Technical description of the CENBG nanobeam line

Two years ago, the CENBG has commissioned the AIFIRA (Application Interdisciplinaire des Faisceaux d’Ions en Aquitaine) facility for the development of an interdisciplinary research program based on a 3.5 MV Singletron^? accelerator (HVEE, The Netherlands). In addition to the existing beam lines, this facility is being equipped with a high demagnification focused beam line allowing the focusing of protons, deuterons and alpha particles down to a sub-micrometer resolution. This so-called “nanobeam line”, based on a long working distance doublet–triplet of Oxford Microbeams Ltd., OM-50^? quadrupoles, is at its final stage of development. The chosen layout of the beam line has been computed in details using the GEANT4 simulation toolkit. In the simulations, experimental measurements of the beam emittance at the entrance slits have been used to obtain more realistic beam distributions and intensities along the full beam line. According to these simulations, a beam resolution of about 300 nm in high current mode and below 100 nm in STIM mode is expected. The components of the beam line have been mounted at the 0° output of the Singletron^? switching magnet and the fine alignment will be performed using the ion beam in the coming weeks.In the present paper, all the major components of the CENBG nanobeam line are described in details.     

First direct-write lithography results on the Guelph high resolution proton microprobe

The recently completed high-resolution proton microprobe at the University of Guelph is Canada’s first one-micron nuclear microprobe, which represents the country’s state-of-the-art technology for various nuclear microprobe applications, e.g. direct-write microlithography. Its probe-forming system is comprised of a triplet Oxford Micro beams magnetic quadrupole lenses, along with high-precision objective slits. High energy protons coming off a 3 MV particle accelerator can achieve a nominal resolution of one micro and a beam current of several hundred of picoamperes when arriving at the target. This proton probe is ideal for the use of direct-write lithography with the incorporation of a magnetic scanning system and motorized sample stage.Preliminary lithography results have been obtained using spin-coated PMMA photoresist as specimen. The beam spot size, beam range and straggling inside the substrate and the exposure conditions are investigated by using scanning electron microscopy. This facility is the first in Canada to perform focused direct-write ion beam lithography, which is ideal for modification and machining of polymer and semiconductor materials for biological, microfluidic and ultimate lab-on-chip applications.     

Design of a compact focusing lens system with short acceleration tube at 300 kV

A compact focusing lens system with high demagnification over 1500 was designed to form an ion nanobeam with 346 keV energy by adding a short distance acceleration tube for beam acceleration and focusing downstream of the existing double acceleration lens system. The demagnification, focusing points and aberrations of the acceleration tube were studied using beam trajectory calculation. The acceleration tube was designed to have a length of 140 mm and a demagnification of 2 at its acceleration tube voltage of 300 kV, which resulted in a new compact focusing lens system with a total length of about 640 mm. In addition, the maximum voltage and electric-field of the acceleration tube were confirmed experimentally on the built device to be 300 kV and 30 kV/cm, respectively. The final beam size formed by the system was estimated to be 130 nm in diameter using the design parameters. The result suggests that an ion nanobeam of 346 keV can be formed by an apparatus having the reasonable length of 2 m, which permits us to develop a system for 1 MV by elongating its tube length.     

A beam optics study of the biomedical beam line at a proton therapy facility

A biomedical beam line has been designed for the experimental area of a proton therapy facility to deliver mm to sub-mm size beams in the energy range of 20-50 MeV using the TRANSPORT/TURTLE beam optics codes and a newly-written program. The proton therapy facility is equipped with a 230 MeV fixed-energy cyclotron and an energy selection system based on a degrader and slits, so that beam currents available for therapy decrease at lower energies in the therapeutic beam energy range of 70-230 MeV. The new beam line system is composed of an energy-degrader, two slits, and three quadrupole magnets. The minimum beam sizes achievable at the focal point are estimated for the two energies of 50 and 20 MeV. The focused FWHM beam size is approximately 0.3 mm with an expected beam current of 20 pA when the beam energy is reduced to 50 MeV from 100 MeV, and roughly 0.8 mm with a current of 10 pA for a 20 MeV beam.     

First results obtained using the CENBG nanobeam line: Performances and applications

A high resolution focused beam line has been recently installed on the AIFIRA (“Applications Interdisciplinaires des Faisceaux d’Ions en Région Aquitaine”) facility at CENBG. This nanobeam line, based on a doublet-triplet configuration of Oxford Microbeam Ltd. OM-50™ quadrupoles, offers the opportunity to focus protons, deuterons and alpha particles in the MeV energy range to a sub-micrometer beam spot. The beam optics design has been studied in detail and optimized using detailed ray-tracing simulations and the full mechanical design of the beam line was reported in the Debrecen ICNMTA conference in 2008. During the last two years, the lenses have been carefully aligned and the target chamber has been fully equipped with particle and X-ray detectors, microscopes and precise positioning stages. The beam line is now operational and has been used for its first applications to ion beam analysis. Interestingly, this set-up turned out to be a very versatile tool for a wide range of applications. Indeed, even if it was not intended during the design phase, the ion optics configuration offers the opportunity to work either with a high current microbeam (using the triplet only) or with a lower current beam presenting a sub-micrometer resolution (using the doublet-triplet configuration).The performances of the CENBG nanobeam line are presented for both configurations. Quantitative data concerning the beam lateral resolutions at different beam currents are provided. Finally, the first results obtained for different types of application are shown, including nuclear reaction analysis at the micrometer scale and the first results on biological samples.     

Creation of 3D microsculptures in PMMA by multiple angle proton irradiation

In recent years the technique of proton beam writing has established itself as a versatile method for the creation of microstructures in resist materials. While these structures can be almost arbitrary in two dimensions, the creation of genuine 3D structures remains a challenge.At the LIPSION accelerator facility a new approach has been developed which combines aspects of ion beam tomography, so far solely an analysis method, with proton beam writing. Key element is the targeted irradiation from multiple angles in order to obtain a much broader range of 3D microstructures than has hitherto been possible.PMMA columns with a diameter of ∼90 μm were used as raw material and placed in an upright position on top of a rotational axis. Using 2.25 MeV protons patterns corresponding to the silhouettes of the desired structures were written from two or more directions. In a subsequent step of chemical etching irradiated portions were dissolved, leaving behind the finished 3D sculpture.Various objects have been created. For the demonstration of the method a 70 μm high model of the Eiffel tower has been sculpted by irradiation from two angles. Using irradiation from three angles a 40 μm wide screw with right-handed thread could be crafted which might find applications in micromachining. Also, a cage structure with a pore size of ca. 20 μm was written with the intention to use it as a scaffold for the growth of biological cells.     

Biomedical research at LIPSION - Present state and future developments

Since its commissioning in 1998 the high energy ion nanoprobe LIPSION has been developed into a versatile tool for a variety of applications in biomedical research. It includes quantitative trace element analysis with sub-micron spatial resolution and 3D-element imaging, as well as 2D- and 3D-microscopy of density distributions. The analytical methods base on particle induced X-ray emission spectrometry (PIXE) and PIXE-tomography, Rutherford backscattering spectrometry (RBS), as well as scanning transmission ion microscopy (STIM) and STIM-tomography.The continuous developments led to improved capabilities for trace element analysis. For sub-micron analysis the spatial resolution could be improved to 0.3 μm for high resolution work and to 0.5 μm for routine analysis. On the other hand, LIPSION was optimized for high sample throughput in quantitative element imaging maintaining a lateral resolution of 1-2 μm. Recently the methods of PIXE- and STIM-tomography of biological specimens have been extended to limited angle tomography to avoid the complicated preparation of free-standing samples.Besides its analytical applications, the nanoprobe is also used for targeted irradiation of living cells with counted single ions for radiobiological research. It is capable of irradiating up to 20,000 cells per hour. Furthermore, we have developed a technique to achieve confined cell growth based on the proton beam writing technique (PBW) and agar. The paper presents an overview of the current biomedical research fields at LIPSION and gives an outlook on prospective developments.     

Creation of microstructures using heavy ion beam lithography

In this work, three-dimensional (3D) structures were produced in PMMA and CR-39 polymer resists using a carbon ion microbeam. To investigate possible advantages of heavy ions compared to the well-established proton beam lithography, the same resist materials were also irradiated with protons that had a range in the materials studied here similar to that of carbon ions. The microstructures produced in different resists were analysed after chemical etching. The quality of the bottom and side walls of the structures produced by protons and carbon ions were compared using scanning electron microscopy (SEM) and atomic force microscopy (AFM). The results showed that, for the resist materials tested, lithographic structures made with the 8 MeV carbon beam had more rough lateral and bottom surfaces compared to those made with 0.6 MeV proton beam lithography.     

Development of a high intensity Al beam from SiC targets for accelerated beam experiments at ISAC

An intense beam of ^26gAl has been developed for accelerated beam experiments at TRIUMF’s ISAC facility. Studies of the on-line production of Al radionuclides from thick silicon carbide targets have been performed as part of a program of beam development for astrophysical reaction studies at ISAC. While the release of short-lived Al nuclides from SiC was found to be slow, development of new target material forms and high-power target containers has allowed operation of SiC targets with proton currents of up to 70 μA on target. In addition, operation with the TRIUMF resonant ionization laser ion source (TRILIS) has produced ^26gAl beam intensities of 5.1 × 10¹⁰ s⁻¹.     

Scanning transmission ion microscopy of polycarbonate nanocapillaries

Polycarbonate membranes containing statistically scattered heavy ion track nanocapillaries have been studied by scanning transmission ion microscopy (STIM) method. The geometry of the samples was characterized by pore diameters of about 172 nm and by 30 μm membrane thickness. The porosity has to be relatively low in order to avoid too many overlapping capillaries. The transparency of the sample is reduced by changing its tilt angle to the beam. While the acceptance angle for transmission of a single capillary is below 0.3°, the STIM results have showed that the angular spread was about 1° full width at half maximum (FWHM). This indicates that the capillaries are not perfectly parallel, i.e. the capillary directions have a finite angular spread.Our results are important for the recent use of these types of insulator membranes in ion guiding studies, and the related potential applications.     

Recharging processes, radiation induced strain and changes of OH bands under H ion implantation in Ti doped lithium niobate

A systematic analysis of variations in structural and optical characteristics of Z-cut plates of titanium doped congruent lithium niobate single crystals implanted with 120 keV proton beam at various fluences of 10¹⁵, 10¹⁶ and 10¹⁷ protons/cm² is presented. Through, high resolution X-ray diffraction, atomic force microscopy, Fourier transform infrared and UV-visible-NIR analysis of congruent lithium niobate, the correlation of properties before and after implantation are discussed. HRXRD (0 0 6) reflection by Triple Crystal Mode shows that both tensile and compressive strain peak are produced by the high fluence implantation. A distinct tensile peak was observed from implanted region for a fluence of 10¹⁶ protons/cm². AFM micrographs indicate mountain ridges, bumps and protrusions on target surface on implantation. UV-visible-NIR spectra reveal an increase in charge transfer between Ti³⁺/Ti⁴⁺ and ligand oxygen for implantation with 10¹⁵ protons/cm², while spectra for higher fluence implanted samples show complex absorption band in the region from 380-1100 nm. Variations of OH⁻ stretching vibration mode were observed for cLN Pure, cLNT2% virgin, and implanted samples with FTIR spectra. The concentration of OH⁻ ion before and after implantation was calculated from integral absorption intensity. The effect of 120 keV proton implantation induced structural, surface and optical studies were correlated.     

Microbeam line with 1.5 MeV helium ions and protons at Osaka

A microprobe for Rutherford backscattering (RBS) and particle-induced X-ray emission (PIXE) measurements has been realized by focusing 1.5 MeV helium-ion or proton beams with a demagnification system consisting of piezo-driven objective slits and a magnetic quadrupole doublet. Minimum beam spot sizes of 1.3 × 2.2 μm² for helium ions and 2.2 × 4.0 μm² for protons have been achieved. The factors which may limit the minimum spot size are discussed using a Monte Carlo simulation procedure. Rutherford backscattering image mapping of 3-dimensional structures is demonstrated.     

Proton elastic scattering and proton induced γ-ray emission cross-sections on Na from 2 to 5 MeV

Differential cross-sections for proton elastic scattering on sodium and for γ-ray emission from the reactions ²³Na(p,p′γ)²³Na (E_γ = 440 keV and E_γ = 1636 keV) and ²³Na(p,α′γ)²⁰Ne (E_γ = 1634 keV) were measured for proton energies from 2.2 to 5.2 MeV using a 63 μg/cm² NaBr target evaporated on a self-supporting thin C film.The γ-rays were detected by a 38% relative efficiency Ge detector placed at an angle of 135° with respect to the beam direction, while the backscattered protons were collected by a Si surface barrier detector placed at a scattering angle of 150°. Absolute differential cross-sections were obtained with an overall uncertainty estimated to be better than ±6.0% for elastic scattering and ±12% for γ-ray emission, at all the beam energies.To provide a convincing test of the overall validity of the measured elastic scattering cross-section, thick target benchmark experiments at several proton energies are presented.     

CTOF measurements and Monte Carlo analyses of neutron spectra for the backward direction from a lead target irradiated with 200-1000 MeV protons

A calorimetric-time-of-flight technique was used for real-time, high-precision measurement of neutron spectra at an angle of 175^o from the initial proton beam direction, which hits a face plane of a cylindrical lead target of 20 cm in diameter and 25 cm thick. A comparison was performed between the neutron spectra predicted by the MARS, RTS&T, MCNP6, and the MCNPX 2.6.0 transport codes and that measured for 200, 400, 600, 800, and 1000 MeV protons. Neutron spectra were measured within the energy range from 0.7 to 250 MeV almost continuously. The transport codes tested here describe with different success the measured spectra, depending on the energy of the detected neutrons and on the incident proton energy, but all the models agree reasonably well with our data.     

Preliminary results of proton beam characterization for a facility of broad beam in vitro cell irradiation

The interaction of charged particles with living matter needs to be well understood for medical applications. Particularly, it is useful to study how ion beams interact with tissues in terms of damage, dose released and dose rate.One way to evaluate the biological effects induced by an ion beam is by the irradiation of cultured cells at a particle accelerator, where cells can be exposed to different ions at different energies and flux.In this paper, we report the first results concerning the characterization of a broad proton beam obtained with our 2 MV tandem accelerator. For broad beam in vitro cell irradiation, the beam has to be stable over time, uniform over a ∼0.5 cm² surface, and a dose rate ranging from 0.1 to 10 Gy/min must be achievable. Results concerning the level of achievement of these requirements are presented in this paper for a 1 MeV proton beam.     

Introduction of conductivity on non-conducting polyaniline by low-energy proton implantation

The semiconductor characteristics of a non-conducting polyaniline pellet can be modified by implantation of low-energy protons, that is, the resistivity became less than 50 Ω cm by proton doping at the fluence rate and fluence of 4 × 10¹¹ ions/cm²/s and 1 × 10¹⁵ ions/cm², respectively. The resistivity increased with the increasing fluence rate of the protons. FT/IR spectra have shown that a new band resulted from the appearance of N⁺-H due to the proton implantation.     

X-ray production cross-sections measurements for high-energy alpha particle beams: New dedicated set-up and first results with aluminum

The “IPNAS” laboratory, in collaboration with the “Centre Européen d’Archéométrie” is partly focused on material analysis by means of IBA techniques: PIXE, PIGE and RBS. A new transport beam line has been developed at our CGR-520 MeV cyclotron to analyze Cultural Heritage objects using these techniques. This facility allows us to produce proton and alpha particle beams with energies up to 20 MeV. A vacuum chamber dedicated to X-ray production and Non-Rutherford cross-section measurements has been recently constructed. After determination of the chamber’s geometry for X-ray detection using thin foils of several elements (11 ? Z ? 82) and 3 MeV proton beams, the measurement of the X-ray production cross-sections in the 6-12 MeV energy range has started using alpha particle beams on light element targets. These experiments contribute to the filling a serious lack of experimental values for alpha particles of this particular energy range in databases. The recent decision to focus our work on the alpha particle interaction with light elements was taken because of the high interest of the low Z elements in the field of archaeometry.     

Suitable test structures for submicron ion beam analysis

For the precise determination of the sizes of submicron beam spots test structures with an excellent edge definition are required. For this purpose a semiconductor heterostructure consisting of an 1.62 μm GaInP epi-layer grown on (0 0 1) GaAs has been made, which provides atomically sharp edges for beam spot size measurements. Since the sample has been thinned down by standard transmission electron microscope (TEM) preparation techniques, it can be used for both PIXE and STIM. The sample has been investigated with a TEM and the ion nanoprobe LIPSION. A one-dimensional beam profile in the low current mode was determined by a STIM measurement using 2 MeV protons and yielded a FWHM of (41±4) nm, which is the smallest value reported so far for high energy nuclear micro- and nanoprobes. Furthermore we present nickel nanowhiskers produced at the GSI Darmstadt by electrochemical preparation of etched ion track membranes that have been used to obtain two-dimensional images of the shapes of submicron beam spots. For these measurements a scan over a single nickel nanowhisker having a diameter of 220 nm and a height of about 6 μm was performed.     

Proton irradiation study of GFR candidate ceramics

This work investigated the microstructural response of SiC, ZrC and ZrN irradiated with 2.6 MeV protons at 800 °C to a fluence of 2.75 × 10¹⁹ protons/cm², corresponding to 0.71-1.8 displacement per atom (dpa), depending on the material. The change of lattice constant evaluated using HOLZ patterns is not observed. In comparison to Kr ion irradiation at 800 °C to 10 dpa from the previous studies, the proton irradiated ZrC and ZrN at 1.8 dpa show less irradiation damage to the lattice structure. The proton irradiated ZrC exhibits faulted loops which are not observed in the Kr ion irradiated sample. ZrN shows the least microstructural change from proton irradiation. The microstructure of 6H-SiC irradiated to 0.71 dpa consists of black dot defects at high density.