Configuration interaction calculations of annihilation rates for positronic complexes of alkali hydrides

Ab initio multireference single- and double-excitation configuration interaction (MRD-CI) wave functions have been employed to compute the annihilation rates (AR) of positronic molecular complexes of four alkali hydrides. The first step in these calculations is the evaluation of integrals of the two-particle Dirac delta function δ₊₋ over pairs of electronic and positronic basis functions. MRD-CI wave functions calculated with the same basis are then employed to obtain expectation values of the δ₊₋ operator (Z_eff), which in turn are proportional to the corresponding annihilation rates (AR) of the associated many-particle states. The importance of removing near-linear dependencies in the basis sets employed is stressed as well as the advisability of placing diffuse (small-exponent) functions in the basis only at the most electronegative center of the molecule. A tendency to underestimate the Z_eff values is noted because of the impracticality of including sufficiently high-l basis functions in the basis for general molecular systems. However, comparison with the relatively accurate values for the four-electron e⁺LiH complex obtained by Quantum Monte-Carlo (QMC) and other methods indicates that the fractional error is nearly constant over a large range of internuclear distance, consistent with the expectation that missing correlation effects in the MRD-CI treatment are predominantly atomic in nature. A scaling procedure based on the asymptotic δ₊₋ value, which is the same for all four alkali hydrides, is then shown to produce good agreement with the QMC AR data for e⁺LiH. The same procedure has been applied to the δ₊₋ values for the positronic complexes of the heavier alkali hydrides for which no other theoretical results are available. Trends in the variation of the AR results with bond distance are discussed.     

Tailoring optical and electrical properties of MgO thin films by 1.5 MeV H implantation to fluences

Thin films of magnesia (MgO) with (1 0 0) dominant orientations were implanted with 1.5 MeV H⁺ ions at room temperature to various fluences of 10¹³, 10¹⁴ and 10¹⁵ ions/cm². X-ray analysis unambiguously showed crystallinity even after a peak damage fluence of 10¹⁵ ions/cm². Rutherford backscattering spectrometry combined with ion channeling (RBS/C) was used to analyze radiation damages and defect distributions. Optical absorption band observed at 5.7 eV in implanted films was assigned to the anion vacancies and the defect was completely disappeared on annealing at 450 °C. Number of F-type defects estimated was 9.42 × 10¹⁵ cm⁻² for the film implanted with 10¹⁵ ions/cm². DC electrical conductivity of 4.02 × 10⁻⁴ S cm⁻¹ was observed in the implanted region which was three orders higher than the as-deposited films. In unison, film surface was modified as a result of the formation of aggregates caused by the atomic mixing of native matrix atoms (Mg and O) and precipitated hydrogen.     

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.     

Alkali ion scattering from Ag(0 0 1) and Ag thin films at low and hyperthermal energies

We have investigated the scattering of K⁺ and Cs⁺ ions from a single crystal Ag(0 0 1) surface and from a Ag-Si(1 0 0) Schottky diode structure. For the K⁺ ions, incident energies of 25 eV to 1 keV were used to obtain energy-resolved spectra of scattered ions at θ_i = θ_f = 45°. These results are compared to the classical trajectory simulation safari and show features indicative of light atom-surface scattering where sequential binary collisions can describe the observed energy loss spectra. Energy-resolved spectra obtained for Cs⁺ ions at incident energies of 75 eV and 200 eV also show features consistent with binary collisions. However, for this heavy atom-surface scattering system, the dominant trajectory type involves at least two surface atoms, as large angular deflections are not classically allowed for any single scattering event. In addition, a significant deviation from the classical double-collision prediction is observed for incident energies around 100 eV, and molecular dynamics studies are proposed to investigate the role of collective lattice effects. Data are also presented for the scattering of K⁺ ions from a Schottky diode structure, which is a prototype device for the development of active targets to probe energy loss at a surface.     

Effect of 200 MeV Ag ion irradiation on structural and electrical transport properties of Fe3O4 thin films

Thin films of Fe₃O₄ have been deposited on single crystal MgO(1 0 0) and Si(1 0 0) substrates using pulsed laser deposition. Films grown on MgO substrate are epitaxial with c-axis orientation whereas, films on Si substrate are highly 〈1 1 1〉 oriented. Film thicknesses are 150 nm. These films have been irradiated with 200 MeV Ag ions. We study the effect of the irradiation on structural and electrical transport properties of these films. The fluence value of irradiation has been varied in the range of 5 × 10¹⁰ ions/cm² to 1 × 10¹² ions/cm². We compare the irradiation induced modifications on various physical properties between the c-axis oriented epitaxial film and non epitaxial but 〈1 1 1〉 oriented film. The pristine film on Si substrate shows Verwey transition (T_V) close to 125 K, which is higher than generally observed in single crystals (121 K). After the irradiation with the 5 × 10¹⁰ ions/cm² fluence value, T_V shifts to 122 K, closer to the single crystal value. However, with the higher fluence (1 × 10¹² ions/cm²) irradiation, T_V again shifts to 125 K.     

Effect of swift heavy ion irradiation on structure, optical, and gas sensing properties of SnO2 thin films

Swift heavy ion irradiation has been successfully used to modify the structural, optical, and gas sensing properties of SnO₂ thin films. The SnO₂ thin films prepared by sol-gel process were irradiated with 75 MeV Ni⁺ beam at fluences ranging from 1 × 10¹¹ ion/cm² to 3 × 10¹³ ion/cm². Structural characterization with glancing angle X-ray diffraction shows an enhancement of crystallinity and systematic change of stress in the SnO₂ lattice up to a threshold value of 1 × 10¹³ ions/cm², but decrease in crystallinity at highest fluence of 3 × 10¹³ ions/cm². Microstructure investigation of the irradiated films by transmission electron microscopy supports the XRD observations. Optical properties studied by absorption and PL spectroscopies reveal a red shift of the band gap from 3.75 eV to 3.1 eV, and a broad yellow luminescence, respectively, with increase in ion fluence. Gas response of the irradiated SnO₂ films shows increase of resistance on exposure to ammonia (NH₃), indicating p-type conductivity resulting from ion irradiation.     

Positron annihilation on the surfaces of SiO2 films thermally grown on single crystal of Cz-Si

Two-detector coincidence system and mono-energetic slow positron beam has been applied to measure the Doppler broadening spectra for single crystals of SiO₂, SiO₂ films with different thickness thermally grown on single crystal of Cz-Si, and single crystal of Si without oxide film. Oxygen is recognized as a peak at about 11.85 × 10⁻³m₀c on the ratio curves. The S parameters decrease with the increase of positron implantation energy for the single crystal of SiO₂ and Si without oxide film. However, for the thermally grown SiO₂-Si sample, the S parameters in near surface of the sample increase with positron implantation energy. It is due to the formation of silicon oxide at the surface, which lead to lower S value. S and W parameters vary with positron implantation depth indicate that the SiO₂-Si system consist of a surface layer, a SiO₂ layer, a SiO₂-Si interface layer and a semi-infinite Si substrate.     

Be AMS measurements at low energies (E < 1 MeV)

The longlived isotope ¹⁰Be is of great importance in earth sciences for dating applications, reconstruction of the solar activity or in climate research. Routine AMS measurements with BeO samples are performed on accelerators with a terminal voltage above 2 MV. Applying the degrader foil technique for boron suppression, first tests with BeO samples on the 0.6 MV ETH/PSI machine were limited by background to a ¹⁰Be/⁹Be ratio of 10⁻¹³. The background was identified as ⁹Be which reaches the detector by scattering processes. By applying an additional magnetic mass filter to the high energy mass spectrometer the background was effectively removed. A ¹⁰Be/⁹Be background ratio of <5 × 10⁻¹⁵ was achieved. The overall efficiency (detected ¹⁰Be compared to BeO⁻ injected into the accelerator) was 7-8%.     

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.     

Luminescence characteristics of Tl ions co-doped RbCl:Eu crystals

RbCl:Eu²⁺ single crystals which are co-doped with thallium display characteristic Eu²⁺ emission around 420 nm and additional emission band at 312 nm with a weak shoulder around 390 nm attributable to centers involving Tl⁺ ions. Additional excitation and emission bands observed in Tl⁺ doped RbCl:Eu²⁺ single crystals are attributed to the presence of Eu²⁺ aggregates and complex centres involving both Eu²⁺ and Tl⁺ ions. Inclusion of Tl⁺ ions in RbCl:Eu²⁺ crystals is found to enhance the intensity of Eu²⁺ emission at 420 nm due to an energy transfer from Tl⁺ → Eu²⁺ ions.     

FTIR and RBS study of ion-beam synthesized buried silicon oxide layers

Single crystal silicon samples were implanted at 140 keV by oxygen (¹⁶O⁺) ion beam to fluence levels of 1.0 × 10¹⁷, 2.5 × 10¹⁷ and 5.0 × 10¹⁷ cm⁻² to synthesize buried silicon oxide insulating layers by SIMOX (separation by implanted oxygen) process at room temperature and at high temperature (325 °C). The structure and composition of the ion-beam synthesized buried silicon oxide layers were investigated by Fourier transform infrared (FTIR) and Rutherford backscattering spectroscopy (RBS) techniques. The FTIR spectra of implanted samples reveal absorption in the wavenumber range 1250-750 cm⁻¹ corresponding to the stretching vibration of Si-O bonds indicating the formation of silicon oxide. The integrated absorption band intensity is found to increase with increase in the ion fluence. The absorption peak was rather board for 325 °C implanted sample. The FTIR studies show that the structures of ion-beam synthesized buried oxide layers are strongly dependent on total ion fluence. The RBS measurements show that the thickness of the buried oxide layer increases with increase in the oxygen fluence. However, the thickness of the top silicon layer was found to decrease with increase in the ion fluence. The total oxygen fluence estimated from the RBS data is found to be in good agreement with the implanted oxygen fluence. The high temperature implantation leads to increase in the concentration of the oxide formation compared to room temperature implantation.     

Molecular model for annihilation rates in positron complexes

The molecular approach for positron interaction with atoms is developed further. Potential energy curves for positron motion are obtained. Two procedures accounting for the nonadiabatic effective positron mass are introduced for calculating annihilation rate constants. The first one takes the bound-state energy eigenvalue as an input parameter. The second is a self-contained and self-consistent procedure. The methods are tested with quite different states of the small complexes HPs, e⁺He (electronic triplet) and e⁺Be (electronic singlet and triplet). For states yielding the positronium cluster, the annihilation rates are quite stable, irrespective of the accuracy in binding energies. For the e⁺Be states, annihilation rates are larger and more consistent with qualitative predictions than previously reported ones.     

Barrier modification of Au/n-GaAs Schottky diode by swift heavy ion irradiation

The effect of swift heavy ion (72.5 MeV ⁵⁸Ni⁶⁺) irradiation on Au/n-GaAs Schottky barrier characteristics is studied using in situ current-voltage measurements. Diode parameters are found to vary as a function of ion irradiation fluence. The Schottky barrier height (SBH) is found to be 0.55(±0.01) eV for the as deposited diode, which decreases with ion irradiation fluence. The SBH decreases to a value of 0.49(±0.01) eV at the highest ion irradiation fluence of 5 × 10¹³ ions cm⁻². The ideality factor is found to be 2.48 for unirradiated diode, and it increases with irradiation to a value of 4.63 at the highest fluence. The modification in Schottky barrier characteristics is discussed considering the energy loss mechanism of swift heavy ion at the metal-semiconductor interface.     

Ionization in symmetric and nearly symmetric low energy ion-surface collisions

Multiply charged ions are emitted following bombardment of Al(1 0 0) and Si(1 1 1) by low energy Si⁺ and P⁺ ions. The ion formation is attributed to inner-shell electron promotion during a hard collision between symmetric or nearly symmetric atomic species, followed by Auger decay outside the surface. The relative yield of triply charged Si ions for Si⁺ → Si(1 1 1) is much smaller than that of triply charged Al ions in direct recoil Si⁺ → Al(1 0 0) experiments. This difference can be explained by assuming that only one 2p hole is produced in a Si atom during the symmetric collision, whereas a double 2p hole is also produced in the Al atom following the nearly symmetric Si-Al collision. Further evidence is provided by the complimentary experiment P⁺ → Si(1 1 1), where Si³⁺ regains its intensity and Si⁴⁺ emerges as a result of a double 2p hole decay with shake-off.     

Coherent pair production by energetic gamma rays incident on quasicrystals

We develop a Born-approximation theory of coherent pair production (CPP) of electrons by energetic gamma rays incident on an icosahedral quasicrystal, described by a schematic model (K model) that includes phonon and phason disorder. Our main result is a formula for the cross-section dσ_cpp/dε₊ for CPP, differential with respect to the positron energy ε₊ and of order α² in the fine-structure constant α ≈ 1/137, but which is otherwise exact. We discuss results of numerical calculations of dσ_cpp/dε₊ versus y = ε₊/k for gamma rays of energies k = 20 MeV, 200 MeV, and 3 GeV, incident on icosahedral Al-Mn-Si, described as a special case of the K model (vertex model). This consists in placing an Mn atom at each vertex of the relevant Ammann tiles. Our calculations include CPP of types A and B. Both types exhibit vertical intensity drops at irregularly distributed y-values, many of these drops being so large that they should be observable experimentally. They are analogous to the large intensity drops exhibited by coherent bremsstrahlung in quasicrystals. We predict that CPP drops also occur for realistic models of i-Al-Mn-Si at the same y-values as for the vertex model, but whose magnitudes may differ from those predicted by this model.     

First-principles investigation on dissolution and diffusion of oxygen in tungsten

Using a first-principles method, we have investigated dissolution and diffusion properties of oxygen (O) in tungsten (W). Single O atom prefers to occupy the tetrahedral interstitial site (TIS). Two interstitial O atoms are attractive and tend to be paired up at two neighboring TIS with a distance of 0.228 nm and a large binding energy of 1.60 eV, which indicates a strong tendency of O clustering in W. O is preferred to diffuse between the most nearest neighboring TIS with a diffusion barrier of 0.17 eV. By the estimation of pre-exponential factor according to an empirical theory, the diffusion coefficient as a function of temperature has been determined, which is 1.50 × 10⁻⁹ m²/s at a typical temperature of 500 K. The results provide a good reference to understand the behavior of O in intrinsic W.     

Autoionization of N (q = 1-3) Rydberg states produced in high-energy collisions with He

Energy spectra of electrons ejected through autoionization decay of high-Rydberg states in high-energy collisions of N^q+ (q = 1-3) with He have been measured with high-resolution by using zero-degree electron spectroscopy. Several series of autoionizing lines were observed, corresponding to decays from N³⁺ 1s²2p(²P)nl Rydberg states produced in N³⁺ + He collisions, from N²⁺ 1s²2s2p(³P)nl Rydberg states produced in N²⁺ + He and from N⁺ 1s²2s2p²(⁴P)nl Rydberg states produced in N⁺ + He, respectively. Angular momentum distributions for the first or second peak of three series of Coster-Kronig electron transitions for N^q+ (q = 1-3) projectiles are also discussed, where the highly excited states are formed by electron excitation.     

Theory of He trapping, diffusion, and clustering in UO2

We have performed ab initio total energy calculations to investigate the behavior of helium and its diffusion properties in uranium dioxide (UO₂). Our investigations are based on the density functional theory within the generalized gradient approximation (GGA). The trapping behavior of He in UO₂ has been modeled with a supercell containing 96-atoms as well as uranium and oxygen vacancy trapping sites. The calculated incorporation energies show that for He a uranium vacancy is more stable than an oxygen vacancy or an octahedral interstitial site (OIS). Interstitial site hopping is found to be the rate-determining mechanism of the He diffusion process and the corresponding migration energy is computed as 2.79 eV at 0 K (with the spin-orbit coupling (SOC) included), and as 2.09 eV by using the thermally expanded lattice parameter of UO₂ at 1200 K, which is relatively close to the experimental value of 2.0 eV. The lattice expansion coefficient of He-induced swelling of UO₂ is calculated as 9 × 10⁻². For two He atoms, we have found that they form a dumbbell configuration if they are close enough to each other, and that the lattice expansion induced by a dumbbell is larger than by two distant interstitial He atoms. The clustering tendency of He has been studied for small clusters of up to six He atoms. We find that He strongly tends to cluster in the vicinity of an OIS, and that the collective action of the He atoms is sufficient to spontaneously create additional point defects around the He cluster in the UO₂ lattice.     

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.