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.     

Effects of MeV Si ions bombardment on the thermoelectric generator from SiO2/SiO2 + Cu and SiO2/SiO2 + Au nanolayered multilayer films

The defects and disorder in the thin films caused by MeV ions bombardment and the grain boundaries of these nanoscale clusters increase phonon scattering and increase the chance of an inelastic interaction and phonon annihilation. We prepared the thermoelectric generator devices from 100 alternating layers of SiO₂/SiO₂ + Cu multi-nano layered superlattice films at the total thickness of 382 nm and 50 alternating layers of SiO₂/SiO₂ + Au multi-nano layered superlattice films at the total thickness of 147 nm using the physical vapor deposition (PVD). Rutherford Backscattering Spectrometry (RBS) and RUMP simulation have been used to determine the stoichiometry of the elements of SiO₂, Cu and Au in the multilayer films and the thickness of the grown multi-layer films. The 5 MeV Si ions bombardments have been performed using the AAMU-Center for Irradiation of Materials (CIM) Pelletron ion beam accelerator to make quantum (nano) dots and/or quantum (quantum) clusters in the multilayered superlattice thin films to decrease the cross plane thermal conductivity, increase the cross plane Seebeck coefficient and cross plane electrical conductivity. To characterize the thermoelectric generator devices before and after Si ion bombardments we have measured Seebeck coefficient, cross-plane electrical conductivity, and thermal conductivity in the cross-plane geometry for different fluences.     

Structural analysis of DC magnetron sputtered and spin coated thin films using RBS, TEM and X-ray reflectivity methods

Metallic thin films such as Au, Cr, Ag, etc., on silicon substrate have many technologically important applications as contact layers in microelectronic industry, as reflecting mirrors in synchrotron radiation research, etc. The native oxide layer on crystalline silicon surface inhibits wetting of few nm thick Au or Ag on native oxide/silicon systems. To obtain continuous thin metallic films (a few nm thick), a Cr layer was first deposited as a adhesion layer on the Si substrate. In this paper, Rutherford backscattering analysis (RBS) of Si/Cr/SiO₂/Si, Si/Au/SiO₂/Si, Si/Au/Cr/SiO₂/Si and Polystyrene (PS) polymer coated on some of these bi- or tri-layer structures has been reported. The X-ray reflectometry and transmission electron microscopy studies were carried out to complement the RBS measurements. The thickness, surface and interface roughness, and crystalline quality have been determined.     

EXPERIMENTS OF MeV ION BEAM INDUCED ATOMIC MIXING

An experimental apparatus for studies of MeV ion beam modification of materials has been established on a 3 MV tandem accelerator at Fudan university. A system of X-Y electrostatic scanning implantation of MeV heavy ions and in situ Rutherford. backscattering analysis was included in it. The uniformity of scanning implantation was checked by the RBS measurement of a Si wafer implanted with 1 MeV Au ions. MeV ion beam mixing of Au/Si, Au/Ge and Ag/Si systems was preliminarily studied. The samples were irradiated by certain fluences of 1 MeV Ag ions at room temperature. The mixed layers were analyzed in situ using the glancing RBS technique with 2 MeV 4He+ ions. For Au/Si system, a uniformly mixed layer with a defined composition is obtained, and the intermixing is much less for Ag/Si system than for Au/Si system.     

Adhesion of proton beam written high aspect ratio hydrogen silsesquioxane (HSQ) nanostructures on different metallic substrates

Hydrogen silsesquioxane (HSQ) behaves as a negative resist under MeV proton beam exposure. HSQ is a high-resolution resist suitable for production of tall (<1.5 μm) high aspect ratio nanostructures with dimensions down to 22 nm. High aspect ratio HSQ structures can be used in many applications, e.g. nanofluidics, biomedical research, etc. Isolated HSQ nanostructures, however, tend to detach from substrates during the development process due to the weak adhesive forces between the resist and the substrate material. Larger proton fluences were observed to promote the adhesion. To determine an optimal substrate material and the proton irradiation doses for HSQ structures, a series of 2 μm long and 60-600 nm wide free-standing lines were written with varying fluences of 2 MeV protons in 1.2 μm thick HSQ resist spun on Ti/Si, Cr/Si and Au/Cr/Si substrates. The results indicate that the Ti/Si substrate is superior in terms of adhesion, while Au/Si is the worst. Cr/Si is not suitable as a substrate for HSQ resist because debris was formed around the structures, presumably due to a chemical reaction between the resist and Cr.     

Synthesis of nanodimensional TiO2 thin films using energetic ion beam

Nanophases of TiO₂ are achieved by irradiating polycrystalline thin films of TiO₂ by 100 MeV Au ion beam at varying fluence. The surface morphology of pristine and irradiated films is studied by atomic force microscopy (AFM). Phase of the film before and after irradiation is identified by glancing angle X-ray diffraction (GAXRD). The blue shift observed in UV-vis absorption edge of the irradiated films indicates nanostructure formation. Electron spin resonance (ESR) studies are carried out to identify defects created by the irradiation. The nanocrystallisation induced by SHI irradiation in polycrystalline thin films is studied.     

Patterned microstructures formed with MeV Au implantation in Si(1 0 0)

Energetic (MeV) Au implantation in Si(1 0 0) (n-type) through masked micropatterns has been used to create layers resistant to KOH wet etching. Microscale patterns were produced in PMMA and SU(8) resist coatings on the silicon substrates using P-beam writing and developed. The silicon substrates were subsequently exposed using 1.5 MeV Au³⁺ ions with fluences as high as 1 × 10¹⁶ ions/cm² and additional patterns were exposed using copper scanning electron microscope calibration grids as masks on the silicon substrates. When wet etched with KOH microstructures were created in the silicon due to the resistance to KOH etching cause by the Au implantation. The process of combining the fabrication of masked patterns with P-beam writing with broad beam Au implantation through the masks can be a promising, cost-effective process for nanostructure engineering with Si.     

Deposition of polycrystalline Si thin films on glass substrates by direct negative Si ion beam deposition

Polycrystalline Si (Poly-Si) thin films were deposited on a glass substrate by direct negative Si (Si⁻) ion beam deposition. The glass substrate temperature was kept constant at 500 °C for all depositions. Prior to deposition, the ion energy spread and ion-to-atom arrival ratio were evaluated as a function of the ion beam energy.The Si⁻ ion energy spread was less than 10% regardless of the ion energy, while the ion-to-atom arrival ratio increased proportionally from 1.3 to 1.6 according to the ion beam energy.Atomic force microscopy images showed that a relatively rough surface was obtained at 50 eV of Si⁻ ion energy and it is also concluded that the Si⁻ ion beam irradiation at 50 eV is effective to deposit Si thin film with small grains as shown in Fig. 3.     

Cross-section for D(p,p)D elastic scattering from 1.8 to 3.2 MeV at the laboratory angles of 155° and 165°

The D(p,p)D cross-sections for elastic scattering of proton on deuterium over incident proton energy range from 1.8 to 3.2 MeV at both laboratory angles of 155° and 165° were measured. A thin solid state target Ni/TiD_x/Ta/Al used for cross-section measurement was fabricated by firstly depositing layers of Ta, Ti and Ni film on the Al foil substrate of about 7 μm in turn using magnetron sputtering and then deuterating under the deuterium atmosphere. The areal density of metal element in each layer of film was measured with RBS analysis by using a 4.0 MeV ⁴He ion beam, while the areal density of the deuterium absorbed in the Ti film was measured with ERD analysis by using a 6.0 MeV ¹⁶O ion beam. The results show that the cross-sections of p-D scattering under this experimental circumstance were much enhanced over the Rutherford cross-section value. It was found that the enhancement increases linearly as the energy of the incident beam increases. The total uncertainty in the measurements was less than 7.5%.     

Lateral straggling and its influence on lateral diffusion in implantation with a focused ion beam

Parallel stripes of nanostructures on an n-type Si substrate have been fabricated by implanting 30 keV Ga⁺ ions from a focused ion beam (FIB) source at three different fluences: 1 × 10¹⁵, 2 × 10¹⁵ and 5 × 10¹⁵ ions/cm². Two sets of implantation were carried out. In one case, during implantation the substrate was held at room temperature and in the other case at 400 °C. Photoemission electron microscopy (PEEM) measurements were carried out on these samples. The implanted parallel stripes, each with a nominal dimension of 4000 × 100 nm², appear as bright regions in the PEEM image. Line scans of the intensities from PEEM images were recorded along and across these stripes. Intensity profile at the edges of a line scan is broader for the implantation carried out at 400 °C compared to room temperature. From the analysis of this intensity profile lateral diffusion coefficient of Ga in silicon was estimated assuming that the PEEM intensity is proportional to Ga concentration. The diffusion coefficient at 400 °C has been estimated to be ∼10⁻¹⁵ m²/s. No significant dependence of diffusion coefficient on ion fluence was observed in the fluence range investigated here. Radiation enhanced diffusion has been discussed in the light of the associated defect distribution due to lateral straggling of the implanted ions.     

Fundamentals of surfactant sputtering

We introduce a new sputter technique, utilizing the steady-state coverage of a substrate surface with up to 10¹⁶ cm⁻² of foreign atoms simultaneously during sputter erosion by combined ion irradiation and atom deposition. These atoms strongly modify the substrate sputter yield on atomic to macroscopic length scales and therefore act as surfactant atoms (a blend of “surface active agent”). Depending on the surfactant-substrate combination, the novel technique allows enhanced surface smoothing, generation of novel surface patterns, shaping of surfaces and formation of ultra-thin films. Sputter yield attenuation is demonstrated for sputtering of Si and Fe substrates and different surfactant species using 5 keV Xe ions at different incidence angles and fluences up to 10¹⁷ cm⁻². Analytical approaches and Monte Carlo simulations are used to predict the sputtering yield attenuation as function of surfactant coverage. For sputtering of Si with Au surfactants we observe high sputter yields despite a steady-state surfactant coverage, which can be explained by strong ion-induced interdiffusion of substrate and surfactant atoms and the formation of a buried Au_xSi surfactant layer in dynamic equilibrium.     

Modification of a pulsed 14-MeV fast neutron generator to a medium-energy ion accelerator for TOF-RBS application

The first drift-tube neutron generator in Thailand, developed during 1980s under the support by the International Atomic Energy Agency (IAEA), was a 150 kV deuteron accelerator-based 14 MeV fast neutron generator. The accelerator was featured by a nanosecond pulsing system consisting of a beam chopper in combination with a beam buncher. Following the rapid development of ion beam technology and increasing needs for materials applications in the laboratory, the accelerator has been upgraded and modified to a large extent into a medium-energy ion-accelerator for time-of-flight Rutherford backscattering spectrometry (TOF-RBS) applications. The modification of the accelerator included the changing of the ion source, the accelerating tube and the mass-analyzing magnet, the upgrading of the pulsing system, and the installation of a TOF-RBS detecting system. The new accelerator is capable of supplying a 400-keV He-ion beam with ns-pulses for nano-layered materials analysis. This paper provides technical details of the modification.     

Defect- and strain-enhanced cavity formation and Au precipitation at nano-crystalline ZrO2/SiO2/Si interfaces

Defect- and strain-enhanced cavity formation and Au precipitation at the interfaces of a nano-crystalline ZrO₂/SiO₂/Si multilayer structure resulting from 2 MeV Au⁺ irradiation at temperatures of 160 and 400 K have been studied. Under irradiation, loss of oxygen is observed, and the nano-crystalline grains in the ZrO₂ layer increase in size. In addition, small cavities are observed at the ZrO₂/SiO₂ interface with the morphology of the cavities being dependent on the damage state of the underlying Si lattice. Elongated cavities are formed when crystallinity is still retained in the heavily-damaged Si substrate; however, the morphology of the cavities becomes spherical when the substrate is amorphized. With further irradiation, the cavities appear to become stabilized and begin to act as gettering sites for the Au. As the cavities become fully saturated with Au, the ZrO₂/SiO₂ interface then acts as a gettering site for the Au. Analysis of the results suggests that oxygen diffusion along the grain boundaries contributes to the growth of cavities and that oxygen within the cavities may affect the gettering of Au. Mechanisms of defect- and strain-enhanced cavity formation and Au precipitation at the interfaces will be discussed with focus on oxygen diffusion and vacancy accumulation, the role of the lattice strain on the morphology of the cavities, and the effect of the binding free energy of the cavities on the Au precipitation.     

Structure and morphology of ion irradiated Au nanocrystals in SiO2

We have investigated the effect of ion irradiation on the structure and morphology of Au nanocrystals (NCs) fabricated by ion beam synthesis in a thin SiO₂ layer on a Si substrate. Extended X-ray absorption fine structure (EXAFS) spectroscopy measurements show a significant drop in the average Au–Au coordination, as well as a loss of medium and long range order with increasing irradiation dose. Small angle X-ray scattering (SAXS) measurements reveal a concomitant reduction in average NC size. These observations are a consequence of structural disorder and collisional mixing induced by the irradiation. The observed reduction in average Au–Au coordination by EXAFS differs significantly from that estimated from the average NC sizes evaluated using SAXS. This behavior can be explained by the dissolution of Au NCs into the SiO₂ matrix. A significant bond-length contraction indicates that part of this material forms small Au clusters (dimers, trimers, etc.) during irradiation that cannot be detected by SAXS. Combining the results from SAXS and EXAFS measurements, we estimate the volume fraction of such clusters.     

Ion beam mixing of Au marker in Pt and Pt marker in Au by 7 MeV Ag ions

Mixing of a thin Au layer in Pt and in reversed conditions mixing of a thin Pt layer in Au due to bombardment with 7 MeV Ag ions has been measured. The Pt-Au multilayers deposited on a Si substrate were irradiated to doses of 1–6 × 10¹⁵ ions cm⁻² at room temperature. The mixed profiles were measured using a SIMS apparatus with O₂⁺ sputter ions at energy 2.5 keV. The width of the Pt marker increased from 90 to 260 Å with increasing dose. The width of the Au marker increased from 80 to 90 Å, respectively. The corresponding mixing efficiencies are 5 ± 3 (Au marker) and 90 ± 30 Å⁵/eV (Pt marker). The experimental results are compared with simulations based on a model which describes the atomic transport from the initial collisional phase to the late thermalized stage. The calculated values for mixing efficiencies agree reasonably well with experimental values.     

High energy Si ions bombardment effects on the properties of nano-layers of SiO2/SiO2 + Ag

We grew 50 periodic SiO₂/SiO₂ + Ag multi-layers by electron beam deposition technique. The co-deposited SiO₂ + Ag layers are 7.26 nm, SiO₂ buffer layers are 4 nm, and total thickness of film was determined as 563 nm. We measured the thickness of the layers using in situ thickness monitoring during deposition, and optical interferometry afterwards. The concentration and distribution of Ag in SiO₂ were determined using Rutherford backscattering spectrometry (RBS). In order to calculate the dimensionless figure of merit, ZT, the electrical conductivity, thermal conductivity and the Seebeck coefficient of the layered structure were measured at room temperature before and after bombardment with 5 MeV Si ions. The energy of the Si ions was chosen such that the ions are stopped deep inside the silicon substrate and only electronic energy due to ionization is deposited in the layered structure. Optical absorption (OA) spectra were taken in the range 200–900 nm to monitor the Ag nanocluster formation in the thin layers.     

HRBS/channeling studies of ultra-thin ITO films on Si

High-resolution Rutherford backscattering spectroscopy (HRBS)/channeling techniques have been utilized for a detailed characterization of ultra-thin indium tin oxide (ITO) films and to probe the nature of the interface between the ITO film and the Si(0 0 1) substrate. Channeling studies provide a direct measure of the lattice strain distribution in the crystalline Si substrate in the case of amorphous over layers. The measurements on DC magnetron sputtered ITO films have been carried out using the recently installed HRBS facility at the Centre for Ion Beam Applications (CIBA). The thickness of the ultra-thin (∼9.8 nm) ITO films was calculated from the HRBS spectra having an energy resolution of about 1.4 keV at the superimposed leading (In + Sn) edge of the ITO film. The films were near stoichiometric and the interface between ITO film and Si was found to include a thin SiO_x transition layer. The backscattering yields from (In + Sn) of ITO were equal in random and channeling directions, thereby revealing the non-crystalline nature of the film. Angular scans of HRBS spectra around the off-normal [1 1 1] axis clearly showed a shift in the channeling minimum indicative of compressive strain of the Si lattice at the SiO_x/Si interface. The observed strain was about 0.8% near the interface and decreased to values below our detection limits at a depth of ∼3 nm from the SiO_x/Si interface.     

High resolution channeling contrast microscopy and channeling analysis of SiGe quantum well structures

High resolution channeling contrast microscopy (CCM) and channeling measurements were carried out to characterize SiGe quantum well structures on micron thick graded layers (i.e. virtual substrates). The virtual substrates were grown by gas source molecular beam epitaxy at a pressure of 10⁻⁵ mbar and low pressure chemical vapor deposition at 10⁻² mbar on boron doped Si(0 0 1) substrates respectively. A homoepitaxial silicon buffer layer was grown prior to the deposition. The nominal structure is a 20 nm Si_0.75Ge_0.25 layer at the surface, followed by 10 nm pure Si, 500 nm Si_0.75Ge_0.25 and a 1000 nm thick graded SiGe (0–26%) layer. RBS was used to measure the depth profiles, and angular scans around the (1 0 0) axis were carried out to assess crystal and interface quality. CCM was used to acquire depth resolved images of micron-sized lateral inhomogenities (‘cross-hatch') present on both samples.     

Changes in metal nanoparticle shape and size induced by swift heavy-ion irradiation

Changes in the shape and size of Co, Pt and Au nanoparticles induced by swift heavy-ion irradiation (SHII) have been characterized using a combination of transmission electron microscopy, small-angle X-ray scattering and X-ray absorption near-edge structure. Elemental nanoparticles of diameters 2-15 nm were first formed in amorphous SiO₂ by ion implantation and thermal annealing and then irradiated at room temperature with 27-185 MeV Au ions as a function of fluence. Spherical nanoparticles below a minimum diameter (4-7 nm) remained spherical under SHII but progressively decreased in size as a result of dissolution into the SiO₂ matrix. Spherical nanoparticles above the minimum diameter threshold were transformed to elongated rods aligned with the ion beamdirection. The nanorod width saturated at an electronic energy deposition dependent value, progressively increasing from 4-6 to 7-10 nm (at 5-18 keV/nm, respectively) while the nanorod length exhibited a broad distribution consistent with that of the unirradiated spherical nanoparticles. The threshold diameter for spherical nanoparticle elongation was comparable to the saturation value of nanorod width. We correlate this saturation value with the diameter of the molten track induced in amorphous SiO₂ by SHII. In summary, changes in nanoparticle shape and size are governed to a large extent by the ion irradiation parameters.     

Ion beam induced amorphization and recrystallization of Si/SiC/Si layer systems

Epitaxial, buried silicon carbide (SiC) layers have been fabricated in (100) and (111) silicon by ion beam synthesis (IBS). In order to study the ion beam induced epitaxial crystallization (IBIEC) of buried SiC layers, the resulting Si/SiC/Si layer systems were amorphized using 2 MeV Si²⁺ ion irradiation at 300 K. An unexpected high critical dose for the amorphization of the buried layers is observed. Buried, amorphous SiC layers were irradiated with 800 keV Si⁺ ions at 320 and 600°C, respectively, in order to achieve ion beam induced epitaxial crystallisation. It is demonstrated that IBIEC works well on buried layers and results in epitaxial recrystallization at considerably lower target temperatures than necessary for thermal annealing. The IBIEC process starts from both SiC/Si interfaces and may be accompanied by heterogenous nucleation of poly-SiC as well as interfacial layer-by-layer amorphization, depending on irradiation conditions. The structure of the recrystallized regions in dependence of dose, dose rate, temperature and crystal orientation is presented by means of TEM investigations.