Development of a TOF-ERDA measurement system for analysis of light elements using a He beam

A time-of-flight ERDA (TOF-ERDA) measurement system has been developed for the analysis of light elements. He ions are used for the incident beam, and recoil light ions are detected with the system. The system consists of a time detector and a silicon detector, and energy and velocity of recoil ion are measured simultaneously. The depth resolution of 21.6 ± 2.2 nm (FWHM) has been obtained by an ERDA measurement of a thin carbon layer onto a silicon wafer using a 5.7 MeV He beam. The mass resolution is better than 1 for elements up to oxygen. Maximum detectable depth of carbon in a PET film is about 650 nm. An ERDA measurement of implanted carbon in a silicon wafer has been demonstrated.     

Micro-ERDA,micro-RBS and micro-PIXE techniques in the investigation of fish otoliths

Elemental distribution in the otolith of the fresh water fish burbot (Lota lota L.) collected in Hungary was measured with Elastic Recoil Detection Analysis (ERDA), Rutherford Backscattering Spectrometry (RBS) and as a complementary technique, Particle-Induced X-ray Emission (PIXE) with a focussed ion beam of 1.5 × 1.5 μm² spot size. The organic- and inorganic-rich regions of the otolith are distinguished and they are presented as hydrogen and calcium maps at depth regions of 0–70, 70–140 and 140–210 nm. The textured surface of the sample and its porosity were characterized from the effect on the RBS spectra. The oxygen and carbon PIXE elemental maps can also be used to identify the organic- and inorganic-rich regions of the otolith. The calcium map was found to be more homogeneous because the otolith structure is averaged in a larger depth. The trace elements Fe, Zn and Sr were detected only in very low concentration by micro-PIXE.     

Determination of the local gold contact morphology on a photoactive polymer film using nanobeam GISAXS

Grazing incidence small-angle X-ray scattering is performed with a nanometer sized X-ray beam (nGISAXS) to probe the local gold contact morphology on a photoactive polymer film. By evaporation a 50 nm thick gold contact is installed on a diblock copolymer film, which consists of a non-conducting poly(styrene) (PS) and a semi-conducting poly(paraphenylene) (PPP) block. The region around the edge of the gold contact of 200 μm is probed with nGISAXS by scanning the sample position in steps of 1 μm with respect to the X-ray beam. The diblock copolymer film has a densely packed micellar structure with a characteristic distance between adjacent micelles of 19 nm which is unaffected by the gold deposition. The gold contact exhibits a tail region which extends its lateral dimension. For the full extended surface area of the gold contact with its tails an interdiffusion of gold into the diblock copolymer film is observed. For comparison imaging ellipsometry, atomic force microscopy and optical microscopy measurements are performed.     

Fabrication of a microreactor by proton beam writing technique

Microreactors are innovative and promising tools in technology nowadays because of their advantages compared to the conventional-scale reactors. These advantages include vast improvements in surface to volume ratio, energy efficiency, reaction speed and yield and increased control of reaction conditions, to name a few examples.The high resolution capability of the micromachining technique utilizing accelerated ion beams in the fabrication technology of microreactors has not yet been taken advantage of. In this work we present the design of a prototype micro-electrochemical cell of 1.5 μL volume (2.5 × 2.5 × 0.240 mm) created with a 3 MeV proton microbeam. The cell can be separated into two half-cells with a suitable membrane applicable to galvanic or fuel cells as well. We deposited gold electrodes on both of the half-cells.The operability of the device was demonstrated by electric current flow between the two electrodes in this micro-electrochemical cell containing a simple electrolyte solution. We used a polycapillary film to separate the two half-cells, hindering the mixing of the anolyte and catholyte solutions. As a result of the minimal mixing caused by the polycapillary film, this cell design can be suitable for electro-synthesis. Due to the high resolution of proton beam writing, it is planned to reduce the dimensions of this kind of microreactor.     

Rearranging a nanoprobe: Line foci,grid shadow patterns and performance tests

After a major modification of the target chamber at the Leipzig high energy ion nanoprobe the probe forming lens system, consisting of two separated quadrupole doublets, had been carefully realigned. This was done by adjusting the line foci position of each individual quadrupole on the centre position defined by the unfocused beam. Using a high magnification microscope the alignment process is very effective and precise. The lens system could be precisely realigned except an intrinsic rotational misalignment which is essentially reduced by a correction lens.Grid shadow patterns have been taken and analysed in order to assess the characteristics of the system. The dominant aberrations are spherical with an additional parasitic octupole.The grid shadow method is also very useful to determine the best position of the aperture diaphragms which minimizes the influence of the aberrations onto the beam spot size.The rearrangement allowed larger aperture diaphragms for higher beam currents at a moderate increase in beam spot sizes. Performance tests yielded proton microbeam currents and half-widths of 4.5 nA at 1.5 μm, 8.3 nA at 1.5 μm and 17.2 nA at 2 μm. For high resolution work the expected beam spots around 0.3 μm at 100 pA were not achieved. The reason is very likely interference on the beam scanner, correlated in x- and y-direction, which results from the insufficiently rectified power supply voltage of the transconductance amplifier.     

Developments in micro-sample 14C AMS at the ANTARES AMS facility

We continue development of micro-sample radiocarbon sample preparation and AMS measurement at the ANTARES AMS facility. We routinely prepare samples containing 10–200 μg of carbon using an iron catalyst with an excess of hydrogen in ～2.5 mL graphitisation reactors. These use a tube furnace to heat the catalyst to 600 °C and a Peltier-cooled water trap. Samples containing just a few micrograms of carbon can be prepared. We describe progress with a 0.5 mL laser-heated ‘microfurnace’ we are developing for the rapid and efficient graphitisation of ～5 μg samples. Following operating experience with a prototype unit, work has commenced on the development of a second-generation device with the goal of fully automated operation with minimal introduction of extraneous carbon.Key to development of micro-sample ¹⁴C AMS is the ability to reliably handle the graphite/iron sample and to mount it in the ion source target holder. We have developed a target holder that permits the sample to be loaded in a 1 mm diameter recess and rear pressed, ensuring a high quality surface finish, at a reproducible depth. Additionally we have developed a method for systematically aligning the sample stage with the cesium beam following ion source servicing.     

Porous iron pellets for AMS 14C analysis of small samples down to ultra-microscale size (10–25 μgC)

We developed the use of a porous iron pellet as a catalyst for AMS ¹⁴C analysis of small samples down to ultra-microscale size (10–25 μgC). It resulted in increased and more stable beam currents through our HVEE 4130 ¹⁴C AMS system, which depend smoothly on the sample size. We find that both the expected decrease of oxalic acid standards and increase of backgrounds with decreasing sample size, due to increasing influence of contamination, are reproducible. Using a mass-dependent background correction for dead (1.0 ± 0.4 μgC) and modern (0.25 ± 0.10 μgC) contamination, we obtain reliable results for small samples down to 10 μgC and possibly smaller. Due to our low graphitization yield for ultra-small samples (increases from 40% to 80% on average with sample size), we measured graphite standards as small as 3 μgC. The standard deviation of the corrected activity is about 5% for a 10-μgC HOxII standard.Here we report the iron pellet technique, which is new to the best of our knowledge. It is generally applicable for AMS ¹⁴C laboratories that want to measure small samples down to ultra-microscale size. As an illustrative test-case, we analyze ¹⁴C data for IAEA-C5, C7 and C8 samples with masses ranging from 15 to 300 μgC.     

Carbon film growth and hydrogenic retention of tungsten exposed to carbon-seeded high density deuterium plasmas

Tungsten (W) targets have been exposed to high density (n_e ? 4 × 10¹⁹ m^?3), low temperature (T_e ? 3 eV) CH₄-seeded deuterium (D) plasma in Pilot-PSI. The surface temperature of the target was ～1220 K at the center and decreased radially to ～650 K at the edges. Carbon film growth was found to only occur in regions where there was a clear CII emission line, corresponding to regions in the plasma with T_e ? 2 eV. The maximum film thickness was ～2.1 μm after a plasma exposure time of 120 s. ³He nuclear reaction (NRA) analysis and thermal desorption spectroscopy (TDS) determine that the presence of a thin carbon film dominates the hydrogenic retention properties of the W substrate. Thermal desorption spectroscopy analysis shows retention increasing roughly linearly with incident plasma fluence. NRA measures a C/D ratio of ～0.002 in these films deposited at high surface temperatures.     

Inactive and mutagenic effects induced by carbon beams of different LET values in a red yeast strain

To evaluate biological action of microorganism exposed to charged particles during the long distance space exploration, induction of inactivation and mutation in a red yeast strain Rhodotorula glutinis AY 91015 by carbon beams of different LET values (14.9–120.0 keV μm^?1) was investigated. It was found that survival curves were exponential, and mutation curves were linear for all LET values. The dependence of inactivation cross section on LET approached saturation near 120.0 keV μm^?1. The mutation cross section saturated when LET was higher than 58.2 keV μm^?1. Meanwhile, the highest RBE_i for inactivation located at 120.0 keV μm^?1 and the highest RBE_m for mutation was at 58.2 keV μm^?1. The experiments imply that the most efficient mutagenic part of the depth dose profile of carbon ion is at the plateau region with intermediate LET value in which energy deposited is high enough to induce mutagenic lesions but too low to induce over kill effect in the yeast cells.     

Experimental set-up for time resolved small angle X-ray scattering studies of nanoparticles formation using a free-jet micromixer

Recently, we have designed, fabricated and tested a free-jet micromixer for time resolved small angle X-ray scattering (SAXS) studies of nanoparticles formation in the <100 μs time range. The microjet has a diameter of 25 μm and a time of first accessible measurement of 75 μs has been obtained. This result can still be improved. In this communication, we present a method to estimate whether a given chemical or biological reaction can be investigated with the micromixer, and to optimize the beam size for the measurement at the chosen SAXS beamline. Moreover, we describe a system based on stereoscopic imaging which allows the alignment of the jet with the X-ray beam with a precision of 20 μm. The proposed experimental procedures have been successfully employed to observe the formation of calcium carbonate (CaCO₃) nanoparticles from the reaction of sodium carbonate (Na₂CO₃) and calcium chloride (CaCl₂). The induction time has been estimated in the order of 200 μs and the determined radius of the particles is about 14 nm.     

Pulsed repetition rate nanosecond laser heating and ablation of the tokamak graphite tile deposited layers

Laser heating and ablation of the plasma-facing surface of a graphite tile from TEXTOR tokamak that was covered by a deposited carbon layer has been studied. Laser heating measurements were performed with a pulsed nanosecond Nd-YAG laser (2nd harmonic, 10 kHz repetition rate, 100 ns pulse duration). Surface temperature measurements were recorded with a home-made pyrometer having a response time of 15 μs (t_99%). The experimental results are simulated with an analytical model of laser heating of a surface covered by a deposited layer and heated repeatedly by laser pulses. The comparison between experimental and theoretical data of the observed temperature excursions enables us to assess the deposited carbon layer physical parameters (thermal conductivity, porosity, etc.) if the thermal and optical properties of the graphite substrate are known. Laser ablation measurements were performed with two pulsed nanosecond Nd-YAG lasers (20 Hz and 10 kHz repetition rate with 5 ns and 100 ns pulse duration, respectively). For a plasma-facing graphite surface covered by a thick (～30–50 μm) deposited carbon layer, the ablation threshold is 4.5 ± 1 kJ/m² regardless of the pulse duration. The obtained ablation threshold is significantly lower than the one measured for a virgin tokamak graphite sample. The comparison of the experimental results and theoretical data demonstrated that the laser ablation mechanisms for tokamak graphite and thick carbon layers deposited on plasma-facing surface are different.     

The impact of thermal fatigue and carbidization on the W coatings deposited on CFC tiles for the ITER-like Wall project at JET

Since August 2011 JET operates with the ITER-like wall comprising bulk Be tiles, bulk W tiles and W coated CFC tiles with a thickness of 10–15 μm and 20–25 μm. In order to evaluate behavior of the W coatings to a cyclic thermal loading relevant to JET operation, high heat flux (HHF) tests have been carried out up to 5100 pulses with an electron beam facility at peak temperatures of 1000 °C, 1250 °C and 1450 °C. The pulse duration was 24 s. Optical inspections of the W layer performed periodically by interrupting the test revealed small delaminations with the size of 50–500 μm. The dependence of the delamination percentage on the number of pulses can be seen as a degradation curve for each particular W coating. In this way the thermo-mechanical properties of the W coatings can be characterized quantitatively. Thermal fatigue and carbidization of the tungsten due to the diffusion of the carbon from the substrate have been recognized as mechanisms for degradation of the coatings. Tungsten carbides have been identified by using TEM (transmission electron microscopy) diffraction analysis on FIB (focused ion beam) prepared cross-section samples subjected to HHF tests. Nano-pores developed at the CFC–Mo and Mo–W interfaces during the tests might be also responsible for the degradation of the coating.     

Ion beam mixing in uranium nitride thin films studied by Rutherford Backscattering Spectroscopy

Thickness, composition, concentration depth profile and ion irradiation effects on uranium nitride thin films deposited on fused silica have been investigated by Rutherford Backscattering Spectroscopy (RBS) using 2 MeV He⁺ ions. The films were prepared by reactive DC sputtering at the temperatures of ?200 °C, +25 °C and +300 °C. A perfect 1U:1N stoichiometry with a layer thickness of 660 nm was found for the film deposited at ?200 °C. An increase of the deposition temperature led to an enhancement of surface oxidation and an increase of the thickness of the mixed U–N–Si–O layers at the interface. The sample irradiation by 1 MeV Ar⁺ ion beam with ion fluence of about 1.2–1.7 × 10¹⁶ ions/cm² caused a large change in the layer composition and a large increase of the total film thickness for the films deposited at ?200 °C and at +25 °C, but almost no change in the film thickness was detected for the film deposited at +300 °C. An enhanced mixing effect for this film was obtained after further irradiation with ion fluence of 2.3 × 10¹⁶ ions/cm².     

Micro and nano patterning by focused ion beam enhanced adhesion

We report a new method of generating nano and micro patterns using focused ion beam (FIB) induced adhesion. The method utilizes selective irradiation of thin metallic films grown on substrates by focused ion beam followed by peel off. After peel off of the irradiated thin film it is observed that the ion beam scanned portions are retained on the substrate, creating nano and micro patterns. The method is suitable for materials of which the adhesion to the substrate can be improved by ion bombardment. The phenomenon has been demonstrated by creating gold nano patterns of different shapes and sizes ranging from 500 nm to 5 μm on SiO₂–Si substrate using 10–30 keV Ga FIB at beam currents up to 10 pA. The mechanism involved in the process has been discussed. The technique could be utilized to prepare micro and nano patterns of thin films deposited on an appropriate substrate for optical, plasmonic and sensor related applications.     

Biological studies using mammalian cell lines and the current status of the microbeam irradiation system,SPICE

The development of SPICE (single-particle irradiation system to cell), a microbeam irradiation system, has been completed at the National Institute of Radiological Sciences (NIRS). The beam size has been improved to approximately 5 μm in diameter, and the cell targeting system can irradiate up to 400–500 cells per minute. Two cell dishes have been specially designed: one a Si₃N₄ plate (2.5 mm × 2.5 mm area with 1 μm thickness) supported by a 7.5 mm × 7.5 mm frame of 200 μm thickness, and the other a Mylar film stretched by pressing with a metal ring. Both dish types may be placed on a voice coil stage equipped on the cell targeting system, which includes a fluorescent microscope and a CCD camera for capturing cell images. This microscope system captures images of dyed cell nuclei, computes the location coordinates of individual cells, and synchronizes this with the voice coil motor stage and single-particle irradiation system consisting of a scintillation counter and a beam deflector. Irradiation of selected cells with a programmable number of protons is now automatable. We employed the simultaneous detection method for visualizing the position of mammalian cells and proton traversal through CR-39 to determine whether the targeted cells are actually irradiated. An immuno-assay was also performed against γ-H2AX, to confirm the induction of DNA double-strand breaks in the target cells.     

Applications to cultural heritage diagnostics at the new nuclear microprobe beam line at CEDAD

A nuclear microprobe beam line has been installed at CEDAD (Centre for Dating and Diagnostics), University of Salento, Lecce, Italy. The beam line is connected to the ?30° port of the high energy switching magnet of a 3 MV HVEE 4130HC Tandetron accelerator. It is based on an Oxford Microbeam magnetic quadrupole triplet and its general features are presented. The results of functional tests are presented showing how a lateral spatial resolution as low as ～2 μm has been achieved in vacuum by analysing standard reference material. The results obtained in the analysis of ancient radiocarbon dated biological tissues are presented for the identification and distribution of toxic elements such as Pb.     

Development of W coatings for fusion applications

The paper gives a short overview on tungsten (W) coatings deposited by various methods on carbon materials (carbon fibre composite – CFC and fine grain graphite – FGG). Vacuum Plasma Spray (VPS), Chemical Vapor Deposition (CVD) and Physical Vapor Deposition (PVD) techniques are analyzed in respect with the characteristics and performances of the W coatings.A particular attention is paid to the Combined Magnetron Sputtering and Ion Implantation (CMSII) technique, which was developed during the last 4 years from laboratory to industrial scale and it is successfully applied for W coating (10–15 μm and 20–25 μm) of more than 2500 tiles for the ITER-like Wall project at JET and ASDEX Upgrade. This technique involves simultaneously magnetron sputtering and high energy (tens of keV) ion implantation. Due to the ion bombardment a stress relief occurs within the coating enabling its growth without delamination to a relatively large thickness. In addition, in order to adjust the thermal expansion mismatch between CFC and W, a Mo interlayer of 2–3 μm is currently used. Experimentally, W/Mo coatings with a thickness up to 50 μm were produced and successfully tested in the GLADIS ion beam facility up to 23 MW/m².     

Study on time resolution of single event TOF-RBS measurement

Flight paths and times of secondary electrons, induced by a focused ion beam, from a sample to a secondary electron detector (SED), were simulated with various shield shapes of a SED for improving the time resolution of time-of-flight Rutherford backscattering spectrometry (TOF-RBS) using the secondary electron signal as a start signal, the results of which were compared with experimental time resolutions of the TOF-RBS measurement. The fluctuation in the flight path and, hence, flight time of the secondary electron deteriorates the time resolution of TOF-RBS. The simulated flight time differences for SEDs with or without a shield were 4.4–41 ns with a shield and 1.0 ns without a shield, respectively, indicating that the SED without the shield would improve the time resolution of the single event TOF-RBS. The time resolutions of TOF-RBS using 150 keV Be⁺ for Au/Si sample with SEDs with and without a shield were 5.6–9.2 and 4.4 ns, respectively. The improved time resolution for SEDs without the shield was confirmed experimentally.     

Angular and lateral spreading of ion beams in biomedical nuclear microscopy

Nuclear scattering from target atoms gives rise to a spatial broadening of energetic ion beams penetrating matter. The spatial broadening of the ion beam presents an ultimate limit to the resolving power that can be achieved in nuclear microscopy methods. The pressing of the attainable resolution limit in biomedical nuclear microscopy to dimensions approaching 10 nm, or so, implies the fundamental limitation from ion-target scattering will become increasingly significant. This effect has been investigated by a combined analytical and numerical computational approach to determine the extent and how single and multiple scattering processes limit the resolution for analysis with 2 MeV ⁴He and ¹H ions of realistic biomedical samples. The cases studied were direct-Scanning Transmission Ion Microscopy (direct-STIM), Particle Induced X-ray Emission (PIXE) studies of 20 μm tissue sections and in vivo single-ion irradiation of cells.     

The improved STIM tomography set-up at LIPSION: Three-dimensional reconstruction of biological samples

The feasibility of tomographic reconstruction of biological specimens using scanning transmission ion microscopy (STIM) has already been demonstrated in the past. However, in previous experiments at Leipzig the resolution was limited by an insufficient accuracy of goniometer motion, which resulted in a blurred alignment of the projections. The new stage and goniometer at the LIPSION accelerator laboratory allow a more precise rotation of the sample. Furthermore, a new software was developed, which includes efficient algorithms to correct misalignment errors. STIM tomography experiments using a proton and a molecular beam respectively were carried out on a rust mite (Aculus schlechtendali), on average 25 μm thick, and on unicellular organisms (Thaumatomonas coloniensis) with a diameter below 5 μm. The backprojection of filtered projections (bfp) algorithm was employed for the three-dimensional reconstruction. The reconstruction revealed many structural details including spherical grains of higher density inside the mite’s body of yet unknown origin.