERN. The experimental results are complemented by state-of-the-art theoretical calculations. The large and unexpected increase of the size of the neutron-rich calcium isotopes beyond N = 28 challenges the doubly-magic nature of 52Ca and opens new intriguing questions on the evolution of nuclear sizes away from stability, which are of importance for our understanding of neutron-rich atomic nuclei., Comment: Submitted version. See original publication (doi:10.1038/nphys3645) for final version

The odd-odd 54;56;58;60;62;64Mn isotopes (Z = 25) were studied using bunched-beam collinear laser spectroscopy at ISOLDE, CERN. From the measured hyperfine spectra the spins and magnetic moments of Mn isotopes up to N = 39 were extracted. The previous tentative ground state spin assignments of 58;60;62;64Mn are now firmly determined to be I = 1 along with an I = 4 assignment for the isomeric states in 58;60;62Mn. The I = 1 magnetic moments show a decreasing trend with increasing neutron number while the I = 4 moments remain quite constant between N = 33 and N = 37. The results are compared to large-scale shell-model calculations using the GXPF1A and LNPS effective interactions. The excellent agreement of the ground state moments with the predictions from the LNPS calculations illustrates the need for an increasing amount of proton excitations across Z = 28 and neutron excitations across N = 40 in the ground state wave functions from N = 37 onwards.

High-resolution bunched-beam collinear laser spectroscopy was used to measure the optical hyperfine spectra of the $^{43-51}$Ca isotopes. The ground state magnetic moments of $^{49,51}$Ca and quadrupole moments of $^{47,49,51}$Ca were measured for the first time, and the $^{51}$Ca ground state spin $I=3/2$ was determined in a model-independent way. Our results provide a critical test of modern nuclear theories based on shell-model calculations using phenomenological as well as microscopic interactions. The results for the neutron-rich isotopes are in excellent agreement with predictions using interactions derived from chiral effective field theory including three-nucleon forces, while lighter isotopes illustrate the presence of particle-hole excitations of the $^{40}$Ca core in their ground state., Comment: Accepted as a Rapid Communication in Physical Review C

\item[Background] Ground-state spins and magnetic moments are sensitive to the nuclear wave function, thus they are powerful probes to study the nuclear structure of isotopes far from stability. \item[Purpose] Extend our knowledge about the evolution of the $1/2^+$ and $3/2^+$ states for K isotopes beyond the $N = 28$ shell gap. \item[Method] High-resolution collinear laser spectroscopy on bunched atomic beams. \item[Results] From measured hyperfine structure spectra of K isotopes, nuclear spins and magnetic moments of the ground states were obtained for isotopes from $N = 19$ up to $N = 32$. In order to draw conclusions about the composition of the wave functions and the occupation of the levels, the experimental data were compared to shell-model calculations using SDPF-NR and SDPF-U effective interactions. In addition, a detailed discussion about the evolution of the gap between proton $1d_{3/2}$ and $2s_{1/2}$ in the shell model and {\it{ab initio}} framework is also presented. \item[Conclusions] The dominant component of the wave function for the odd-$A$ isotopes up to $^{45}$K is a $\pi 1d_{3/2}^{-1}$ hole. For $^{47,49}$K, the main component originates from a $\pi 2s_{1/2}^{-1}$ hole configuration and it inverts back to the $\pi 1d_{3/2}^{-1}$ in $^{51}$K. For all even-$A$ isotopes, the dominant configuration arises from a $\pi 1d_{3/2}^{-1}$ hole coupled to a neutron in the $\nu 1f_{7/2}$ or $\nu 2p_{3/2}$ orbitals. Only for $^{48}$K, a significant amount of mixing with $\pi 2s_{1/2}^{-1} \otimes \nu (pf)$ is observed leading to a $I^{\pi}=1^{-}$ ground state. For $^{50}$K, the ground-state spin-parity is $0^-$ with leading configuration $\pi 1d_{3/2}^{-1} \otimes \nu 2p_{3/2}^{-1}$., Comment: 12 pages, 10 figures, 7 tables

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

We report on the measurement of optical isotope shifts for $^{38,39,42,44,46\text{-}51}$K relative to $^{47}$K from which changes in the nuclear mean square charge radii across the N=28 shell closure are deduced. The investigation was carried out by bunched-beam collinear laser spectroscopy at the CERN-ISOLDE radioactive ion-beam facility. Mean square charge radii are now known from $^{37}$K to $^{51}$K, covering all $\nu f_{7/2}$-shell as well as all $\nu p_{3/2}$-shell nuclei. These measurements, in conjunction with those of Ca, Cr, Mn and Fe, provide a first insight into the $Z$ dependence of the evolution of nuclear size above the shell closure at N=28.