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.     

Evaluation of soft error rates using nuclear probes in bulk and SOI SRAMs with a technology node of 90 nm

The difference of soft error rates (SERs) in conventional bulk Si and silicon-on-insulator (SOI) static random access memories (SRAMs) with a technology node of 90 nm has been investigated by helium ion probes with energies ranging from 0.8 to 6.0 MeV and a dose of 75 ions/μm². The SERs in the SOI SRAM were also investigated by oxygen ion probes with energies ranging from 9.0 to 18.0 MeV and doses of 0.14–0.76 ions/μm². The soft error in the bulk and SOI SRAMs occurred by helium ion irradiation with energies at and above 1.95 and 2.10 MeV, respectively. The SER in the bulk SRAM saturated with ion energies at and above 2.5 MeV. The SER in the SOI SRAM became the highest by helium ion irradiation at 2.5 MeV and drastically decreased with increasing the ion energies above 2.5 MeV, in which helium ions at this energy range generated the maximum amount of excess charge carriers in a SOI body. The soft errors occurred by helium ions were induced by a floating body effect due to generated excess charge carriers in the channel regions. The soft error occurred by oxygen ion irradiation with energies at and above 10.5 MeV in the SOI SRAM. The SER in the SOI SRAM gradually increased with energies from 10.5 to 13.5 MeV and saturated at 18 MeV, in which the amount of charge carriers induced by oxygen ions in this energy range gradually increased. The computer calculation indicated that the oxygen ions with energies above 13.0 MeV generated more excess charge carriers than the critical charge of the 90 nm node SOI SRAM with the designed over-layer thickness. The soft errors, occurred by oxygen ions with energies at and below 12.5 MeV, were induced by a floating body effect due to the generated excess charge carriers in the channel regions and those with energies at and above 13.0 MeV were induced by both the floating body effect and generated excess carriers. The difference of the threshold energy of the oxygen ions between the experiment and the computer calculation might be due to the difference between the designed and real structures.     

The live cell irradiation and observation setup at SNAKE

We describe a new setup at the ion microprobe SNAKE (Superconducting Nanoscope for Applied nuclear (Kern-) physics Experiments) at the Munich 14 MV Tandem accelerator that facilitates both living cell irradiation with sub micrometer resolution and online optical imaging of the cells before and after irradiation by state of the art phase contrast and fluorescence microscopy. The cells are kept at standard cell growth conditions at 37 °C in cell culture medium. After irradiation it is possible to switch from single ion irradiation conditions to cell observation within 0.5 s. First experiments were performed targeting substructures of a cell nucleus that were tagged by TexasRed labeled nucleotides incorporated in the cellular DNA by 55 MeV single carbon ion irradiation. In addition we show first online sequences of short time kinetics of Mdc1 protein accumulation in the vicinity of double strand breaks after carbon ion irradiation.     

Aperture edge scattering in focused MeV ion beam lithography and nuclear microscopy: An application for the GEANT4 toolkit

Collimators are widely used to define MeV ion beams. Recent studies have shown the capability of combinations of collimators and lenses to define beams of MeV ions with sub-100 nanometre dimensions. Such nanometre beams have potential applications in MeV ion beam lithography, which is the only maskless technique capable of producing extremely high aspect ratio micro- and nano-structrures, as well as in high resolution MeV ion beam based imaging. The ion scattering from the collimator-edges can be a resolution restricting factor in these applications. Scattering processes at edges are difficult to study using conventional simulation codes because of the complicated geometry. In this work we overview the possibilities and pitfalls in using the GEANT4 toolkit as a simulation tool for studying the behaviour of ions impinging onto, or in close proximity to aperture edges. Results from simulations of scattering of 2 MeV protons incident on a 5 mm in diameter cylindrical beam defining tungsten carbide (WC) aperture blade, such as used in nuclear micro- and nanobeams as object and scraper apertures, are presented. The bubble formation at the aperture edges due to the implantation of H was first believed to cause edge roughening and hence the beam quality degradation. The concentration profile of implanted H in a WC cylinder shows that the bubble formation is not likely to be the edge roughening factor, but rather other mechanisms of beam induced topographical changes such as ion beam induced morphological changes and cracking of hydrocarbons.     

Development of a real-time beam current monitoring system for microbeam scanning-PIXE analysis using a ceramic channel electron multiplier

Microbeam scanning-PIXE (micro-PIXE) analysis is a useful method for obtaining information of multi-elemental distribution in samples by two-dimensional images of sample surfaces such as mammalian cells, tissues, and other environmental monitoring species. In addition to elemental distribution information, quantitative analysis is in demand for further investigations of environmental and biomedical studies concerning heavy metals accumulated in terms of cells and sub-cellular organelles. To make quantitative analysis possible, a real-time beam monitoring system that gives a precise number of ions, and an output independent from a sample that enables one to keep a beam resolution of micrometer size is required. In this paper, we report on the development of beam current monitoring. The beam current was monitored using a ceramic channel electron multiplier (CEM) to detect secondary electrons induced from a 50 nm thick carbon film (10 μg/cm²). This carbon film was attached to a sample holder, which was set at the targeted sample position. The output value of the CEM was proportional to the Faraday cup installed just after the sample position. The beam resolution was measured using off-axis STIM by scanning a copper grid, and was estimated at 1.79 and 1.72 μm for the horizontal and vertical directions, respectively, sufficient for routine micro-PIXE analysis.     

Elastic scattering of 7Li + 27Al at several angles in the 7–11 MeV energy range

Elastic cross sections for the ⁷Li + ²⁷Al system were measured at laboratory energies between 7 and 11 MeV in steps of 0.25 MeV, and angles between 135° and 170° in steps of 5°. Excitation functions for the elastic scattering were measured using an array of eight Si surface-barrier detectors whereas a solid-state telescope was used to estimate and subtract background from other reactions. Contamination from α particles arising from the ⁷Li breakup process at E_lab ? 10 MeV makes the use of these energies inadvisable for RBS applications. The present results are compared with previous data obtained at 165° (E_lab ? 6 MeV), 140° and 170° (E_lab ? 8 MeV). The experimental data were analyzed in terms of the Optical Model. Two different energy-independent potentials were found. These optical potentials allow an interpolation with physical meaning to other energies and scattering angles. The experimental cross sections will be uploaded to the IBANDL database.     

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.     

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.     

The structure of ion beam amorphised zirconolite studied by grazing angle X-ray absorption spectroscopy

Ti K edge X-ray absorption spectroscopy (XAS) was applied to determine the Ti co-ordination environment in the surface amorphised layer formed on zirconolite ceramics by 2 MeV Kr⁺ irradiation, to a fluence of 5 × 10¹⁵ ions cm^?2. The application of XAS in a grazing angle geometry was demonstrated to be essential in order to probe only the surface damaged layer (<1000 nm thick), in isolation of the undamaged interior of the specimen. 2 MeV Kr⁺ irradiation induced a change in the Ti co-ordination environment from majority six fold to majority five fold in the amorphised surface layer. This finding is consistent with the formation of five fold Ti in metamict natural zirconolite, as reported previously and confirmed in this study, despite the difference in dose rate of at least 10¹² between ion beam irradiated and naturally metamict materials. This study therefore opens the door to systematic investigation of composition – structure – property relations in materials designed for radioactive waste immobilisation, through the combined application of ion beam irradiation and grazing angle XAS.     

Thermal and irradiation induced interdiffusion in Fe3O4/MgO(0 0 1) thin film

The interface reactions in an epitaxial 10 nm-thick Fe₃O₄/MgO(0 0 1) film were investigated by using Rutherford Backscattering spectrometry (RBS), channeling (RBS-C) and X-ray reflectometry (XRR). The as-grown film had a good crystallinity indicated by the minimum yield and the half-angle value for Fe, respectively, χ_min(Fe) = 22% and ψ_1/2(Fe) = 0.62°. Annealing the films under partial argon pressure up to 600 °C led to a large enhancement of Mg out-diffusion into the film forming a wustite-type phase, but the total layer thickness did not change much. Ion irradiation of the film by 1 MeV Ar ion beam caused a strong Fe ion mixing resulting in a large interfacial zone with a thickness of 23 nm.     

Fabrication of nanowires by varying energy microbeam lithography using heavy ions at the TIARA

In TIARA facility of Japan Atomic Energy Agency (JAEA) Takasaki, we have produced three-dimensional micro/nano-structures with high aspect ratio using cross linking process based on negative resist such as SU-8 by a technique of mask less ion beam lithography. By bombarding high energy heavy ions such as 450 MeV Xe²³⁺ to SU-8, on the other hand, it appeared that a nanowire could be produced just with a single ion hitting. Then we tried to produce nanowires, of which both ends were fixed in the three-dimensional structure. This paper shows a preliminary experiment for this purpose using a combination of 15 MeV Ni⁴⁺ ion microbeam patterning and the 450 MeV ¹²⁹Xe²³⁺ hitting on SU-8.     

Ion beam induced luminescence of polyethylene terephthalate foils under MeV H and He ion bombardment

The evolution of the ion beam induced luminescence (IBIL) of the polyethylene terephthalate (PET) foils was studied under the irradiation of H and He ions of MeV energy. The optical and chemical changes of the samples were also examined by photo-stimulated luminescence and optical absorption measurements after the irradiation. A prominent broad emission peak of IBIL appeared at around 380 nm, and its intensity monotonically decreased during the ion irradiation. The decay curves of the emission intensity were quantitatively explained as a function of the electronic energy deposition of the incident H and He ions. On the contrary, to the decrease of the main emission peak, a growth of new peaks was observed in the wavelengths between 500 and 600 nm.     

Swift heavy ion induced modifications of optical and microstructural properties of silver–fullerene C60 nanocomposite

In this paper, we study the optical and microstructural properties of silver–fullerene C₆₀ nanocomposite and their modifications induced by swift heavy ion irradiation. Silver nanoparticles embedded in fullerene C₆₀ matrix were synthesized by co-deposition of silver and fullerene C₆₀ by thermal evaporation. The nanocomposite thin films were irradiated by 120 MeV Ag ions at different fluences ranging from 1 × 10¹² to 3 × 10¹³ ions/cm². Optical absorption studies revealed that the surface plasmon resonance of Ag nanoparticles showed a blue shift of ～49 nm with increasing ion fluence up to 3 × 10¹³ ions/cm². Transmission electron microscopy and Rutherford backscattering spectroscopy were used to quantify particle size and metal atomic fraction in the nanocomposite film. Growth of Ag nanoparticles was observed with increasing ion fluence. Raman spectroscopy was used to understand the effect of heavy ion irradiation on fullerene matrix. The blue shift in plasmonic wavelength is explained by the transformation of fullerene C₆₀ matrix into amorphous carbon.     

Nanoparticle architecture in carbonaceous matrix upon swift heavy ion irradiation of polymer–metal nanocomposites

Distinct nanoparticle self-organization in the nanocomposites (∼100 nm) of Teflon AF containing different metallic clusters is reported upon swift heavy ion irradiation of 120 MeV Au beams at different ion fluences ranging from 1 × 10¹¹ to 3 × 10¹² ions/cm². Two dimensionally distributed Au clusters are found to be transformed into long cluster chains of seemingly helical pattern in the organic matrix like pearls on a string. Comparatively diluted three dimensionally arranged Ag nanoparticles are observed to be concentrated in the formed mesh of carbon-enriched nanoregions upon irradiation. The nanoparticle self-organization in such carbonaceous nanowires (diameter ∼ 25 nm) finally leads to a quasi-one-dimensional distribution at the highest fluence with several particles apparently being aligned. It appears most probable that a high Au cluster concentration in the polymer matrix leads to direct ion–cluster interaction. This probably initiates irradiation-enhanced and thermally assisted diffusion of the clusters coupled with intermixing in the polymer layers. Moving clusters are assumed to be trapped in the ion beam induced additional free volume leading to a long string of helical-type nanoscale configuration. On the other hand, with diluted clusters arrangement, irradiation induced electronically excited inter-cluster organic regions are interpreted to act as trapping centres for the nanoparticles that self-organize along the ion damaged zones. Transmission electron microscopic investigations have been applied to analyse the irradiated and pristine nanocomposites.     

Annealing of ion implanted 4H–SiC in the temperature range of 100–800 °C analysed by ion beam techniques

Ion implantation induced damage formation and subsequent annealing in 4H–SiC in the temperature range of 100–800 °C has been investigated. Silicon Carbide was implanted at room temperature with 200 keV ⁴⁰Ar ions with two implantation fluences of 4 × 10¹⁴ and 2 × 10¹⁵ ions/cm². The samples were characterized by Rutherford backscattering and nuclear reaction analysis techniques in channeling mode using 2.00 and 4.30 MeV ⁴He ion beams for damage buildup and recovery in the Si and C sublattices, respectively. At low ion fluence, the restoration of the Si sublattice is evident already at 200 °C and a considerable annealing step occurs between 300 and 400 °C. Similar results have been obtained for the C sublattice using the nuclear resonance reaction for carbon, ¹²C(α,α)¹²C at 4.26 MeV. For samples implanted with the higher ion fluence, no significant recovery is observed at these temperatures.     

Excitation functions for proton-induced reactions on natural hafnium: Production of 177Lu for medical use

There is an increasing interest in using radioisotopes of rare earth elements for internal radiotherapy and for imaging in nuclear medicine. ¹⁷⁷Lu is one of the promising radionuclides. This article reports on the first measurements of the excitation function for the production of ¹⁷⁷Lu with proton-beam energies up to 17 MeV on natural hafnium targets. The experimental cross sections for the reaction ^natHf(p,x)¹⁷⁷Lu were obtained by the activation of a stacked-foil target and subsequent gamma spectrometry. Theoretical cross sections were calculated up to 35 MeV with the EMPIRE nuclear reaction model code. The measured and calculated cross sections were used for deriving the thick-target yields and for estimating the production of other nuclides than ¹⁷⁷Lu. Measured production cross sections of ^{175,176,177,178}Ta on the same target are also presented.     

SHI induced re-crystallization of Ge implanted SiO2 films

Ge nanocrystals embedded in SiO₂ matrix have been synthesized by swift heavy ion irradiation of Ge implanted SiO₂ films. In the present study, 400 keV Ge⁺ ions were implanted into SiO₂ films at dose of 3 × 10¹⁶ ions/cm² at room temperature. The as-implanted samples were irradiated with 150 MeV Ag¹²⁺ ions with various fluences. Similarly 400 keV Ge⁺ ions implanted into Silicon substrate at higher fluence at 573 K have been irradiated with 100 MeV Au⁸⁺ ions at room temperature (RT). These samples were subsequently characterized by XRD and Raman to understand the re-crystallization behavior. The XRD results confirm the presence of Ge crystallites in the irradiated samples. Rutherford backscattering spectrometry (RBS) was used to quantify the concentration of Ge in the SiO₂ matrix. Variation in the nanocrystal size as a function of ion fluence is presented. The basic mechanism of ion beam induced re-crystallization has been discussed.     

Development of CrN precipitates during the initial stages of PIII nitriding of stainless steel thin films

Stainless steel thin films produced by ion beam sputtering (IBS) were used as a model system to investigate the nitrogen diffusion and CrN formation after 10 min of nitrogen plasma immersion ion implantation (PIII) at 350 °C and 450 °C. At 350 °C, a thin nitrided layer of 70 nm is formed, with additional diffusion of nitrogen along grain boundaries and the growth of CrN precipitates along these grain boundaries. For 450 °C, a complete nitriding of the whole 400 nm thick layer was observed, with the lower 75 nm consisting of an expanded phase and the upper 330 nm of a decomposed phase with CrN precipitates formed inside the original grains. Such a layered structure capturing the transformation process has not been observed before. A determination of time–temperature dependencies of this process and the transfer of these results for bulk material should be possible.     

Investigation of avalanche silicon detectors for low energy single ion implantation applications

Avalanche silicon photodiodes have potential applications to detect low energy single ions for counting single ion impacts in shallow implant depths for the deterministic doping of nanoscale electronic devices. This paper reports the investigation of avalanche photodiode detectors in the linear operation mode for detection of 0.5–2 MeV helium ions. The measured charge gain was found to be up to 100 depending on bias voltage. The charge gain was found to saturate at a level that correlated with the ion stopping depth in silicon. The measured charge gain for energetic ions, which have a well-defined depth in a silicon substrate for the deposition of ionization energy, is compared with that of X-rays and photons, which deposit the ionization energy over a wider range of depth. This allowed the identification of a suitable structure for an avalanche photodiode optimised for the detection of sub-10 keV heavy ions with an internal charge gain above 10 achievable. This offers significant advantages over conventional PIN devices where the signals from such ions would be lost in the noise.     

Photon production through multi-step processes important in nuclear resonance fluorescence experiments

We present calculations describing the production of photons through multi-step processes occurring when a beam of gamma-rays interacts with a macroscopic material. These processes involve the creation of energetic electrons through Compton scattering, photo-absorption and pair production, the subsequent scattering of these electrons, and the creation of energetic photons occurring as these electrons are slowed through Bremsstrahlung emission. Unlike single Compton collisions, during which an energetic photon that is scattered through a large angle loses most of its energy, these multi-step processes result in a sizable flux of energetic photons traveling at large angles relative to an incident photon beam. These multi-step processes are also a key background in experiments that measure nuclear resonance fluorescence by shining photons on a thin foil and observing the spectrum of back-scattered photons. Effective cross sections describing the production of back-scattered photons are presented in a tabular form that allows simple estimates of backgrounds expected in a variety of experiments. Incident photons with energies between 0.5 MeV and 8 MeV are considered. These calculations of effective cross sections may be useful for those designing NRF experiments or systems that detect specific isotopes in well-shielded environments through observation of resonance fluorescence.