The quantum-mechanical nuclear-shell structure determines the stability and limits of the existence of the heaviest nuclides with large proton numbers Z ≳ 100 (refs. 1-3). Shell effects also affect the sizes and shapes of atomic nuclei, as shown by laser spectroscopy studies in lighter nuclides4. However, experimental information on the charge radii and the nuclear moments of the heavy actinide elements, which link the heaviest naturally abundant nuclides with artificially produced superheavy elements, is sparse5. Here we present laser spectroscopy measurements along the fermium (Z = 100) isotopic chain and an extension of data in the nobelium isotopic chain (Z = 102) across a key region. Multiple production schemes and different advanced techniques were applied to determine the isotope shifts in atomic transitions, from which changes in the nuclear mean-square charge radii were extracted. A range of nuclear models based on energy density functionals reproduce well the observed smooth evolution of the nuclear size. Both the remarkable consistency of model prediction and the similarity of predictions for different isotopes suggest a transition to a regime in which shell effects have a diminished effect on the size compared with lighter nuclei.

Here we report online results with the in-gas-Jet Resonance Ionization Spectroscopy (JetRIS) apparatus. The S01↔P11 transition of No254 was successfully measured with sub-GHz resolution, marking a fivefold improvement over previous measurements. Recent developments in laser spectroscopy have allowed access to more exotic nuclei, but measurements of the heavy actinide region have been limited by line broadening mechanisms, limiting the precision with which nuclear properties can be deduced from the hyperfine spectrum. JetRIS provides a method to measure the heavy actinide region with a high level of sensitivity and higher resolution than previous experiments. The offline and online characterizations of the system are reported, and future perspectives are presented. Published by the American Physical Society 2024

In this paper we present the first high-resolution laser spectroscopy results obtained at the GISELE laser laboratory of the GANIL-SPIRAL2 facility, in preparation for the first experiments with the S$^3$-Low Energy Branch. Studies of neutron-deficient radioactive isotopes of erbium and tin represent the first physics cases to be studied at S$^3$. The measured isotope-shift and hyperfine structure data are presented for stable isotopes of these elements. The erbium isotopes were studied using the $4f^{12}6s^2$ $^3H_6 \rightarrow 4f^{12}(^3 H)6s6p$ $J = 5$ atomic transition (415 nm) and the tin isotopes were studied by the $5s^25p^2 (^3P_0) \rightarrow 5s^25p6s (^3P_1)$ atomic transition (286.4 nm), and are used as a benchmark of the laser setup. Additionally, the tin isotopes were studied by the $5s^25p6s (^3P_1) \rightarrow 5s^25p6p (^3P_2)$ atomic transition (811.6 nm), for which new isotope-shift data was obtained and the corresponding field-shift $F_{812}$ and mass-shift $M_{812}$ factors are presented.

The radiation detection resonance ionization spectroscopy (RADRIS) technique enables laser spectroscopic investigations of the heaviest elements which are produced in atom-at-a-time quantities from fusion-evaporation reactions. To achieve a high efficiency, laser spectroscopy is performed in a buffer-gas environment used to thermalize and stop the high-energy evaporation residues behind the velocity filter SHIP. The required cyclic measurement procedure in combination with the applied filament collection for neutralization as well as confinement of the stopped ions and subsequent pulse-heat desorption constrains the applicability of the technique. Here, some of these limitations and also opportunities that arise from this unique measurement setup will be evaluated.

The Super Separator Spectrometer-Low Energy Branch (S3-LEB) is a low-energy radioactive ion beam experiment under commissioning as part of the GANIL-SPIRAL2 facility. It will be used for the production and study of exotic nuclei by in-gas laser ionization and spectroscopy (IGLIS), decay spectroscopy, and mass spectrometry. We report recent results from the off-line commissioning of S3-LEB, including first laser spectroscopy measurements in both the gas cell and the supersonic gas jet, the determination of the transport efficiency of laser ions from the gas cell through the RFQ chain, and time-of-flight measurements with the multi-reflection time-of-flight mass spectrometer PILGRIM. The measurements were performed using erbium, introduced by evaporation from a heated filament in the gas environment. The reported laser spectroscopy results include a characterization of the pressure broadening in the gas cell, proof-of-principle isotope shift measurements, and hyperfine-structure measurements.

The in-gas laser ionization and spectroscopy (IGLIS) technique has been a cornerstone in the study of heavy elements. The addition of a convergent–divergent (de Laval) nozzle to perform laser ionization in a cold hypersonic gas jet greatly improves the achievable resolution. Recent efforts have focused on preparing the in-gas-jet method for the study of the low-lying 229Th isomer. Tailor-made recoil sources of 233U are installed inside a fast extraction gas cell to provide the (isomeric) thorium ions. A level search above the second ionization potential (IP) uncovered several auto-ionizing states, greatly improving the laser ionization efficiency of singly charged thorium ions.

Laser resonance ionization spectroscopy of atomic thulium (Tm) has been performed at TRIUMF's off-line laser ion source test stand with a system of pulsed titanium sapphire (Ti:Sa) lasers. Automated continuous laser frequency scans across Rydberg states and autoionizing (AI) states were carried out using a pulsed, frequency doubled grating-tuned Ti:Sa laser. A combined analysis of the convergence limits resulting from odd-parity Rydberg series and AI Rydberg series improved the value for the ionization potential to 49,880.57(6)stat(4)sys cm−1, one order of magnitude more precise than the currently accepted value of 49,879.8(5) cm−1. An efficient resonance ionization scheme has been deduced from the photoionization spectra, and applied to online radioactive Tm isotope beam delivery at ISAC-TRIUMF. The ionization scheme will be useful for the extraction of Tm isotopes for nuclear medicine. The production yields of 153–165Tm were measured by evaluating the characteristic γ lines of the Tm isotopes at the ISAC yield station.

We present the first results obtained from the S3 Low-Energy Branch, the gas cell setup at SPIRAL2-GANIL, which will be installed behind the S3 spectrometer for atomic and nuclear spectroscopy studies of exotic nuclei. The installation is currently being commissioned offline, with the aim to establish optimum conditions for the operation of the radio frequency quadrupole ion guides, mass separation and ion bunching, providing high-efficiency and low-energy spatial spread for the isotopes of interest. Transmission and mass-resolving power measurements are presented for the different components of the S3-LEB setup. In addition, a single-longitudinal-mode, injection-locked, pumped pulsed-titanium–sapphire laser system has been recently implemented and is used for the first proof-of-principle measurements in an offline laser laboratory. Laser spectroscopy measurements of erbium, which is the commissioning case of the S3 spectrometer, are presented using the 4f126s23H6→4f12(3H)6s6p optical transition.

RAdiation-Detected Resonance Ionization Spectroscopy (RADRIS) is a versatile method for highly sensitive laser spectroscopy studies of the heaviest actinides. Most of these nuclides need to be produced at accelerator facilities in fusion-evaporation reactions and are studied immediately after their production and separation from the primary beam due to their short half-lives and low production rates of only a few atoms per second or less. Only recently, the first laser spectroscopic investigation of nobelium (Z=102) was performed by applying the RADRIS technique in a buffer-gas-filled stopping cell at the GSI in Darmstadt, Germany. To expand this technique to other nobelium isotopes and for the search for atomic levels in the heaviest actinide element, lawrencium (Z=103), the sensitivity of the RADRIS setup needed to be further improved. Therefore, a new movable double-detector setup was developed, which enhances the overall efficiency by approximately 65% compared to the previously used single-detector setup. Further development work was performed to enable the study of longer-lived (t1/2>1 h) and shorter-lived nuclides (t1/2<1 s) with the RADRIS method. With a new rotatable multi-detector design, the long-lived isotope 254Fm (t1/2=3.2 h) becomes within reach for laser spectroscopy. Upcoming experiments will also tackle the short-lived isotope 251No (t1/2=0.8 s) by applying a newly implemented short RADRIS measurement cycle.

The in-gas-jet laser spectroscopy method relies on the production of uniform and low-temperature gas jets to fully resolve the atomic hyperfine structure and efficiently determine fundamental nuclear properties of short-lived isotopes from, e.g., the hardly accessible actinide and transactinide elements. In this article we present the studies devoted to designing, producing, and characterizing the flow properties of a convergent-divergent (de Laval) hypersonic nozzle with a superior performance for laser spectroscopy applications. A novel flow mapping technique, based on resonance ionization spectroscopy (RIS), has been employed to characterize the local flow properties of an argon gas jet formed by this nozzle, revealing a 61.5-mm long, highly collimated atomic jet at a uniform low temperature of 16.6(5) K [Mach 8.11(12)] that will enable laser spectroscopy experiments on heavy-exotic nuclei with an unprecedented spectral resolution and a high efficiency. These results have been compared with those obtained by planar laser induced fluorescence spectroscopy (PLIFS) studies and show a good agreement between the two techniques and a significant improvement in efficiency of the RIS mapping method with respect to PLIFS. The data are compared to state-of-the-art fluid-dynamics calculations that were carried out to obtain the nozzle contour and simulate its performance, as well as to explain the observation of a possible onset of argon nucleation.

Using TRIUMF's off-line laser ion source test stand with a system of tunable titanium sapphire lasers, the polarization dependence of laser resonance ionization has been investigated using beryllium. A significant polarization dependence was observed for the excitation path S-1(0) -> P-1 degrees(1) -> S-1(0), which are typical transitions for alkaline-earth and alkaline-earth like elements. This polarization dependence was further verified on Be radioactive isotopes at TRIUMF's isotope separator and accelerator facility (ISAC). Laser polarization was proven to be an important parameter in operating resonance ionization laser ion sources (RILIS). The polarization spectroscopy was performed off-line both on the 2p(2) S-1(0) autoionizing (AI) state and high-n Rydberg states of the 2sns S-1(0) and 2snd D-1(2) series. The energy of the 2p(2) S-1(0) AI state and ionization potential (IP) of beryllium were extracted as 76,167(6) cm(-1) and 75,192.59(3) cm(-1). Polarization spectroscopy can be used to determine the J values of newly found states in in-source spectroscopy of the complex/radioactive alkaline-earth like elements such as Ra, Sm, Yb, Pu and No.

Hot cavity resonant ionization laser ion sources (RILIS) provide a multitude of radioactive ion beams with high ionization efficiency and element selective ionization. However, in hot cavity RILIS there still remains isobaric contamination in the extracted beam from surface ionized species. An ion guide-laser ion source (IG-LIS) has been implemented at TRIUMF’s isotope separator and accelerator (ISAC) facility that decouples the hot isotope production region from the laser ionization volume. A number of IG-LIS runs have been conducted to provide isobar free radioactive ion beams for experiments. Isobar suppression of up to 106 has been achieved, e.g. for Mg, Cd, Ga and other isotopes, IG-LIS however, still suffers from an intensity loss of 50-100× as compared to hot cavity RILIS. The work towards operating the IG-LIS in an optimized fashion and possible design improvements to the operational prototype for efficient and robust (radiation hard) on-line operation and recent SIMION ion optics simulation results as well as the ongoing development status of the IG-LIS are presented.

In the search of efficient laser resonance ionization schemes and optimal source parameters, offline laser ion source development is of importance for successful online radioactive beam delivery. An overview and update on recent TRIUMF's resonance ionization laser ion sources (TRILIS) offline developments is presented. This includes titanium-sapphire (Ti:Sa) laser development and the investigation of the laser ionization efficiency dependence on source temperature and laser polarization.

The novel and sensitive In-Gas Laser Ionization Spectroscopy (IGLIS) technique enables high-precision laser spectroscopy of the heaviest elements and isotopes very far from stability that are produced in fusion-evaporation reactions at in-flight separators. Powerful and dedicated laser systems are required in these facilities to realize in-gas jet laser spectroscopy with optimal spectral resolution and efficiency. The performance with respect to the requirements for IGLIS studies at the low energy front-end of the Super Separator Spectrometer (S-3) at GANIL, France, of Dye and Ti:sapphire laser systems is investigated. In addition, a number of specific experimental cases on key isotopes of the elements Ag, Sn, Ac, and No are discussed in detail.