Status and research programs of the multinuclide accelerator mass spectrometry system at the University of Tsukuba

We present the current status and research programs of a multinuclide accelerator mass spectrometry (AMS) system on the 12UD Pelletron tandem accelerator at the University of Tsukuba (Tsukuba AMS system), Japan. A maximum terminal voltage of 12 MV is available for the AMS system. The Tsukuba AMS system can measure environmental levels of long-lived radioisotopes of ¹⁴C, ²⁶Al, ³⁶Cl and ¹²⁹I by employing a molecular pilot beam. Recently, enhancements in AMS techniques and equipment, including sample preparation, the ion source and the data acquisition system, have improved the performance of ³⁶Cl-AMS. The standard deviation of fluctuations is typically ±2%, and the machine background level for the ³⁶Cl/Cl ratio is lower than 1 × 10^?15 with a halite sample. We have measured over 500 samples in 1 year, including samples for earth and environmental sciences and nuclear safety research.     

The French accelerator mass spectrometry facility ASTER: Improved performance and developments

Following the installation and acceptance test of the French 5 MV AMS facility ASTER, the focus has been on improving the capability for routine measurements of ¹⁰Be and ²⁶Al. Quality assurance has been established by the introduction of traceable AMS standards for each nuclide, by self-monitoring through participation in round-robin exercises and proficiency testing, and by surveillance of long- and short-time variability of blank and reference materials. A background level of 3 × 10^?14 makes ASTER well-suited for measuring ⁴¹Ca/⁴⁰Ca in the10^?12 region, which is sufficient for a wide range of applications. Routine AMS measurements of volatile elements like ³⁶Cl and ¹²⁹I will most likely become feasible in the very near future as the result of significant improvements in the ion source design.     

Fluorides or hydrides? 41Ca performance at VERA’s 3-MV AMS facility

Recent improvements in isobaric suppression for medium-mass isotopes, e.g. ⁴¹Ca, offer new possibilities for tandem accelerators with terminal voltages of 3 MV or lower; i.e. when dealing with particle energies ?1 MeV/amu. In particular, detection of ⁴¹Ca requires sufficient discrimination of the stable isobar ⁴¹K. We explored the limits of ⁴¹Ca detection at our 3-MV AMS facility by means of different types of particle detectors: The ΔTOF method, which is based on the different flight-time of isobars after passing a thick absorber foil. The second method makes use of a new type of compact ionization chamber: ⁴¹K and ⁴¹Ca are separated in energy due to their different energy loss in the detector entrance foil and the detector gas, which is measured via a segmented anode.At VERA we measured ⁴¹Ca/Ca ratios below 10^?13 for commercial CaF₂ material serving as blank samples. CaH₂ sputter targets, with the extraction of ${\text{CaH}}_3^{-}$, yielded background ratios as low as ⁴¹Ca/Ca = 1 × 10^?15. The typical measurement precision at VERA for ⁴¹Ca measurements was between 2% and 5%. These results demonstrate that AMS facilities based on 3-MV tandems have reached the sensitivity level of larger AMS facilities for a wide range of applications, with the advantage of high overall efficiency and sample throughput.     

Comparison of detector systems for the separation of 36Cl and 36S with a 3-MV tandem

The possibility of detecting ³⁶Cl for geological exposure dating has been explored for several years at VERA (the Vienna Environmental Research Accelerator). First results on real samples were obtained with an ionization chamber (developed at the ETH/PSI, Zürich, Switzerland) with two anodes. To improve the suppression of ³⁶S, we equipped the ionization chamber with an exit window and added a Time-of-Flight (TOF) system with a double-sided silicon strip detector (50 × 50 mm²) as stop detector. We optimized the TOF setup by using silicon nitride foils to reduce scattering tails in the energy spectra.At 3 MV terminal voltage, corresponding to a particle energy of 24 MeV of ³⁶Cl⁷⁺, we achieved a ³⁶S⁷⁺-suppression of 21,500 (50% ³⁶Cl-detector-efficiency).     

Comparison of 41Ca analysis on 0.5 MV and 5 MV-AMS systems

A comparative study was made between the compact AMS system at the PSI/ETH Laboratory of Ion Beam Physics in Zurich with 0.5 MV terminal voltage and the 5 MV-AMS system at the Scottish Universities Environmental Research Centre (SUERC), Glasgow. Overall 34 urinary samples with ⁴¹Ca/⁴⁰Ca ratios in the range from 4 × 10^?11 to 3 × 10^?10 were processed to CaF₂ and aliquots of the same material were measured on both instruments.Measurements on the compact AMS system were performed in charge state 3+ achieving a transmission of 4% at 1.7 MeV beam energy. Under these conditions a suppression of the interference ⁴¹K is virtually impossible. However, samples with an excess of potassium can be identified by a shift of the ⁴¹Ca/⁴¹K peak in the ΔE ? E histogram of the gas ionization detector employed and a criterion for data rejection can be defined. An overall precision of ～4% and a ⁴¹Ca/⁴⁰Ca background level of 5 × 10^?12 have been reached.For studies with higher demands on the detection limit AMS systems like the one at SUERC are attractive: in charge state 5+ and using a gas stripper beam energy of 27 MeV, a transmission of 5%, a ⁴¹K suppression factor of ～500 and a ⁴¹Ca/⁴⁰Ca background level of 3 × 10^?14 are achieved.We demonstrate that both systems are well suited for large-scale ⁴¹Ca biomedical applications.     

Improved 36Cl AMS at 5 MV

Small changes to our ion source and gas ionization detector have significantly improved Cl measurement by reducing source memory and increasing interference rejection. Gas stripped low energy 30 MeV ³⁶Cl⁵⁺ ions are still efficiently transported to the detector but ³⁶S vs. ³⁶Cl separation is improved by an order of magnitude. Accordingly ³⁶Cl/Cl background is <10^?15 before additional interference correction that is also newly automated. ³⁵Cl^? currents have increased to 30 μA and ³⁶Cl/Cl inter-cathode repeatability is 3%.     

AMS measurement technique after 30 years: Possibilities and limitations of low energy systems

A brief summary of the development of AMS over the last 30 years is given and major development steps for the measurement technique are described. With the appearance of compact low energy AMS systems 10 years ago, a new category of AMS instruments has been introduced. This has resulted in a boom of new AMS facilities with more than 20 installations over the last 5 years. But low energy AMS is not limited to radiocarbon only and there is a great potential for ¹⁰Be, ²⁶Al, ¹²⁹I and actinides measurements at compact AMS systems. The latest developments towards the low energy limit of AMS resulted in two new types of systems, the NEC Single Stage AMS and ETH MICADAS operating with terminal voltages of about 200 kV only. These systems have enormous impact, not only on the use of AMS in biomedical research but also on radiocarbon dating. Precision limits of radiocarbon dating will be discussed for the MICADAS type instruments.     

Highly sensitive AMS measurements of 53Mn

Our AMS system, with the gas-filled detector system GAMS, has been optimized for measurements with ⁵³Mn. A high sensitivity has been achieved. A newly installed cesium sputter ion source yields an improved emittance, and thus a higher mass resolution. By the extraction of the manganese molecule MnF^? instead of MnO^? we can suppress the isobaric chromium background in the ion source by more than a factor of three. The GAMS system achieves an isobaric suppression factor of about 3 × 10⁸. Measurements on blank samples yielded upper limits for the ⁵³Mn/⁵⁵Mn ratios of 7 × 10^?15.     

14C analysis via intracavity optogalvanic spectroscopy

A new ultra sensitive laser-based analytical technique, intracavity optogalvanic spectroscopy (ICOGS), allowing extremely high sensitivity for detection of ¹⁴C-labeled carbon dioxide has recently been demonstrated. Capable of replacing accelerator mass spectrometers (AMS) for many applications, the technique quantifies zeptomoles of ¹⁴C in sub micromole CO₂ samples. Based on the specificity of narrow laser resonances coupled with the sensitivity provided by standing waves in an optical cavity, and detection via impedance variations, limits of detection near 10^{?15 14}C/¹²C ratios have been obtained with theoretical limits much lower. Using a 15 W ¹⁴CO₂ laser, a linear calibration with samples from 5 × 10^?15 to >1.5 × 10^?12 in ¹⁴C/¹²C ratios, as determined by AMS, was demonstrated. Calibration becomes non-linear over larger concentration ranges due to interactions between CO₂ and buffer gas, laser saturation effects and changes in equilibration time constants. The instrument is small (table top), low maintenance and can be coupled to GC or LC input. The method can also be applied to detection of other trace entities. Possible applications include microdosing studies in drug development, individualized sub-therapeutic tests of drug metabolism, carbon dating and real time monitoring of atmospheric radiocarbon.     

SUERC AMS ion detection

In a short time Be, C, Al, Cl, Ca and I accelerator mass spectrometry (AMS) have been established on the National Electrostatics Corporation (NEC) 5 MV pelletron system at the Scottish Universities Environmental Research Centre (SUERC). While summarising the present performance of the system, this report will focus on the details of ion detection, which sample materials are used and the analytical procedures employed for each individual species during routine analysis.All rare isotope detection is with a single flexible detector and ion event analysis system, but switching of analysed species typically requires a detector reconfiguration. Configurations for routine ¹⁰Be, ¹⁴C, ²⁶Al, ³⁶Cl, ⁴¹Ca and ¹²⁹I detection have been established and will be presented here. Notably, there has proven to be sufficient suppression of the isobaric interferences of ³⁶Cl and ⁴¹Ca in the 5+ charge state using an argon gas stripper at a terminal voltage of 5.0 MV to allow for routine analysis of these isotopes.     

On the measurement of 10Be on the 1 MV compact AMS system at the Centro Nacional de Aceleradores (Spain)

In this work we present the most recent improvements performed by our group on ¹⁰Be measurements on the 1 MV AMS system recently set up at the CNA (Centro Nacional de Aceleradores), in Seville (Spain). Our efforts have been focused on the study of the viability of our system for BeO and BeF^? measurements. To achieve this, different standard materials have been measured to demonstrate the reliability of the system for BeO measurements in a wide ¹⁰Be/⁹Be atomic ratio range and several environmental samples have been studied both at the 1 MV AMS CNA facility and at the 6 MV AMS ETH-PSI facility of Zurich to validate our measurements. The results show a good agreement between laboratories. New experiments also have been carried out selecting 1+ and 2+ charge states at the exit of the accelerator and inserting Si₃N_3.1 foils with different thicknesses to separate ¹⁰Be from its isobar, ¹⁰B. The influence of each foil on the overall transmission (detected ¹⁰Be compared to BeO^? injected into the accelerator) and background level was also assessed. In addition some tests were also done to assess the viability of BeF₂ and BaBeF₄ measurements at our system. Several metal matrices and cathode preparation procedures for BeO samples were investigated to maximize current and cathode lifetime.     

Competitive 10Be measurements below 1 MeV with the upgraded ETH–TANDY AMS facility

Competitive ¹⁰Be measurements at energies as low as 0.75 MeV are now possible with the compact ETH AMS system TANDY. In this paper we describe and discuss the modifications that led to the significantly improved performance for ¹⁰Be at the 0.6 MV accelerator. Results from the first routine measurement show that ¹⁰Be on the upgraded TANDY is now fully competitive with larger AMS systems with respect to background and measurement precision. The total efficiency for ¹⁰Be is comparable to our large 6 MV Tandem system and thus sufficient for the full range of applications in the Earth and Environmental Sciences.     

Design of a large irradiation channel at MNSR facility in Ghana

In the design of new slant tube for large sample irradiation in the Ghana Research Reactor-1 facility, Monte Carlo N-Particle Code version 5 (MCNP-5) was employed to simulate the neutron flux profile of the new design. The results show that the neutron flux peaks at different points, at an average thermal neutron flux of (1.1406 ± 0.0046) × 10¹¹, (1.1849 ± 0.0047) × 10¹¹ and (1.0580 ± 0.0044) × 10¹¹ n cm^?2 s^?1 around the reactor vessel. The first two peaks happened to coincide with pneumatic transfer pipes in the pool, but the third peak happened to be in line with the slant tube position. It was observed that as the diameter of the tube varies from 3.90 cm to 23.40 cm, the average thermal neutron flux decreased exponentially from (1.1849 ± 0.0047)10¹¹ n cm^?2 s^?1 to (3.3241 ± 0.0100) × 10¹⁰ n cm^?2 s^?1. The average thermal neutron flux decreases exponentially along the diameter of the designed slant tube from (1.0366 ± 0.0042) × 10¹¹ n cm^?2 s^?1 to (9.7396 ± 0.0136) × 10⁹ n cm^?2 s^?1. From the results, it is evident that a slant tube of diameter 15.00 cm can be installed at the original slant tube position for large sample irradiation.     

Improvement of initial vacuum condition along 2008–2010 KSTAR campaign by vessel baking

Korea Superconducting Tokamak Advanced Research (KSTAR) is upgraded for its KSTAR 3rd campaign for new target mission to produce the D-shaped plasma with a target plasma current of 500 kA and/or pulse length of 5 s. New Plasma Facing Components (PFCs) are installed which leads to the increase of the surface area of the vessel by a factor of about 5. The vacuum conditioning such as the vessel baking has been performed in order to remove various kinds of impurities including H₂O, carbon and oxygen for the plasma. The total outgassing rate in the KSTAR 1st campaign was measured as 1.5 × 10^?4 mbar ? s^?1 which is increased by a factor of 3 (6.49 × 10^?4 mbar ? s^?1) in the KSTAR 3rd campaign. Nevertheless, the outgassing rates per unit area have been decreased from 9.31 × 10^?5 mbar ? m^?2 s^?1 to 1.22 × 10^?5 mbar ? m^?2 s^?1 due to the upgrade of baking system and series of baking operation.     

Nickel,Zn and Cd localisation in seeds of metal hyperaccumulators using μ-PIXE spectroscopy

Metal hyperaccumulators are a rare group of plant species that accumulate exceptionally high concentrations of metals in above ground tissues without showing symptoms of phytotoxicity. Quantitative localisation of the accumulated metals in seed tissues is of considerable interest to help understand the eco-physiology of these unique plant species. We investigated the spatial localisation of metals within seeds of Ni hyperaccumulating Hybanthus floribundus subsp. adpressus, H. floribundus subsp. floribundus and Pimelea leptospermoides and dual-metal (Cd and Zn) hyperaccumulating Thlaspi caerulescens using quantitative micro-proton induced X-ray emission (μ-PIXE) spectroscopy. Intact seeds were hand-sectioned, sandwiched between Formvar films and irradiated using the 3 MeV high energy heavy ion microprobe at ANSTO. Elemental maps of whole H. floribundus subsp. adpressus seeds showed an average Ni concentration of 5.1 × 10³ mg kg^?1 dry weight (DW) with highest Ni concentration in cotyledonary tissues (7.6 × 10³ mg kg^?1 DW), followed by the embryonic axis (4.4 × 10³ mg kg^?1 DW). Nickel concentration in whole H. floribundus subsp. floribundus seeds was 3.5 × 10² mg kg^?1 DW without a clear pattern of Ni localisation. The average Ni concentration in whole P. leptospermoides seeds was 2.6 × 10² mg kg^?1 DW, and Ni was preferentially localised in the embryonic axis (4.3 × 10² mg kg^?1 DW). In T. caerulescens, Cd concentrations were similar in cotyledon (4.5 × 10³ mg kg^?1 DW) and embryonic axis (3.3 × 10³ mg kg^?1 DW) tissues, whereas Zn was highest in cotyledonary tissues (1.5 × 10³ mg kg^?1 DW). In all species, the presence of the accumulated metal within the cotyledonary and embryonic axis tissues indicates that the accumulated metal was able to move apoplastically within the seed.     

A simple way to analyze infrared reflectivity spectra of p-type Hg0.78Cd0.22Te implanted in various conditions

Different ion-implanted p-type Hg_0.78Cd_0.22Te samples were analyzed by infrared reflectivity in the 2–20 μm wavelength range. We show how to derive some characteristic values of the free carriers induced by ion implantation from simple models of the implanted samples. For low energy implantations (Al (320 keV)) an excess of electrons with concentration n⁺ ≈ 5 × 10¹⁷ cm⁻³ for doses 10¹² and 10¹⁴ ions cm⁻² is observed between the surface and the projected range R_p of the ions, in agreement with the well-known change of type of the free carriers induced by the ion implantation in this kind of samples. High energy α particle (0.8 and 2 MeV, 10¹⁴ ions cm⁻²) implantations lead to a pronounced inhomogeneous concentration of free electrons with n⁺ ≈ 9.2 × 10¹⁶ cm⁻³ between the surface and R_p where a negligible amount of defects due to the nuclear energy loss is formed, and n⁺ ≈ 1.6 × 10¹⁷ cm⁻³ between R_p and R_p + ΔR_p, ΔR_p being the longitudinal straggling, where the defect production rate through the nuclear energy loss mechanism is maximum.     

Selective isobar suppression for accelerator mass spectrometry and radioactive ion-beam science

A new method of selective isobar suppression by photodetachment in a radio-frequency quadrupole ion cooler is being developed at HRIBF with a twofold purpose: (1) increasing the AMS sensitivity for certain isotopes of interest and (2) purifying radioactive ion beams for nuclear science. The potential of suppressing the ³⁶S contaminants in a ³⁶Cl beam using this method has been explored with stable S^? and Cl^? ions and a Nd:YLF laser. In the study, the laser beam was directed along the experiment’s beam line and through a RF quadrupole ion cooler. Negative ³²S and ³⁵Cl ions produced by a Cs sputter ion source were focused into the ion cooler where they were slowed by collisions with He buffer gas; this increased the interaction time between the negative-ion beam and the laser beam. As a result, suppression of S^? by a factor of 3000 was obtained with about 2.5 W average laser power in the cooler while no reduction in Cl^? current was observed.     

Vacuum system of SST-1 Tokamak

Vacuum chambers of Steady State Superconducting (SST-1) Tokamak comprises of the vacuum vessel and the cryostat. The plasma will be confined inside the vacuum vessel while the cryostat houses the superconducting magnet systems (TF and PF coils), LN₂ cooled thermal shields and hydraulics for these circuits. The vacuum vessel is an ultra-high (UHV) vacuum chamber while the cryostat is a high-vacuum (HV) chamber. In order to achieve UHV inside the vacuum vessel, it would be baked at 150 °C for longer duration. For this purpose, U-shaped baking channels are welded inside the vacuum vessel. The baking will be carried out by flowing hot nitrogen gas through these channels at 250 °C at 4.5 bar gauge pressure. During plasma operation, the pressure inside the vacuum vessel will be raised between 1.0 × 10^?4 mbar and 1.0 × 10^?5 mbar using piezoelectric valves and control system. An ultimate pressure of 4.78 × 10^?6 mbar is achieved inside the vacuum vessel after 100 h of pumping. The limitation is due to the development of few leaks of the order of 10^?5 mbar l/s at the critical locations of the vacuum vessel during baking which was confirmed with the presence of nitrogen gas and oxygen gas with the ratio of ～3.81:1 indicating air leak. Similarly an ultimate vacuum of 2.24 × 10^?5 mbar is achieved inside the cryostat. Baking of the vacuum vessel up to 110 °C with ±10 °C deviation was achieved with a net mass flow rate of 0.8 kg/s at 1.5 bar gauge inlet pressure and supply temperature of 230 °C at the heater end. Also during gas feed system installation, the pressure inside the VV was raised from 3.01 × 10^?5 mbar to 1.72 × 10^?4 mbar by triggering a pulse of lower amplitude of 25 voltage direct current (VDC) for 100 s to piezoelectric valve. This paper describes in detail the design and implementation of the various vacuum subsystems including relevant experimental results.     

Damage evolution of yttria-stabilized zirconia induced by He irradiation

The study presents an investigation of damage evolution of yttria-stabilized zirconia (YSZ) induced by irradiation of 100 keV He ions at room temperature as a function of fluence. Transmission electron microscopy (TEM), X-ray diffraction (XRD) and atomic force microscopy (AFM) were used in order to study the nature and evolution of structural damage at different levels. Our study shows that various kinds of defects are formed with the increasing fluence. Firstly, at low fluences, from 1 × 10¹⁶ to 4 × 10¹⁶ cm^?2, of which maximum values of displacement per atom (dpa) range from 0.29 to 1.17, an elastic strain which is attributed to the accumulation of irradiation-induced discrete point defects, is presented. Secondly, in the intermediate fluences ranging from 8 × 10¹⁶ to 1 × 10¹⁷ cm^?2 with corresponding dpa varying from 2.33 to 2.91, a large drop of elastic strain occurs accompanied by presence of an intensive damage region, which is comprised by large and interacted defect clusters. Thirdly, at the two high fluences of 2 × 10¹⁷ and 4 × 10¹⁷ cm^?2, of which dpa are 5.83 and 11.65 respectively, a great amount of ribbon-like He bubbles with granular structure and cracks are presented at the depth of maximum concentration of deposited He atoms. The structural damage evolution and the mechanism of formation of He bubbles are discussed.     

Dose-dependent bonding environment of oxygen implanted in GaN

The bonding environment of oxygen implanted in GaN is studied using Near Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy. The implantation of 70 keV O ions in GaN results in the formation of a 200 nm – thick subsurface layer that is highly defective or amorphous depending on the implantation fluence which ranges from 1 × 10¹⁵ to 1 × 10¹⁷ cm^?2. The NEXAFS spectra are simulated using the FEFF8 code assuming models that account for the formation of point defects (various configurations of O interstitial and O substitutional in N and Ga sites) as well as chemical effects such as the formation of various polymorphs of Ga oxides and oxynitrides. The implantation-induced lattice disorder is modeled by displacing atoms from their equilibrium positions by adding to their Cartesian coordinates random numbers that belong to normal distributions. The simulations reveal that when the fluence is 1 × 10¹⁵ cm^?2, the O implants occupy interstitial sites preferentially in the empty channels aligned parallel to the c-axis in the plane that contains the Ga atoms and/or in the columns that consist of Ga and N atoms along the c-axis. When the fluence is equal to 1 × 10¹⁶ cm^?2 the O ions substitute for N while at 1 × 10¹⁷ cm^?2 they participate in the formation of mixed GaO_xN_y phases.