On-line implementation and first operation of the Laser Ion Source and Trap at ISOLDE/CERN

13 pags.; 12 figs.; 2 tab.; Open Access funded by CERN

Probing Sizes and Shapes of Nobelium Isotopes by Laser Spectroscopy

Until recently, ground-state nuclear moments of the heaviest nuclei could only be inferred from nuclear spectroscopy, where model assumptions are required. Laser spectroscopy in combination with modern atomic structure calculations is now able to probe these moments directly, in a comprehensive and nuclear-model-independent way. Here we report on unique access to the differential mean-square charge radii of ^{252,253,254}No, and therefore to changes in nuclear size and shape. State-of-the-art nuclear density functional calculations describe well the changes in nuclear charge radii in the region of the heavy actinides, indicating an appreciable central depression in the deformed proton densi…

Determination of a three-step excitation and ionization scheme for resonance ionization and ultratrace analysis of Np-237

Abstract The long-lived radio isotope 237 Np is generated within the nuclear fuel cycle and represents a major hazard in the final disposal of nuclear waste. Related geochemical research requires sensitive methods for the detection of ultratrace amounts of neptunium in environmental samples. Resonance ionization mass spectrometry (RIMS) has proven to be one of the most sensitive methods for the detection of plutonium. A precondition for the application of RIMS to ultratrace analysis of neptunium is the knowledge of an efficient and selective scheme for optical excitation and ionization. Therefore, a multitude of medium to high-lying atomic levels in neptunium was located by applying in-sour…

Measurement of the first ionization potential of astatine by laser ionization spectroscopy

The radioactive element astatine exists only in trace amounts in nature. Its properties can therefore only be explored by study of the minute quantities of artificially produced isotopes or by performing theoretical calculations. One of the most important properties influencing the chemical behaviour is the energy required to remove one electron from the valence shell, referred to as the ionization potential. Here we use laser spectroscopy to probe the optical spectrum of astatine near the ionization threshold. The observed series of Rydberg states enabled the first determination of the ionization potential of the astatine atom, 9.31751(8) eV. New ab initio calculations are performed to sup…

Triple-resonance autoionization of uranium optimized for diode laser excitation

Abstract The photoionization of uranium via three-step excitation has been optimized for isotope selective trace analysis. A search found 13 new J = 6, 7, and 8 odd-parity states in the 36,850–37,200 cm− 1 region that allow blue–red–red three-photon excitation at wavelengths favorable for commercial diode laser systems. From each of these 13 states, near-threshold autoionization spectra were recorded at a resolution of 3 × 10− 4 cm− 1. Some 30 even-parity autoionizing levels with J = 5 to 9 have also been observed and characterized. Comparison of the spectra allows J assignment for the new intermediate levels as well as selection of an optimized path for trace analysis. We show that, for a …

Opportunities and limitations of in-gas-cell laser spectroscopy of the heaviest elements with RADRIS

International audience; 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…

Detection of missing low-lying atomic states in actinium

Two lowest-energy odd-parity atomic levels of actinium, 7s^27p 2P^o_1/2, 7s^27p 2P^o_3/2, were observed via two-step resonant laser-ionization spectroscopy and their respective energies were measured to be 7477.36(4) cm^-1 and 12 276.59(2) cm^-1. The lifetimes of these states were determined as 668(11) ns and 255(7) ns, respectively. In addition, these properties were calculated using a hybrid approach that combines configuration interaction and coupled-cluster methods in good agreement. The data are of relevance for understanding the complex atomic spectra of actinides and for developing efficient laser-cooling and ionization schemes for actinium, with possible applications for high-purity…

A Progress Report on Laser Resonance Chromatography

Atoms 10(3), 87 (2022). doi:10.3390/atoms10030087

Hot-cavity studies for the Resonance Ionization Laser Ion Source

International audience; The Resonance Ionization Laser Ion Source (RILIS) has emerged as an important technique in many Radioactive Ion Beam (RIB) facilities for its reliability, and ability to ionize target elements efficiently and element selectively. GISELE is an off-line RILIS test bench to study the implementation of an on-line laser ion source at the GANIL separator facility. The aim of this project is to determine the best technical solution which combines high selectivity and ionization efficiency with small ion beam emittance and stable long term operation. The ion source geometry was tested in several configurations in order to find a solution with optimal ionization efficiency an…

Detection of the Lowest-Lying Odd-Parity Atomic Levels in Actinium

Two lowest-energy odd-parity atomic levels of actinium, 7s27pP21/2o, 7s27pP23/2o, were observed via two-step resonant laser-ionization spectroscopy and their respective energies were measured to be 7477.36(4) and 12 276.59(2) cm-1. The lifetimes of these states were determined as 668(11) and 255(7) ns, respectively. In addition, we observed the effect of the hyperfine structure on the line for the transition to P23/2o. These properties were calculated using a hybrid approach that combines configuration interaction and coupled-cluster methods, in good agreement with the experiment. The data are of relevance for understanding the complex atomic spectra of actinides and for developing efficien…

Performance of Dye and Ti:sapphire laser systems for laser ionization and spectroscopy studies at S3

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 (S3) at GANIL, France, of Dye and Ti:sapphire laser systems is investigated. In addition, a number of specific experimental cases on key isotopes of t…

Production of negative osmium ions by laser desorption and ionization.

The interest to produce negative osmium ions is manifold in the realm of high-accuracy ion trap experiments: high-resolution nearly Doppler-free laser spectroscopy, antihydrogen formation in its ground state, and contributions to neutrino mass spectrometry. Production of these ions is generally accomplished by sputtering an Os sample with Cs(+) ions at tens of keV. Though this is a well-established method commonly used at accelerators, these kind of sources are quite demanding and tricky to operate. Therefore, the development of a more straightforward and cost effective production scheme will be of benefit for ion trap and other experiments. Such a scheme makes use of desorption and ionizat…

Characterization of a pulsed injection-locked Ti:sapphire laser and its application to high resolution resonance ionization spectroscopy of copper

A high repetition rate pulsed Ti:sapphire laser injection-locked to a continuous wave seed source is presented. A spectral linewidth of 20 MHz at an average output power of 4W is demonstrated. An enhanced tuning range from 710-920 nm with a single broadband mirror set is realized by the inclusion of a single thin birefringent quartz plate for suppression of unseeded emission. The spectral properties have been analyzed using both a scanning Fabry-P´erot interferometer as well as crossed beam resonance ionization spectroscopy of the hyperfine levels of natural copper. Delayed ionization of the long-lived excited state is demonstrated for increased resolution. For the excited state hyperfine c…

Determination of the ground-state hyperfine structure in neutral229Th

The ground-state hyperfine structure of neutral 229Th has been measured for the first time using high-resolution resonance ionization spectroscopy. The measurements were performed as a preparatory work aimed at the identification of the predicted low-lying 7.6 eV isomer in 229Th through an investigation of its hyperfine structure. The hyperfine coupling constants have been extracted for the atomic ground state as well as for three excited states at 26 096, 26 113 and 38 278 cm−1. Due to rather small splittings not all hyperfine components were completely resolved and therefore an extensive χ2-error analysis was performed to achieve reliable results. The ground-state transition to the excite…

Towards high-resolution laser ionization spectroscopy of the heaviest elements in supersonic gas jet expansion

Resonant laser ionization and spectroscopy are widely used techniques at radioactive ion beam facilities to produce pure beams of exotic nuclei and measure the shape, size, spin and electromagnetic multipole moments of these nuclei. However, in such measurements it is difficult to combine a high efficiency with a high spectral resolution. Here we demonstrate the on-line application of atomic laser ionization spectroscopy in a supersonic gas jet, a technique suited for high-precision studies of the ground- and isomeric-state properties of nuclei located at the extremes of stability. The technique is characterized in a measurement on actinium isotopes around the N=126 neutron shell closure. A…

Advancing Radiation-Detected Resonance Ionization towards Heavier Elements and More Exotic Nuclides

Atoms 10(2), 41 (2022). doi:10.3390/atoms10020041

New Developments in the Production and Research of Actinide Elements

Atoms 10(2), 61 (2022). doi:10.3390/atoms10020061

Atom-at-a-time laser resonance ionization spectroscopy of nobelium

Resonance ionization spectroscopy of nobelium (atomic number 102) reveals its ground-state transition and an upper limit for its ionization potential, paving the way to characterizing even heavier elements via optical spectroscopy. Characterizing the heaviest elements in the periodic table is a gruelling task because they are radioactive, exist only for split seconds at a time and need to be artificially produced in sufficient quantities by complicated procedures. The heaviest element that has been characterized by optical spectroscopy is fermium, which has an atomic number of 100. Mustapha Laatiaoui et al. extend the methods used for fermium to perform optical spectroscopy on nobelium (ato…

Ultra Trace Determination Scheme for26Al by High-Resolution Resonance Ionization Mass Spectrometry using a Pulsed Ti:Sapphire Laser

We propose an ultra trace analysis approach for 26Al by high-resolution Resonance Ionization Mass Spectrometry (RIMS) using a pulsed narrow band-width Ti:Sapphire laser. For ensuring efficient ionization and high isotopic selectivity in RIMS of Al, we developed an injection seeded pulsed Ti:Sapphire laser with high repetition rate operation at up to 10 kHz. The laser produced an output power of 2 W and a spectral band-width of ~20 MHz with a repetition rate of 7 kHz. A first demonstration of its performance was done by detecting stable 27Al using RIMS.

Precision Measurement of the First Ionization Potential of Nobelium

One of the most important atomic properties governing an element's chemical behavior is the energy required to remove its least-bound electron, referred to as the first ionization potential. For the heaviest elements, this fundamental quantity is strongly influenced by relativistic effects which lead to unique chemical properties. Laser spectroscopy on an atom-at-a-time scale was developed and applied to probe the optical spectrum of neutral nobelium near the ionization threshold. The first ionization potential of nobelium is determined here with a very high precision from the convergence of measured Rydberg series to be 6.626 21±0.000 05  eV. This work provides a stringent benchmark for st…

Performance of a high repetition pulse rate laser system for in-gas-jet laser ionization studies with the Leuven laser ion source @ LISOL

The Leuven Isotope Separator On-Line (LISOL) facility at the Cyclotron Research Center (CRC) Louvain-la-Neuve; The laser ionization efficiency of the Leuven gas cell-based laser ion source was investigated under on- and off-line conditions using two distinctly different laser setups: a low-repetition rate dye laser system and a high-repetition rate Ti:sapphire laser system. A systematic study of the ion signal dependence on repetition rate and laser pulse energy was performed in off-line tests using stable cobalt and copper isotopes. These studies also included in-gas-jet laser spectroscopy measurements on the hyperfine structure of 63Cu. A final run under on-line conditions in which the ra…

Developments towards in-gas-jet laser spectroscopy studies of actinium isotopes at LISOL

To study exotic nuclides at the borders of stability with laser ionization and spectroscopy techniques, highest efficiencies in combination with a high spectral resolution are required. These usually opposing requirements are reconciled by applying the in-gas-laser ionization and spectroscopy (IGLIS) technique in the supersonic gas jet produced by a de Laval nozzle installed at the exit of the stopping gas cell. Carrying out laser ionization in the low-temperature and low density supersonic gas jet eliminates pressure broadening, which will significantly improve the spectral resolution. This article presents the required modifications at the Leuven Isotope Separator On-Line (LISOL) facility…

High-resolution laser spectroscopy of long-lived plutonium isotopes

Long-lived isotopes of plutonium were studied using two complementary techniques, high-resolution resonance ionisation spectroscopy (HR-RIS) and collinear laser spectroscopy (CLS). Isotope shifts have been measured on the $5f^67s^2\ ^7F_0 \rightarrow 5f^56d^27s\ (J=1)$ and $5f^67s^2\ ^7F_1 \rightarrow 5f^67s7p\ (J=2)$ atomic transitions using the HR-RIS method and the hyperfine factors have been extracted for the odd mass nuclei $^{239,241}$Pu. Collinear laser spectroscopy was performed on the $5f^67s\ ^8F_{1/2} \rightarrow J=1/2\; (27523.61\text{cm}^{-1})$ ionic transition with the hyperfine $A$ factors measured for $^{239}$Pu. Changes in mean-squared charge radii have been extracted and s…

In-gas-cell laser ionization studies of plutonium isotopes at IGISOL

Abstract In-gas-cell resonance laser ionization has been performed on long-lived isotopes of Pu at the IGISOL facility, Jyvaskyla. This initiates a new programme of research towards high-resolution optical spectroscopy of heavy actinide elements which can be produced in sufficient quantities at research reactors and transported to facilities elsewhere. In this work a new gas cell has been constructed for fast extraction of laser-ionized elements. Samples of 238–240,242 Pu and 244 Pu have been evaporated from Ta filaments, laser ionized, mass separated and delivered to the collinear laser spectroscopy station. Here we report on the performance of the gas cell through studies of the mass spec…

Ion production from solid state laser ion sources.

Laser ion sources based on resonant excitation and ionization of atoms are well-established tools for selective and efficient production of radioactive ion beams. Recent developments are focused on the use of the state-of-the-art all solid-state laser systems. To date, 35 elements of the periodic table are available from laser ion sources based on tunable Ti:sapphire lasers. Recent progress in this field regarding the establishment of suitable optical excitation schemes for Ti:sapphire lasers are reported.

High-resolution laser resonance ionization spectroscopy of $^{143-147}$Pm

The European physical journal / A 56(2), 69 (2020). doi:10.1140/epja/s10050-020-00061-8

High-resolution laser system for the S3-Low Energy Branch

International audience; 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 $5s^25p^2 (^3P_0) \rightarrow 5s^25p6s (^3P_1)$…

Study of the radiative decay of the low-energy isomer in ${}^{229}$Th

Recent progress in laser spectroscopy of the actinides

The interest to perform laser spectroscopy in the heaviest elements arises from the strong impact of relativistic effects, electron correlations and quantum electrodynamics on their atomic structure. Once this atomic structure is well understood, laser spectroscopy also provides access to nuclear properties such as spins, mean square charge radii and electromagnetic moments in a nuclear-model independent way. This is of particular interest for the heaviest actinides around $N = 152$, a region of shell stabilized deformed nuclei. The experimental progress of laser spectroscopy in this region benefitted from continuous methodological and technical developments such as the introduction of buff…

Resolution Characterizations of JetRIS in Mainz Using 164Dy

Atoms 10(2), 57 (2022). doi:10.3390/atoms10020057

Impact of buffer gas quenching on the $^1S_0$ $\to$ $^1P_1$ ground-state atomic transition in nobelium

International audience; Using the sensitive Radiation Detected Resonance Ionization Spectroscopy (RADRIS) techniquean optical transition in neutral nobelium (No, Z = 102) was identified. A remnant signal when delaying the ionizing laser indicated the influence of a strong buffer gas induced de-excitation of the optically populated level. A subsequent investigation of the chemical homologue, ytterbium (Yb, Z = 70), enabled a detailed study of the atomic levels involved in this process, leading to the development of a rate equation model. This paves the way for characterizing resonance ionization spectroscopy (RIS) schemes used in the studyof nobelium and beyond, where atomic properties are c…

Simulation studies of the laser ablation ion source at the SHIPTRAP setup

Hyperfine interactions 241(1), 46 (2020). doi:10.1007/s10751-020-01708-0

Resonance ionization spectroscopy of thorium isotopestowards a laser spectroscopic identification of the low-lying 7.6 eV isomer of 229Th

International audience; In-source resonance ionization spectroscopy was used to identify an efficient and selective three step excitation/ionization scheme of thorium, suitable for titanium:sapphire (Ti:sa) lasers. The measurements were carried out in preparation of laser spectroscopic investigations for an identification of the low-lying 229 m Th isomer predicted at 7.6 ± 0.5 eV above the nuclear ground state. Using a sample of 232 Th, a multitude of optical transitions leading to over 20 previously unknown intermediate states of even parity as well as numerous high-lying odd parity auto-ionizing states were identified. Level energies were determined with an accuracy of 0.06 cm −1 for inte…

Recent developments in resonance ionization mass spectrometry for ultra-trace analysis of actinide elements

Abstract Resonance ionization mass spectrometry is an efficient tool to detect minute amounts of long-lived radio-isotopes in environmental samples. Applying resonant excitation and ionization with pulsed laser radiation within a hot cavity atomizer enables the sensitive detection and precise quantification of long-lived actinide isotopes. Due to the inherently element selective ionization process, this method ensures ultimate suppression of contaminations from other elements and molecules. The characterization of in-source resonance ionization of the actinide elements U, Th, Np, and Am using a compact quadrupole mass spectrometer (QMS) setup are discussed.

Study of Low Work Function Materials for Hot Cavity Resonance Ionization Laser Ion Sources

The selectivity of a hot cavity resonance ionization laser ion source (RILIS) is most often limited by contributions from competing surface ionization on the hot walls of the ionization cavity. In this article we present investigations on the properties of designated high-temperature, low-work function materials regarding their performance and suitability as cavity material for RILIS. Tungsten test cavities, impregnated with a mixture of barium oxide and strontium oxide (BaOSrO on W), or alternatively gadolinium hexaboride (GdB6) were studied in comparison to a standard tungsten RILIS cavity as being routinely used for hot cavity laser ionization at ISOLDE. Measurement campaigns took place …