Determination of90Sr in environmental samples with resonance ionization spectroscopy in collinear geometry

A new, fast technique for trace analysis of the radioactive isotopes89Sr and90Sr in environmental samples has been developed. Conventional mass separation is combined with resonance ionization spectroscopy in collinear geometry, which provides high selectivity and sensitivity. In addition, a chemical separation procedure for sample preparation has been developed. The described technique was used to determine the90Sr content in ≈ 870 m3 air samples collected near Munich during and shortly after the Chernobyl reactor accident in April 1986. The content of90Sr was measured to be 1.4 mBq per m3, corresponding to 1.6 × 109 atoms of90Sr per sample. This value is in good agreement with the results…

A highly selective laser ion source for bunched, low emittance beam release

A novel type of resonance ionization laser ion source (RILIS) is under development, which combines the advantages of laser ionization with those of a source-implemented ion trap. This laser ion source trap (LIST) system, based on a gas-filled linear radio-frequency quadrupole ion trap, decouples the evaporation and ionization process by introduction of a primary surface ion repeller. Apart from significantly enhancing the selectivity in radioactive ion beam production, optimum control on the temporal pulse structure and the emittance of the generated laser ion bunch is obtained. A variety of operational modes from quasi-dc to microseconds-bunched ion beams with variable repetition rate can …

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

Atomic transitions and the first ionization potential of promethium determined by laser spectroscopy

The atomic spectrum of neutral promethium has been studied extensively by laser resonance ionization spectroscopy. We report on more than 1000 atomic transitions in the blue and near infrared spectral ranges, most of them between high excited energy levels. As Rydberg convergences could not be assigned unambiguously in the dense spectrum at high excitation energies, the first ionization potential (IP) was determined via field ionization of weakly bound states within a static electric field. By applying the saddle-point model, a value of IP ( Pm ) = 45 020.8 ( 3 ) cm − 1 [ 5.58188 ( 4 ) eV ] was derived, which confirms previous expectations of 45 027 ( 80 ) and 44 985 ( 140 ) cm − 1 , which …

Lineshapes and optical selectivity in high-resolution double-resonance ionization mass spectrometry

Abstract Lineshapes expected in high-resolution double-resonance ionization spectroscopy are calculated using the density matrix formalism, integrated over experimentally realistic conditions including atomic velocity and angular distributions as well as laser intensity profiles. The results of these calculations are compared with experimental measurements on the system 4s2 1S0 → 4s4p 1P1 → 4s4d 1D1 → ion for calcium. The measurements of lineshape, with a dynamic range of >106, reveal and confirm subtle effects predicted by theory. These include the shape, position and intensity of the laser-induced structure in the spectra and the simultaneous presence of coherent and incoherent excitation…

Laser spectroscopy of the 1001nm ground state transition in dysprosium

We present a direct excitation of the presumably ultranarrow $1001\ensuremath{-}\mathrm{nm}$ ground-state transition in atomic dysprosium. By using resonance ionization spectroscopy with pulsed Ti:sapphire lasers at a hot cavity laser ion source, we were able to measure the isotopic shifts in the $1001\ensuremath{-}\mathrm{nm}$ line between all seven stable isotopes. Furthermore, we determined the upper level energy from the atomic transition frequency of the $^{164}\mathrm{Dy}$ isotope as $9991.004(1)\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ and confirm the level energy listed in the NIST database. Since a sufficiently narrow natural linewidth is an essential prerequisit…

Relativistic J-dependence of the isotope shift in the 6s-6p doublet of Ba II

The collinear laser-ion beam technique has been used to measure the isotope shift and hyperfine structure in the 6s-6p doublet (4,934A, 4,554A) of Ba II for all seven stable isotopes. The influence of the excited2P1/2 and2P3/2 states on the field shift leads to a difference of 2.5(3)% in the electronicF factors. The specific mass shifts differ by {A′-A} 2.2(3) MHz which corresponds to about 12% of the normal mass shift.

Continuously tunable diamond Raman laser for resonance ionization experiments at CERN

We demonstrate a highly efficient, continuously tunable, diamond Raman laser operating in the blue region of the spectrum. The linewidth and tunability characteristics of a frequency-doubled Ti:Sapphire laser were transferred directly to the Stokes output, offering great potential for spectroscopic applications using an all-solid-state platform.

The Collinear Resonance Ionization Spectroscopy (CRIS) experimental setup at CERN-ISOLDE

The CRIS setup at CERN-ISOLDE is a laser spectroscopy experiment dedicated to the high-resolution study of the spin, hyperfine structure and isotope shift of radioactive nuclei with low production rates (a few per second). It combines the Doppler-free resolution of the in-flight collinear geometry with the high detection efficiency of resonant ionisation. A recent commissioning campaign has demonstrated a 1% experimental efficiency, and as low as a 0.001% non-resonant ionisation. The current status of the experiment and its recent achievements with beams of francium isotopes are reported. The first identified systematic effects are discussed. publisher: Elsevier articletitle: The Collinear …

Terbium Medical Radioisotope Production: Laser Resonance Ionization Scheme Development

Terbium (Tb) is a promising element for the theranostic approach in nuclear medicine. The new CERN-MEDICIS facility aims for production of its medical radioisotopes to support related R&D projects in biomedicine. The use of laser resonance ionization is essential to provide radioisotopic yields of highest quantity and quality, specifically regarding purity. This paper presents the results of preparation and characterization of a suitable two-step laser resonance ionization process for Tb. By resonance excitation via an auto-ionizing level, the high ionization efficiency of 53% was achieved. To simulate realistic production conditions for Tb radioisotopes, the influence of a surplus of Gd at…

Laser resonance ionization for efficient and selective ionization of rare species

Abstract Due to the steady development and refinement of powerful pulsed as well as continuous-wave lasers, resonance ionization has developed into an extremely versatile tool for numerous applications. Apart from suppressing isobaric interferences and contributing to isotopic selectivity already in the ionization process, resonant optical excitation and ionization with laser light ensures high overall efficiency and good temporal and spatial controls of the ions delivered to mass spectrometric applications. In the field of rare isotope research laser resonance ionization has nowadays become one of the key techniques, including similarly the determination of long-lived or stable ultra-trace…

First demonstration of Doppler-free 2-photon in-source laser spectroscopy at the ISOLDE-RILIS

Abstract Collinear Doppler-free 2-photon resonance ionization has been applied inside a hot cavity laser ion source environment at CERN-ISOLDE. An injection-seeded Ti:sapphire ring laser was used to generate light pulses with a Fourier-limited linewidth for high-resolution spectroscopy. Using a molybdenum foil as a reflective surface positioned at the end of the target transfer line, rubidium was successfully ionized inside the hot cavity. The results are presented alongside previously obtained data from measurements performed at the RISIKO mass separator at Mainz University, where collinear and perpendicular ionization geometries were tested inside an RFQ ion guide. This work is a pre-curs…

Evaluation of the magnetic moments of radium isotopes

Using the relativistic linked cluster many-body perturbation procedure we have obtained the hyperfine field at the nucleus of the Ra+ ion in the2S1/2 ground state. There is good agreement between the calculated magnetic moment of213Ra and the results of a recent Zeeman measurement by the collinear laser beam technique. Detailed comparison is carried out between our result and earlier ones.

Laser ion beam production at CERN-ISOLDE: New features – More possibilities

Abstract This article summarizes the current specifications and the latest features of the CERN-ISOLDE resonance ionization laser ion source (RILIS). This includes a description of the optical layout and the newly designed reference system. The ionization schemes for the laser ionized beams at ISOLDE are tabulated, including six new elements. All RILIS schemes are also made publicly available in the RILIS elements on-line database. Finally, we announce a paradigm shift in RILIS operation – the combination of a machine protection and a monitoring and control system has enabled on-call operation of the laser ion source for selected beams in 2014 and has become the standard mode of operation i…

Ultratrace analysis and isotope ratio measurements of long-lived radioisotopes by resonance ionization mass spectrometry (RIMS).

Resonance Ionization Mass Spectrometry (RIMS) is a sensitive and selective method for ultratrace analysis of long-lived radioisotopes and isotope ratio measurements. It provides extremely high isobaric suppression and good overall efficiency. The experimental limits of detection are as low as 10(6) atoms per sample and isotopic selectivities of 5x10(12) have been obtained. The widespread potential of RIMS, using different experimental arrangements, is demonstrated for the determination of the radiotoxic isotopes Pu-238 to Pu-244 and Sr-89/Sr-90 in various environmental samples as well as for Ca-41 in nuclear reactor components and biomedical samples.

Resonance ionization mass spectrometry for ultratrace analysis of plutonium with a new solid state laser system

Abstract Resonance ionization mass spectrometry (RIMS) is well-suited for isotope selective ultratrace analysis of long-lived radioactive isotopes due to its high element and isotope selectivity and good sensitivity. For the analysis of plutonium with a pulsed RIMS apparatus, a powerful, reliable and easy to handle Nd:YAG pumped titanium–sapphire laser system has been developed and combined with a time-of-flight mass spectrometer. Spectroscopic measurements led to an efficient three step excitation and ionization scheme for plutonium with λ1 = 420.76 nm, λ2 = 847.28 nm, and λ3 = 767.53 nm. The isotope shifts in this scheme for the plutonium isotopes 238 Pu through 244 Pu have been determine…

Laser and decay spectroscopy of the short-lived isotope Fr214 in the vicinity of the N=126 shell closure

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

Isotopes with an odd number of neutrons are usually slightly smaller in size than their even-neutron neighbours. In charge radii of short-lived copper isotopes, a reduction of this effect is observed when the neutron number approaches fifty. 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 …

Nuclear moments of strongly deformed strontium isotopes

Nuclear spins, moments and mean square charge radii of78–100Sr have been obtained by fast ion-beam collinear laserspectroscopy. The experiments performed at ISOLDE have been extended to include99Sr, measured by a non-optical detection scheme with a two-step optical pumping sequence. The results for the strongly deformed isotopes are discussed in the frame of the particle-plus-deformed core model.

Laser Spectroscopy of Neutron-Rich Hg207,208 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 d…

Quadrupole moments of radium isotopes from the 7p 2 P 3/2 hyperfine structure in Ra II

The hyperfine structure and isotope shift of221–226Ra and212,214Ra have been measured in the ionic (Ra II) transition 7s 2 S 1/2–7p 2 P 3/2 (λ=381.4 nm). The method of on-line collinear fast-beam laser spectroscopy has been applied using frequency-doubling of cw dye laser radiation in an external ring cavity. The magnetic hyperfine fields are compared with semi-empirical and ab initio calculations. The analysis of the quadrupole splitting by the same method yields the following, improved values of spectroscopic quadrupole moments:Q s (221Ra)=1.978(7)b,Q s (223Ra)=1.254(3)b and the reanalyzed valuesQ s (209Ra)=0.40(2)b,Q s (211Ra)=0.48(2)b,Q s (227Ra)=1.58(3)b,Q s (229Ra)=3.09(4)b with an ad…

Precision measurements of the charge radii of potassium isotopes

International audience; Precision nuclear charge radii measurements in the light-mass region are essential for understanding the evolution of nuclear structure, but their measurement represents a great challenge for experimental techniques. At the Collinear Resonance Ionization Spectroscopy (CRIS) setup at ISOLDE-CERN, a laser frequency calibration and monitoring system was installed and commissioned through the hyperfine spectra measurement of $^{38–47}$K. It allowed for the extraction of the hyperfine parameters and isotope shifts with better than 1 MHz precision. These results are in excellent agreement with available literature values and they demonstrate the suitability of the CRIS tec…

Quadrupole moment of Fr 203

The spectroscopic electric quadrupole moment of the neutron-deficient francium isotope 203Fr was measured by using high-resolution collinear resonance ionization spectroscopy (CRIS) at the CERN Isotope Separation On-Line Device (ISOLDE)facility. A remeasurement of the 207Fr quadrupole momentwas also performed, resulting in a departure from the established literature value. A sudden increase in magnitude of the 203Fr quadrupole moment, with respect to the general trend in the region, points to an onset of static deformation at N =116 in the 87Fr isotopic chain. Calculation of the static and total deformation parameters show that the increase in static deformation only cannot account for the o…

Tagungsnachlese Berlin: Atome, Moleküle, Quantenoptik und Plasmen (AMOP), Chemische und Polymerphysik

Trace detection of radiotoxic isotopes by resonance ionization mass spectrometry

Resonance ionization spectroscopy combined with mass spectrometry (RIMS) has become an important technique for ultratrace environmental analysis, and is particularly well suited for the detection of long-lived radio-toxic isotopes. A variety of experimental approaches have been developed to address the specific requirements posed by individual isotopes, which have widely differing physical, chemical, and environmental properties. In this paper we discuss the principles and recent progress in the development of three different methods that are being used for the analysis of radiotoxic species. These include measurement of actinides using triple-resonance ionization and time-of-flight mass sp…

Intrinsic quantum chaos and spectral fluctuations within the protactinium atom

Narrow linewidth operation of the RILIS titanium: Sapphire laser at ISOLDE/CERN

Abstract A narrow linewidth operating mode for the Ti:sapphire laser of the CERN ISOLDE Resonance Ionization Laser Ion Source (RILIS) has been developed. This satisfies the laser requirements for the programme of in-source resonance ionization spectroscopy measurements and improves the selectivity for isomer separation using RILIS. A linewidth reduction from typically 10 GHz down to 1 GHz was achieved by the intra-cavity insertion of a second (thick) Fabry-Perot etalon. Reliable operation during a laser scan was achieved through motorized control of the tilt angle of each etalon. A scanning, stabilization and mode cleaning procedure was developed and implemented in LabVIEW. The narrow linew…

Nuclear orientation of radon isotopes by spin exchange optical pumping

This paper reports the first demonstration of nuclear orientation of radon atoms. The method employed was spin exchange with potassium atoms polarized by optical pumping. The radon isotopes were produced at the ISOLDE isotope separator of CERN. The nuclear alignment of /sup 209/Rn and /sup 223/Rn has been measured by observation of ..gamma..-ray anisotropies and the magnetic dipole moment for /sup 209/Rn has been measured by the nuclear-magnetic-resonance method to be chemically bond..mu..chemically bond = 0.838 81(39)..mu../sub N/.

High efficiency resonance ionization of palladium with Ti:sapphire lasers

This work presents the development and testing of highly efficient excitation schemes for resonance ionization of palladium. To achieve the highest ionization efficiencies, a high-power, high repetition rate Ti:sapphire laser system was used and 2-step, 3-step and 4-step schemes were investigated and compared. Starting from different excited steps, the frequencies of the final ionization steps were tuned across the full accessible spectral range of the laser system, revealing several autoionizing Rydberg series, which converge towards the energetically higher lying state of the Pd+ ion ground state configuration. Through proper choice of these excitation steps, we developed a highly efficie…

High-resolution triple-resonance autoionization of uranium isotopes

Abstract The near-threshold autoionization (AI) spectrum of uranium has been investigated by triple-resonance excitation with single-mode continuous lasers. Spectra were recorded over the first ∼30 cm − 1 above the first ionization limit at a resolution of 3 × 10 − 4 cm − 1 using intermediate states with different J values (6, 7, 8) to assign AI level total angular momentum J AI  = 5 to 9. Resonances with widths ranging from 8 MHz to 30 GHz were observed; the strongest ones have J AI  = 9 and widths of ∼60 MHz. Hyperfine structures for 235 U and isotope shifts for 234, 235 U have been measured in the two intermediate levels and in the final AI level for the most favorable excitation path. T…

Production, isolation and characterization of radiochemically pure 163Ho samples for the ECHo-project

Abstract Several experiments on the study of the electron neutrino mass are based on high-statistics measurements of the energy spectrum following electron capture of the radionuclide 163Ho. They rely on the availability of large, radiochemically pure samples of 163Ho. Here, we describe the production, separation, characterization, and sample production within the Electron Capture in Holmium-163 (ECHo) project. 163Ho has been produced by thermal neutron activation of enriched, prepurified 162Er targets in the high flux reactor of the Institut Laue-Langevin, Grenoble, France, in irradiations lasting up to 54 days. Irradiated targets were chemically processed by means of extraction chromatogr…

Resonance ionization mass spectrometry for trace analysis of long-lived radionuclides

Resonance ionization mass spectrometry (RIMS) is a sensitive and selective method for the determination of extremely low abundances of long-lived radionuclides. The detection limits are about 106 atoms per sample and an isotopic selectivity up to 1013 has been achieved. The potential of RIMS using different experimental arrangements is outlined for the determination of isotope ratios and lowest abundances of long-lived radioisotopes of interest like 238–244Pu, 90Sr, and 41Ca. Recent developments in improving detection limits and the spatial resolution of this technique are briefly discussed.

Continuously tunable diamond Raman laser for resonance laser ionization.

We demonstrate a highly efficient, tunable, ∼5 GHz line- width diamond Raman laser operating at 479 nm. The diamond laser was pumped by a wavelength-tunable intra- cavity frequency-doubled titanium sapphire (Ti:Sapphire) laser operating at around 450 nm, at a repetition rate of 10 kHz with a pulse duration of 50 ns. The Raman reso- nator produced a continuously tunable output with high stability, high conversion efficiency (28%), and beam quality (M$^{2}$ <1.2). We also demonstrate that the linewidth and tunability of the pump laser is directly transferred to the Stokes output. Our results show that diamond Raman lasers offer great potential for spectroscopic applications, such as resonance…

Excited atomic energy levels in protactinium by resonance ionization spectroscopy

We present high-resolution data of the single-excitation spectrum of protactinium, reaching slightly beyond the first-ionization threshold. Within this work, more than 1500 energy levels are recorded in different excitation energy ranges below $50\phantom{\rule{0.16em}{0ex}}000\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Our experimental results show that the tabulated data in the literature severely underestimate the density of states particularly regarding the highly excited spectral range.

Development of a laser ion source at IGISOL

FURIOS, the Fast Universal laser IOn Source, is under development at the IGISOL (Ion Guide Isotope Separator On-Line) mass separator facility in Jyvaskyla, Finland. This new laser ion source will combine a state-of-the-art solid state laser system together with a dye laser system, for the selective and efficient production of exotic radioactive species without compromising the universality and fast release inherent in the IGISOL system. The motivation for, and development of, this ion source is discussed in relation to the programme of research ongoing at this mass separator facility.

Spin, moments, and mean square nuclear charge radius ofSr77

The neutron deficient $^{77}\mathrm{Sr}$ nucleus was studied by fast ion beam collinear laser spectroscopy with a detection scheme based on optical pumping, state selective neutralization, and atom counting. From the measured hyperfine splitting and isotope shift of the Sr II transition 5s $^{2}$${\mathit{S}}_{1/2}$\ensuremath{\rightarrow}5p $^{2}$${\mathit{P}}_{3/2}$ the nuclear spin I=5/2, the nuclear moments \ensuremath{\mu}=-0.348(4)${\mathrm{\ensuremath{\mu}}}_{\mathit{N}}$, ${\mathit{Q}}_{\mathit{s}}$=1.40(11) b, and the change in mean square charge radius \ensuremath{\delta}〈${\mathit{r}}^{2}$${\mathrm{〉}}^{88,77}$=0.248(12) ${\mathrm{fm}}^{2}$ were deduced. These ground-state proper…

A complementary laser system for ISOLDE RILIS

The Resonance Ionization Laser Ion Source (RILIS) is a powerful tool for efficient and selective production of radioactive ion beams at Isotope Separator On Line (ISOL) facilities. To avoid isobaric background, highly selective stepwise resonant ionization is applied, using up to three different laser wavelengths. Due to their advantages in terms of stability and reliability, an all solid-state titanium:sapphire (Ti:Sa) system is used or is planned to be installed at the majority of on-line facilities worldwide. Such an all solid-state Ti:Sa laser system is going to be installed at the ISOLDE RILIS at CERN alongside the well-established dye laser system.

Atomic spectroscopy studies of short-lived isotopes and nuclear isomer separation with the ISOLDE RILIS

The Resonance Ionization Laser Ion Source (RILIS) at the ISOLDE on-line isotope separator is based on the selective excitation of atomic transitions by tunable laser radiation. Ion beams of isotopes of 20 elements have been produced using the RILIS setup. Together with the mass separator and a particle detection system it represents a tool for high-sensitive laser spectroscopy of short-lived isotopes. By applying narrow-bandwidth lasers for the RILIS one can study isotope shifts (IS) and hyperfine structure (HFS) of atomic optical transitions. Such measurements are capable of providing data on nuclear charge radii, spins and magnetic moments of exotic nuclides far from stability. Although t…

New developments of the in-source spectroscopy method at RILIS/ISOLDE

At the CERN ISOLDE facility, long isotope chains of many elements are produced by proton-induced reactions in target materials such as uranium carbide. The Resonance Ionization Laser Ion Source (RILIS) is an efficient and selective means of ionizing the reaction products to produce an ion beam of a chosen isotope. Coupling the RILIS with modern ion detection techniques enables highly sensitive studies of nuclear properties (spins, electromagnetic moments and charge radii) along an isotope chain, provided that the isotope shifts and hyperfine structure splitting of the atomic transitions can be resolved. At ISOLDE the campaign to measure the systematics of isotopes in the lead region (Pb, Bi…

A dedicated decay-spectroscopy station for the collinear resonance ionization experiment at ISOLDE

A newdecay-spectroscopystation(DSS)has been developed to be coupled to the collinear resonance ionization spectroscopy (CRIS) beam line at CERN-ISOLDE. The system uses a rotatable wheel with ten 20 mg=cm2 carbon foils as beam implantation sites for the efficient measurement of charged decay products. Silicon detectors are placed on either side of the carbon foil in an optimal geometry to cover a large solid angle for detecting these charged particles. In addition to the silicon detectors at the on-beam axis position, a second pair of off-beam axis detectors are placed at the wheel position 108 deg. away, allowing longer-lived species to be studied. Up to three high purity germanium detector…

CRIS: A new method in isomeric beam production

The Collinear Resonance Ionization Spectroscopy (CRIS) experiment at ISOLDE, CERN, uses laser radiation to stepwise excite and ionize an atomic beam for the purpose of ultra-sensitive detection of rare isotopes, and hyperfine-structure measurements. The technique also offers the ability to purify an ion beam that is heavily contaminated with radioactive isobars, including the ground state of an isotope from its isomer, allowing decay spectroscopy on nuclear isomeric states to be performed. The isomeric ion beam is selected by resonantly exciting one of its hyperfine structure levels, and subsequently ionizing it. This selectively ionized beam is deflected to a decay spectroscopy station (DS…

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…

Total angular momenta of even-parity autoionizing levels and odd-parity high-lying levels of atomic uranium

Using three-step resonance ionization spectroscopy, over 200 even-parity autoionizing (AI) levels of atomic uranium, including Rydberg series converging to the second lowest ionic level (6L 11/2o), were observed in the 49 930–51 200 cm−1 energy range. Total angular momenta (J values) of these levels were determined by a polarization combination method as well as a method based on the J-momentum selection rule. Using the AI levels of which J values were determined unambiguously, unique J values were also assigned for about 70 high-lying odd-parity levels. The observed J-dependence on autoionization linewidth is interpreted as being due to a centrifugal potential barrier.

Isotope shift of182Hg and an update of nuclear moments and charge radii in the isotope range181Hg-206Hg

The technique of collinear fast-beam laser spectroscopy has been used to measure the isotope shifts of the even-even isotopes of Hg (Z=80) in the mass range 182≤A≤198 at the on-line mass separator ISOLDE at CERN. The atomic transition studied (6s 6p 3 P 2- 6s7s 3 S 1,λ=546.1 nm) starts from a metastable state, which is populated in a quasi resonant charge transfer process. The resulting changes in nuclear mean square charge radii show clearly that182Hg follows the trend of the heavier, even, weakly oblate isotopes. Correspondingly the huge odd-even shape staggering in the light Hg isotopes continues and the nuclear shape staggering and shape coexistence persists down to the last isotope inv…

A novel scheme for a highly selective laser ion source

A new type of resonance ionization laser ion source, which shall combine the advantages of a laser ion source with those of an ion trap, is proposed. The primary purpose of such a laser ion source trap, which is based on a gas-filled linear radio-frequency quadrupole ion trap system, is the decoupling of evaporation and ionization processes. Furthermore optimum temporal control on the generated ion bunch is obtained. Both effects will lead to a significantly increased isobaric selectivity and ion beams of low emittance. A large variety of operational modes, ranging from quasi-dc to microseconds-bunched radioactive ion beams with variable pulse width and repetition rate, can be chosen freely…

Upgrades of the GANDALPH photodetachment detector towards the determination of the electron affinity of astatine

The Gothenburg ANion Detector for Affinity measurements by Laser PHotodetachment (GANDALPH) has recently been built for measurements of electron affinities (EA) of radioisotopes. A first measurement campaign is aimed towards the determination of the EA of astatine, the rarest naturally occurring element on earth. In this work we present several upgrades of GANDALPH which have been implemented in order to facilitate EA measurements of radioisotopes where only low intensity ion beams (< 1pA) can be produced.

Resonant laser–SNMS for spatially resolved and element selective ultra-trace analysis of radionuclides

The newly developed resonant laser–SNMS system at the IRS Hannover combines the high spatial and decent mass resolution of a TOF-SIMS instrument with the element-selective process of resonant laser ionization. This setup was characterized by use of synthetic uranium, plutonium and technetium samples to prepare and demonstrate the performance for measurements on environmental samples. The laser–SNMS system will be applied for the detection, visualization and ultra-trace analysis of radionuclide containing nanoparticles in environmental samples with strongly reduced or even completely omitted chemical preparation. The necessary suppression of isobaric contamination was demonstrated as well as…

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…

Hyperfine structure study of Tc97,98,99 in a new laser ion source for high-resolution laser spectroscopy

Using a novel concept for efficient laser spectroscopy, we investigated the hyperfine splittings of three different atomic transitions in the long-lived isotopes $^{97\ensuremath{-}99}\mathrm{Tc}$. Despite the refractory character of the element technetium, sample sizes as low as ${10}^{11}$ atoms were sufficient to achieve excellent signal-to-noise ratios at a spectroscopic linewidth of less than 100 MHz. The obtained spectra were analyzed in detail, which results in a very good consistency for the extracted hyperfine parameters from the different transitions. The presented measurements provide the first hyperfine structure data for the isotopes $^{97,98}\mathrm{Tc}$ from which, in combina…

The electron affinity of astatine

One of the most important properties influencing the chemical behavior of an element is the electron affinity (EA). Among the remaining elements with unknown EA is astatine, where one of its isotopes, 211At, is remarkably well suited for targeted radionuclide therapy of cancer. With the At− anion being involved in many aspects of current astatine labeling protocols, the knowledge of the electron affinity of this element is of prime importance. Here we report the measured value of the EA of astatine to be 2.41578(7) eV. This result is compared to state-of-the-art relativistic quantum mechanical calculations that incorporate both the Breit and the quantum electrodynamics (QED) corrections and…

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…

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 $\delta\langle r^{2}\rangle^{A,221}$ 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 sugges…

Very high specific activity erbium 169Er production for potential receptor-targeted radiotherapy

Erbium 169Er is one of the most interesting radiolanthanides for new potential receptor-targeted β− therapy applications due to its low energy β− emissions, very low intensity ɣ rays and the possibility to use 68Ga or 44Sc as companion for diagnostic in a theranostics approach. Currently it can be produced in reactors through the neutron activation of highly enriched 168Er. The low specific activity of the produced carrier-added 169Er is limiting its use for receptor-targeted therapy. Nonetheless it is used for radiosynoviorthesis of small joints. The aim of this work is to develop a new large-scale production method for the supply of very high specific activity 169Er. Highly enriched 168Er…

Depletion of the excited state population in negative ions using laser photodetachment in a gas-filled RF quadrupole ion guide

International audience; The depopulation of excited states in beams of negatively charged carbon and silicon ions was demonstrated using collisional detachment and laser photodetachment in a radio frequency quadrupole ion guide filled with helium. The high lying, loosely bound 2 D excited state in C − was completely depleted through collisional detachment alone, which was quantitatively determined within 6%. For Si − the combined signal from the population in the 2 P and 2 D excited states was only partly depleted through collisions in the cooler. The loosely bound 2 P state was likely to be completely depopulated and the more tightly bound 2 D state was partly depopulated through collision…

Data acquisition, remote control and equipment monitoring for ISOLDE RILIS

Abstract With a steadily increasing on-line operation time up to a record 3000 h in the year 2012, the Resonance Ionization Laser Ion Source (RILIS) is one of the key components of the ISOLDE on-line isotope user facility at CERN. Ion beam production using the RILIS is essential for many experiments due to the unmatched combination of ionization efficiency and selectivity. To meet the reliability requirements the RILIS is currently operated in shift duty for continuous maintenance of crucial laser parameters such as wavelength, power, beam position and timing, as well as ensuring swift intervention in case of an equipment malfunction. A recent overhaul of the RILIS included the installation…

Development of High Resolution Resonance Ionization Mass Spectrometry for Neutron Dosimetry Technique with93Nb(n,n')93mNb Reaction

We have proposed an advanced technique to measure the 93mNb yield precisely by Resonance Ionization Mass Spectrometry, instead of conventional characteristic X-ray spectroscopy. 93mNb-selective resonance ionization is achievable by distinguishing the hyperfine splitting of the atomic energy levels between 93Nb and 93mNb at high resolution. In advance of 93mNb detection, we could successfully demonstrate high resolution resonant ionization spectroscopy of stable 93Nb using an all solid-state, narrowband and tunable Ti:Sapphire laser system operated at 1 kHz repetition rate. peerReviewed

Determination of the154Sm ionization energy by high-precision laser spectroscopy

High-resolution resonance ionization mass spectrometry has been used to determine the ionization energy of 154Sm. Three-step resonant excitation with single-frequency lasers populates a series of ? = 3, J = 4 Rydberg levels in the range of n = 60?160, covering the range of 30 cm?1 to 4 cm?1 below the first ionization limit. Although samarium has a complex electronic structure with eight valence electrons, series of nearly unperturbed levels could be observed. Analysis includes shifts caused by a single perturbing state, an extended Ritz term for quantum defect variation at lower n, and corrections for residual electric fields. The resulting series convergence limit has an uncertainty of 4 ?…

The New Generation of Resonant Laser Ionization Mass Spectrometers: Becoming Competitive for Selective Atomic Ultra-Trace Determination?

A critical assessment of the present status of resonant laser ionization mass spectrometry (RIMS) as a specialized analytical technique for the field of atomic ultra-trace determination is attempted and a comparison with established mass spectrometric methods is made. Within the last years RIMS on atomic species has rapidly developed towards becoming a versatile experimental technique, in particular addressing those applications that require high selectivity in respect of isobaric or isotopic interferences. This progress is mainly based on the advent of easy-to-handle tunable solid-state laser systems for both pulsed and continuous operation, which are used in combination with modern compac…

Resonance Ionization Laser Ion Source - Off-line tests at TRIUMF

Resonance ionization laser ion sources (RILIS) developed into the most powerful tool for radioactive ion beam production at on-line facilities, as they provide a selective ionization process with inherent suppression of unwanted isobaric contaminations at the ion source. While typical tunable laser systems for these applications are based on dye lasers, we developed an all solid state laser system which consists of three pulsed titanium:sapphire (ti:sa) lasers pumped by a single high repetition rate Nd:YAG laser. Each ti:sa laser provides up to 2.5 W average output power at 12 kHz repetition rate in the wavelength region of 700-950 nm with optional frequency doubling in BBO crystals. This l…

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…

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 predomina…

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…

Development of resonance ionization in a supersonic gas-jet for studies of short-lived and long-lived radioactive nuclei

High-resolution resonance ionization spectroscopy (RIS) is required for laser spectroscopy and trace analysis of short-lived and long-lived radioactive nuclei. We have proposed high-resolution resonance ionization spectroscopy in a gas jet combined with a narrow band-width injection-locked Ti:Sapphire laser. Resonance ionization of stable 93Nb in a gas jet was demonstrated using a broad bandwidth Ti:Sapphire laser. In addition, a setup for high-resolution RIS in a gas-jet was designed using numerical simulations of the gas-jet conditions based on computational fluid dynamics.

Three-photon resonance ionization of atomic Mn in a hot-cavity laser ion source using Ti:sapphire lasers

Three-photon resonance ionization of atomic manganese (Mn) in a hot-cavity ion source using Ti:sapphire lasers has been demonstrated. Three-step ionization schemes employing different intermediate levels and Rydberg or autoionizing (AI) states in the final ionization step are established. Strong AI resonances were observed via the 3d54s5s f 6S5/2 level at 49 415.35 cm−1, while Rydberg transitions were reached from the 3d54s4d e 6D9/2,7/2,5/2 levels at around 47 210 cm−1. Analyses of the strong Rydberg transitions associated with the 3d54s4d e 6D7/2 lower level indicate that they belong to the dipole-allowed 4d → nf 6F°9/2,7/2,5/2 series converging to the 3d54s 7S3 ground state of Mn II. Fro…

Trace Analysis of the Radionuclides90Sr and89Sr in Environmental Samples I: Laser Mass Spectrometry

High-resolution laser spectroscopy with the Collinear Resonance Ionisation Spectroscopy (CRIS) experiment at CERN-ISOLDE

The Collinear Resonance Ionisation Spectroscopy (CRIS) experiment at CERN has achieved high-resolution resonance ionisation laser spectroscopy with a full width at half maximum linewidth of 20(1) MHz for 219;221Fr, and has measured isotopes as short lived as 5 ms with 214Fr. This development allows for greater precision in the study of hyperfine structures and isotope shifts, as well as a higher selectivity of singleisotope, even single-isomer, beams. These achievements are linked with the development of a new laser laboratory and new data-acquisition systems. publisher: Elsevier articletitle: High-resolution laser spectroscopy with the Collinear Resonance Ionisation Spectroscopy (CRIS) exp…

Development of two-color resonance ionization scheme for Th using an automated wide-range tunable Ti:sapphire laser system

Two-color resonance ionization schemes of Th were investigated by an automated wide-range tunable, grating-assisted Ti:Sa laser system with intracavity SHG option. A two-color ionization scheme via autoionizing state (1st step: 372.049 nm and 2nd step: 401.031 nm) was developed and its relative efficiency was lower by factor of three compared to a known three color scheme. peerReviewed

Atom beam emersion from hot cavity laser ion sources

Abstract Ion sources exploiting laser resonance ionization offer efficient and element-selective radioactive ion beam production at the leading isotope separation on-line facilities worldwide. Most commonly, laser resonance ionization takes place inside a resistively heated atomizer tube directly coupled to the production target, where the element of interest is evaporated and provided as atomic vapor. While naturally the majority of atoms is ionized inside this hot cavity, a fraction of the neutrals effuses towards the high voltage beam extraction system of the subsequent mass separator. We report on several systematic investigations on this phenomenon regarding its significance and implic…

Evaluation of the magnetic moment ofRa213

The hyperfine field at the nucleus of singly ionized radium has been investigated using the relativistic linked-cluster many-body-perturbation-theory procedure, including the effects of distributed charge and magnetization over the nucleus. The total hyperfine field of 1239 T, when combined with the experimentally observed hyperfine constant for $^{213}\mathrm{Ra}^{+}$, yields a nuclear moment of 0.607(12)${\mathrm{\ensuremath{\mu}}}_{\mathit{N}}$, in excellent agreement with the experimentally observed moment of 0.6133(18)${\mathrm{\ensuremath{\mu}}}_{\mathit{N}}$ from Zeeman measurements. Our investigation leads to exchange core-polarization and correlation contributions of 14% and 13%, r…

Recent developments in isotope ratio measurements by resonance ionization mass spectrometry

Resonance ionization mass spectrometry (RIMS) has become a sensitive and highly selective technique for the determination of extremely low elemental or isotopic abundances, involving isotope ratio measurements with dynamical ranges of 109 and beyond. The experimental detection limits are as low as 106 atoms per sample, and isotopic selectivities of up to 1013 have been achieved under optimal conditions. The potential of RIMS using different experimental systems is outlined in the determination of lowest abundances and isotope ratios of long-lived radioisotopes of general importance like Pu238–244, 41Ca, and 236U for studies in geosciences, environmental, bio-medical or fundamental research.

Isotope shifts and hyperfine structure in calcium 4snp and 4snf F Rydberg states

Isotope shifts and hyperfine structure have been measured in 4snp 1 P1 and Rydberg states for all stable calcium isotopes and the radioisotope 41Ca using high-resolution laser spectroscopy. Triple-resonance excitation via Rydberg state was followed by photoionization with a CO2 laser and mass selective ion detection. Isotope shifts for the even-mass isotopes have been analyzed to derive specific mass shift and field shift factors. The apparent isotope shifts for 41Ca and 43Ca exhibit anomalous values that are n-dependent. This is interpreted in terms of hyperfine-induced fine-structure mixing, which becomes very pronounced when singlet-triplet fine-structure splitting is comparable to the h…

Selective detection of 13C by laser photodetachment mass spectrometry

Abstract In this paper, we demonstrate how laser photodetachment mass spectrometry (LPMS) can be used to selectively detect 13C− ions in the presence of 12C− ions in a low energy ion beam. An isotopically enriched beam of carbon ions consisting of equal amounts of 13C− and 12C− ions was extracted from an ion source. The ions interacted with a laser beam in a collinear geometry over a distance of 70 cm. Residual atoms produced in the photodetachment process were detected in a neutral particle detector placed downstream of the collinear interaction region. By making use of the Doppler effect we were able to selectively photodetach 13C− ions. The number of detected 13C atoms was 13 times large…

Nuclear moments and charge radii of rare-earth isotopes studied by collinear fast-beam laser spectroscopy

The collinear fast-beam laser technique is being used to measure systematically hyperfine structures and isotope shifts of unstable nuclides in the rare-earth region. This brief report gives a general survey of the results obtained for the even-Z elements64Gd,66Dy,68Er and70Yb, with emphasis on the nuclear spins and moments. They allow a rather complete mapping of the single-particle structure and the development of nuclear deformation in the N > 82 region. The spins, magnetic moments and spectroscopic quadrupole moments of159–169Yb are presented in detail.

Shape staggering of midshell mercury isotopes from in-source laser spectroscopy compared with density-functional-theory and Monte Carlo shell-model calculations

Neutron-deficient Hg177-185 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 α-decay tagging or multireflection time-of-flight gating for isotope identification. 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 Hg177-180. 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 s…

A study of on-line gas cell processes at IGISOL

Abstract The laser ion source at the IGISOL facility, Jyvaskyla, has been used to study the effects of the passage of a primary beam through an ion guide via the dynamic time profiles of yttrium and related molecular compounds. The accessibility of a neutral fraction for laser ionization is shown to be restricted to the nozzle region in the presence of a weak plasma. The survival of this neutral fraction cannot be explained by recombination of the buffer gas alone and perhaps indicates a suppression of the transport of ions due to a plasma-generated electric field. The concept of a competition between the processes that create and destroy the ion of interest is used to explain the different…

Time profile of ion pulses produced in a hot-cavity laser ion source.

The time spreads of Mn ions produced by three-photon resonant ionization in a hot-cavity laser ion source are measured. A one-dimensional ion-transport model is developed to simulate the observed ion time structures. Assuming ions are generated with a Maxwellian velocity distribution and are guided by an axial electric field, the predictions of the model agree reasonably well with the experimental data and suggest that the ions are radially confined in the ion source and a substantial fraction of the ions in the transport tube are extracted.

Determination of nuclear spins and moments in a series of radium isotopes

Abstract The first investigation of hyperfine structure in radium isotopes has enabled the determination of nuclear spins, magnetic dipole and electric quadrupole moments of the isotopes with mass numbers A = 211, 213, 221, 223, 225, 227 and 229. Isotope shifts in the mass range A = 208−232 have also been measured. These studies were carried out using the technique of on-line collinear fast beam laser spectroscopy.

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…

Systematics of nuclear ground state properties inSr78–100by laser spectroscopy

Hyperfine structures and isotope shifts of strontium isotopes with A=78 to A=98 and A=100 were measured by collinear fast beam laser spectroscopy. Nuclear spins, moments and changes in mean square charge radii are extracted from the data. The spins and moments of most of the odd isotopes are explained in the framework of the single particle model. The changes in mean square charge radii are compared with predictions of the droplet model and of Hartree-Fock-plus-BCS calculations. For the isotopes in the transitional regions below and above the N=50 shell closure, the inclusion of quadrupole zero point motion in the Droplet model describes part of the observed shell effect. An additional chan…

Counting IndividualCa41Atoms with a Magneto-Optical Trap

Atom trap trace analysis, a novel method based upon laser trapping and cooling, is used to count individual atoms of $^{41}\mathrm{Ca}$ present in biomedical samples with isotopic abundance levels between ${10}^{\ensuremath{-}8}$ and ${10}^{\ensuremath{-}10}$. The method is calibrated against resonance ionization mass spectrometry, demonstrating good agreement between the two methods. The present system has a counting efficiency of $2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$. Within 1 h of observation time, its $3\mathrm{\text{\ensuremath{-}}}\ensuremath{\sigma}$ detection limit on the isotopic abundance of $^{41}\mathrm{Ca}$ reaches $4.5\ifmmode\times\else\texttimes\fi{}{10…

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…

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 the…

RADIOISOTOPE MASS SPECTROMETRY

Mass spectrometric methods are very sensitive and enable in many cases a multielement determination of trace and ultratrace elements combined with a good isotopic analysis ( Bacon et al. , 2001 ). Therefore, these techniques are also applied for the detection of long-lived radionuclides ( Becker and Dietze, 2000 ) mainly in environmental samples ( Adriaens et al. , 1992 ; Bailey et al. , 1993 ; Bibler et al. , 1998 ; Eroglu et al. , 1998 ; Edmonds et al. , 1998 ; Becker and Dietze, 1999 ; Wendt et al. , 1999 ), nuclear materials ( Betti, 1997 ; Chartier et al. , 1999 ), glass and ceramics ( Rohr et al. , 1994 ; Fukuda and Sayama, 1997 ), and in high-purity substances ( Beer and Heumann, 199…

Efficient and robust photo-ionization loading of beryllium ions

We demonstrate the efficient generation of Be$^+$ ions with a 60 ns and 150 nJ laser pulse near 235 nm for two-step photo-ionization, proven by subsequent counting the number of ions loaded into a linear Paul trap. The bandwidth and power of the laser pulse are chosen in such a way that a first, resonant step fully saturates the entire velocity distribution of beryllium atoms effusing from a thermal oven. The second excitation step is driven by the same light field causing efficient non-resonant ionization. Our ion-loading scheme is more than 15 times more efficient as compared to former pathways using two-photon continuous wave laser excitation.

Quantitative Detection of Strontium-90 and Strontium-89 in Environmental Samples by Laser Mass Spectrometry

Parallel to the strongly growing public concern about environmental problems, new ideas for trace detection and analysis of toxic and radioactive material are being developed. One of these new and outstanding experimental techniques is the application of analytical laser spectroscopy. Most interesting in this context is the method of resonance ionization spectroscopy (RIS), as proposed1 already in 1972 combining very high sensitivity in the detection of the element or isotope under investigation with high selectivity in the suppression of contaminants2–4.

Optimization of a laser ion source for $^{163}$Ho isotope separation

To measure the mass of the electron neutrino, the “Electron Capture in Holmium-163” (ECHo) collaboration aims at calorimetrically measuring the spectrum following electron capture in 163Ho. The success of the ECHo experiment depends critically on the radiochemical purity of the 163Ho sample, which is ion-implanted into the calorimeters. For this, a 30 kV high transmission magnetic mass separator equipped with a resonance ionization laser ion source is used. To meet the ECHo requirements, the ion source unit was optimized with respect to its thermal characteristics and material composition by means of the finite element method thermal-electric calculations and chemical equilibrium simulation…

Dipole and quadrupole moments of Cu73–78 as a test of the robustness of the Z=28 shell closure near Ni78

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…

Radium ionization scheme development: The first observed autoionizing states and optical pumping effects in the hot cavity environment

© 2018 The Authors This paper reports on resonance ionization scheme development for the production of exotic radium ion beams with the Resonance Ionization Laser Ion Source (RILIS) of the CERN-ISOLDE radioactive ion beam facility. During the study, autoionizing states of atomic radium were observed for the first time. Three ionization schemes were identified, originating from the 7s2 1S0 atomic ground state. The optimal of the identified ionization schemes involves five atomic transitions, four of which are induced by three resonantly tuned lasers. This is the first hot cavity RILIS ionization scheme to employ optical pumping effects. The details of the spectroscopic studies are described …

First Offline Results from the S3 Low-Energy Branch

International audience; 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-lo…

TRIGA-SPEC: the prototype of MATS and LaSpec

Investigation of short-lived nuclei is a challenging task that MATS and LaSpec will handle at the low energy branch of Super-FRS at FAIR. The groundwork for those experiments is laid-out already today at the TRIGA-SPEC facility as a powerful development platform located at the research reactor TRIGA Mainz. The latest status, new developments and first results of commissioning runs are presented here.

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…

An evaluation procedure for scanning interferometer based wavemeters

Abstract A common approach to wavelength measurement is the travelling interferometer (wavemeter). We present an evaluation procedure that allows to achieve high precision with a compact device. The zero crossings of the interference signal corresponding to the reference laser is used to sample the signal of the probe laser. Electronic noise and fluctuations of the laser frequency cancel due to the large number of sample points. The evaluation procedure has been applied to a wavemeter based on a continuously moving Mach–Zehnder interferometer. A travelling path of 10 cm was sufficient to yield 3σ-accuracy of Δ λ / λ =3.2×10 −9 , demonstrated by comparison with cesium saturation spectroscopy.

Nuclear spins, moments, and changes of the mean square charge radii of sup.(140-153)Eu

The hyperfine structures and isotope shifts of 14 isotopes of Eu (Z=63) in the mass range 140≦A≦153, partly with isomeric states, have been measured in the atomic transitions at 4,594 A and 4,627 A, using the technique of collinear fast-beam laser spectroscopy at the ISOLDE facility at CERN. The nuclear spins, the magnetic dipole and electric quadrupole moments, and the changes in the mean square charge radii have been evaluated. These nuclear parameters clearly reflect the effects of theN=82 neutron-shell closure in the single-proton hole states with respect to the semi-magic gadolinium (Z=64), and theN=88−90 shape transition.

First laser ions at an off-line mass separator of the ISAC facility at TRIUMF

For efficient and in particular for selective production of radioactive ion beams at on-line mass separator facilities the technique of resonance ionization laser ion sources (RILIS) has become the most powerful tool. In facilities like ISOLDE at CERN they nowadays represent the most commonly used type of ion source for rare short-lived isotopes, delivering highest suppression of isobaric contaminations. For a first off-line demonstration preparing the development and installation of such a laser ion source at the new ISAC facility at TRIUMF in Vancouver (Canada), an all solid state laser system developed at the University of Mainz (Germany), was transferred and tested there at an off-line …

Off-line studies of the laser ionization of yttrium at the IGISOL facility

A laser ion source is under development at the IGISOL facility, Jyvaskyla, in order to address deficiencies in the ion guide technique. The key elements of interest are those of a refractory nature, whose isotopes and isomers are widely studied using both laser spectroscopic and high precision mass measurement techniques. Yttrium has been the first element of choice for the new laser ion source. In this work we present a new coupled dye-Ti:Sapphire laser scheme and give a detailed discussion of the results obtained from laser ionization of yttrium atoms produced in an ion guide via joule heating of a filament. The importance of not only gas purity, but indeed the baseline vacuum pressure in…

Nuclear Magnetic Moment ofTl207

The magnetic moment 1.876(5)${\mathrm{\ensuremath{\mu}}}_{\mathit{N}}$ of 4.77-min $^{207}\mathrm{Tl}$, the only heavy nucleus with a doubly magic core plus a single ${s}_{\frac{1}{2}}$ particle or hole, was measured from the hfs by collinear fast-beam laser spectroscopy at ISOLDE (isotope separator at the CERN synchrotron). The result is of theoretical importance as a test case for core polarization since the nuclear structure is relatively simple and the orbital part of the magnetic moment, including strong pion-exchange contribution, is expected to be zero.

Peak shape for a quadrupole mass spectrometer: comparison of computer simulation and experiment

Abstract Computer simulations of ion trajectories have been used to evaluate the performance of a quadrupole mass spectrometer. Consideration has been given to realistic fields modeled on a commercial system as well as experimental distributions with respect to ion entry position, axial and radial velocity and relative phase of the quadrupole field. Determination of the mass filter acceptance-area as a function of the mass setting yields mass peak shapes with a dynamic range of more than seven orders of magnitude and thus provides estimates for abundance sensitivity. Results from these simulations are found to give excellent agreement with experimental measurements for different elements in…

Optimization of a hot-cavity type resonant ionization laser ion source

TuePS05; International audience; Resonant Ionization Laser Ion Source (RILIS) is nowadays an important technique in many RadioactiveIon Beam (RIB) facilities for its reliability and ability to ionize efficiently and element selectively.Grand Accélérateur National d’Ions Lourds (GANIL) Ion Source using Electron Laser Excitation(GISELE) is an off-line test bench for RILIS developed to study a fully operational resonant laserion source at GANIL facility. The ion source body has been designed as a modular system toinvestigate different experimental approaches by varying the design parameters, to develop the futureon-line laser ion source. The aim of this project is to determine the best technic…

Novel photoreception system in sponges?

Abstract Sponges (phylum Porifera) of the classes Hexactinellida and Demospongiae possess a skeleton composed of siliceous spicules, which are synthesized enzymatically. The longest spicules are found among the Hexactinellida, with the stalk spicules (length: 30 cm; diameter: 300 μm) of Hyalonema sieboldi as prominent examples. These spicules are constructed around a central axial filament, which is formed by approximately 40 siliceous layers. The stratified spicules function as optical glass fibers with unique properties. If free-spaced coupled with a white light source (WLS), the entire fiber is illuminated. Special features of the light transmission: (i) only wavelengths between 615 and …

Certification of a 41Ca dose material for use in human studies (IRMM-3703) and a corresponding set of isotope reference materials for 41Ca measurements (IRMM-3701)

Abstract The long-living radioisotope 41Ca could overcome current limitations in assessing the impact of interventions on bone health in controlled human studies. Changes in bone Ca metabolism can be identified directly via the induced changes in 41Ca excretion from 41Ca-labelled bones via the n(41Ca)/n(40Ca) ratio in urine. A 41Ca dose material (IRMM-3703), for use in human studies, was produced by IRMM within the EC funded project OSTEODIET. The 41Ca base material was purified and the purified solution is certified for both isotopic composition and amount content by isotope dilution mass spectrometry. The 44Ca-enriched isotope reference material, IM-6009, was used as spike and the natural…

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…

High-resolution γ-ray spectroscopy: a versatile tool for nuclear β-decay studies at TRIUMF-ISAC

High-resolution γ-ray spectroscopy is essential to fully exploit the unique, high-quality beams available at the next generation of radioactive ion beam facilities such as the TRIUMF isotope separator and accelerator (ISAC). The 8π spectrometer, which consists of 20 Compton-suppressed HPGe detectors, has recently been reconfigured for a vigorous research programme in weak interaction and nuclear structure physics. With the addition of a variety of ancillary detectors it has become the world's most powerful device dedicated to β-decay studies. This paper provides a brief overview of the apparatus and highlights from recent experiments.

Nuclear ground state spins of short-lived strontium isotopes

Nuclear ground state spins of the odd-mass strontium isotopes between A=79 and 97 were determined by measurements of the hyperfine structure in the ionic transition 5s2S1/2−5p2P3/2. The spins of93Sr and97Sr are revised to I=5/2 and I=1/2, respectively, while assignments for the remaining isotopes are confirmed.

Resonance laser ionization spectroscopy of tellurium

Abstract Resonance ionization schemes for tellurium are investigated with a resonance ionization laser ion source and Ti:Sapphire lasers for fundamental research applications. We present the first three-step resonance ionization spectra of atomic Te. Several autoionizing Rydberg series converging to the first excited state of Te+ are observed and assigned to 5p3 (2Do3/2) ns and nd configurations. Our results include confirmation and significant expansion of the Rydberg series previously reported as well as observation of three new series. From the series convergence limits the ionization potential of tellurium is revised to be 72,669.006(42)stat(20)sys cm−1.

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…

Spurenbestimmung der Radionuclide90Sr und89Sr in Umweltproben I: Laser-Massenspektrometrie

Development of a sequential data correction method for isotope ratio analysis by resonance ionization mass spectrometry

A sequential data correction method using several experimental parameters of pulsed resonance ionization mass spectrometry was developed to reduce mass discrimination effects for isotope ratio analysis as well as fluctuations in the ion count rate. This correction method was applied to isotope ratio determination of stable titanium isotopes using a two-step, single color ionization scheme. A significant improvement of the precision of the measured isotopic ratio of stable titanium isotopes was demonstrated after correction with a parameter set consisting of laser power, atmospheric pressure, and laser frequency.

Combined high-resolution laser spectroscopy and nuclear decay spectroscopy for the study of the low-lying states inFr206,At202, andBi198

High-resolution laser spectroscopy was performed on $^{206}\mathrm{Fr}$ with the collinear resonance ionization spectroscopy (CRIS) experiment at CERN-ISOLDE. The hyperfine structure and isotope shift of the ground, first isomeric and second isomeric states were measured. The hyperfine components were unambiguously assigned to each nuclear state by means of laser-assisted nuclear decay spectroscopy. The branching ratios in the $\ensuremath{\alpha}$ decay of $^{206}\mathrm{Fr}$ and $^{202}\mathrm{At}$ were also measured for the first time with isomerically purified beams. The extracted hindrance factors allow determination of the spin of the ground, first isomeric, and second isomeric states…

Isotope shifts and hyperfine structure in the $\mathsf{ 3d ^2D_J \rightarrow 4p ^2P_J}$ transitions in calcium II

The isotope shift and hyperfine structure in the three \(\) - transitions in Ca II have been studied by fast ion beam collinear laser spectroscopy for all stable Ca isotopes. The metastable 3d states were populated within the surface ionization source of a mass separator with a probability of about 0.1%. After resonant excitation to the 4p levels with diode laser light around 850 nm the uv photons from the \(\) transitions to the ground state were used for detection. Hyperfine structure parameters A and B for the odd isotope 43Ca, as evaluated from the splittings observed, agree well with theoretical predictions from relativistic many-body perturbation theory. Field shift constants \(\) and…

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.

Lifetime measurements of highly excited Rydberg states of strontium I

Lifetimes of Rydberg states of the triplet-series 5s ns3S1 withn = 19–23, 35 and 5s nd3D3 withn = 18–20, 23–28 in the spectrum of neutral strontium have been determined. Observation of the exponential decay after excitation by a pulsed laser in a fast atomic beam and subsequent state-selective field ionization was employed. The lifetimes of the states of the3S1-series show the expectedn*3 dependence on the effective principal quantum number, while the3D3-series is disturbed by configuration mixing. Furthermore, state re-populations induced by black-body radiation have been observed.

Collisional ionization as a sensitive detection scheme in collinear laser-fast-beam spectroscopy

Abstract State-selective collisional ionization of fast atomic beams is used to detect optical pumping. Counting of these ions is superior in sensitivity by several orders of magnitude to the conventional fluorescence detection, provided that the energy levels involved in the optical pumping process are sufficiently well separated. A straightforward application is envisaged in the collinear laser-fast-beam spectroscopy of rare-gas isotopes far from stability of which only very weak beams are available from on-line isotope separators.

Isotope shifts and hyperfine structure in the transitions of stable calcium isotopes and calcium-41

Isotope shifts and hyperfine structure in the 4s2 1S0 → 4s4p 1P1 and 4s2 1S0 → 4s4d 1D2 transitions of calcium have been measured with high-precision laser spectroscopy. Calcium atoms in an atomic beam were excited with single-frequency cw dye and titanium sapphire lasers and then photoionized with the 363.8 nm or 514.5 nm line of an argon ion laser. The resulting ions were analyzed and detected with a quadrupole mass spectrometer. Isotope shifts for all stable calcium isotopes and the radionuclide 41Ca have been measured in both transitions. The corresponding field shift and specific mass shift coefficients as well as hyperfine structure constants for the isotopes 41, 43Ca have been derive…

Use of a Continuous Wave Laser and Pockels Cell for Sensitive High-Resolution Collinear Resonance Ionization Spectroscopy

New technical developments have led to a 2 orders of magnitude improvement of the resolution of the collinear resonance ionization spectroscopy (CRIS) experiment at ISOLDE, CERN, without sacrificing the high efficiency of the CRIS technique. Experimental linewidths of 20(1) MHz were obtained on radioactive beams of francium, allowing us for the first time to determine the electric quadrupole moment of the short lived [t1/2=22.0(5) ms]219Fr Qs=−1.21(2) eb, which would not have been possible without the advantages offered by the new method. This method relies on a continuous-wave laser and an external Pockels cell to produce narrow-band light pulses, required to reach the high resolution in t…

Development of accelerator mass spectrometry assisted by isotope-selective laser photodetachment for monitoring 129I

Abstract A prototype system was developed to investigate an isotope-selective laser photodetachment technique for a 129 I accelerator mass spectrometer. A pulsed ion source for negative iodine ions (I − ) that employed laser ablation proved to be suitable for isotope-selective laser photodetachment. Laser photodetachment of pulsed negative iodine ions was estimated to have an efficiency of about 81% based on a model calculation for the prototype system with a tunable pulsed Ti:sapphire laser.

Simulation and optimization of the implantation of holmium atoms into metallic magnetic microcalorimeters for neutrino mass determination experiments

Abstract Several novel experiments designed to investigate the electron neutrino mass in the sub-eV region are based on the calorimetric measurement of the 163Ho electron capture spectrum. For this the 163Ho source, with a required activity of the order of 1 to 100 Bq , needs to be enclosed in the detector, having a volume smaller than 10 − 3 mm 3 . Ion implantation is presently considered to be the most reliable method to enclose this source in the detector homogeneously distributed in a well defined volume. We have investigated the distribution of implanted holmium ions in different target materials and for different implantation energies by means of Monte Carlo simulations based on the S…

Laser resonance ionization spectroscopy on lutetium for the MEDICIS project

The MEDICIS-PROMED Innovative Training Network under the Horizon 2020 EU program aims to establish a network of early stage researchers, involving scientific exchange and active cooperation between leading European research institutions, universities, hospitals, and industry. Primary scientific goal is the purpose of providing and testing novel radioisotopes for nuclear medical imaging and radionuclide therapy. Within a closely linked project at CERN, a dedicated electromagnetic mass separator system is presently under installation for production of innovative radiopharmaceutical isotopes at the new CERN-MEDICIS laboratory, directly adjacent to the existing CERN-ISOLDE radioactive ion beam …

Selective ultra trace isotope determination in environmental and biomedical studies by high-resolution resonance ionization mass spectrometry

The precise determination of relative abundances of ultra trace isotopes in the range below 10 -9 is of importance for a wide spectrum of applications in fields like environmental protection, cosmo-chemistry, bio-medical tracer studies or geological and geo-chronological investigations. The necessary high isotopic selectivity, rather complete isobaric suppression and good overall efficiency for these investigations is provided by high-resolution resonance ionization mass spectrometry. Multi-step continuous wave laser excitation and ionization using diode lasers at a compact quadrupole mass spectrometer has been optimized to become a powerful and reliable experimental method, which is just b…

Resonance ionization spectroscopy for trace analysis and fundamental research

Resonance ionization spectroscopy (RIS) and its combination with mass spectrometry (RIMS) have grown to become powerful techniques, which offer high sensitivity as well as elemental and isotopic selectivity. The principles of RIS and RIMS are introduced; they primarily concern the analysis of the optical spectra for the choice of efficient excitation schemes and the suitable design of the experimental apparatus. Recent applications span from studies of short-lived isotopes at on-line mass separators to a wide variety of trace analysis applications for radioactive isotopes, which can range from measurements of solar neutrino flux to environmental assessment.

Resonant ionization spectroscopy of autoionizing Rydberg states in cobalt and redetermination of its ionization potential

Multi-step resonance ionization spectroscopy of cobalt has been performed using a hot-cavity laser ion source and three Ti:Sapphire lasers. The photoionization spectra revealed members of five new autoionizing Rydberg series that originate from three different lower levels of 3d74s5s h4F9/2, 3d74s4d f4G11/2, and 3d74s4d f4H13/2 and converge to the first four excited states of singly ionized Co. The analyses of the Rydberg series yield 63564.689 �� 0.036 cm-1 as the first ionization potential of Co, which is an order of magnitude more accurate than the previous estimation. Using a three-step resonance ionization scheme that employs an autoinizing Rydberg state in the last transition, we obta…

Resonant laser ionization mass spectrometry: An alternative to AMS?

Resonant laser ionization mass spectrometry (RIMS) has developed into a versatile experimental method particularly concerning applications for highly selective ultratrace analysis. Apart from providing nearly complete isobaric suppression and high overall efficiency, the possibility for combining optical isotopic selectivity with that of the mass spectrometer leads to remarkable specifications. The widespread analytical potential and applicability of different techniques based on resonant laser ionization is demonstrated in investigations on stable and radioactive ultratrace isotopes with the focus on applications which require high selectivity, concerning, e.g., the noble gas isotopes 81,8…

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…

Achterbahn fahren im Physikunterricht. Physikdidaktik

Abstract in German Das Messen von Beschleunigungen und Hohen wahrend einer Achterbahnfahrt bietet die Moglichkeit, den Physikunterricht anwendungsbezogen zu gestalten. Dieser Ansatz erlaubt einen erlebnisorientierten Zugang speziell im Bereich der oftmals als langweilig empfundenen Mechanik. Das Beispiel der Achterbahn Kanonen in Goteborg demonstriert die vielen Moglichkeiten der Datenauswertung. Auserdem generiert das eigenstandige Experimentieren mit einem modernen Messsystem und die Datenauswertung mit Analyse am Computer einen zusatzlichen Lerneffekt.

The laser ion source and trap (LIST) – A highly selective ion source

A combined structure consisting of a laser ion source and a linear Paul trap (LIST) has been designed to produce radioactive ion beams of high purity and optimal temporal and spacial brilliance at on-line isotope separator (ISOL) facilities. The functionality of the LIST was experimentally demonstrated in off-line tests using the RISIKO off-line mass separator together with an all solid state Ti:sapphire laser system at the University of Mainz. Two different ion trap designs were tested extracting the performance of these devices regarding ionization efficiency and selectivity as well as time structure and transverse emittance of the produced ion beam. The results of these measurements are …

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…

Collinear Resonance Ionization Spectroscopy of Neutron-Deficient Francium Isotopes

The magnetic moments and isotope shifts of the neutron-deficient francium isotopes 202-205Fr were measured at ISOLDE-CERN with use of collinear resonance ionization spectroscopy. A production-to-detection efficiency of 1% was measured for 202Fr. The background from nonresonant and collisional ionization was maintained below one ion in 105 beam particles. Through a comparison of the measured charge radii with predictions from the spherical droplet model, it is concluded that the ground-state wave function remains spherical down to 205Fr, with a departure observed in 203Fr (N = 116). ispartof: Physical Review Letters vol:111 issue:21 pages:212501-4 ispartof: location:United States status: pub…

Rydberg and autoionizing states of tellurium studied by laser resonance ionization spectroscopy

Multistep laser-resonance-ionization spectroscopy of tellurium (Te) has been performed at TRIUMF's off-line laser ion source test stand. Six clean and regular even-parity Rydberg series $5{p}^{3}$ $({^{4}S}_{3/2}^{\ensuremath{\circ}})$ $np\phantom{\rule{4pt}{0ex}}^{3}P_{0,1,2}$, $np\phantom{\rule{4pt}{0ex}}^{5}P_{1,2}$, and $nf\phantom{\rule{4pt}{0ex}}^{3}F_{2}/^{5}F_{1,2}$ were observed. The ionization potential of Te was extracted from the measured series as $72669.114{(56)}_{\mathrm{stat}}{(45)}_{\mathrm{sys}}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Excited from two different intermediate levels, seven odd-parity autoionization Rydberg series converging to the $5{s}^{2}…

Isotope shifts and hyperfine structure in the transitions of gadolinium

High-resolution resonance ionization mass spectrometry has been used to measure isotope shifts and hyperfine structure in all (J = 2-6) and the transitions of gadolinium (Gd I). Gadolinium atoms in an atomic beam were excited with a tunable single-frequency laser in the wavelength range of 422-429 nm. Resonant excitation was followed by photoionization with the 363.8 nm line of an argon ion laser and resulting ions were mass separated and detected with a quadrupole mass spectrometer. Isotope shifts for all stable gadolinium isotopes in these transitions have been measured for the first time. Additionally, the hyperfine structure constants of the upper states have been derived for the isotop…

Feasibility of photodetachment isobar suppression of WF with respect to HfF

Abstract The feasibility of using laser photodetachment as a means for isobar suppression in accelerator mass spectrometry has been investigated for the special case of HfF 5 − /WF 5 − . A method for absolute photodetachment cross section measurements was applied and the cross sections of tungsten pentafluoride and hafnium pentafluoride negative ions were measured. The measurements indicate that the photodetachment cross section for WF 5 − is at least 100 times larger than for HfF 5 − at the wavelength of the fourth harmonic of the Nd:YAG laser at 266 nm. The absolute cross section for WF 5 − at this photon energy was found to be (2.8 ± 0.3) × 10 −18  cm 2 , while an upper limit of 2 × 10 −…

First observation of the blue optical lines of francium

We report here the first wave-length measurements in the second resonance doublet of francium, D1'(7s2S1/2-8p2P 1/2) and D2'(7s2S1/2-8p2P 3/2), carried out by collinear fast-beam laser spectroscopy. The transition wave numbers are D1' = 23112.9603(50) cm-1 and D2' = 23658.3058(40) cm-1, corresponding to a 8p fine-structure splitting of δW8p = 545.3454(70) cm-1. In addition the hyperfine structure in both lines and the isotope shift in the D2' line for the isotopes 212,213,220,221Fr have been measured. The results are discussed with special emphasis on the analysis of the atomic structure in the heaviest alkali element and compared with theoretical predictions, as well as the only earlier sp…

Determination of the first ionization potential of actinide elements by resonance ionization mass spectroscopy

Abstract Resonance ionization mass spectroscopy (RIMS) in the presence of an external static electric field has been used for the determination of photoionization thresholds. Extrapolation of the thresholds obtained with different electric field strengths to zero field strength directly leads to the first ionization potential (IP). The ionization potentials of the transplutonium elements americium, curium, berkelium and californium could be measured for the first time. Due to the high sensitivity of RIMS, samples of only 1012 atoms have been used. The results are: IPAm = 5.9738(2)eV, IPCm = 5.9915(2)eV, IPBk = 6.1979(2)eV and IPCf = 6.2817(2)eV. The same technique was applied to thorium, ne…

Temporal Control of Pulses from a High-Repetition-Rate Tunable Ti:Sapphire Laser by Active Q-switching

We investigated the lasing characteristics of a Ti:sapphire laser pumped by a pulsed high-repetition-rate Nd:YAG laser. The pump laser has a pulsewidth of 450 ns, while the Ti:sapphire laser shows a significantly shorter pulse width of 25 ns for suitably intense pumping. The energy conversion efficiency of the laser is more than 10%. To synchronize different lasers and to avoid multiple spiking during one pump pulse, we use a Brewster-cut Pockels cell in the resonator for Q-switching. The temporal profile and conversion efficiency are determined and compared to theoretical estimates.

Erratum to ‘Simulation of the relative atomic populations of elements 1≤Z ≤89 following charge exchange tested with collinear resonance ionization spectroscopy of indium’ [Spectrochimica Acta Part B 153 (2019) 61–83]

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…

Laser photodetachment of radioactive $^{128}$I$^−$

International audience; The first experimental investigation of the electron affinity (EA) of a radioactive isotope has been conducted at the CERN-ISOLDE radioactive ion beam facility. The EA of the radioactive iodine isotope (128)I (t (1/2) = 25 min) was determined to be 3.059 052(38) eV. The experiment was conducted using the newly developed Gothenburg ANion Detector for Affinity measurements by Laser PHotodetachment (GANDALPH) apparatus, connected to a CERN-ISOLDE experimental beamline. (128)I was produced in fission induced by 1.4 GeV protons striking a thorium/tantalum foil target and then extracted as singly charged negative ions at a beam energy of 20 keV. Laser photodetachment of th…

In-gas laser ionization and spectroscopy of actinium isotopes near the N=126 closed shell

The in-gas laser ionization and spectroscopy (IGLIS) techniquewas applied on the $^{212–215}$Ac isotopes, produced at the Leuven Isotope Separator On-Line (LISOL) facility by using the in-gas-cell and the in-gas-jet methods. The first application under on-line conditions of the in-gas-jet laser spectroscopy method showed a superior performance in terms of selectivity, spectral resolution, and efficiency in comparison with the in-gas-cell method. Following the analysis of both experiments, the magnetic-dipole moments for the $^{212–215}$Ac isotopes, electric-quadrupole moments and nuclear spins for the $^{214,215}$Ac isotopes are presented and discussed. A good agreement is obtained with lar…

High-Precision Multiphoton Ionization of Accelerated Laser-Ablated Species

We demonstrate that the pulsed-time structure and high-peak ion intensity provided by the laser-ablation process can be directly combined with the high resolution, high efficiency, and low background offered by collinear resonance ionization spectroscopy. This simple, versatile, and powerful method offers new and unique opportunities for high-precision studies of atomic and molecular structures, impacting fundamental and applied physics research. We show that even for ion beams possessing a relatively large energy spread, high-resolution hyperfine-structure measurements can be achieved by correcting the observed line shapes with the time-of-flight information of the resonantly ionized ions.…

MELISSA: Laser ion source setup at CERN-MEDICIS facility. Blueprint

The Resonance Ionization Laser Ion Source (RILIS) has become an essential feature of many radioactive ion beam facilities worldwide since it offers an unmatched combination of efficiency and selectivity in the production of ion beams of many different chemical elements. In 2019, the laser ion source setup MELISSA is going to be established at the CERN-MEDICIS facility, based on the experience of the workgroup LARISSA of the University Mainz and CERN ISOLDE RILIS team. The purpose is to enhance the capability of the radioactive ion beam supply for end users by optimizing the yield and the purity of the final product. In this article, the blueprint of the laser ion source, as well as the key …

CERN-MEDICIS: A Review Since Commissioning in 2017

The CERN-MEDICIS (MEDical Isotopes Collected from ISolde) facility has delivered its first radioactive ion beam at CERN (Switzerland) in December 2017 to support the research and development in nuclear medicine using non-conventional radionuclides. Since then, fourteen institutes, including CERN, have joined the collaboration to drive the scientific program of this unique installation and evaluate the needs of the community to improve the research in imaging, diagnostics, radiation therapy and personalized medicine. The facility has been built as an extension of the ISOLDE (Isotope Separator On Line DEvice) facility at CERN. Handling of open radioisotope sources is made possible thanks to i…

Ultratrace analysis of calcium with high isotopic selectivity by diodelaser resonance ionisation mass spectrometry

A resonance ionisation mass spectrometer for the ultratrace determination of calcium isotopes is presented. It achieves high overall efficiency, ultra-high isotopic abundance sensitivity of more than 1010 and complete suppression of isobars. The system can be used for isotope ratio studies on stable and long-lived trace isotopes with the final goal of radiodating via 41Ca-determination. For the different applications optical one-, two- or three-step resonance excitation and subsequent ionisation is applied using simple and inexpensive diodelasers. Additional mass analysis is accomplished in a commercial quadrupole mass spectrometer. The experimental set-up and first results on synthetical a…

Double-resonance-ionization mapping of the hyperfine structure of the stable Cu isotopes using pulsed narrowband Ti:sapphire lasers

We present two approaches to enhance the resolving power for measuring hyperfine structure constants using resonance ionization spectroscopy. The first method employs a 2D-resonance ionization spectroscopy scanning technique with pulsed, narrowband Ti:sapphire lasers (1 GHz linewidth), allowing us to resolve hyperfine components that cannot be separated using the standard 1D-scanning method across only one optical transition. In a second refinement, the resolving power is further enhanced through the use of a ring design of the laser cavity. This layout leads to a reduction of the laser linewidth from 1 GHz to below 50 MHz, resulting in experimental linewidths of about 150 MHz. Motivated by…

Laser photodetachment mass spectrometry

We demonstrate that the technique of laser photodetachment spectroscopy on atomic negative ions can be used as a sensitivity enhancement tool in mass spectrometry, useful for suppressing both isotopic as well as molecular isobaric interferences. In the experiment a beam of negative ions and a laser beam are merged in a collinear geometry and the wavelength of the laser is tuned across the photodetachment threshold region. Due to the large differential Doppler shifts associated with the fast moving ions of different masses, it is possible to selectively detach ions of certain isotopes while leaving others unaffected. By choosing co-propagating laser and ion beams, the heavier isotopes of an …

Development of the CRIS (Collinear Resonant Ionisation Spectroscopy) beam line

The CRIS (Collinear Resonant Ionisation Spectroscopy) beam line is a new experimental set up at the ISOLDE facility at CERN. CRIS is being constructed for highresolution laser spectroscopy measurements on radioactive isotopes. These measurements can be used to extract nuclear properties of isotopes far from stability. The CRIS beam line has been under construction since 2009 and testing of its constituent parts have been performed using stable and radioactive ion beams, in preparation for its first on-line run. This paper will present the current status of the CRIS experiment and highlight results from the recent tests. ispartof: pages:012070-6 ispartof: Journal of Physics: Conference Serie…

Spectroscopy of short-lived radioactive molecules

Molecular spectroscopy offers opportunities for the exploration of the fundamental laws of nature and the search for new particle physics beyond the standard model1–4. Radioactive molecules—in which one or more of the atoms possesses a radioactive nucleus—can contain heavy and deformed nuclei, offering high sensitivity for investigating parity- and time-reversal-violation effects5,6. Radium monofluoride, RaF, is of particular interest because it is predicted to have an electronic structure appropriate for laser cooling6, thus paving the way for its use in high-precision spectroscopic studies. Furthermore, the effects of symmetry-violating nuclear moments are strongly enhanced5,7–9 in molecu…

Isotope Shifts of Radium Monofluoride Molecules

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.

Three-step resonant photoionization spectroscopy of Ni and Ge: ionization potential and odd-parity Rydberg levels

In preparation of a laser ion source, we have investigated multi-step laser ionization via Rydberg and autoionizing states for atomic Ni and Ge using a mass separator with an ion beam energy of 20 keV. For both elements resonant three-step excitation schemes suitable for modern Ti:sapphire laser systems were developed. Rydberg series in the range of principal quantum numbers 20 n 80 were localized, assigned and quantum numbers were allocated to the individual resonances. Ionization potentials (IP) were extracted from fits of the individual series and quantum defects of individual levels were analysed for confirmation of series assignment. For Ni the ionization potential could be extracted w…

A New Sensitive Technique for Laser Spectroscopic Studies of Radioactive Rare-Gas Isotopes

The concept of laser ionization has been widely used in spectroscopy studies and for the detection of minute samples of atoms. Being based on ion counting, it avoids the sensitivity problems of conventional fluorescence spectroscopy, which are due to low detection efficiency and large background from scattered laser light. We report the first application of an alternative ionization scheme which we have developed for collinear laser spectroscopy on fast atomic beams /1/. Here the increase in sensitivity has considerably enlarged the range of isotopes very far from stability, for which nuclear moments and radii can be investigated in hyperfine structure and isotope shift measurements.

Properties and performance of a quadrupole mass filter used for resonance ionization mass spectrometry

Abstract The performance of commercial quadrupole mass spectrometers (QMS) with a number of imperfections, as compared to the ideal hyperbolic geometry, has been characterized using the computer simulation program simion 3d version 6.0. The analysis of simulated QMS geometries focuses primarily on modeling of the internal potential, the study of field deviations, and the influence of finite length on performance of the QMS. The computer simulation of ion trajectories in the QMS field yields predictions for optimum working conditions and provides estimates for the resolving power and the maximum isotopic abundance sensitivity. Experimental measurements that confirm these expectations are pre…

Ion beam production and study of radioactive isotopes with the laser ion source at ISOLDE

At ISOLDE the majority of radioactive ion beams are produced using the resonance ionization laser ion source (RILIS). This ion source is based on resonant excitation of atomic transitions by wavelength tunable laser radiation. Since its installation at the ISOLDE facility in 1994, the RILIS laser setup has been developed into a versatile remotely operated laser system comprising state-of–the-art solid state and dye lasers capable of generating multiple high quality laser beams at any wavelength in the range of 210–950 nm. A continuous programme of atomic ionization scheme development at CERN and at other laboratories has gradually increased the number of RILIS-ionized elements. At present, …

Progress of resonant ionization laser ion source development at GANIL.

SPIRAL2 (Systeme de Production d’Ions Radioactifs Acceleres en Ligne) is a research facility under construction at GANIL (Grand Accelerateur National d’Ions Lourds) for the production of radioactive ion beams by isotope separation on-line methods and low-energy in-flight techniques. A resonant ionization laser ion source will be one of the main techniques to produce the radioactive ion beams. GISELE (GANIL Ion Source using Electron Laser Excitation) is a test bench developed to study a fully operational laser ion source available for Day 1 operations at SPIRAL2 Phase 2. The aim of this project is to find the best technical solution which combines high selectivity and ionization efficiency w…

First online operation of TRIGA-TRAP

Abstract We report on the successful coupling of the Penning-trap mass spectrometry setup TRIGA-TRAP to the research reactor TRIGA Mainz. This offers the possibility to perform direct high-precision mass measurements of short-lived nuclei produced in neutron-induced fission of a 235 U target located near the reactor core. An aerosol-based gas-jet system is used for efficient transport of short-lived neutron-rich nuclei from the target chamber to a surface ion source. In conjunction with new ion optics and extended beam monitoring capabilities, the experimental setup has been fully commissioned. The design of the surface ion source, efficiency studies and first results are presented.

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.

Intercomparison measurements between accelerator and laser based mass spectrometry for ultra-trace determination of 41Ca in the 10−11–10−10 isotopic range

Abstract Selective ultra-trace determination of the long-lived radioisotope 41 Ca has applications in environmental and biomedical research, as well as in cosmochemistry. We have conducted an intercomparison between the two currently available methods for measurement at these low (radio) activities: accelerator mass spectrometry (AMS) and resonance ionization mass spectrometry (RIMS). Three artificially produced 41 Ca samples, primarily of cosmochemical importance, with isotopic abundances in the range of 10 −11 –10 −10 were used and results of these measurements show good agreement between the two methods, within the experimental uncertainties.

Moments and Radii of 78–100Sr

The chain of Sr isotopes ranges from the neutron-shell closure at N = 50 into both the N = 38 and N = 60 deformation regions which represent the main topic of this workshop. For a detailed understanding of the nature of these nuclei, laser spectroscopy can provide the ground state spins and moments, as well as the the changes in the mean square charge radii as a function of the neutron number N. Recent experiments at Karlsruhe [1] and at Daresbury [2] essentially cover the neutron-deficient and stable Sr isotopes between N = 40 and N = 50. In order to complement these results, and to extend the measurements into the region of neutron-rich isotopes, we have performed an experiment at the ISO…

Laser ion source tests at the HRIBF on stable Sn, Ge and Ni isotopes

Abstract As one step in the ion source development for the Rare Isotope Accelerator, a hot-cavity laser ion source using an all-solid-state titanium–sapphire laser system has been tested at the Holifield Radioactive Ion Beam Facility. Resonance ionization of stable isotopes of Sn, Ge and Ni has been studied in a Ta hot cavity. Efficient three step resonant ionization schemes applying frequency tripling for the first excitation step and using auto-ionizing or atomic Rydberg states in the ionizing step have been identified for all three elements, resulting in laser ion beams of typically around 100 nA. By saturating most of the optical excitation steps involved, ionization efficiencies of 22%…

Highly efficient isotope separation and ion implantation of  163Ho for the ECHo project

Abstract The effective electron neutrino mass measurement in the framework of the ECHo experiment requires radiochemically pure 163 Ho, which is ion implanted into detector absorbers. To meet the project specifications in efficiency and purity, the entire process chain of ionization, isotope separation , and implantation of 163Ho was optimized. A new two-step resonant laser ionization scheme was established at the 30 kV magnetic mass separator RISIKO. For ionization and separation, an average efficiency of 69 ( 5 )  stat(4)sys% was achieved using intra-cavity frequency doubled Ti:sapphire lasers. The implantation of undesired 166 m Ho, which is present in trace amounts in the initial  163Ho…

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

Resonant three-photon ionization spectroscopy of atomic Fe

Laser spectroscopic investigations on high-lying states around the ionization potential (IP) in the atomic spectrum of Fe have been carried out for the development of a practical three-step resonance ionization scheme accessible by Ti: sapphire lasers. A hot cavity laser ion source, typically used at on-line radioactive ion beam production facilities, was employed in this work. Ionization schemes employing high-lying Rydberg and autoionizing states populated by three-photon excitations were established. Five new Rydberg and autoionizing Rydberg series converging to the ground and to the first four excited states of Fe II are reported. Analyses of the Rydberg series yield the value 63 737.68…

Resonance ionization of holmium for ion implantation in microcalorimeters

Abstract The determination of the electron neutrino mass by calorimetric measurement of the 163 Ho electron capture spectrum requires ultra-pure samples. Several collaborations, like ECHo or HOLMES, intend to employ microcalorimeters into which 163 Ho is implanted as an ion beam. This makes a selective and additionally very efficient ion source for holmium mandatory. For this purpose, laser resonance ionization of stable holmium 165 Ho was studied, using a three step excitation scheme driven by pulsed Ti:sapphire lasers. Five measurements with sample sizes of 10 14 and 10 15 atoms were performed for the efficiency investigation. In average, an excellent ionization efficiency of 32(5) % coul…

Optical spectroscopy and performance tests with a solid state laser ion source at HRIBF

An ISOLDE-type hot-cavity laser ion source based on high-repetition-rate Ti:Sapphire lasers has been set up at the Holifield radioactive ion beam facility. To assess the feasibility of the all-solid-state laser system for applications at advanced radioactive ion beam facilities, spectroscopy and performance tests have been conducted with this source. The results of recent studies on excitation schemes, source efficiency, beam emittance and ion time structure are presented.

RILIS-ionized mercury and tellurium beams at ISOLDE CERN

This paper presents the results of ionization scheme development for application at the ISOLDE Resonance Ionization Laser Ion Source (RILIS). Two new ionization schemes for mercury are presented: a three-step three-resonance ionization scheme, ionizing via an excitation to a Rydberg level and a three-step two-resonance ionization scheme, with a non-resonant final step to the ionization continuum that corresponded to a factor of four higher ionization efficiency. The efficiency of the optimal mercury ionization scheme was measured, together with the efficiency of a new three-step three resonance ionization scheme for tellurium. The efficiencies of the mercury and tellurium ionization schemes…

The CERN/ISOLDE Laser Ion Source

Laser resonance photo-ionization an essential aspect of radioactive ion beam production for fundamental and applied physics research. The laser ion source of the ISOLDE facility, described here, is the most versatile of its type worldwide.

Nuclear spin and magnetic moment of 11Li

Abstract Nuclear spin and magnetic moment of 11Li have been measured by optical pumping of a fast atomic beam. The angular asymmetry of the β-radiation from the polarized nuclei was used to detect the hfs of the 2s 2 S 1 2 −2 p 2 P 1 2 resonance line and the NMR signal cubic LiF crystal lattice. The results I= 3 2 and μI=3.6673(25) n.m. indicate a pure 1p 3 2 state of the valence proton.

New horizons in microparticle forensics: Actinide imaging and detection of 238Pu and 242mAm in hot particles

Description

Hyperfine structure in 5s 4d 3 D ?5snf transitions of87Sr

The hyperfine spectra of the 5s4d3D1-5s20f, 5s4d3D2-5s23f, and 5s 4d3D3-5s32f transitions of87Sr (I=9/2) have been measured by collinear fast beam laser spectroscopy. The structure in the upper configurations is highly perturbed by fine structure splitting that is of comparable size to the hyperfine interaction energy. These perturbations can be adequately treated with conventional matrix diagonalization methods, using the 5s-electron magnetic dipole interaction terma5s and the unperturbed fine structure splittings as input parameters. Additionally, hyperfine constants for the lower 5s4d3D configurations, including theA- andB-factors and a separation of the individuals- andd-electron contri…

Laser assisted decay spectroscopy at the CRIS beam line at ISOLDE

A new collinear resonant ionization spectroscopy (Cris)beam line has recently been installed at Isolde, Cern utilising lasers to combine collinear laser spectroscopy and resonant ionization spectroscopy. The combined technique offers the ability to purify an ion beam that is heavily contaminated with radioactive isobars, including the ground state of an isotope from its isomer, allowing sensitive secondary experiments to be performed. A new programme aiming to use the Cris technique for the separation of nuclear isomeric states for decay spectroscopy will commence in 2011. A decay spectroscopy station, consisting of a rotating wheel implantation system for alpha decay spectroscopy, and thre…

Trace determination of 90Sr and 89Sr in environmental samples by collinear resonance ionization spectroscopy

Collinear resonance ionization spectroscopy has been developed as a sensitive technique for fast trace detection of 90Sr and 89Sr in the environment. A detection limit for 90Sr of 107 atoms in the presence of 1017 atoms in the presence of 1017 atoms of stable Strontium has been achieved, while the applicability of the method has been demonstrated on real world samples. After collection and chemical separation, strontium is surface ionized, accelerated to 33keV and mass separated. The ions are neutralized and the emerging fast atoms interact with an argon ion laser beam (γ=364 nm) in a quasi‐collinear geometry. Optical excitation starts from the long‐lived 5s4d3 D2 state of strontium, which …

3D-Printable Model of a Particle Trap: Development and Use in the Physics Classroom

Quadrupole ion traps are modern and versatile research tools used in mass spectrometers, in atomic frequency and time standards, in trapped ion quantum computing research, and for trapping anti-hydrogen ions at CERN. Despite their educational potential, quadrupole ion traps are seldom introduced into the physics classroom not least because commercial quadrupole ion traps appropriate for classroom use are expensive and difficult to set up. We present an open hardware 3D-printable quadrupole ion trap suitable for the classroom, which is capable of trapping lycopodium spores. We also provide student worksheets developed in an iterative design process, which can guide students while discovering…

Hyperfine structure studies in the 6s 6p3P2-level of barium

The hfs of the3P2 state of the 6s 6p configuration of atomic barium has been determined for137Ba, applying the collinear fast-beam laser spectroscopy. The data fill the last gap in the experimental information on low lying 6s2, 6s 6p, 6s 5d and 6p 5d configurations of this alcaline earth system. The results are analyzed in terms for the existing semi-empirical modified Breit-Wills theory (MBWT), working with two basic wave functions, as well as by an extension to six-component wave functions of inclusion of configuration interaction. The semi-empirical approaches lead to a consistent description of the different hyperfine structures; they are compared with the results from recent ab initio …

Charge radii and electromagnetic moments of At195–211

Hyperfine-structure parameters and isotope shifts of At195-211 have been measured for the first time at CERN-ISOLDE, using the in-source resonance-ionization spectroscopy method. The hyperfine structures of isotopes were recorded using a triad of experimental techniques for monitoring the photo-ion current. The Multi-Reflection Time-of-Flight Mass Spectrometer, in connection with a high-resolution electron multiplier, was used as an ion-counting setup for isotopes that either were affected by strong isobaric contamination or possessed a long half-life; the ISOLDE Faraday cups were used for cases with high-intensity beams; and the Windmill decay station was used for short-lived, predominantl…

Nuclear ground state properties of 99Sr by collinear laser spectroscopy with non-optical detection

Abstract Collinear fast-beam laser spectroscopy, with improved sensitivity for ions with hyperfine split transitions, is performed to measure the hyperfine structure and the isotope shift of the well deformed short-lived 99Sr. The new method consists in ground state depopulation by a two-step optical pumping sequence prior to state selective neutralization and fast-atom counting. A definitive nuclear spin value I = 3 2 , the change in mean square charge radius δ〈r2〉98,99 and the nuclear moments are derived. These results are compared to nuclear spectroscopy information and are interpreted in the frame of the particle plus deformed core model.

Simulation of the relative atomic populations of elements 1 ≤ Z ≤89 following charge exchange tested with collinear resonance ionization spectroscopy of indium

© 2019 The Authors Calculations of the neutralisation cross-section and relative population of atomic states were performed for ions beams (1 ≤ Z ≤ 89) at 5 and 40 keV incident on free sodium and potassium atoms. To test the validity of the calculations, the population distribution of indium ions incident on a vapour of sodium was measured at an intermediate energy of 20 keV. The relative populations of the 5s 2 5p 2 P 1/2 and 5s 2 5p 2 P 3/2 states in indium were measured using collinear resonance ionization spectroscopy and found to be consistent with the calculations. Charge exchange contributions to high-resolution lineshapes were also investigated and found to be reproduced by the calc…

Studies of narrow autoionizing resonances in gadolinium

The autoionization (AI) spectrum of gadolinium between the first and second limits has been investigated by triple-resonance excitation with high-resolution cw lasers. A large number of narrow AI resonances have been observed and assigned total angular momentum J values. The resonances are further divided into members of AI Rydberg series converging to the second limit or other ''interloping'' levels. Fine structure in the Rydberg series has been identified and interpreted in terms of Jc j coupling. A number of detailed studies have been performed on the interloping resonances: These include lifetime determination by lineshape analysis, isotope shifts, hyperfine structure, and photoionizati…

Unexpectedly large charge radii of neutron-rich calcium isotopes

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 theo…

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

Time profiles of ions produced in a hot-cavity resonant ionization laser ion source

Abstract The time profiles of Cu, Sn, and Ni ions extracted from a hot-cavity resonant ionization laser ion source are investigated. The ions are produced in the ion source by three-photon resonant ionization with pulsed Ti:Sapphire lasers. Measurements show that the time spread of these ions generated within laser pulses of about 30 ns duration could be larger than 100 μs when the ions are extracted from the ion source. A one-dimensional ion-transport model using the Monte Carlo method is developed to simulate the time dependence of the ion pulses. The prediction of the model agrees reasonably well with the experimental data. To reproduce the observed ion time profiles, we find it necessar…

A White Paper on keV sterile neutrino Dark Matter

We present a comprehensive review of keV-scale sterile neutrino Dark Matter, collecting views and insights from all disciplines involved - cosmology, astrophysics, nuclear, and particle physics - in each case viewed from both theoretical and experimental/observational perspectives. After reviewing the role of active neutrinos in particle physics, astrophysics, and cosmology, we focus on sterile neutrinos in the context of the Dark Matter puzzle. Here, we first review the physics motivation for sterile neutrino Dark Matter, based on challenges and tensions in purely cold Dark Matter scenarios. We then round out the discussion by critically summarizing all known constraints on sterile neutrin…

A graphene-based neutral particle detector

A neutral particle detector is presented, in which the traditionally used target material, indium tin oxide (ITO), is replaced by graphene. The graphene-based detector enables collinear photodetachment measurements at a significantly shorter wavelength of light down to 230 nm compared to ITO-based detectors, which are limited at 335 nm. Moreover, the background signal from the photoelectric effect is drastically reduced when using graphene. The graphene based detector, reaching 1.7 eV further into the UV energy range, allows increased possibilities for photodetachment studies of negatively charged atoms, molecules, and clusters.A neutral particle detector is presented, in which the traditio…

In-source laser spectroscopy of dysprosium isotopes at the ISOLDE-RILIS

A number of radiogenically produced dysprosium isotopes have been studied by in-source laser spectroscopy at ISOLDE using the Resonance Ionization Laser Ion Source (RILIS). Isotope shifts were measured relative to $^{152}$Dy in the 4 f$^{ 10}$6s$^{2}$ $^5$I$_8$ (gs) $\rightarrow$ 4 f$^{ 10}$6s6p (8,1)$^8_o$ (418.8 nm$_{vac}$) resonance transition. The electronic factor, F, and mass shift factor, M, were extracted and used for determining the changes in mean-squared charge radii for $^{145m}$Dy and $^{147m}$Dy for the first time. A number of radiogenically produced dysprosium isotopes have been studied by in-source laser spectroscopy at ISOLDE using the Resonance Ionization Laser Ion Source (…

The laser ion source trap for highest isobaric selectivity in online exotic isotope production

The improvement in the performance of a conventional laser ion source in the laser ion source and trap (LIST) project is presented, which envisages installation of a repeller electrode and a linear Paul trap/ion guide structure. This approach promises highest isobaric purity and optimum temporal and spatial control of the radioactive ion beam produced at an online isotope separator facility. The functionality of the LIST was explored at the offline test separators of University of Mainz (UMz) and ISOLDE/CERN, using the UMz solid state laser system. Ionization efficiency and selectivity as well as time structure and transversal emittance of the produced ion beam was determined. Next step aft…

First application of the Laser Ion Source and Trap (LIST) for on-line experiments at ISOLDE

The Laser Ion Source and Trap (LIST) provides a new mode of operation for the resonance ionization laser ion source (RILIS) at ISOLDE/CERN, reducing the amount of surface-ionized isobaric contaminants by up to four orders of magnitude. After the first successful on-line test at ISOLDE in 2011 the LIST was further improved in terms of efficiency, selectivity, and reliability through several off-line tests at Mainz University and at ISOLDE. In September 2012, the first on-line physics experiments to use the LIST took place at ISOLDE. The measurements of the improved LIST indicate more than a twofold increase in efficiency compared to the LIST of the 2011 run. The suppression of surface-ionize…

Intracavity Frequency Doubling and Difference Frequency Mixing for Pulsed ns Ti:Sapphire Laser Systems at On-Line Radioactive Ion Beam Facilities

Intra-cavity second harmonic generation of a Titanium:sapphire (Ti:sa) laser system has been used to improve the conversion efficiency to the second harmonic. Over the course of several experiments performance data spanning the whole wavelength range of a Ti:sa has been collected, which may be used as a guideline for future experiments. An average output power of up to 3.7 W was achieved, resulting in a conversion efficiency of >75 % to the second harmonic. A wavelength coverage from 340-525 nm has been demonstrated. To extend the wavelength range of the solid state laser system, difference frequency mixing has been applied to the intra-cavity doubled light and the fundamental output of a s…

Characterization of the shape-staggering effect in mercury nuclei

In rare cases, the removal of a single proton (Z) or neutron (N) from an atomic nucleus leads to a dramatic shape change. These instances are crucial for understanding the components of the nuclear interactions that drive deformation. The mercury isotopes (Z = 80) are a striking example1,2: their close neighbours, the lead isotopes (Z = 82), are spherical and steadily shrink with decreasing N. The even-mass (A = N + Z) mercury isotopes follow this trend. The odd-mass mercury isotopes 181,183,185Hg, however, exhibit noticeably larger charge radii. Due to the experimental difficulties of probing extremely neutron-deficient systems, and the computational complexity of modelling such heavy nucl…

A new resonant Laser-SNMS system for environmental ultra-trace analysis: Installation and optimization

Abstract Localization, analysis and mobility of radioactive contaminated particles is of major concern for assessment of contamination threads and nuclear forensics. For this purpose, a new resonant Laser-SNMS system was developed and set up at the Institute for Radioecology and Radiation Protection for spatially resolved ultra-trace analysis of low concentrated radionuclides directly on environmental samples. This paper describes the adaption and combination of a dedicated Ti:sapphire laser system with a commercial TOF-SIMS instrument for resonant Laser-SNMS. The project includes computer simulations for optimization of the TOF analyzer. Results on synthetic uranium and technetium samples …

Direct high-precision mass measurements onAm241,243,Pu244, andCf249

The absolute masses of four long-lived transuranium nuclides, $^{241,243}\mathrm{Am}$, $^{244}\mathrm{Pu}$, $^{244}\mathrm{Pu}$, and $^{249}\mathrm{Cf}$, in the vicinity of the deformed $N=152$ neutron shell closure have been measured directly with the Penning-trap mass spectrometer TRIGA-TRAP. Our measurements confirm the AME2012 mass values of $^{241,243}\mathrm{Am}$ and $^{244}\mathrm{Pu}$ within one standard deviation, which were indirectly determined, by decay spectroscopy studies. In the case of the $^{249}\mathrm{Cf}$ mass, a discrepancy of more than three standard deviations has been observed, affecting absolute masses even in the superheavy element region. The implementation of the…

Recent developments in and applications of resonance ionization mass spectrometry

Resonance Ionization Mass Spectrometry (RIMS) has nowadays reached the status of a routine method for sensitive and selective ultratrace determination of long-lived radioactive isotopes in environmental, biomedical and technical samples. It provides high isobaric suppression, high to ultra-high isotopic selectivity and good overall efficiency. Experimental detection limits are as low as 106 atoms per sample and permit the fast and sensitive determination of ultratrace amounts of radiotoxic contaminations. Experimental arrangements for the detection of different radiotoxic isotopes, e.g. 236–244Pu, 89,90Sr and 99Tc in environmental samples are described, and the application of RIMS to the ul…

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…

Hyperfine structure and isotope shift investigations in $^{202-222}$Rn for the study of nuclear structure beyond Z = 82

The hyperfine structure (hfs) and isotope shift (IS) in the isotopic chain of the radioactive element radon have been studied for the first time. The measurements were carried out by collinear fast-beam laser spectroscopy at the mass separator facility ISOLDE at CERN. The IS between 16 isotopes in the mass range 202≦A≦222 and the hfs of 7 odd-A isotopes were determined in the transitions 7s [3/2]2-7p [5/2]3 (745 nm) of Rn I. The nuclear spins and moments, as well as the observed inversion of the odd-even staggering for218–222Rn, can be associated with the effects of octupole instability around N=134.

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.

Multi-color resonance ionization of laser ablated gadolinium at high laser power

Abstract Spectroscopic and analytical properties of a trace analytical method using multi-step resonance ionization at high laser intensities (>kW/cm 2 ) have been investigated with gadolinium as a test element. Strongly saturated transitions are observed, which have been used for a temperature determination of the atoms in the laser ablated plume. Regimes of multi-step resonance ionization and multiphoton ionization could be distinguished. Analytical performances due to resonance enhancement and resulting discrimination against non-resonant background, precision in isotope ratio determination and overall detection efficiency 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 …

Measurement of the laser resonance ionization efficiency for lutetium

Abstract The development of a highly efficient resonance ionization scheme for lutetium is presented. A laser ion source, based on the all-solid-state Titanium:sapphire laser system, was used at the 30 keV RISIKO off-line mass separator to characterize different possible optical excitation schemes in respect to their ionization efficiency. The developed laser resonance ionization scheme can be directly applied to the use at radioactive ion beam facilities, e. g. at the CERN-MEDICIS facility, for large-scale production of medical radioisotopes.

A laser desorption/resonance enhanced photoionisation TOF-system for the spatially resolved trace analysis of elements

Abstract A novel method for direct and spatially resolved elemental trace analysis with high sensitivity and elemental selectivity is presented. The concept is based on the combination of a commercial MALDI-TOF mass spectrometer with a pulsed laser system for resonant postionisation of neutrals. While the MALDI method is usually applied for investigations of large organic compounds and biomolecules, the technique discussed here concerns the low mass range around 1 ⩽ A ⩽ 300. The analytical performances of the setup with respect to mass analysis, spatial resolution and overall detection efficiency are discussed.