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

Chemical studies of Fl (element 114): Heaviest chemically studied element

Spectroscopic Tools Applied to Flerovium Decay Chains

Abstract An upgraded TASISpec setup, with the addition of a veto DSSD and the new Compex detector-germanium array, has been employed with the gas-filled recoil separator TASCA at the GSI Helmholtzzentrum für Schwerionenforschung Darmstadt, to study flerovium (element 114) decay chains. The detector upgrades along with development of new analytical techniques have improved the sensitivity of the TASISpec setup for measuring α-photon coincidences. These improvements have been assessed with test reactions. The reaction 48Ca+206,207Pb was used for verification of experimental parameters such as transmission to implantation DSSD and target-segment to α-decay correlations. The reaction 48Ca+ nat …

Direct detection of the 229Th nuclear clock transition

Today’s most precise time and frequency measurements are performed with optical atomic clocks. However, it has been proposed that they could potentially be outperformed by a nuclear clock, which employs a nuclear transition instead of an atomic shell transition. There is only one known nuclear state that could serve as a nuclear clock using currently available technology, namely, the isomeric first excited state of 229Th (denoted 229mTh). Here we report the direct detection of this nuclear state, which is further confirmation of the existence of the isomer and lays the foundation for precise studies of its decay parameters. On the basis of this direct detection, the isomeric energy is const…

Sensitive laser spectroscopy on trapped barium ions by quenching with hydrogen

The sensitivity of laser spectroscopy on barium ions stored in a radio frequency quadrupole trap was drastically increased by using hydrogen for quenching the optically pumped metastable states. The attained fluorescence intensity per ion permits the detection of single ions. The method will be applied to environmental studies on actinides.

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…

Nuclear Forensics: A methodology applicable to Nuclear Security and to Non-Proliferation

Nuclear Security aims at the prevention and detection of and response to, theft, sabotage, unauthorized access, illegal transfer or other malicious acts involving nuclear material". Nuclear Forensics is a key element of nuclear security. Nuclear Forensics is defined as a methodology that aims at re-establishing the history of nuclear material of unknown origin. It is based on indicators that arise from known relationships between material characteristics and process history. Thus, nuclear forensics analysis includes the characterization of the material and correlation with production history. To this end, we can make use of parameters such as the isotopic composition of the nuclear material…

Trennung von Spaltprodukten durch Extraktionschromatographie

The possibilities for the separation of a complex fission product mixture by extraction chromatography have been investigated. Here the partition coefficients between three solvents and hydrochloric acid are reported for the following elements: Zn(II), Ge(IV), As(III), As(V), Se(IV), Zr(IV), Nb(V), Mo(VI), Tc(IV) Ru(III), Ru(IV), Rh(III), Ag(I), Cd(II), In(III), Sn(IV), Sb(III), Sb(V), Te(IV), I(oxidized), Cs(I), Ce(III), Tb(III), Tm(III), Ac(III), Th(IV), Pa(V), U(VI), Np(IV), Np(VI). As solvents tri-n-butylphosphate (TBP), tri-n-octylamine (TOA) and di-(2-ethylhexyl)-orthophosphoric acid (HDEHP) have been used. The partition coefficients have been measured by batch-experiments in which th…

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.

A compact apparatus for mass selective resonance ionization spectroscopy in a buffer gas cell

Abstract An ultra-sensitive laser spectroscopic method for the investigation of transuranium nuclides has been developed based on resonance ionization in an argon buffer gas cell. This method has been combined with ion-guide extraction and mass selective direct detection of the resonantly ionized atoms. Using argon as a buffer gas, recoils of fusion reactions can be thermalized even at low pressure. The differential pumping system consists of only one roots pump and two turbo molecular pumps. The set-up has been tested with 243 Am evaporated from a filament located inside the optical gas cell. Resonance ionization is performed using a two-step excitation with an excimer-dye-laser combinatio…

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…

Alpha-Photon Coincidence Spectroscopy Along Element 115 Decay Chains

Produced in the reaction 48Ca+243Am, thirty correlated α-decay chains were observed in an experiment conducted at the GSI Helmholzzentrum fur Schwerionenforschung, Darmstadt, Germany. The decay chains are basically consistent with previous findings and are considered to originate from isotopes of element 115 with mass numbers 287, 288, and 289. A set-up aiming specifically for high-resolution charged particle and photon coincidence spectroscopy was placed behind the gas-filled separator TASCA. For the first time, γ rays as well as X-ray candidates were observed in prompt coincidence with the α-decay chains of element 115.

HIGH SPIN STATES OF 232Th, 234U AND 236U+

Phosphonomethyl-substituted phenols are readily obtained from o-hydroxymethylated phenols and trialkyl phosphites. The free acids, incorporated into phenol-formaldehyde resins, act as cation exchangers with remarkable selectivity for different metal ions.

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,…

First Aqueous Chemistry with Seaborgium (Element 106)

Verfl�chtigung von Spaltprodukten aus festem Uran(IV)-fluorid und anderen Fluoriden

In der Kernehemie sueht man nach temperaturund strahlenresistenten Targetsystemen, aus denen naeh Kernreaktionen kurzlebige Nuklide kontinu: ierlich abgetrennt werden kSnne n. Dies ist insbesondere im Hinblick auf die yon der Gesellschaft fiir Sehwerionenforsehung in Darmstadt geplanten Experimente interessan~, bei denen die Synthese neuer, iibersehwerer Elemente versucht wird. Als Modell fiir Verdampfungsstudien aus festen Targets wurde die tr~gerfreie Verfliichtigung yon Spaltprodukten aus festem Uran(IV)-fluorid gew~hlt [1--3]. Im fliiehtigen Anteil konnten folgende Elemente identifiziert werden: Se, Kr, Zr, Iqb, Me, Te, Ru, Sn, Sb, Te, J und Xe. In einem Rohr mit Temperaturgradienten l~…

The Study of Prompt and Delayed Muon Induced Fission; II. Mean life times of negative muons bound to 237Np, 242Pu and 244Pu

The mean life times of negative muons bound to actinide nuclei have been measured by detecting the time difference between a stopped muon and the arrival of fragments from delayed fission after muon capture. The deduced capture rates c are 1.392(4)·107/s for237Np, 1.290(7)·107/s for242Pu and 1.240(7)·107/s for244Pu. The results are compared with published data for the fission and the neutron decay channels and for the electron decay of the bound muon. Including a former measurement of c for239Pu, an isotopic dependence of the muon capture rates in the Pu isotopes is clearly observed.

Recoil-α-fission and recoil-α–α-fission events observed in the reaction 48Ca + 243Am

Products of the fusion-evaporation reaction 48Ca + 243Am were studied with the TASISpec set-up at the gas-filled separator TASCA at the GSI Helmholtzzentrum für Schwerionenforschung, Darmstadt, Germany. Amongst the detected thirty correlated α-decay chains associated with the production of element Z=115, two recoil-α-fission and five recoil-α-α-fission events were observed. The latter five chains are similar to four such events reported from experiments performed at the Dubna gas-filled separator, and three such events reported from an experiment at the Berkeley gas-filled separator. The four chains observed at the Dubna gas-filled separator were assigned to start from the 2n-evaporation ch…

First ionization potential of the heaviest actinide lawrencium, element 103

The first ionization potential (IP1 ) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP 1 value is 4.9630.08 0.07 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s 2 5f 14 7p 1 1/2 , which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens t…

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…

Determination of the content in uranium oxide particles by fission track analysis

Abstract One of the most important tasks of nuclear safeguards is to control the activities in nuclear facilities worldwide. These activities include the enrichment of 235 U . To identify enrichments above the maximum authorised level in commercial enrichment plants (usually 5% 235 U ) swipe tests are performed and the 235 U enrichment is determined in the sampled uranium oxide particles. A method is described that allows to measure the 235 U content in small particles (around 1 μm in diameter) by the use of fission tracks. It is based on the fact that in uranium fuel, only 235 U atoms are fissile with thermal neutrons and contribute to the amount of fission tracks counted for individual pa…

Laser resonant ionization of plutonium

Resonance ionization mass spectrometry (RIMS) has been tested for the isotope-selective determination of trace amounts of plutonium. An atomic beam is formed by evaporating plutonium atoms from a rhenium-filament heated to 1800 °C. The radiation of a pulsed dye laser excites the atoms in a two-photon process (λ=595.2 nm) followed by photoionization of the excited atoms. Mass selectivity is obtained by use of a time-of-flight spectrometer. A resonant signal of239Pu was measured with 1013 atoms deposited on the filament.

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.

Evidence for Shape Coexistence in Neutron-Rich Rh and Ag Nuclei

Neutron-rich nuclei of Rh and Ag have been investigated by γ-ray spectroscopic measurements as well as single-particle transfer reactions like (d,3He) and (3He,d). The obtained level schemes of 105,107,109,111Rh and 113,115Ag show two different types of excitation: (I) proton-hole states related to a spherical shape of the nucleus and (II) proton-particle states with a rotational band-like structure (intruder band) pointing towards deformation of the nucleus. The “fingerprints” for such a shape coexistence and resulting systematics in these nuclei and the possible interpretation of the intruder band as a rotational band built upon the 1/2+[431] Nilsson configuration are discussed.

Search for Superheavy Elements in theU238+U238Reaction

A search was made for spontaneously fissioning superheavy elements in damped collisions of two uranium nuclei. Different techniques were applied covering the elements 108 to 118 and approx. =126, and a half-life range from 1 ms to more than 1 yr. No evidence for superheavy elements was found at upper cross-section limits of 10/sup -32/, 10/sup -33/, and 10/sup -35/ cm/sup 2/ for half-lives from 1 to 100 ms, 100 ms to 1 d, and 1 d to 1 yr, respectively.

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}…

Radiation detected resonance ionization spectroscopy on208Tl and242fAm

An ultra-sensitive laser spectroscopic method has been developed for the hyperfine spectroscopy of short-lived isotopes far off stability produced by heavy ion induced nuclear reactions at very weak intensity (> 1/s). It is based on resonance ionization spectroscopy in a buffer gas cell with radiation detection of the ionization process (RADRIS). As a first on-line application of RADRIS optical spectroscopy at242fAm fission isomers is in progress at the low target production rate of 10/s. The resonance ionization has been performed in two steps utilizing an excimer dye laser combination with a repetition rate of 300 Hz. The first resonant step proceeds through terms which correspond to wave…

Systematic evidence for quasifission in Be9−, C12−, and O16 -induced reactions forming No258,260

Isotope Distributions in the Reaction ofU238withU238

Radiochemically determined cross sections $\ensuremath{\sigma}(Z, A)$ were used to construct charge and mass distributions for the reaction of 1785-MeV $^{238}\mathrm{U}$ ions with thick $^{238}\mathrm{U}$ targets. Fission of the colliding nuclei is found to dominate. For the surviving uraniumlike fragments an enhancement of yields compared to the Kr + U and Xe + U reactions is observed. The formation of heavy actinides is shown to be associated with the low-energy tails of the broad excitation energy distributions in damped collisions.

Miss Piggy, a californium-252 fission fragment source as a generator of short-lived radionuclides

Abstract Carrier-free short-lived nuclides are employed in many different fields of modern nuclear chemistry. The two main production strategies are either thermal neutron-induced fission of 235U or 239Pu at nuclear reactors or spallation neutron sources or charged particle-induced nuclear reactions at accelerator facilities. An alternative method is to use a spontaneously fissioning nuclide. A facility applying this technique (“Miss Piggy”) was built at the University of Berne (Switzerland). Californium-252 (252Cf), which has a 3% fission branch and a half-life of 2.645 a, is used for the production of short-lived fission products that are stopped in an adjacent recoil chamber. Short-lived…

Precise energies of gamma rays from the 230Th and 228Th decay

Abstract Energies up to 300 keV of prominent gamma rays from the decay of 230 Th, 228 Th and some of the 228 Th descendants have been precisely measured by use of Ge(Li) detectors.

Evidence for intruder states in111Rh

Levels in111Rh have been investigated via the γ -rays following the β−-decay of 2.1 s111Ru. The Ru activity was produced in the fission of249Cf and separated chemically from the fission product mixture. The emitted γ-rays were studied by γ singles and γ(t) coincidence measurements. Evidence for intruder states in111Rh has been obtained. Their properties are discussed and compared with those in the lighter Rh isotopes.

Low-lying states in Ra219 and Rn215 : Sampling microsecond α -decaying nuclei

Short-lived α-decaying nuclei "northeast" of 208Pb in the chart of nuclides were studied using the reaction 48Ca+243Am with the decay station TASISpec at TASCA, GSI Darmstadt. Decay energies and times from pile-up events were extracted with a tailor-made pulse-shape analysis routine and specific α-decay chains were identified in a correlation analysis. Decay chains starting with the even-even 220Ra and its odd-A neighbors, 219Fr, and 219,221Ra, with a focus on the 219Ra→215Rn decay, were studied by means of α-γ spectroscopy. A revised α-decay scheme of 219Ra is proposed, including a new decay branch from a previously not considered isomeric state at 17 keV excitation energy. Conclusions on …

Application of Resonance Ionization Mass Spectrometry for Ultratrace Analysis of Technetium

This work shows the ability of resonance ionization mass spectrometry (RIMS) to determine 99gTc at the ultratrace level. The characterization of the prepared samples by X-ray photoelectron spectroscopy (XPS) and optimization of the RIMS setup for this purpose, as well as the application of the RIMS method to a soil sample, are presented in this article. 97Tc was used as a tracer isotope to determine the amount of 99gTc in a soil sample with RIMS. With 8.8 × 1010 atoms of 97Tc as the tracer, the concentration of 99gTc was found to be 1.5 × 109 atoms per gram of dried sample material, demonstrating the sensitivity of the method. Furthermore, it could be shown that the 97Tc solution contained …

Trace detection of plutonium by three-step photoionization with a laser system pumped by a copper vapor laser

Laser photoionization has been used to detect trace amounts of plutonium. A high sensitivity and selectivity has been achieved by applying three-step excitation and ionization of the plutonium atoms with high pulse-repetition rates and additional mass determination by time-of-flight measurements. A laser system was developed which consists of a copper vapor laser pumping three dye lasers simultaneously. Samples containing between 1010 and 1012 atoms of239Pu on Re filaments were measured yielding strong resonance signals with maximum ion count rates of several kHz at a vanishingly low background. A detection efficiency of 10−7 was determined allowing the detection of about 108 plutonium atom…

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…

Nuclear reactions in collisions of very heavy ions at energies below and near the barrier

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…

Cross sections for nuclear reactions in collisions of238U+238U and238U +197Au near and below the coulomb barrier

Cross sections for nuclear reactions at beam energies near and below the spherical Coulomb barrier V c were measured in the very heavy collision systems238U +238U and238U +197Au. The most probable reaction channel with mass transfer is the one-neutron transfer. Its excitation function is understood in terms of Rutherford trajectories together with the quantal process of neutron tunnelling over large distances. In addition, the exchange of up to 15 nucleons is observed down to 0.90 V c . The excitation functions for the multi-nucleon transfer products have much steeper slopes than that for one-neutron transfer, and are steeper for238U +197Au than for238U +238U, suggesting that nuclear contac…

An improved system for fast, continuous chemical separations (“SISAK 2”) in nuclear spectroscopic studies

Abstract An improved rapid, continuous solvent extraction system (“SISAK 2”) is described. The system is connected to a gas-jet installed at the Mainz reactor. It allows single or multistage chemical separations of liquid phases by means of specially designed centrifuges within ∼1 s per stage. The application of this system to study short-lived nuclides is exemplified for neutron-rich lanthanum and cerium isotopes produced by fission.

Odd neutron nuclei near A=100: Rotational bands in103Mo and105Mo populated in the? ? decays of103Nb and105Nb

Theβ − decays of103Nb and105Nb have been studied at the fission product separators JOSEF and LOHENGRIN. Half-lives of (1.5±0.2) s and (2.95±0.06) s, respectively, have been determined for these decays. Fromγ singles andγ-γ coincidence measurements extended level schemes for103Mo and105Mo have been established for the first time. The lowest energy levels of these nuclei are consistent with the interpretation as members of rotational bands built on a 3/2+ [411] Nilsson state. Evidence is presented for the location of the 9/2+ [404] configuration.

A high-temperature laser ion source for trace analysis and other applications

We report here on the development of a high-temperature laser ion source useful for trace analysis and other applications. It consists of a high temperature ionization chamber, three tunable dye lasers pumped by copper vapor lasers for stepwise resonant ionization and a Mattauch-Herzog mass spectrometer for the analysis of photo-ions. The principle of the laser ion source and its theoretical efficiency are discussed, where the efficiency of a laser ion source is the ratio of photo-ions extracted out to the number of atoms introduced into the cavity. Experimentally, an efficiency of 2×10−3 has been achieved for technetium. The scheme of gated detection is described which is used for suppress…

The decay of 8.7 min237Pa

The beta and gamma radiations of237Pa have been investigated employing semiconductor and scintillation spectrometers and coincidence techniques. Sources of237Pa were obtained after bombardments of238U with bremsstrahlung and 14-MeV neutrons and subsequent chemical separation. From the total of 18γ-rays following the decay of 8.7±0.2 min237Pa 17 transitions, representing 99.9% of theγ-ray intensity, could be placed in a level scheme of237U. AQ β- value of 2.25±0.1 MeV has been determined.

Resonance ionization mass spectroscopy for trace analysis of neptunium

Resonance ionization mass spectroscopic (RIMS) measurements for trace analysis and spectroscopy of 237Np, the ecologically most important isotope of neptunium, are described. The chemical procedure for the separation of neptunium from aqueous samples as well as the preparation of filaments for RIMS are outlined. Several two- and three-step excitation schemes have been investigated in order to find suitable conditions for the sensitive detection of 237Np. Using a three-step, three-color excitation and ionization scheme an overall detection efficiency of 3×10−8 was obtained, resulting in a detection limit of 4×108 atoms (160 fg) of 237Np. The hyperfine structure splittings of the levels under…

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…

Search for superheavy elements in monazites using chemical enrichment

Evidence for the existence of superheavy elements in monazite inclusions embedded in Madagascan mica and surrounded by giant radioactive haloes was given by Gentry et al.1 who observed photons with energies corresponding to predicted Lα1 X-ray energies of element 126 (at 27.25 keV) and also of elements 116, 124 and 127 in irradiations of such crystals with collimated proton beams. For an unambiguous identification, the detection of further members of the L X-ray series would be most important. In X-ray spectra of monazite samples these transitions are buried under the strong K X-ray peaks of the lanthanide elements. They should, however, become visible after chemical enrichment of the super…

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

New nuclides: Neptunium-243 and neptunium-244

We have observedγ-rays following the β−-decay of243Np and244Np after chemical isolation of neptunium isotopes from the products of the reaction of 835 MeV136Xe with244Pu. The ground-state of 1.85-min243Np hasJ=5/2. The decay of 2.29-min244Np (probableJπ=7−) populates high-spin members of the ground state rotational band in244Pu.

Beta-decay of148,150,152Pr into levels of148,150,152Nd

Theβ−-decay of148,150,152Pr into levels of148,150,152Nd has been studied byγ-singles,γγ-coincidence and for148Pr also byγγ-angular correlation measurements. The praseodymium activities have been obtained by thermal neutron-induced fission of235U followed by on-line mass separation with the helium-jet coupled mass separator HELIOS. Decay schemes for these heaviest praseodymium nuclides are proposed. From the angular correlation measurements spin values for the seven lowest levels of148Nd are deduced. Spin and parity assignments for the lower levels in150,152Nd have been extrapolated from level systematics.

Speciation and interactions of plutonium with humic substances and kaolinite in aquifer systems

Abstract The speciation of plutonium (Pu) in contact with humic substances (HS) and kaolinite has been performed in aquifer systems. Mainly the redox behavior, complexation, and sorption of plutonium are discussed here. The redox behavior of Pu(VI) in contact with HS was studied and it was found that Pu(VI) is reduced to Pu(III) and Pu(IV) within a couple of weeks. The complexation constants (log  β LC ) of Pu(III) and Pu(IV) with HS have been determined by means of the ultrafiltration method. Furthermore, the sorption of Pu(III) and Pu(IV) onto kaolinite has been investigated as a function of pH by batch experiments under aerobic and anaerobic conditions.

Actinide Production in Collisions ofU238withCm248

Cross sections for the production of heavy actinides in damped collisions of $^{238}\mathrm{U}$ ions with $^{248}\mathrm{Cm}$ targets are reported and compared with similar data for other projectiles. The relatively small differences in the formation rates of a given isotope made by different projectiles indicate a balance between increased mass transfer probability with increasing projectile mass and a concurrent decrease in survivability because of an increase in excitation energy.

Search for supermassive nuclei in nature

We report on a search for supermassive nuclei in nature with masses up to 107 amu. Such exotic nuclei might consist, for example, of stable strange matter, which comprises a mixture of up, down, and strange quarks, or of relic particles from the early Universe. The experiments are based on Rutherford backscattering of heavy ions, preferably238U, from various target samples. The measured parameters of a detected particle are its time-of-flight, scattering angle, and specific ionization. From this information the mass of the target nucleus can be inferred. Upper limits for the abundance of strange supermassive nuclei with massesA−4·102 to 107 amu relative to the number of nucleons were found …

Uran aus deutschen Nuklearprojekten der 1940er Jahre – eine nuklearforensische Untersuchung

Wir berichten hier uber eine nuklearforensische Analyse verschiedener Uranmaterialien aus deutschen Nuklearprojekten der 1940er Jahre, bei denen Uranmetall in verschiedenen Geometrien verwendet wurde. Mithilfe des 230Th/234U-Isotopenverhaltnisses konnte fur das Metall ein Produktionszeitraum von 1940 bis 1943 bestimmt werden. Die geographische Herkunft des Urans wurde anhand des Spurengehalts an Seltenerdelementen und der Strontium-Isotopenverhaltnisse bestimmt. Die Ergebnisse zeigen, dass das bei den deutschen Nuklearprojekten verwendete Uran aus Minen in der Tschechischen Republik stammt. 236U und 239Pu wurden in Spuren nachgewiesen. Diese entsprechen in etwa der Haufigkeit dieser Isotope…

Digital liquid-scintillation counting and effective pulse-shape discrimination with artificial neural networks

Abstract A typical problem in low-level liquid scintillation (LS) counting is the identification of α particles in the presence of a high background of β and γ particles. Especially the occurrence of β-β and β-γ pile-ups may prevent the unambiguous identification of an α signal by commonly used analog electronics. In this case, pulse-shape discrimination (PSD) and pile-up rejection (PUR) units show an insufficient performance. This problem was also observed in own earlier experiments on the chemical behaviour of transactinide elements using the liquid-liquid extraction system SISAK in combination with LS counting. α-particle signals from the decay of the transactinides could not be unambigu…

Level lifetimes in neutron-rich Ru isotopes

The neutron-rich Ru isotopes are situated between the strongly deformed Sr-Zr region with axial deformation of f l _ 0.40 [1] and the spherical Cd-Sn region. Evidence for triaxiality of even-even Ru isotopes has been presented in [2-5], and lifetimes of some of their 2 + states have been measured in fission studies [6-9]. It seems, however, that in these experiments the nearly identical energies of the 2 + ---* 0 + transitions in l~ and 11~ could not be separated. Therefore, high-resolution measurements are required in order to perceive the evolution of deformation with increasing neutron number. So far only few measurements by the delayed-coincidence method [10] have been performed on chem…

Erste Messung der Ionisationsenergie von Americium und Curium

Performance of the on-line isotope separation facility HELIOS at the Mainz reactor

Abstract The helium-jet on-line isotope eparation facility HELIOS is in operation at the Mainz reactor for spectroscopic studies on mass separated neutron-rich nuclides far from the line of beta-stability. The basic features and achievements of the facility are reported. A total of 45 isotopes of the elements Rb, Sr, Y, Sn, Sb, Te, Cs, Ba, La, Ce, Pr and Nd have been separated and identified so far. Overall efficiencies up to 2% have been obtained using the integrated skimmer ion source arrangement either in a hollow cathode or in a high temperature surface ionization mode. The delay time for the HELIOS system was determined to be about 1 s.

Estimates of the Nuclear Time Delay in Dissipative U + U and U + Cm Collisions Derived from the Shape of Positron andδ-Ray Spectra

Positron and delta-ray spectra have been measured in coincidence with quasielastic scattered particles and fission fragments from the bombardment of Pd, U, and Cm targets with U beams of energies between 5.9 and 8.4 MeV/u. For collisions leading to a fission reaction, the atomic positron and delta-ray spectra fall off more steeply at high energies than expected from calculations based on pure Rutherford trajectories. A quantitative analysis of this effect is in accord with a nuclear contact time of about 10/sup -21/ s.

Resonance ionization spectroscopy in a buffer gas cell with radioactive decay detection, demonstrated usingTl208

An ultrasensitive laser spectroscopic method has been developed to perform hyperfine spectroscopy of heavy-ion-induced reaction products. It is based on resonance ionization in a buffer gas cell combined with radioactive decay detection. The feasibility has been demonstrated using the \ensuremath{\beta}-active ${\mathrm{isotope}}^{208}$ Tl. A sensitivity of 1.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}3}$ of the two-step resonance-ionization process via the n=17 Rydberg level has been determined, utilizing a pulsed excimer-dye-laser combination. The previously unknown nuclear magnetic moment \ensuremath{\mu}${(}^{208}$Tl) = 0.292(13)${\mathrm{\ensuremath{\mu}}}_{\mathi…

Zeptosecond contact times for element Z=120 synthesis

The synthesis of new superheavy elements beyond oganesson (Z=118) requires fusion reactions with projectile nuclei with proton numbers larger than that of $^{48}$Ca (Z=20), which has been successfully employed for the synthesis of elements with Z=112-118. In such reactions, fusion is drastically hindered by fast non-equilibrated dynamical processes. Attempts to produce nuclei with Z=120 using the $^{64}$Ni+$^{238}$U, $^{58}$Fe+$^{244}$Pu, $^{54}$Cr+$^{248}$Cm, and $^{50}$Ti+$^{249}$Cf reactions have been made, which all result in larger Coulomb forces than for $^{48}$Ca-induced reactions, but no discovery has been confirmed to date. In this work, mass and angle distributions of fission frag…

Application of fast solvent extraction processes to studies of exotic nuclides

Fast solvent extraction is a chemical separation method, which can be applied to study exotic nuclides. Since about 1970 the SISAK technique, which is an on-line method based on multi-stage solvent extraction separations, has been successfully used to investigate the nuclear properties of β-decaying nuclides with half-lives down to about one second. During the last decade it has become possible to produce transactinide elements in high enough yields to investigate their chemical properties on a one-atom-at-a-time scale. For this purpose it was necessary to improve and change the detection part of the SISAK system in order to be capable to detect spontaneously fissioning and α-decaying nucli…

Preparation of thin counting samples by volatilization-condensation

Abstract We describe a technique for the preparation of thin counting samples of metallic elements for a α-particle and fission-fragment spectroscopy. The elements are volatilized in a carrier gas stream through a capillary and condensed on a cooled thin collector foil.

Principle and analytical applications of resonance lonization mass spectrometry

Resonance ionization mass spectrometry (RIMS) is a very sensitive analytical technique for the detection of trace elements. This method is based on the excitation and ionization of atoms with resonant laser light followed by mass analysis. It allows element and, in some cases, isotope selective ionization and is applicable to most of the elements of the periodic table. A high selectivity can be achieved by applying three step photoionization of the elements under investigation and an additional mass separation for an unambiguous isotope assignment. An effective facility for resonance ionization mass spectrometry consists of three dye lasers which are pumped by two copper vapor lasers and of…

Fission in238U+238U collisions below the Coulomb barrier

Integral fission cross sections in the system238U+238U were measured at beam energies below the interaction barrierVC. Scattering angle dependent probabilities and integral cross sections for Coulomb fission were calculated. It is concluded that earlier observed discrepancies between measured and calculated angular distributions for the one-neutron transfer product239U cannot be explained by sequential fission. Multi-nucleon transfer induced fission is observed down to energies (0.90±0.02)×VC.

The probability of prompt and delayed fission of muonic237Np

Fission fragments from the reaction237Np(μ−,γ,f) have been measured in coincidence with muonic X-rays. The efficiency of the fission fragment detector is determined from (μ−,γ,f)-data of the same experiment. The total fission probability perμ-stopPt has been measured as well as the fission probabilities Pf of the non-radiative muonic (3d→1s)- and (2p→1s)-transitions; the latter has been divided into two parts leading to different mean excitation energiesE:P t =(54±17)%,P f (3d→1s)=(41±21)%,P f (2p→1s,E=6.218 MeV)=(61±19)%, andP f (2p→1s,E=6.525 MeV)=(57±18)%. The influence of the muon on the fission barrier is discussed. The fission probability after muon capture is compared with a calculat…

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

Electrolytic preparation of actinide filaments for laser resonance ionization spectroscopy

Abstract For the determination of trace amounts of actinide elements by resonance ionization mass spectroscopy, atomic beams of these elements are produced by evaporation from rhenium substrates. The actinides are deposited by electrolysis as hydroxides in a 2 mm spot on a rhenium foil and covered electrolytically with a thin layer of rhenium or platinum. During heating of such a sandwich reduction occurs to the metallic state while diffusing through the overplated layers and the actinides are evaporated as atoms from the surface. With lead-doped platinum, efficient release is observed already at 1700°C in contrast to rhenium where 2100°C is required and a higher background is produced.

Realization of a broad band neutron spin filter with compressed, polarized 3He gas

The strongly spin dependent absorption of neutrons in nuclear spin polarized 3He opens the possibility to polarize beams of thermal and epithermal neutrons. An effective 3He neutron spin filter (NSF) requires high 3He nuclear polarization as well as a filter thickness corresponding to a gas amount of the order of 1 barl. We realized such a filter using direct optical pumping of metastable 3He∗ atoms in a 3He plasma at 1 mbar. Metastable exchange scattering transfers the angular momentum to the whole ensemble of 3He atoms. At present 3 × 1018 3He-atoms/s are polarized up to 64%. Subsequent polarization preserving compression by a two stage compressor system enables to prepare NSF cells of ab…

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.

Heavy isotopes of actinium: 229Ac, 230Ac, 231Ac and 232Ac

Abstract By irradiation of 232Th with 150-MeV bremsstrahlung and with 14-MeV neutrons, three new neutron-rich isotopes of actinium, 230Ac, 231Ac and 232Ac, were produced and identified and the previously reported isotope, 229Ac, was confirmed. The actinium isotopes were chemically isolated by a fast procedure based on elution with α-hydroxyisobutyric acid from cation exchange resins. For 229Ac, a half-life of 62·7 ± 0·5 min and a β-ray energy of 1·14 ± 0·15 MeV were found; 35 γ-rays were observed, the strongest ones with the following energies and relative intensities: 135·3(34), 146·4(35), 164·6(100), 252·2(24), 261·9(39), 317·0(23), 539·9(20), 569·1(91), and 605·2 keV(23). For 230Ac, a ha…

A heavy-ion identification system for the detection of rare events

Abstract A large area detection system is described which consists of twelve low-pressure multi-wire proportional counters and is used in the search for exotic super-massive nuclei. The experiments are based on Rutherford backscattering of heavy ions, preferably 208Pb or 238U, from various target samples. The measured parameters of a detected particle are its time-of-flight, scattering angle, and specific ionization. From this information the mass of the target nucleus can be inferred. The present experimental sensitivity for the detection of exotic nuclei with at least twice the mass of the projectile is about 10−12 relative to the number of nucleons.

Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)

AbstractThe behaviour of plutonium with respect to its migration in the aquifer has been studied under conditions close to nature. Most relevant under these conditions are Pu(III) and Pu(IV) in contact with humic substances (HS) and minerals. As a model for the host rock, kaolinite (KGa-1b) was chosen. The complexation of Pu(III) and Pu(IV) with Aldrich humic acid (AHA) in aqueous solution at ionic strength 0.1 M was investigated by the ultrafiltration method. The sorption of Pu(III) and Am(III) onto kaolinite (K) as a function of pH and metal-ion concentration was studied under aerobic and anaerobic conditions. The pH edge was found at pH∼5.5 independent of the metal-ion concentration and …

Studies of short-lived fission products by means of the multistage solvent extraction system SISAK

The multistage solvent extraction system SISAK is described. The system is used for online studies of nuclides with half-lives down to ∼1 s. Some of the chemical separation procedures are presented, and a survey is given on the results obtained so far. The possiblity to gain access to nuclides with even shorter half-lives is also discussed.

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…

Continuous separation and identification of neutronrich neptunium isotopes from heavy-ion reactions by means of the centrifuge system “sisak”

Abstract Neutron-rich neptunium isotopes formed in direct transfer reactions between 136 Xe projectiles and targets of 244 Pu have been separated from other reaction products with the on-line liquid-liquid extraction system SISAK. A four-detector delay method was used to determine the half-lives of the previously unknown isotopes 243 Np and 244 Np. From the decay of the 287.4 keV γ-line a half-life of 1.8 ± 0.3 min was determined for 243 Np. From the decay curves of the γ-lines at 162.7 and 216.7 keV, which fit into the known level scheme of 244 Pu, a half-life of 2.5 ± 0.3 min results for 244 Np.

Rapid continous radiochemical separations by thermochromatography in connection with a gas-jet recoil-transport system

Abstract A combination of a gas-jet recoil-transport system with a thermochromatographic system has been studied as a technique for rapid, continuous radiochemical separations. Fission products were used as a model for complex mixtures of elements. A nitrogen gas-jet containing potassium chloride clusters was applied to transport nuclides produced in a reactor from the target area to the thermochromatographic column. Conversion of the reaction products carried by the gas-jet volatile species was achieved by stopping the clusters in a quartz-wool plug located in the column and kept at high temperatures and feeding a reactive gas into the column. Several reactive gases producing volatile chlo…

Ca48+Bk249Fusion Reaction Leading to ElementZ=117: Long-Livedα-DecayingDb270and Discovery ofLr266

The superheavy element with atomic number Z=117 was produced as an evaporation residue in the 48Ca+249Bk fusion reaction at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. The radioactive decay of evaporation residues and their α-decay products was studied using a detection setup that allowed measuring decays of single atomic nuclei with half-lives between sub-μs and a few days. Two decay chains comprising seven α decays and a spontaneous fission each were identified and are assigned to the isotope 294-117 and its decay products. A hitherto unknown α-decay branch in 270Db (Z=105) was observed, which populated the new isotope 266Lr (Z=103). The identification of the long-liv…

TRIGA-SPEC: A setup for mass spectrometry and laser spectroscopy at the research reactor TRIGA Mainz

The research reactor TRIGA Mainz is an ideal facility to provide neutron-rich nuclides with production rates sufficiently large for mass spectrometric and laser spectroscopic studies. Within the TRIGA-SPEC project, a Penning trap as well as a beam line for collinear laser spectroscopy are being installed. Several new developments will ensure high sensitivity of the trap setup enabling mass measurements even on a single ion. Besides neutron-rich fission products produced in the reactor, also heavy nuclides such as 235-U or 252-Cf can be investigated for the first time with an off-line ion source. The data provided by the mass measurements will be of interest for astrophysical calculations on…

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…

Fast volatilization of some lanthanide and actinide elements from titanium surfaces

The ad- and desorption of trace quantities of the lanthanide elements lanthanum, praseodymium, neodymium, samarium, europium, gadolinium, dysprosium, and ytterbium and of the actinide elements americium and curium were investigated by thermochromatographic and isothermal measurements with hot titanium columns. The adsorption enthalpies deduced from the experimental data are in reasonable agreement with calculated values which indicate considerable variations in volatility under such conditions. More volatile elements can quickly be separated from less volatile elements by heating the mixture on titanium in high vacuum.

Release Studies of Atomic Technetium

Application of a laser ion source (LIS) is a promising new technique for trace analysis with high efficiency and selectivity. One of the problems which can limit its efficiency attained in practice is the adsorption of sample atoms on the hot walls of the LIS cavity. We have studied the release of atomic technetium from different wall materials at temperatures up to 2500 K. For these investigations resonance ionization of technetium atoms applying a copper vapour pumped dye laser system and γ-spectrometry of 6-h 99mTc have been used. Theoretical calculations of the heat of desorption for technetium on different wall materials are presented and compared with experimental data. Though the res…

Search for strange matter by Rutherford backscattering

According to a number of suggestions, stable strange matter could exist in the form of supermassive nuclei (or 'strange nuggets')1,2. In contrast to ordinary nuclei, which contain only 'up' and 'down' quarks, a piece of strange matter should comprise a mixture of 'up', 'down' and 'strange' quarks in roughly equal proportions. Small amounts of strange matter could have survived from the early stages of the Universe1. Alternatively, strange matter might reach the Earth as a flux of strange nuggets produced in collisions of neutron stars3. Limits to the cosmic flux of strange nuggets with masses in the range from 10−4 to 250 g have been obtained in a search for light produced by the nuggets in…

Search for superheavy elements in damped collisions betweenU238andCm248

Negative results for the production of superheavy elements in damped collisions between $^{238}\mathrm{U}$ projectiles and $^{248}\mathrm{Cm}$ targets are reported. This reaction was believed to permit a closer and more widespread approach to the predicted island of stability near Z=114 and N=184 than any practical fusion reaction. Aqueous and gas phase chemistry techniques were used to isolate superheavy element fractions. The fractions were counted for spontaneous fission activity, fragment kinetic energies, and neutron multiplicities. Cross-section limits for half-lives from hours to several years are g4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}35}$ ${\mathrm{cm}}^{…

Excitation functions for production of heavy actinides from interactions ofCa40andCa48ions withCm248

Excitation functions have been measured for production of isotopes of Bk through Fm in bombardments of /sup 248/Cm with 234- to 294-MeV /sup 40/Ca ions and with 239- to 318-MeV /sup 48/Ca ions. The maxima of the isotopic distributions for these elements occur at only 2 to 3 mass numbers larger for /sup 48/Ca than for /sup 40/Ca reactions. The shapes of the distributions and the half-widths of about 2.5 mass numbers are quite similar to those observed previously for reactions of /sup 16/O, /sup 18/O, /sup 20/Ne, and /sup 22/Ne with /sup 248/Cm. In general, the excitation functions for /sup 40/Ca show maxima near the Coulomb barrier while those for /sup 48/Ca are about 20 MeV above the barrie…

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 …

The decay of105Tc to levels in105Ru

Theβ−-decay of 7.6-min105Tc has been investigated byβ- andγ-ray singles and coincidence measurements. The activities have been produced by thermal-neutron-induced fission of235U or239Pu and subsequent chemical separation of the technetium fraction from the fission product mixture. AQβ-value of 3.2±0.2 MeV has been determined. In a delayed coincidence experiment the lifetime of the first excited state in105Ru at 20.55 keV has been measured to be 340±15 nsec. A level scheme of105Ru is proposed and compared with the results of recent nuclear reaction studies like104Ru(d, p) and104Ru(n, γ). From beta branching ratios to levels in105Ru, ground state spin and parity of 5/2+ can be suggested for10…

Trennung von spaltprodukten durch Extraktionschromatographie

The separation of fission products which form anionic species in mineral acids and of uranium and neptunium from samples of neutron-irradiated uranium is described. The method used is extraction chromatography with tri-n-butylphosphate (TBP) and di-(2-ethylhexyl)-orthophosphoric acid (HDEHP) as extractants and polytrifluoromonochloroethylene powder as the solid support. In the first column Zr, U and Np are extracted with TBP from 8N HNO3/NaClO3. In the second column, HDEHP is applied as extractant and 9N HCl/NaClO3 as the mobile phase for the isolation of Nb, Sb, and I, and in the third column (HDEHP), the rare earths and Mo are extracted from 0.1N HCl. Finally with the fourth column (TBP),…

Levels in104Ru populated by the ??-decay of104Tc

Theβ− — andγ-activities of 18.4 min104Tc have been studied with singles and coincidence measurements. Sources were prepared by chemical separation of technetium from the fission products of thermal-neutron-induced fission of235U. A revised level scheme of104Ru up to an excitation energy of 4.26 MeV is proposed. Fromβ-γ coincidence measurements, aQβ-value of 5.62±0.07 MeV has been obtained.

Chemical investigation of hassium (element 108).

The periodic table provides a classification of the chemical properties of the elements. But for the heaviest elements, the transactinides, this role of the periodic table reaches its limits because increasingly strong relativistic effects on the valence electron shells can induce deviations from known trends in chemical properties. In the case of the first two transactinides, elements 104 and 105, relativistic effects do indeed influence their chemical properties, whereas elements 106 and 107 both behave as expected from their position within the periodic table. Here we report the chemical separation and characterization of only seven detected atoms of element 108 (hassium, Hs), which were…

The on-line isotope separation facility helios at the mainz reactor

Abstract The on-line isotope separation facility HELIOS consisting of a helium-jet transport system coupled to a high transmission mass separator is described. The main characteristics of the system were determined from γ-ray measurements on neutron-rich nuclides. The transmission from the target to the skimmer is about 60%; the overall efficiency for typical fission product elements is 0.05–0.2% and the transit time for Cs is about 1.0 s.

Shape coexistence near the double-midshell nucleus 111Rh

The decay of 111Ru obtained from fast on-line chemical and mass separation has been investigated by β-γ-t and γ-γ coincidence techniques. Earlier spin and parity assignments of 111Rh levels based on extrapolations of level systematics are confirmed. In particular, the K=1/2 intruder band is supported by the hindrance of E2 transitions between deformed and spherical states and enhancement of intraband E2 transitions. The excitation energies of intruder band members in Rh isotopes show a minimum at 109Rh64, with two neutrons less than 111Rh at the N=66 midshell. This trend, which differs from the one in the higher-Z neighbouring elements Ag and Cd with minima at N=66, follows the evolution of…

Spurenbestimmung der Radionuclide90Sr und89Sr in Umweltproben I: Laser-Massenspektrometrie

Separation of plutonium and neptunium species by capillary electrophoresis-inductively coupled plasma-mass spectrometry and application to natural groundwater samples.

Capillary electrophoresis (CE) was coupled to ICPMS in order to combine the good performance of this separation technique with the high sensitivity of the ICPMS for the analysis of plutonium and neptunium oxidation states. The combination of a fused-silica capillary with a MicroMist AR 30-I-FM02 nebulizer and a Cinnabar small-volume cyclonic spray chamber yielded the best separation results. With this setup, it was possible to separate a model element mixture containing neptunium (NpO2(+)), uranium (UO2(2+)), lanthanum (La3+), and thorium (Th4+) in 1 M acetic acid. The same conditions were also suitable for the separation of various oxidation states of plutonium and neptunium in different a…

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…

A laser ion source for trace analysis

A laser ion source has been set up which is based on resonant stepwise excitation and ionization of atomic vapor confined in an ionization chamber. Using a pulsed copper vapor/dye laser system with a high repetition rate (6.5 kHz) one expects high efficiency and high selectivity for this new type of ion source. First test experiments with lead are reported.

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…

Determination of trace elements by resonant ionization mass spectrometry (RIMS)

A resonant ionization mass spectrometer has been developed as an analytical tool for the detection of trace elements, especially of plutonium and other radionuclides. The sample, deposited on a rhenium filament, is evaporated by electrical heating and the atoms of the element under investigation are selectively ionized by laser light delivered from three dye lasers pumped by a copper vapour laser. The resulting photoions are detected in a time-of-flight spectrometer with a channelplate detector. For plutonium a mass resolution of M/δM=1500 was obtained and an overall detection efficiency of 4×10−6 was determined for stepwise excitation and ionization via autoionizing states. With a laser li…

Measurement of the first ionization potential of lawrencium (element 103)

Lawrencium, with atomic number 103, has an isotope with a half-life of 27 seconds; even so, its first ionization potential has now been measured on an atom-at-a-time scale and agrees well with state-of-the-art theoretical calculations that include relativistic effects. The most dramatic modern revision of Mendeleev's periodic table of elements came in 1944 when Glenn T. Seaborg placed a new series of elements, the actinides (atomic numbers 89–103), below the lanthanides. In this issue of Nature, Yuichiro Nagame and colleagues report the first measurement of one of the basic atomic properties of element 103 (lawrencium), namely its first ionization potential. Lawrencium is only accessible vi…

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…

Realization of a broad-band neutron spin filter with compressed, polarized 3He gas

The strongly spin-dependent absorption of neutrons in nuclear spin polarized 3He opens the possibility to polarize beams of thermal and epithermal neutrons. An effective 3He neutron spin filter (NSF) requires high 3He nuclear polarization as well as a filter thickness corresponding to amount of gas in the order of 1 bar 1. We realized such a filter using direct optical pumping of metastable 3He∗ atoms in a 3He plasma at 1 mb. Metastable exchange scattering transfers the angular momentum to the whole ensemble of 3He atoms. At present 3.6 × 1018 3He-atoms s−1 are polarized up to 68%. Subsequent polarization preserving compression by a two-stage compressor system enables to prepare NSF cells o…

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.

Quantitative molecular plating of large-area 242Pu targets with improved layer properties

Abstract For measurements of the neutron-induced fission cross section of 242Pu, large-area (42 cm2) 242Pu targets were prepared on Ti-coated Si wafers by means of constant current density molecular plating. Radiochemical separations were performed prior to the platings. Quantitative deposition yields (>95%) were determined for all targets by means of alpha-particle spectroscopy. Layer densities in the range of 100–150 μg/cm2 were obtained. The homogeneity of the targets was studied by radiographic imaging. A comparative study between the quality of the layers produced on the Ti-coated Si wafers and the quality of layers grown on normal Ti foils was carried out by applying scanning electron…

Attempts to chemically investigate element 112

Summary Two experiments aiming at the chemical investigation of element 112 produced in the heavy ion induced nuclear fusion reaction of 48Ca with 238U were performed at the Gesellschaft für Schwerionenforschung (GSI), Darmstadt, Germany. Both experiments were designed to determine the adsorption enthalpy of element 112 on a gold surface using a thermochromatography setup. The temperature range covered in the thermochromatography experiments allowed the adsorption of Hg at about 35 °C and of Rn at about -180 °C. Reports from the Flerov Laboratory for Nuclear Reactions (FLNR), Dubna, Russia claim production of a 5-min spontaneous fission (SF) activity assigned to 283112 for the 238U(48Ca,3n)…

Review of the SISAK system in transactinide research

Abstract The performance of the SISAK 1 liquid–liquid extraction system applied in transactinide experiments has been improved with respect to the equipment itself and the way it is operated. The improvements were checked in on-line experiments, under conditions similar to those during transactinide experiments. As a result, the yield of the separation system was increased by a factor >5. Furthermore, a cleaner organic scintillation phase was obtained due to a better phase separation. This reduced the β-background, which disturbs the α-measurements. The sensitivity of the SISAK apparatus, including the gasjet and the detection system has been improved by more than one order of magnitude.

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…

Cover Picture: Uranium from German Nuclear Power Projects of the 1940s— A Nuclear Forensic Investigation (Angew. Chem. Int. Ed. 45/2015)

Direct identification of 103–107Mo by a rapid chemical separation procedure

Abstract The nuclides 103–107Mo have been identified by means of γ-ray spectroscopy after the separation of molybdenum from fission products of 235U and 239Pu by a rapid chemical procedure. Half-lives of 67.5 ± 1.5 s for 103Mo, 59.4 ± 0.8 s for 104Mo, 36.7 ± 1.0 s for 105Mo, 8.4 ± 0.5 s for 106Mo and 3.5 ± 0.5 s for 107Mo have been determined and the main γ-lines were assigned to the decay of these isotopes. Some evidence for 108Mo with a half-life ≤2 s has also been obtained.

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…

Reactions of40Ar with233U,235U, and238U at the barrier

Production cross sections for target-like transfer products in reactions of40Ar with233,235,238U at the barrier were determined using radiochemical techniques. The heaviest products detected are isotopes of californium (Z=98). In addition to the quasi-elastic component of the isotopic distributions observed in the vicinity of uranium, there are also relaxed contributions throughout the entire region. The peak positions of the isotope distributions of this component for fixed atomic number, after the transfer of > 3 charges, approach closely the minimum of the potential energy surfaces (PES). The experimental results thus indicate the cold formation of the reaction products. A search for lon…

Search for long-lived superheavy elements in the reaction of136Xe with238U

A search with radiochemical methods for long-lived superheavy elements in 238U targets bombarded with intense beams of136Xe ions produced negative results. A formation cross section of ≤1×10−35 cm2 is deduced at 95% confidence level for nuclides with half-lives between 1 and 200 d.

Isotope Shift Measurements for Superdeformed Fission Isomeric States

Optical isotope shift measurements have been performed for the ${}^{240,242}{\mathrm{Am}}^{f}$ fission isomers with low target production rates of $10{\mathrm{s}}^{\ensuremath{-}1}$ employing resonance ionization spectroscopy in a buffer gas cell. Isotope shift ratios ${\mathrm{IS}}^{240f,241}/{\mathrm{IS}}^{243,241}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}39.2(8)$ and ${\mathrm{IS}}^{242f,241}/{\mathrm{IS}}^{243,241}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}41.4(8)$ have been measured at the 500.02 nm transition. A difference in the nuclear mean charge radii $\ensuremath{\delta}〈{r}^{2}{〉}_{\mathrm{opt}}^{242f,241}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}5.34(2…

The deformedN=60 nucleus 41 101 Nb

The β− decay of101Zr has been investigated at the fission-product separators JOSEF and LOHENGRIN. The half-life of101Zr has been determined to 2.5(1) s and a level scheme for101Nb has been established fromγ ray singles as well as X/3-γ and γ—γ coincidence measurements. Conversion coefficients for transitions in101Nb and level half-lives between 10 ps and 2 ns have been determined. Three rotational bands are identified among the low-lying levels with band heads at 0 keV, 206 keV and 208 keV. The bands are probably based on the Nilsson configurations [422 5/2+], [301 3/2−] and [303 5/2−], respectively. The deformation has been determined to βq=0.40(4) and 0.41(8) for the ground state band and…

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…

Search for elements 119 and 120

A search for production of the superheavy elements with atomic numbers 119 and 120 was performed in the 50Ti+249Bk and 50Ti+249Cf fusion-evaporation reactions, respectively, at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. Over four months of irradiation, the 249Bk target partially decayed into 249Cf, which allowed for a simultaneous search for both elements. Neither was detected at cross-section sensitivity levels of 65 and 200 fb for the 50Ti+249Bk and 50Ti+249Cf reactions, respectively, at a midtarget beam energy of Elab=281.5 MeV. The nonobservation of elements 119 and 120 is discussed within the concept of fusion-evaporation reactions including various theoretical pr…

Half-life ofTi44

The half-life of $^{44}\mathrm{Ti}$ has been measured to be ${T}_{\frac{1}{2}}=54.2\ifmmode\pm\else\textpm\fi{}2.1$ yr, somewhat higher than previously published values of 46.4\ifmmode\pm\else\textpm\fi{}1.7 and 48.2\ifmmode\pm\else\textpm\fi{}0.9 yr. The present value was obtained from the specific activity and the radioisotope concentration of several Ti${\mathrm{O}}_{2}$ samples, each spiked with a $^{44}\mathrm{Ti}$ activity of about 1.2 \ensuremath{\mu}Ci. The specific activity was measured via the 1157 keV $\ensuremath{\gamma}$ line from the decay of the $^{44}\mathrm{Sc}$ daughter. $^{44}\mathrm{Ti}$/Ti concentrations were measured with the Argonne FN tandem accelerator in conjunctio…

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…

Comparison of ultracold neutron sources for fundamental physics measurements

Ultracold neutrons (UCNs) are key for precision studies of fundamental parameters of the neutron and in searches for new CP violating processes or exotic interactions beyond the Standard Model of particle physics. The most prominent example is the search for a permanent electric dipole moment of the neutron (nEDM). We have performed an experimental comparison of the leading UCN sources currently operating. We have used a 'standard' UCN storage bottle with a volume of 32 liters, comparable in size to nEDM experiments, which allows us to compare the UCN density available at a given beam port.

VERFLÜCHTIGUNG VON SPALTPRODUKTEN AUS FESTEM URAN(IV)-FLUORID UND ANDEREN FLUORIDEN

In der Kernehemie sueht man nach temperaturund strahlenresistenten Targetsystemen, aus denen naeh Kernreaktionen kurzlebige Nuklide kontinu: ierlich abgetrennt werden kSnne n. Dies ist insbesondere im Hinblick auf die yon der Gesellschaft fiir Sehwerionenforsehung in Darmstadt geplanten Experimente interessan~, bei denen die Synthese neuer, iibersehwerer Elemente versucht wird. Als Modell fiir Verdampfungsstudien aus festen Targets wurde die tr~gerfreie Verfliichtigung yon Spaltprodukten aus festem Uran(IV)-fluorid gew~hlt [1--3]. Im fliiehtigen Anteil konnten folgende Elemente identifiziert werden: Se, Kr, Zr, Iqb, Me, Te, Ru, Sn, Sb, Te, J und Xe. In einem Rohr mit Temperaturgradienten l~…

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…

Decay of the heaviest isotope of neodymium:154Nd

The neutron-rich isotope154Nd has been separated from235U fission products with the HELIum-jet On-line mass Separator HELIOS and investigated by γ-singles, γγ- and γX-coincidence measurements. The Z- and A-assignment have been confirmed by the observation of promethium KX-rays and by the genetic relationship to the daughter product 1.7-min154Pm. A half-life of 26±2 s has been obtained for154Nd, and a partial decay scheme is proposed. A 40 s activity previously assigned to154Nd could not be confirmed.

Radiochemical study of the kinematics of multi-nucleon transfer reactions in 48Ca + 248Cm collisions 10% above the Coulomb barrier

Abstract The kinematics of multi-nucleon transfer reactions in 48Ca + 248Cm collisions at 262 MeV (center of target) was investigated by using a stacked-foil technique and radiochemical separations of trans-curium elements. Trans-curium isotopes were identified by α-particle spectroscopy. For Fm isotopes, by comparing the centroids of the measured post-neutron emission isotope distributions with the most probable primary mass number predicted by Volkov's generalized Q g g systematics, the missing mass (number of evaporated neutrons) is estimated. The latter is compared with that deduced from the measured centroid of the laboratory angular distribution peaked closely to the grazing angle and…

Hafnium and Lutetium Isomers Produced in Heavy-lon Collisions of 7.6 MeV/u 40Ar, 8.5 MeV/u 84 Kr and 8.5 MeV/u 136Xe on natW Targets

The decay of 31 sec98Zr, 2.9 sec98Nb and 51 min98Nb

TheΒ- andγ-radiations of98Zr and98m, g Nb have been investigated employing scintillation and semiconductor spectrometers and coincidence techniques. Sources of98Nb were produced by the98Mo(n, p)98Nb reaction, sources of98Zr by fission of235U with thermal neutrons applying chemical separations. For98Zr, a half-life of 30.7±0.4 sec and aQ β-value of 2.3±0.2 MeV were obtained, for the98Nb isomers, half-lives of 2.86±0.06 sec and 51.3±0.4 min, andQ β-values of 4.8±0.2 MeV and 4.5±0.2 MeV, respectively. Noγ-rays were observed in the decay of98Zr. The decay of 2.9 sec98Nb was found to involve 11γ-ray transitions. In the decay of 51 min98Nb, 54γ-transitions were detected. Spin and parity of 1+ and…

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.

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…

Decay properties of265Sg(Z=106)and266Sg(Z=106)

The presently known most neutron-rich isotopes of element 106 (seaborgium, Sg), {sup 265}Sg and {sup 266}Sg, were produced in the fusion reaction {sup 22}Ne+{sup 248}Cm at beam energies of 121 and 123 MeV. Using the On-Line Gas chemistry Apparatus OLGA, a continuous separation of Sg was achieved within a few seconds. Final products were assayed by {alpha}-particle and spontaneous fission (SF) spectrometry. {sup 265}Sg and {sup 266}Sg were identified by observing time correlated {alpha}-{alpha}-({alpha}) and {alpha}-SF decay chains. A total of 13 correlated decay chains of {sup 265}Sg (with an estimated number of 2.8 random correlations) and 3 decay chains of {sup 266}Sg (0.6 random correlat…

Preparation of targets by electrodeposition for heavy element studies

Abstract For heavy element studies at GSI, lanthanide and actinide targets have been prepared by molecular plating. The deposition occurs from an isopropanolic solution at 1000–1200 V with current densities of a few mA/cm 2 . Several lanthanide targets have been prepared for test experiments. With nat Gd deposited on a 10 μm thick Be backing foil a target density of 1100 μg/cm 2 could be achieved. Gd-targets were used for the production of α-emitting isotopes of Os, the homologue of hassium (Hs; Z =108), in order to develop a chemical separation procedure for Hs. 248 Cm targets with densities up to 730 μg/cm 2 have been produced for recent experiments to investigate the chemical behaviour o…

Titelbild: Uran aus deutschen Nuklearprojekten der 1940er Jahre – eine nuklearforensische Untersuchung (Angew. Chem. 45/2015)

Evidence for rotational bands in103Nb

The nucleus103Nb62 has been studied through the s− decay of the fission product103Zr at LOHENGRIN and JOSEF. The energies of the lowlying levels and the γ transitions indicate rotational bands based on the Nilsson proton configurations [422 5/2+] [303 5/2−] and [301 3/2−] at 0, 164 and 248 keV, respectively. The measured half-lives of (4.7±0.5) ns and (2.0±0.6) ns of the levels at 164 and 248 keV are consistent with the Nilsson-model estimates including pairing.

Schnelle Extraktion durch quasi-feste Extraktionsmittel

Losungsmittelextraktionen lassen sich erheblich beschleunigen, indem man das Extraktionsmittel an einen feinkornigen TrAger adsorbiert und die zu extrahierende Losung rasch durch eine dunne Schicht dieses Materials saugt. Funfwertiges Antimon und Protactinium werden durch Diisobutylcarbinol und Di-2-Athylhexyl-orthophosphorsAure, gebunden an PolytrifluormonochlorAthylen, selbst bei maximaler Sauggeschwindigkeit von 2–3 ml/sec nahezu quantitativ extrahiert. Die Anwendung dieser Technik bei kernchemischen Studien wird an folgenden schnellen Trennungen demonstriert: Protactinium-234 m aus Uran, Antimon aus Tellur nach (n, p)-Proze\, Antimon aus Spaltprodukten und wiederholtes Abmelken von Tell…

Development of new centrifuges for fast solvent extraction of transactinide elements

The H-0.3 liquid-liquid centrifuge applied for rapid and efficient separation of two liquid phases, and the HG-0.1 gas-liquid centrifuge used to separate the gas phase stemming from a gas jet transportation system and the liquid phase, have been further improved. New centrifuges have been produced of PEEK, a plastic material, which makes them resistant to most aqueous and organic solutions. The performance with respect to time behavior and phase purity is comparable to the titanium centrifuges used so far. The H-0.3 centrifuge has been applied to solvent extraction studies of Zr, Nb, Mo, Hf, Ta, W and Pa from HF solutions into tri-n-octylamine.

Isotope shift and hyperfine structure measurements at the242f Am fission isomer

Istope shift and hyperfine structure measurements have been performed for the242fAm fission isomer with target production rates of only a few per second. The method is based on resonance ionization spectroscopy (RIS) in a buffer gas cell with radioactive decay detection of the ionization process (RADRIS). A relative isotope shift ratioX exp=IS242f,241/ IS243,241=41.7±0.9 has been measured for the 500.02 nm transition corresponding to a nuclear parameter Λ242f,241=5.4±0.3 fm2. The analysis of the quadrupole moment based on the deformed Fermi-model of the nuclear charge distribution including second order corrections results inQ 20=38.2 ±1.4( −0.8 +0.4 )model eb. The measurement of the hyperf…

First Determination of the Ionization Potential of Americium and Curium

Evidence for the formation of sodium hassate(VIII)

SummaryHassium, element 108, was produced in the fusion reaction between26Mg and248Cm. The hassium recoils were oxidizedin-situto a highly volatile oxide, presumably HsO4, and were transported in a mixture of He and O2to a deposition and detection system. The latter consisted of 16 silicon PIN-photodiodes facing a layer of NaOH, which served, in the presence of a certain partial pressure of water in the transport gas, as reactive surface for the deposition of the volatile tetroxides. Six correlated α-decay chains of Hs were detected in the first 5 detectors centred around detection position 3. In analogy to OsO4, which forms Na2[OsO4(OH)2], an osmate(VIII), with aqueous NaOH, HsO4presumably…

An efficient excitation scheme for resonance ionization of tin in a laser ion source

An efficient three-colour, three-step resonant excitation/ionization scheme has been found for tin that leads from the 5p23P2 level of the ground-state multiplet via two excited atomic levels (λ1 = 317.51 nm and λ2 = 811.40 nm) to an autoionizing state 9s3P2(λ3 = 823.49 nm) at 59375.9 cm−1. This excitation path permits the saturation of all transitions with the limited power available from a copper vapour laser pumped dye laser system (Esat ≈ 1.5 mJcm2 for λ3). The high repetition rate of such a laser system is essential for a highly efficient laser ion source.

Decay properties of neutron-rich niobium isotopes

The decay of neutron-rich niobium isotopes in the mass region $A\ensuremath{\simeq}100$ has been investigated by $\ensuremath{\gamma}$-ray singles and $\ensuremath{\gamma}$-$\ensuremath{\gamma}$ coincidence measurements. The isotopes were produced by thermal-neutron induced fission of $^{235}\mathrm{U}$, $^{239}\mathrm{Pu}$, and $^{249}\mathrm{Cf}$, and niobium was separated from fission-product mixtures with an automated chemical procedure. Isomerism was found in the even-mass niobium isotopes with the following half-lives: 1.5 and 3.1 sec for $^{100}\mathrm{Nb}$, 1.3 and 4.3 sec for $^{102}\mathrm{Nb}$, and 0.8 and 4.8 sec for $^{104}\mathrm{Nb}$. Half-lives and $\ensuremath{\gamma}$ rays…

Anomalous Behavior of High-Spin States inCm248

The ground-state band of $^{248}\mathrm{Cm}$ has been studied up to spin ${28}^{+}$ and tentatively to ${30}^{+}$ by observing $\ensuremath{\gamma}$ rays following multiple Coulomb excitation with use of $^{208}\mathrm{Pb}$ ions at 5.3 MeV/u. A smooth, gradual increase in the effective moment of inertia is seen at lower spin with an anomalous forward bend above spin ${22}^{+}$. Calculations are presented which indicate that this behavior including the forward bend can be understood in terms of the alignment of single-particle angular momenta along the rotation axis.

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 …

Gas phase synthesis of 4d transition metal carbonyl complexes with thermalized fission fragments in single-atom reactions

Abstract The formation of carbonyl complexes using atom-at-a-time quantities of short-lived transition metals from fusion and fission reactions was reported in 2012. Numerous studies focussing on this chemical system, which is also applicable for the superheavy elements followed. We report on a novel two-chamber approach for the synthesis of such complexes that allows spatial decoupling of thermalization and gas-phase carbonyl complex synthesis. Neutron induced fission on 235U and spontaneous fission of 248Cm were employed for the production of the fission products. These were stopped inside a gas volume behind the target and flushed with an inert-gas flow into a second chamber. This was fl…

Uranium from German Nuclear Power Projects of the 1940s— A Nuclear Forensic Investigation

Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence.

SIMSISAK – a Method to Model Nuclide Transport in the SISAK System

A computer model that calculates the transport yield of a nuclide through an arbitrary SISAK experimental set-up has been developed. The model is intended to be used for two types of calculations connected to chemical studies of the heaviest elements. If the production cross section and the nuclide half-life are known, it can be used to estimate the number of decay events to be expected at the detection site. Consequently, if the number of atoms decaying in the detection cells is known, it can be used to estimate the production cross section or the half-life, provided that one of these properties is known.

Subshell closure effects on the collectivity of 36 88 Kr52 and the beta decay of88Br to levels in88Kr

The level structure of88Kr has been investigated by measurements on chemically separated bromine samples. A total of 146γ-rays have been assigned to the decay of88Br, and a level scheme with 58 levels is proposed. The collectivity of88Kr has been investigated within the framework of the Interacting Boson Approximation (IBA-2 model). Comparison of our detailedγ-ray data and calculations have led to the establishment of a protonhole boson desciption rather than protonparticle nature. This supports recent works establishingZ=40 as a major subshell closure.

Fusion reaction Ca48+Bk249 leading to formation of the element Ts ( Z=117 )

The heaviest currently known nuclei, which have up to 118 protons, have been produced in 48Ca induced reactions with actinide targets. Among them, the element tennessine (Ts), which has 117 protons, has been synthesized by fusing 48Ca with the radioactive target 249Bk, which has a half-life of 327 d. The experiment was performed at the gas-filled recoil separator TASCA. Two long and two short α decay chains were observed. The long chains were attributed to the decay of 294Ts. The possible origin of the short-decay chains is discussed in comparison with the known experimental data. They are found to fit with the decay chain patterns attributed to 293Ts. The present experimental results confi…

Chemical reactions in a gas-jet recoil-transport system: Continuous separation procedure for selenium and tellurium from fission products

Abstract Chemical selectivity in a gas-jet recoil-transport system can be achieved by chemical reactions with the carrier gas. This is demonstrated for an ethylene-nitrogen jet in which volatile species of selenium and tellurium are formed by passing the gas through a reaction zone heated to 860°C. Rapid continuous separation procedures for selenium and tellurium from fission products based on this effect are described and some decay data of the neutron-rich nuclides 85–88Se and 135–137Te obtained with these methods are given.

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…

Study of non-fusion products in the Ti50+Cf249 reaction

The isotopic distribution of nuclei produced in the 50Ti + 249Cf reaction has been studied at the gas-filled recoil separator TASCA at GSI Darmstadt, which separates ions according to differences in magnetic rigidity. The bombardment was performed at an energy around the Bass barrier and with the TASCA magnetic fields set for collecting fusion-evaporation reaction products. Fifty-three isotopes located “north-east” of 208Pb were identified as recoiling products formed in non-fusion channels of the reaction. These recoils were implanted with energies in two distinct ranges; besides one with higher energy, a significant low-energy contribution was identified. The latter observation was not ex…

Rapid chemical separation procedures

Fast, discontinuous separation procedures are described for zirconium, niobium, technetium and antimony from fission products. Other rapid separation methods from aqueous solutions are summarized. The combination of a gas jet recoil transport system with a continuous solvent extraction technique and with a thermochromatographic separation method is presented. The application of such procedures to the investigation of new and already known short-lived nuclides is illustrated by some examples.

The collective structure of106,108Ru

Levels in106,108Ru have been studied by measuringγγ coincidences andγγ directional correlations of theγ-rays following theβ−-decay of 36 s106Tc and 5 s108Tc. Tc activities were separated chemically from the fission products of thermal neutron induced fission of239Pu by the continuously running system “SISAK 2” and theγ-radiation was measured on-line. An extended level scheme for108Ru, spin assignments,E2/M1 multipole mixing ratios andB(E2) ratios for106Ru and108Ru have been obtained. The collective structure of the two nuclei is discussed in the framework of different nuclear models.

Spectroscopy along Flerovium Decay Chains: Discovery ofDs280and an Excited State inCn282

A nuclear spectroscopy experiment was conducted to study α-decay chains stemming from isotopes of flerovium (element Z=114). An upgraded TASISpec decay station was placed behind the gas-filled separator TASCA at the GSI Helmholtzzentrum fur Schwerionenforschung in Darmstadt, Germany. The fusion-evaporation reactions ^{48}Ca+^{242}Pu and ^{48}Ca+^{244}Pu provided a total of 32 flerovium-candidate decay chains, of which two and eleven were firmly assigned to ^{286}Fl and ^{288}Fl, respectively. A prompt coincidence between a 9.60(1)-MeV α particle event and a 0.36(1)-MeV conversion electron marked the first observation of an excited state in an even-even isotope of the heaviest man-made eleme…

Production of monodisperse uranium oxide particles and their characterization by scanning electron microscopy and secondary ion mass spectrometry

Abstract Secondary ion mass spectrometry (SIMS) can be confidently used to measure uranium isotopic ratios in single particles. Dense particles of known isotopic composition and size allow the precision and the accuracy of the applied procedure to be estimated. These particles can be obtained by dissolving standard reference uranium materials, nebulizing the solution in droplets of proper diameter and collecting the particles after the desolvation and calcination of the droplets. A new instrumental set up, based on a commercial vibrating orifice aerosol generator to generate monodisperse droplets of the solutions from four uranium oxide reference materials, is described. The droplets were d…

TASCAを用いたCn, Nh, Fl化学実験のためのHg, Tl, PbのSiO2及びAu表面に対するオンライン化学吸着研究

Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO$_{2}$ and Au surfaces were carried out using short-lived radioisotopes with half-lives in the range of 4-49 s. This is a model study to measure adsorption enthalpies of superheavy elements Cn, Nh, and Fl. The short-lived isotopes were produced and separated by the gas-filled recoil separator TASCA at GSI. The products were stopped in He gas, and flushed into gas chromatography columns made of Si detectors whose surfaces were covered by SiO$_{2}$ or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO$_{2}$ surface at room temperature. On the other hand, the Hg did no…

Fast preparation and gas-chromatographic separation of lanthanide and actinide hexafluoroacetylacetonates

A fast method for the separation of lanthanide elements by gas chromatography of their hexafluoroacetylacetonates is described. Individual lanthanides can be isolated within a few minutes, and the whole group can be separated in less than 10 min. The hexafluoroacetylacetonates are applied in form of mixed complexes with tri-n-butyl phosphate or trioctylphosphine oxide prepared by fast extraction into quasi-solid solvents. The applicability of this method for the separation of trivalent actinide elements is shown, including the fast preparation of thin counting samples.

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…

Speciation of the oxidation states of plutonium in aqueous solutions by UV/Vis spectroscopy, CE-ICP-MS and CE-RIMS

For the speciation of the plutonium oxidation states in aqueous solutions, the online coupling of capillary electrophoresis (CE) with inductively coupled plasma mass spectrometry (ICP-MS) has been developed. Depending on the radius/electrical charge ratio, the oxidation states III, IV, V, and VI of plutonium are separated by CE, based on the different migration times through the capillary and are detected by ICP-MS. The detection limit is 20 ppb,i.e.109–1010atoms (10-12–10-13g) for one oxidation state with an uncertainty of the reproducibility of the migration times of ≤1% and ≤5% for the peak area. The redox kinetics of the different plutonium oxidation states in the presence of humic subs…

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…

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…

Educational programs in nuclear and radiochemistry at the University of Mainz and in Germany

A survey is given of the educational programs at German universities and research institutions. The program at the University of Mainz is outlined in some detail.

Sensitive search for near-symmetric and super-asymmetric fusion-fission of the superheavy element Flerovium (Z=114)

Physics letters / B 820, 136601 (2021). doi:10.1016/j.physletb.2021.136601

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.

Electromagnetic and nuclear fission of238U in the reaction of 100, 500, and 1000 A�MeV208Pb with238U

The folding- and azimuthal-angle and velocity distributions for the238U fission fragments have been measured in reactions with 100, 500, and 1000 A·MeV208Pb. These distributions were used to decompose the fission cross section into its electromagnetic and nuclear components. The fraction of electromagnetic fission was found to be 0.16±0.07, 0.48±0.08, and 0.60±0.04, respectively. The electromagnetic fission cross section as a function of the208Pb nucleus energy is compared with theoretical predictions. The measured fission cross section from nuclear reactions (≈1.5 b) is approximately constant between 100 and 1000 A·MeV.

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.