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K. M. Lynch

Publications and source records attributed to K. M. Lynch.

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Energies and lifetimes of the 9p and 10p excited states in atomic francium

We present the first measurement of 9p 2P1/2,3/2 and 10p 2P1/2,3/2 excited levels absolute wavenumbers and radiative lifetime in francium. We used the Collinear Resonance Ionization Spectroscopy (CRIS) technique, applied on a beam of 221Fr atoms. Prior to this work, no experimental data existed for francium p-states with n > 8. The results provide a precision experimental test of relativistic coupled-cluster theory for the heaviest alkali, showing good agreement for lifetimes and relative excitation energies, despite a residual global offset in absolute energies.

physics.atom-ph

$^{61}$Cr as a Doorway to the N = 40 Island of Inversion

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 $μ(^{61}$Cr$)=+0.539(7)~μ_N$ 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.

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Laser spectroscopy and CP-violation sensitivity of actinium monofluoride

The apparent invariance of the strong nuclear force under combined charge conjugation and parity (CP) remains an open question in modern physics. Precision experiments with heavy atoms and molecules can provide stringent constraints on CP violation via searches for effects due to permanent electric dipole moments and other CP-odd properties in leptons, hadrons, and nuclei. Radioactive molecules have been proposed as highly sensitive probes for such searches, but experiments with most such molecules have so far been beyond technical reach. Here we report the first production and spectroscopic study of a gas-phase actinium molecule, $^{227}$AcF. We observe the predicted strongest electronic transition from the ground state, which is necessary for efficient readout in searches of symmetry-violating interactions. Furthermore, we perform electronic- and nuclear-structure calculations for $^{227}$AcF to determine its sensitivity to various CP-violating parameters, and find that a realistic, near-term experiment with a precision of 1 mHz would improve current constraints on the CP-violating parameter hyperspace by three orders of magnitude. Our results thus highlight the potential of $^{227}$AcF for exceptionally sensitive searches of CP violation.

physics.atom-ph

Reduction in nuclear size and quadrupole deformation of high-spin isomers of 127,129In

We employed laser spectroscopy of atomic transitions to measure the nuclear charge radii and electromagnetic properties of the high-spin isomeric states in neutron-rich indium isotopes (Z = 49) near the closed proton and neutron shells at Z = 50 and N = 82. Our data reveal a reduction in the nuclear charge radius and intrinsic quadrupole moment when protons and neutrons are fully aligned in 129In(N = 80), to form the high spin isomer. Such a reduction is not observed in 127In(N = 78), where more complex configurations can be formed by the existence of four neutron-holes. These observations are not consistently described by nuclear theory.

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Pinning down electron correlations in RaF via spectroscopy of excited states and high-accuracy relativistic quantum chemistry

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.

physics.atom-ph

Electromagnetic Properties of Indium Isotopes Elucidate the Doubly Magic Character of $^{100}$Sn

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.

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Radiative lifetime of the A 2Π1/2 state in RaF with relevance to laser cooling

The radiative lifetime of the $A$ $^2 Π_{1/2}$ (v=0) state in radium monofluoride (RaF) is measured to be 35(1) ns. The lifetime of this state and the related decay rate $Γ= 2.86(8) \times 10^7$ $s^{-1}$ are of relevance to the laser cooling of RaF via the optically closed $A$ $^2 Π_{1/2} \leftarrow X$ $^2Σ_{1/2}$ 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.

physics.atom-ph

Charge radii, moments and masses of mercury isotopes across the N = 126 shell closure

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.

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Laser spectroscopy of neutron-rich $^{207,208}$Hg isotopes: Illuminating the kink and odd-even staggering in charge radii across the $N=126$ shell closure

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.

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Measurement and microscopic description of odd-even staggering of charge radii of exotic copper isotopes

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.

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Analytic Response Relativistic Coupled-Cluster Theory: The first application to indium isotope shifts

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.

physics.atom-ph

Shape staggering of mid-shell mercury isotopes from in-source laser spectroscopy compared with Density Functional Theory and Monte Carlo Shell Model calculations

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 $πh_{9/2}$ and neutron $νi_{13/2}$ orbitals.

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Dipole and quadrupole moments of $^{73-78}$Cu as a test of the robustness of the $Z=28$ shell closure near $^{78}$Ni

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.

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Study of the long-lived excited state in the neutron deficient nuclides $^{195,197,199}$Po by precision mass measurement

Direct mass measurements of the low-spin $3/2^{(-)}$ and high-spin $13/2^{(+)}$ states in the neutron-deficient isotopes $^{195}$Po, $^{197}$Po, and high-spin $13/2^{(+)}$ state in $^{199}$Po were performed with the Penning-trap mass spectrometer ISOLTRAP at ISOLDE-CERN. These measurements allow the determination of the excitation energy of the isomeric state arising from the $ν$i$_{13/2}$ orbital in $^{195,197}$Po. Additionally, the excitation energy of isomeric states of lead, radon, and radium isotopes in this region were obtained from $α$-decay chains. The new excitation energies complete the knowledge of the energy systematics in the region and confirm for the first time that the $13/2^{(+)}$ states remain isomeric, independent of the number of valence neutrons.

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Laser spectroscopy of francium isotopes at the borders of the region of reflection asymmetry

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 $δ\langle r^{2}\rangle^{A,221}$ 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 $π1h_{9/2}$ shell model configuration for the ground state. The $g(^{229,231}\text{Fr})$ values support the tentative $I^π(^{229,231}\text{Fr}) = (1/2^{+})$ spin, and point to a $πs_{1/2}^{-1}$ intruder ground state configuration.

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Decay-assisted collinear resonance ionization spectroscopy: Application to neutron-deficient francium

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.

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