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…

Die experimentelle Bestimmung der Ionisationsenergien von Berkelium und Californium

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 …

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…

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…

Frequency tripling for resonance ionization spectroscopy (RIS) of Cd

To explore the nucleosynthesis of heavy elements in the rapid neutron-capture process, investigations on short- lived, very neutron-rich Cd isotopes are planned that require pure samples. These will be produced at the CERN-ISOLDE on-line mass separator in combination with a chemically se- lective laser ion source. The excitation scheme for resonance ionization of Cd was tested in Mainz with a copper-vapor- pumped dye laser system. Due to the high ionization potential of Cd, frequency tripling was required for the first excita- tion step.1D 228: 8n m/. Laser light with an average power of 2m Wwas obtained after frequency tripling and was suc- cessfully used for RIS test measurements on cadmi…

Efficient three-step, two-color ionization of plutonium using a resonance enhanced 2-photon transition into an autoionizing state

Resonance ionization mass spectrometry (RIMS) has proven to be a powerful method for isotope selective ultra-trace analysis of long-lived radioisotopes. For plutonium detection limits of $\rm 10^{6}$ to $\rm 10^{7}$ atoms have been achieved for various types of samples. So far a three-step, three-color laser excitation scheme was applied for efficient ionization. In this work, a two-photon transition from an excited state into a high-lying autoionizing state, will be presented, yielding a similar overall efficiency as the three-step, three-color ionization scheme. In this way, only two tunable lasers are needed, while the advantages of a three-step, three-color excitation (high selectivity,…

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…

Isotope shift and hyperfine structure of stable platinum isotopes

Isotope shift (IS) and hyperfine structure (hfs) measurements have been performed on seven lines of the platinum I spectrum with interference as well as laser fluorescence spectroscopy. In the latter case a frequency-doubled single-mode cw dye laser was applied. The IS of190Pt with a natural abundance of only 0.01% was determined to beδν 190, 192=−38.65(8) mK in theλ306.47 nm transition. The IS parameters and the effective hfs integrals in the configuration (5d+6s)10 were determined in intermediate coupling by a least squares fit of the IS and hfs data with eigenvectors obtained from the platinum fine structure (fs). The results are compared with theoretical values and yield improvedδ〈r 2〉 …

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…

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.

First Observation of Atomic Levels for the Element Fermium (Z=100)

The atomic level structure of the element fermium was investigated for the first time using a sample of $2.7\ifmmode\times\else\texttimes\fi{}{10}^{10}$ atoms of the isotope $^{255}\mathrm{F}\mathrm{m}$ with a half-life of 20.1 h. The atoms were evaporated from a filament and stored in the argon buffer gas of an optical cell. Atomic levels were sought by the method of resonance ionization spectroscopy using an excimer-dye-laser combination. Two atomic levels were found at wave numbers $(25\text{ }099.8\ifmmode\pm\else\textpm\fi{}0.2)$ and $(25\text{ }111.8\ifmmode\pm\else\textpm\fi{}0.2)\text{ }\text{ }{\mathrm{c}\mathrm{m}}^{\ensuremath{-}1}$. Partial transition rates to the $5{f}^{12}7{s}…

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…

Fast, low-level detection of strontium-90 and strontium-89 in environmental samples by collinear resonance ionization spectroscopy

Environmental assessment in the wake of a nuclear accident requires the rapid determination of the radiotoxic isotopes 89Sr and 90Sr. Useful measurements must be able to detect 108 atoms in the presence of about 1018 atoms of the stable, naturally occurring isotopes. This paper describes a new approach to this problem using resonance ionization spectroscopy in collinear geometry, combined with classical mass separation. After collection and chemical separation, the strontium from a sample is surface-ionized and the ions are accelerated to an energy of about 30 keV. Initially, a magnetic mass separator provides an isotopic selectivity of about 106. The ions are then neutralized by charge exc…

First Experimental Determination of the Ionization Potentials of Berkelium and Californium

First Determination of the Ionization Potential of Actinium and First Observation of Optical Transitions in Ferminm

For the determination of the first ionization potential of actinium, 227Ac was electrodeposited on a Ta backing and covered with ~1 μm Zr. From this filament, Ac atoms were evaporated at ≥ 1250 °C. By resonant excitation with UV light of 388.67 nm and subsequent excitation with light of ca. 568 nm, Ac was ionized in an external electrical field. By determining the ionization thresholds as a function of the electrical field strength and by extrapolation to zero field strength, the first ionization potential of 43398(3) cm−1 = 5.3807(3) eV was measured.About 1 ng of 255Fm, half life 20.1 h, was prepared at ORNL by milking from 255Es produced in the High Flux Isotope Reactor and shipped to Mai…

Resonance ionization spectroscopy of fermium (Z=100)

Laser spectroscopy has been applied for the first time to measure resonant transition frequencies of fermium (Zs 100). A number of 2.7=10 atoms was electrodeposited on a Ta filament and covered with a 1 mm Ti layer. Fm 10

Erste Messung der Ionisationsenergie von Americium und Curium

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…

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.

Trace analysis of plutonium in environmental samples by resonance ionization mass spectroscopy (RIMS)

Resonance ionization mass spectroscopy (RIMS) is well suited for trace analysis of long-lived radioisotopes in environmental, biological and technical samples. By multiple resonant laser excitation and ionization of the elemental atoms under investigation, an extremely high element selectivity can be achieved. In addition, isotope selectivity is obtained by subsequent mass analysis. The excellent sensitivity results from the large atomic cross-sections in the excitation–ionization process and the good detection efficiency for ions. The element selectivity of RIMS allows a simplified procedure for the chemical preparation of the samples compared to the requirements of thin sources for α-spec…

Resonance ionization mass spectroscopy for trace determination of plutonium in environmental samples

Resonance ionization mass spectroscopy (RIMS) is a sensitive and isotope selective method and well suited for trace analysis of plutonium in the environment. After the chemical isolation of plutonium from soil, air filters or urine, e.g., it is electrolytically deposited as hydroxide on a tantalum backing and covered with a thin titanium layer. By heating such a sandwich filament in the RIMS-apparatus under vacuum an atomic beam of plutonium is produced. The atoms are ionized by a three-step resonant excitation using pulsed dye lasers, and the ions are mass-selectively detected with a time-of-flight (TOF) spectrometer and a multi channel plate detector. RIMS yields a low detection limit of …

Isotope selective ultratrace analysis of plutonium by resonance ionisation mass spectrometry

Abstract Resonance ionisation mass spectrometry (RIMS) is a sensitive and selective method for isotopically resolved ultratrace analysis of long-lived radionuclides. For the routine analysis of plutonium three titanium–sapphire lasers pumped by a pulsed Nd:YAG laser in combination with a time-of-flight mass spectrometer are used. The detection limit of this system is as low as 106–107 atoms for the plutonium isotopes 238Pu to 244Pu. The RIMS technique was applied to investigate the isotopic composition and the content of plutonium in a depleted uranium penetrator as used during the Balkan conflict delivering important information on the origin of the depleted uranium in this type of ammunit…

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.

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…

Ground-state properties of neutron-deficient platinum isotopes

The hyperfine structure splitting and the isotope shift in the λ=266 nm transition of Pt isotopes within the mass range 183 ≦A≦ 198 have been determined by Resonance Ionization Mass Spectroscopy (RIMS) in combination with Pulsed-Laser Induced Desorption (PLID). The Pt isotopes were obtained at the on-line isotope separator ISOLDE-3/CERN as daugthers of the primarily produced Hg isotopes. Magnetic moments, quadrupole moments, and changes in the mean-square charge radii are deduced and compared with results of a particle-triaxial rotor model and mean field calculations. Good agreement with experimental data (including nuclear level schemes and transition probabilities) can only be obtained if…

Beta decay of the new isotope101Sn

The very neutron-deficient isotope 101Sn was produced in a 50Cr(58Ni, 2p5n) reaction and its decay properties were determined for the first time. By using chemically selective ion sources of an on-line mass separator, the energy spectrum and the half-life (3 ± 1 s) of beta-delayed protons of 101Sn were measured. These results are compared to theoretical predictions.

First Determination of the Ionization Potential of Americium and Curium

The charge radii of $^{198}$Pt - $^{183}$Pt

The changes of the mean-square charge radii have been measured for198Pt-183Pt by means of resonance ionization mass spectroscopy (RIMS) at the new on-line isotope separator ISOLDE-3/CERN. As in the case of the neighbouring isotopes of Au and Hg, a strong nuclear deformation of ¦β2¦ −-0.24 is reached at the neutron mid-shell nucleus183Pt, but no indication for a sharp shape transition is observed from the study of the isotope shifts.

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 …

Determination of the first ionization potential of einsteinium by resonance ionization mass spectroscopy (RIMS)

Abstract The first ionization potential of einsteinium (IP Es ) was determined by resonance ionization mass spectroscopy (RIMS) using samples with ≤10 12 atoms of 254 Es ( T 1/2 =276 days). This method is based on the measurement of photoionization thresholds as a function of applied electric field strength, followed by extrapolation to zero field strength to yield IP Es . An atomic beam of Es was created by heating a filament on which einsteinium was electrodeposited from an aqueous solution onto a tantalum backing and covered with titanium metal. Es atoms were ionized via a three-step excitation scheme, and the ions mass-selectively detected in a time-of-flight (TOF) mass spectrometer. Th…

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…

Observation of strongly deformed ground-state configurations in $^{184}$Au and $^{183}$Au by laser spectroscopy

Resonance ionization mass spectroscopy (RIMS) and pulsed-laser induced desorption (PLID) have been combined in order to study the isotope shift (IS) and hyperfine structure (HFS) of184Au (T1/2=53 s) and183Au (T1/2=42 s) in the 6s2S1/2 → 6p2P1/2 (λ=267 nm) transition. The Au isotopes were obtained as daughters in the decay of184,183Hg produced and mass separated at the new ISOLDE-3 facility at CERN. It was found that the strong deformationβ2}-0.25 setting in at186Au persists down to183Au.

Determination of the first ionization potential of nine actinide elements by resonance ionization mass spectroscopy (RIMS)

The high sensitivity of RIMS enables the precise determination of the first ionization potential of actinide elements with a sample size of ≤1012 atoms. By multiple resonant laser excitation, the actinide atoms under investigation are ionized in the presence of an electric field, and the ions are mass-selectively detected in a time-of-flight spectrometer. The first ionization potential is obtained by scanning the wavelength of the laser used for the last excitation step across the ionization threshold Wth—indicated by a sudden increase of the ion count rate—at various electric field strengths. Extrapolation of Wth to electric field strength zero leads directly to the first ionization potent…

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.

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.