Structural studies of silicon oxynitride layers formed by low energy ion implantation

Silicon oxynitride (Si_xO_yN_z) layers were synthesized by implanting ¹⁶O₂⁺ and ¹⁴N₂⁺ 30 keV ions in 1:1 ratio with fluences ranging from 5 × 10¹⁶ to 1 × 10¹⁸ ions cm⁻² into single crystal silicon at room temperature. Rapid thermal annealing (RTA) of the samples was carried out at different temperatures in nitrogen ambient for 5 min. The FTIR studies show that the structures of ion-beam synthesized oxynitride layers are strongly dependent on total ion-fluence and annealing temperature. It is found that the structures formed at lower ion fluences (∼1 × 10¹⁷ ions cm⁻²) are homogenous oxygen-rich silicon oxynitride. However, at higher fluence levels (∼1 × 10¹⁸ ions cm⁻²) formation of homogenous nitrogen rich silicon oxynitride is observed due to ion-beam induced surface sputtering effects. The Micro-Raman studies on 1173 K annealed samples show formation of partially amorphous oxygen and nitrogen rich silicon oxynitride structures with crystalline silicon beneath it for lower and higher ion fluences, respectively. The Ellipsometry studies on 1173 K annealed samples show an increase in the thickness of silicon oxynitride layer with increasing ion fluence. The refractive index of the ion-beam synthesized layers is found to be in the range 1.54-1.96.     

Determination of mass attenuation coefficients, effective atomic and electron numbers for Cr, Fe and Ni alloys at different energies

The total mass attenuation coefficients (μ_m), for Cr, Fe, Ni and Fe_xNi_1−x (x = 0.8, 0.7, 0.6, 0.5, 0.4, 0.3 and 0.2), Fe_xCr_yNi_1−(x+y) (x = 0.7, y = 0.1; x = 0.5, y = 0.2; x = 0.4, y = 0.3; x = 0.3, y = 0.3; x = 0.2, y = 0.2 and x = 0.1, y = 0.2) and Ni_xCr_1−x (x = 0.8, 0.6, 0.5, 0.4 and 0.2) alloys were measured at 22.1, 25.0, 59.5 and 88.0 keV photon energies. The samples were irradiated with 10 mCi Cd-109 and 100 mCi Am-241 radioactive point source using transmission arrangement. The γ- and X-rays were counted by a Si(Li) detector with a resolution of 160 eV at 5.9 keV. Total atomic and electronic cross-sections (σ_t and σ_e), effective atomic and electron numbers (Z_eff and N_eff) were determined experimentally and theoretically using the obtained mass attenuation coefficients for investigated 3d alloys. The theoretical mass attenuation coefficients of each alloy were estimated using mixture rule. The experimental values were compared with the calculated values for all samples.     

Thermal conductivities of hypostoichiometric (U, Pu, Am)O2−x oxide

The thermal conductivities of (U_0.68Pu_0.30Am_0.02)O_2.00−x solid solutions (x = 0.00-0.08) were studied at temperatures from 900 to 1773 K. The thermal conductivities were obtained from the thermal diffusivities measured by the laser flash method. The thermal conductivities obtained experimentally up to about 1400 K could be expressed by a classical phonon transport model, λ = (A + BT)⁻¹, A(x) = 3.31 × x + 9.92 × 10⁻³ (mK/W) and B(x) = (−6.68 × x + 2.46) × 10⁻⁴ (m/W). The experimental A values showed a good agreement with theoretical predictions, but the experimental B values showed not so good agreement with the theoretical ones in the low O/M ratio region. From the comparison of A and B values obtained in this study with the ones of (U,Pu)O_2−x obtained by Duriez et al. [C. Duriez, J.P. Alessandri, T. Gervais, Y. Philipponneau, J. Nucl. Mater. 277 (2000) 143], the addition of Am into (U, Pu)O_2−x gave no significant effect on the O/M dependency of A and B values.     

Structural characterization of buried nitride layers formed by nitrogen ion implantation in silicon

The synthesis of buried silicon nitride insulating layers was carried out by SIMNI (separation by implanted nitrogen) process using implantation of 140 keV nitrogen (¹⁴N⁺) ions at fluence of 1.0 × 10¹⁷, 2.5 × 10¹⁷ and 5.0 × 10¹⁷ cm⁻² into 〈1 1 1〉 single crystal silicon substrates held at elevated temperature (410 °C). The structures of ion-beam synthesized buried silicon nitride layers were studied by X-ray diffraction (XRD) technique. The XRD studies reveal the formation of hexagonal silicon nitride (Si₃N₄) structure at all fluences. The concentration of the silicon nitride phase was found to be dependent on the ion fluence. The intensity and full width at half maximum (FWHM) of XRD peak were found to increase with increase in ion fluence. The Raman spectra for samples implanted with different ion fluences show crystalline silicon (c-Si) substrate peak at wavenumber 520 cm⁻¹. The intensity of the silicon peak was found to decrease with increase in ion fluence.     

The use of HI-ERDA/RBS and NRA/RBS to depth profile N in GaAs1−xNx thin films

N profiles of several GaAs_1−xN_x epitaxial layers with different N mole fractions in the range 0 < x < 0.14 were obtained by using (1) heavy-ion elastic recoil detection analysis (HI-ERDA) along with Rutherford backscattering spectrometry (RBS) using a 35 MeV Si⁶⁺ beam, and (2) nuclear reaction analysis (NRA) with the ¹⁴N(α, p)¹⁷O reaction, also with RBS, using a 3.7 MeV ⁴He⁺ beam. The results from the two techniques are compared and the advantages, disadvantages and capabilities are discussed.     

Depth profiling of carbon in silicon using the C(p, p′γ) reaction

An analytical method has been developed for the measurement of a carbon depth profile of the region a few tens of μm from the surface, using a ¹²C(p, p′γ) reaction. Measurements for a SiC sample coated with a silicon layer and a carbon-implanted silicon sample were performed using this method. Two charged particle detectors and two γ-ray detectors were utilized for the coincident detection of scattered protons and γ-rays from the first excited state (E_x = 4.4 MeV) of ¹²C. The measured depth profiles agree well with results obtained using a surface profiler and an Auger microprobe. These results demonstrate that this method is useful for the non-destructive analysis of carbon at depths of a few tens of μm from the surface.     

Oxygen potential and thermal conductivity of (U, Pu) mixed oxides

(U, Pu) mixed oxides, (U_1−yPu_y)O_2−x, with y = 0.21 and 0.28 are being considered as fuels for the Prototype Fast Breeder Reactor (PFBR) in India. The use of urania-plutonia solid solutions in PFBR calls for accurate measurement of physicochemical properties of these materials. Hence, in the present study, oxygen potentials of (U_1−yPu_y)O_2−x, with y = 0.21 and 0.28 were measured over the temperature range 1073-1473 K covering an oxygen potential range of −550 to −300 kJ mol⁻¹ (O/M ratio from 1.96 to 2.000) by employing a H₂/H₂O gas equilibration technique followed by solid electrolyte EMFmeasurement. (U_1−yPu_y)O_2−x, with y = 0.40 is being used in the Fast Breeder Test Reactor (FBTR) in India to test the behaviour of fuels with high plutonium content. However, data on the oxygen potential as well as thermal conductivity of the mixed oxides with high plutonium content are scanty. Hence, the thermal diffusivity of (U_1−yPu_y)O₂, with y = 0.21, 0.28 and 0.40 was measured and the results of the measurements are reported.     

Electrical properties of silicon diodes with pn junctions irradiated with Au swift heavy ions

Electrical properties of silicon diodes with p⁺n junctions irradiated with ¹⁹⁷Au⁺²⁶ swift heavy ions (energy E = 350 MeV, fluences of 10⁷ cm⁻² and 10⁸ cm⁻²) and silicon diodes irradiated with electrons (energy E = 3.5 MeV, fluences of 10¹⁵ cm⁻², 5 × 10¹⁵ cm⁻² and 10¹⁶ cm⁻²) have been investigated. Frequency dependences of the impedance, current-voltage characteristics and switching characteristics of these devices have been studied. Irradiation of the diodes with ¹⁹⁷Au⁺²⁶ ions at a fluence of 10⁸ cm⁻² leads to the formation of a quasi-continuous layer of irradiation-induced defects that enable a combination of characteristics such as a reverse resistance recovery time and direct voltage drop that are better than those for electron-irradiated diodes. Still, the irradiation of high-energy ions results in an increase in recombination currents that are larger than those obtained with electron irradiation, and causes more complicated frequency dispersion of the diode parameters.     

Effects of ion irradiation on the mechanical properties of SiNawOxCyHz sol-gel derived thin films

A study of the effects of ion irradiation of hybrid organic/inorganic modified silicate thin films on their mechanical properties is presented. NaOH catalyzed SiNa_wO_xC_yH_z thin films were synthesized by sol-gel processing from tetraethylorthosilicate (TEOS) and methyltriethoxysilane (MTES) precursors and spin-coated onto Si substrates. After drying at 300 °C, the films were irradiated with 125 keV H⁺ or 250 keV N²⁺ at fluences ranging from 1 × 10¹⁴ to 2.5 × 10¹⁶ ions/cm². Nanoindentation was used to characterize the films. Changes in hardness and reduced elastic modulus were examined as a function of ion fluence and irradiating species. The resulting increases in hardness and reduced elastic modulus are compared to similarly processed acid catalyzed silicate thin films.     

Ion-induced electron emission monitoring of the structure and morphology evolution in HOPG

The temperature dependences of the ion-induced electron emission yield γ of highly-oriented pyrolytic graphite (HOPG) under high-fluence (10¹⁸-10¹⁹ ions/cm²) 30 keV Ar⁺ ion irradiation at ion incidence angles from θ = 0^o (normal incidence) to 80^o have been measured to trace both the structure and morphology changes in the basal oriented samples. The target temperature has been varied during continuous irradiation from T = −180 to 400 ^oC. The surface analysis has been performed by the RHEED and SEM techniques. The surface microgeometry was studied using laser goniophotometry (LGF). The dependences of γ(T) were found to be strongly non-monotonic and essentially different from the ones for Ar⁺ and N₂⁺ ion irradiation of the polygranular graphites. A sharp peak at irradiation temperature T_p ≈ 150 ^oC was found. A strong influence of electron transport anisotropy has been observed, and ion-induced microgeometry is discussed.     

Effects of ion irradiation on the structural transformation of sol-gel derived TEOS/MTES thin films

Ion beam processing of organic/inorganic thin films has been shown to be an effective means in converting polymeric films into their final ceramic-like state. In this study, hybrid sol-gel derived thin films based on TEOS (tetraethylorthosilicate) Si(OC₂H₅)₄ and MTES (methyltriethoxysilane) CH₃Si(OC₂H₅)₃ were prepared and deposited on Si substrates by spin coating. After the films were allowed to air dry, they were heat treated at 300 °C for 10 min. Ion irradiation was performed at room temperature using 125 keV H⁺ and 250 keV N²⁺ ions with fluences ranging from 1 × 10¹⁴ to 5 × 10¹⁶ ions/cm². FT-IR and Raman spectroscopies were used to quantify the chemical structural transformations which occurred including the evolution of the organic components, the cross-linking of silica clusters, and the clustering of carbon.     

On the emission of MoCs molecular ions from Cs irradiated molybdenum surface

The present paper deals with the emission of atomic and molecular ions from elemental molybdenum surface under Cs⁺ bombardment to explore the MCs⁺ formation mechanism with changing Cs surface coverage. Integrated count of MoCs⁺ shows a monotonic increase with increasing primary ion energy (1-5 keV). Change in MoCs⁺ intensity is attributed to the variation of surface work function ? and cesium surface concentration c_Cs due to varying impact energies. Variation of c_Cs has been obtained from the expression, c_Cs ∝ 1/(1 + Y) where Y is the elemental sputtering yield estimated from TRIM calculations. Systematic study of the energy distributions of all species emerging from Mo target has been done to measure the changes in surface work function. Changing slopes of the leading parts of Cs⁺ energy distributions suggest a substantial depletion in surface work function ? with decreasing primary ion energies. Δ? shows a linear dependence on c_Cs. The maximum reduction in surface work function Δ?_max = 0.69 eV corresponds to the highest value of c_Cs = 0.5. A phenomenological model, based on the linear dependence of ? on c_Cs, has been employed to explain the MoCs⁺ data.     

Proton beam induced luminescence of silicon dioxide implanted with silicon

Light emission from a silicon dioxide layer enriched with silicon has been studied. Samples used had structures made on thermally oxidized silicon substrate wafers. Excess silicon atoms were introduced into a 250-nm-thick silicon dioxide layer via implantation of 60 keV Si⁺ ions up to a fluence of 2 × 10¹⁷ cm⁻². A 15-nm-thick Au layer was used as a top semitransparent electrode. Continuous blue light emission was observed under DC polarization of the structure at 8-12 MV/cm. The blue light emission from the structures was also observed in an ionoluminescence experiment, in which the light emission was caused by irradiation with a H₂⁺ ion beam of energy between 22 and 100 keV. In the case of H₂⁺, on entering the material the ions dissociated into two protons, each carrying on average half of the incident ion energy. The spectra of the emitted light and the dependence of ionoluminescence on proton energy were analyzed and the results were correlated with the concentration profile of implanted silicon atoms.     

Study of surface activation of PET by low energy (keV) Ni and N ion implantation

Polyethyleneterephthalate (PET) has been modified by 100 keV Ni⁺ and N⁺ ions using metal ion from volatile compound (MIVOC) ion source to fluence ranging from 1 × 10¹⁴ to 1 × 10¹⁶ ions/cm². The increasing application of polymeric material in technological and scientific field has motivated the use of surface treatment to modify the physical and chemical properties of polymer surfaces. When a material is exposed to ionization radiation, it suffers damage leading to surface activation depending on the type. The surface morphology was observed by atomic force microscopy (AFM). That show the roughness increases with fluence in both the cases. The Ni particles as precipitation in PET were observed by cross-section transmission electron microscopy (XTEM). The optical band gap (E_g) deduced from absorption spectra; was calculated by Tau’c relation. Raman spectroscopy shows quantitatively the chemical nature at the damage caused by the Ni⁺ and N⁺ bombardment. The ration of I_D/I_G shows graphite-like structure is formed on the surface. A layer of hydrogenated amorphous carbon is formed on the surface, which has confirmed by XPS results also.     

New local model for electronic energy loss and its application to computer simulations of channeling

We used the average of the Thomas-Fermi (TF) electron distribution instead of that of Hartree-Fock (HF) electron distribution as the screening length of an isolated atom. Based on the Firsov theory, we proposed a new Firsov formula of the electronic energy loss which has a simple form ΔE_e(E, b) ∞ S_e(E) exp(γb)/(1 + βb)⁶, where S_e(E) is the electronic stopping cross section, b = p/a, p and a are the impact parameter and the screening length, respectively, and β and γ are the fitting parameters. Using the present screening lengths with the shell effect and the new Firsov formula, the depth distributions of channeling were simulated by the ACOCT code for 20 keV B⁺ ions impinging along the [1 1 0] channel direction of silicon (1 1 0) surface. The ACOCT depth profiles of channeling using the new Firsov (solid) local model for the AMLJ potential are in good agreement with the experimental ones.     

Ion induced segregation in gold nanostructured thin films on silicon

We report a direct observation of segregation of gold atoms to the near surface regime due to 1.5 MeV Au²⁺ ion impact on isolated gold nanostructures deposited on silicon. Irradiation at fluences of 6 × 10¹³, 1 × 10¹⁴ and 5 × 10¹⁴ ions cm⁻² at a high beam flux of 6.3 × 10¹² ions cm⁻² s⁻¹ show a maximum transported distance of gold atoms into the silicon substrate to be 60, 45 and 23 nm, respectively. At a lower fluence (6 × 10¹³ ions cm⁻²) transport has been found to be associated with the formation of gold silicide (Au₅Si₂). At a high fluence value of 5 × 10¹⁴ ions cm⁻², disassociation of gold silicide and out-diffusion lead to the segregation of gold to defect - rich surface and interface regions.     

Optical contrast formation in amorphous silicon carbide with high-energy focused ion beams

Thin films (d ～ 1 μm) of hydrogenated amorphous silicon carbide (a-Si_1?xC_x:H), deposited by RF reactive magnetron sputtering with different carbon content x, have been implanted with high fluences (Φ = 1016–1017 cm^?2) of high-energy (E = 0.2–1 MeV) He⁺ ions as the implant species. The induced structural modification of the implanted material results in a considerable change of its optical properties, best manifested by a significant shift of the optical absorption edge to lower photon energies as obtained from photo-thermal-deflection spectroscopy (PDS) data. This shift is accompanied by a remarkable increase of the absorption coefficient over one order of magnitude (photo-darkening effect) in the measured photon energy range (0.6–3.8 eV), depending on the ion fluence, energy and carbon content of the films. These effects could be attributed both to additional defect introduction and increased graphitization, as confirmed by Raman spectroscopy and infra-red (IR) optical transmission measurements. The optical contrast thus obtained (between implanted and unimplanted film material) could be made use of in the area of high-density optical data storage using focused high-energy He⁺ ion beams.     

Channeling study of thermal decomposition of III-N compound semiconductors

GaN thermal stability is the limiting factor of the growth rate for epitaxially grown films and of the thermal annealing of defects. As a consequence, this issue has been extensively studied for more than one decade. There are, however, substantial differences in the reported kinetics and presumed mechanisms of decomposition, which are primarily related to the reactor design thus, reflecting the complexity of chemical reactions involved. We report here on the use of 1.7 MeV He-ion RBS/channeling for the study of thermal decomposition of MOVPE grown GaN and Al_xGa_1−xN (x = 0.05-0.5) layers. These layers with thickness of 320 nm were grown on sapphire substrates with 20 nm AlN nucleation layer. Prior to annealing samples were characterized by RBS/channeling, selected samples were also studied by SEM. Thermal treatment was performed in the MOVPE reactor in the temperature range 900-1200 °C in the N₂ atmosphere. RBS/channeling analysis provided data on layer thickness, composition and evolution of ingrown defects. GaN decomposition starts at 900 °C and results in the reduction of the layer thickness without observable changes of the film composition. The presence of large density of GaN hillocks on the surface was revealed by SEM after annealing at 1000-1050 °C. Remarkable stability of Al_xGa_1−xN was observed, this alloy remains unchanged upon annealing at 1200 °C/6 h even for x as low as 0.05.     

Microstructure evolution of Ge implanted silicon oxide thin films upon annealing treatments

The structural evolution of silicon oxide films with Ge⁺ implantation was traced with a positron beam equipped with positron annihilation Doppler broadening and lifetime spectrometers. Results indicate that the film structure change as a function of the annealing temperature could be divided into four stages: (I) T < 300 °C; (II) 300 °C ? T ? 500 °C; (III) 600 °C ? T ? 800 °C; (IV) T ? 900 °C. In comparison with stage I, the increased positron annihilation Doppler broadening S values during stage II is ascribed to the annealing out of point defects and coalescence of intrinsic open volumes in silicon oxides. The obtained long positron lifetime and high S values without much fluctuation in stage III suggest a rather stable film structure. Further annealing above 900 °C brings about dramatic change of the film structure with Ge precipitation. Positron annihilation spectroscopy is thereby a sensitive probe for the diagnosis of microstructure variation of silicon oxide thin films with nano-precipitation.     

Synthesis, characterization and thermal expansion measurements on uranium-cerium mixed oxides

Uranium-cerium mixed oxides (U_1−yCe_y)O₂ (y = 0.2, 0.4, 0.6, 0.8) were prepared by combustion synthesis using citric acid as the fuel. Sintering of the solid solutions was carried out at 1873 K under reduced atmosphere. From the room temperature XRD patterns of the sintered samples it was found that the solid solutions form single phase fluorite structure. The room temperature lattice parameters of (U_1−yCe_y)O₂ (y = 0.2, 0.4, 0.6, 0.8) are 0.5458, 0.5446, 0.5434 and 0.5422 nm respectively. Thermal expansion of (U_1−yCe_y)O₂ (y = 0.2, 0.4, 0.6, 0.8) in the temperature range 298-1973 K was measured by high temperature X-ray diffraction (HTXRD). The coefficients of thermal expansion increase with increase in CeO₂ content in the sample and the measured data in the temperature range 298-1973 K, for (U_1−yCe_y)O₂ (y = 0.2, 0.4, 0.6, 0.8) are 18.23, 19.91, 21.59, 23.29 × 10⁻⁶ K⁻¹, respectively.