Monte Carlo study of ion-induced backward and forward secondary electron emission from thin Al foil

A direct Monte Carlo program has been developed to calculate the backward (γ_b) and forward (γ_f) electron emission yields from 20 nm thick Al foil for impact of C⁺, Al⁺, Ar⁺, Cu⁺ and Kr⁺ ions having energies in the range of 0.1-10 keV/amu. The program incorporates the excitation of target electrons by projectile ions, recoiling target atoms and fast primary electrons. The program can be used to calculate the electron yields, distribution of electron excitation points in the target and other physical parameters of the emitted electrons. The calculated backward electron emission yield and the Meckbach factor R = γ_f/γ_b are compared with the available experimental data, and a good agreement is found. In addition, the effect of projectile energy and mass on the longitudinal and lateral distribution of the excitation points of the electrons emitted from front and back of Al target has been investigated.     

Pure ionization cross section of helium and ionization mechanism

Pure target ionization was investigated for 0.4-6.4 MeV C^q+(q = 1-4) + He and O^q+(q = 1-4) + He collisions. The double-to-single target ionization ratios R₂₁ were measured using coincidence techniques. We compare our results with existing experimental results and find they are in good agreement. The ratio R₂₁ is nearly independent of projectile charge state. The relation of R₂₁ ∼ V is analyzed using the over barrier model (OBM) and ionization probability, which is described in our extended over barrier model. Our calculation agrees well with the experimental results.     

A neutronic evaluation of the (Pu–U) and (Am–Pu–U) insertion in a typical fuel of Angra-I

The goal is to evaluate the neutronic behavior when (Pu–U) and (Am–Pu–U) mixed oxide are inserted in a typical cell of a Pressurized Water Reactor (PWR) such as Angra-I. Four types of fuels were studied: (1) MOX fuel enriched at 3.1% and V_m/V_f = 1.15; (2) MOX fuel enriched at 4.5% and V_m/V_f = 1.15; (3) MOX fuel enriched at 4.5% and V_m/V_f = 2.0 and (4) MOX fuel enriched at 4.5%, with 1% of Americium insertion in its composition (62.8% of Am²⁴¹, 0.1% of Am^242m and 37.1% of Am²⁴³) and with V_m/V_f = 2.0. The first case represents the standard state of Angra I, but with Pu. The second case is similar to the first but the enrichment is increased. To evaluate the Americium insertion, a study of the V_m/V_f was made and better results were obtained with V_m/V_f = 2.0 and to compare, this case was too evaluated to (Pu–U) in the third and fourth cases. The idea is to verify the possibility of using these fuels in Angra-I analyzing neutronic parameters such as infinite multiplication factor, hardening spectrum, Boron worth and reactivity temperature coefficients. The results show that it is possible to use all the studied fuels in Angra-I as well as to burn Am inserted in the MOX fuel by a considerable quantity during PWR operation. The WIMS-D5 code was used to perform a simplified neutronic and burnup simulations to evaluate this possibility.     

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.     

Interaction potentials for modeling of ion-surface scattering

Accurate potential data for system Ar⁺, С⁺, Cd⁺, Kr⁺, Ne⁺, Xe⁺, Zn⁺-Xe, Ar⁺-Ar and Ne⁺-Ne were obtained by analyzing the scattering cross-sections. These data extend the existing database of potentials obtained experimentally. To fit better the existing data, a new analytical form of the potential is proposed. The fitting errors analysis shows that the universal potential can be used only for the systems with nuclear charges Z > 18 and in the region where the distances of closest approach are less than R < 8 a_f (here a_f is the Firsov screening length (see below)). The model of individual potentials is suggested, which extends the region of potential application and minimizes the fitting errors.     

Thermal conductivity of (U,Pu,Np)O2 solid solutions

The thermal conductivities of (U_,Pu_,Np)O₂ solid solutions were studied at temperatures from 900 to 1770 K. Thermal conductivities were obtained from the thermal diffusivity measured by the laser flash method. The thermal conductivities obtained below 1400 K were analyzed with the data of (U,Pu,Am)O₂ obtained previously, assuming that the B-value was constant, and could be expressed by a classical phonon transport model, λ = (A + BT)⁻¹, A(z₁, z₂) = 3.583 × 10⁻¹ × z₁ + 6.317 × 10⁻² × z₂ + 1.595 × 10⁻² (m K/W) and B = 2.493 × 10⁻⁴ (m/W), where z₁ and z₂ are the contents of Am- and Np-oxides. It was found that the A-values increased linearly with increasing Np- and Am-oxide contents slightly, and the effect of Np-oxide content on A-values was smaller than that of Am-oxide content. The results obtained from the theoretical calculation based on the classical phonon transport model showed good agreement with the experimental results.     

Energy levels in Ag-like (4d4f, 4d5? (? = 0-3)), Pd-like (4d4f [J = 1], 4d5p [J = 1], 4d5f [J = 1]), and Rh-like (4d [J = 5/2, 3/2]) ions with Z ? 86

Relativistic perturbation theory with a model potential is used for the calculation of energy levels of the states 4f_5/2, 4f_7/2, 5s_1/2, 5p_1/2, 5p_3/2, 5d_3/2, 5d_5/2, 5f_5/2, and 5f_7/2 above the 1s²2s²2p⁶3s²3p⁶3d¹⁰4s²4p⁶4d¹⁰ core, with one vacancy , in the same core, in the silver and rhodium isoelectronic sequences with the maximum nuclear charge Z = 86. The method of extrapolation of the model potential parameter is applied to calculate one-electron and one-vacancy wavefunctions. The wavefunctions of Ag- and Rh-like ions were used to calculate the energies of resonance transitions to the ground state ¹S₀ in Pd-like ions. Good agreement between the theoretical and the experimental energies of the resonance transitions in Pd-like ions indicates the reliability of the results obtained.     

Approach for the fission fragment total kinetic energy TKE(A) calculation: Application to prompt neutron emission models

A simple approach for the calculation of the fission fragment total kinetic energy, TKE(A), based on the electrostatic repulsion between the fragments connected by a neck in the pre-scission configuration is described. The calculated TKE(A) is obtained in good agreement with the experimental data for many fissioning systems, such as ^233,235U(n_th, f), ²³⁹Pu(n_th, f), ²³⁷Np(n, f), ²⁴²Pu(SF), with minor adjustment of only one parameter. Due to the fact that the present approach can provide with enough trust TKE(A) distributions for fissioning systems for which experimental TKE(A) data do not exist, the possibilities to use the refined Point by Point model of prompt neutron emission can be considerably extended.     

Optical properties of UO2 and PuO2

We perform first-principles calculations of electronic structure and optical properties for UO₂ and PuO₂ based on the density functional theory using the generalized gradient approximation (GGA) + U scheme. The main features in orbital-resolved partial density of states for occupied f and p orbitals, unoccupied d orbitals, and related gaps are well reproduced compared to experimental observations. Based on the satisfactory ground-state electronic structure calculations, the dynamical dielectric function and related optical spectra, i.e., the reflectivity, adsorption coefficient, energy-loss, and refractive index spectrum, are obtained. These results are consistent with the available experiments.     

Growth of silicon nitride films by bombarding amorphous silicon with N ions: MD simulation

In this study, the molecular dynamics simulation method was employed to investigate the growth of silicon nitride films by using N⁺ ions, with energies of 50, 100, 150 and 200 eV, to bombard an amorphous silicon surface at 300 K. After an initial period of N⁺ bombardment, saturation of the number of N atoms deposited on the surface is observed, which is in agreement with experiments. During subsequent steady state deposition, a balance between uptake of N by the surface and sputtering of previously deposited N is established. The Si(N_x) (x = 1-4) and N(Si_y) (y = 1-3) bond configurations in the grown films are analyzed.     

Photostimulated luminescence studies of γ-irradiated KBr1−xIx:TlI mixed crystals

Results on photoluminescence and photostimulated luminescence studies of KBr_1−xI_x:TlI (0.01 and 0.05 mol%) mixed crystals grown in vacuum and air are presented. Photoluminescence spectra of the mixed crystals excited in the A-absorption band of KBr:Tl⁺ exhibited the characteristic emission bands of Tl⁺ ions in KBr:Tl⁺. When excited in the low energy tail of A-band absorption, additional emission bands were observed. Compared with earlier reports, excitation bands observed around 4.8, 4.6 and 4.4 eV are attributed to complex thallium centres of the form TlBr_6−nI_n (n = 0, 1, 2, 3). Photostimulated luminescence of γ-irradiated KBr_1−xI_x:TlI mixed crystals showed the presence of emission bands similar to the characteristic photoluminescence of Tl⁺ ions. The photostimulated luminescence slightly shifted towards the low energy side with increasing iodide composition x. The mechanism of emission in these mixed crystals is discussed. Dose response and storage stability (fading characteristics) in these mixed crystals are reported.     

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.     

First-principles study of electronic structure and insulating properties of uranium and plutonium dioxides

First-principles density functional theory calculations were carried out to investigate the electronic structure and the degree of 5f states localization of the Mott-Hubbard type insulators UO₂ and PuO₂. We used the fully relativistic cluster discrete variational method (RDV) with the local exchange-correlation potential. The energies of one-electron transition between occupied and vacant 5f^5/2 states of neighboring actinide atoms were evaluated on the base of the ground state and the excited state calculations. It is found that in UO₂ and PuO₂ the energy difference between 5f^5/2 levels of nearest metal sites in the lattice are close to 1.0 eV and 0.9 eV, despite the results of conventional band structure approach predicting that both oxides are good conductors.     

Enthalpy measurements of La2Te3O9 and La2Te4O11

Enthalpy increment measurements on La₂Te₃O₉(s) and La₂Te₄O₁₁(s) were carried out using a Calvet micro-calorimeter. The enthalpy values were analyzed using the non-linear curve fitting method. The dependence of enthalpy increments with temperature was given as: H°(T) − H°(298.15 K) (J mol⁻¹) = 360.70T + 0.00409T² + 133.568 × 10⁵/T − 149 923 (373 ? T (K) ? 936) for La₂Te₃O₉ and H°(T) − H°(298.15 K) (J mol⁻¹) = 331.927T + 0.0549T² + 29.3623 × 10⁵/T − 114 587 (373 ? T (K) ? 936) for La₂Te₄O₁₁.     

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.     

Study on the behavior of oxygen atoms in swift heavy ion irradiated CeO2 by means of synchrotron radiation X-ray photoelectron spectroscopy

To study the effects of swift heavy ion irradiation on cerium dioxide (CeO₂), CeO₂ sintered pellets were irradiated with 200 MeV Xe ions at room temperature. For irradiated and unirradiated samples, the spectra of X-ray photoelectron spectroscopy (XPS) were measured. XPS spectra for the irradiated samples show that the valence state of Ce atoms partly changes from +4 to +3. The amount of Ce³⁺ state was quantitatively obtained as a function of ion-fluence. The relative amount of oxygen atom displacements, which are accompanied by the decrease in Ce valence state, is 3-5%. This value is too large to be explained in terms of elastic interactions between CeO₂ and 200 MeV ions. The experimental result suggests the contribution of 200 MeV Xe induced electronic excitation to the displacements of oxygen atoms.     

Bulk properties and photoelectron spectroscopy of the ζ-U-Pu phase

The ζ-phase, existing between 35% and 70% U in Pu, belongs to the high-density phases seen from the point of view of systematics of allotropic modifications of Pu metal. Despite the volume per actinide atom only slightly higher than for α-Pu, it magnetic susceptibility is much higher than for α-Pu and exceeds even the δ-Pu value. Similarly, the Sommerfeld coefficient γ > 40 mJ/mol Pu K² exceeds the experimental δ-Pu value. The data confirm that the volume is not the primary control parameter affecting the situation around the Fermi level of common Pu phases and they point against the traditional belief that they are essentially narrow 5f band systems. Electronic structure calculations suggest that the 5f states of Pu have slightly lower occupancy comparing with δ-Pu. A tendency to the 5f localization can be seen in the Pu dilution situation in the photoelectron spectra.     

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.     

Studies on new neutron-sensitive dosimeters using an optically stimulated luminescence technique

The neutron response of detectors prepared using α-Al₂O₃:C phosphor developed using a melt processing technique and mixed with neutron converters was studied in monoenergetic neutron fields. The detector pellets were arranged in two different pairs: α-Al₂O₃:C + ⁶LiF/α-Al₂O₃:C + ⁷LiF and α-Al₂O₃:C + high-density polyethylene/α-Al₂O₃:C + Teflon, for neutron dosimetry using albedo and recoil proton techniques. The optically stimulated luminescence response of the Al₂O₃:C + ^6,7LiF dosimeter to radiation from a ²⁵²Cf source was 0.21, in terms of personal dose equivalent H_p(10) and relative to radiation from a ¹³⁷Cs source. This was comparable to results obtained with similar detectors prepared using commercially available α-Al₂O₃:C phosphor. The H_p(10) response of the α-Al₂O₃:C + ^6,7LiF dosimeters was found to decrease by more than two orders of magnitude with increasing neutron energy, as expected for albedo dosimeters. The response of the α-Al₂O₃:C + high-density polyethylene/α-Al₂O₃:C + Teflon dosimeters was small, of the order of 1% to 2% in terms of Hp(10) and relative to radiation from a ¹³⁷Cs source, for neutron energies greater than 1 MeV.     

The (He, tf) as a surrogate reaction to determine (n, f) cross sections in the 10-20 MeV energy range

The surrogate reaction ²³⁸U(³He, tf) is used to determine the ²³⁷Np(n, f) cross section indirectly over an equivalent neutron energy range from 10 to 20 MeV. A self-supporting ∼761 μg/cm² metallic ²³⁸U foil was bombarded with a 42 MeV ³He²⁺ beam from the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory (LBNL). Outgoing charged particles and fission fragments were identified using the Silicon Telescope Array for Reaction Studies (STARS) consisted of two 140 μm and one 1000 μm Micron S2 type silicon detectors. The ²³⁷Np(n, f) cross sections, determined indirectly, were compared with the ²³⁷Np(n, f) cross section data from direct measurements, the Evaluated Nuclear Data File (ENDF/B-VII.0), and the Japanese Evaluated Nuclear Data Library (JENDL 3.3) and found to closely follow those datasets. Use of the (³He, tf) reaction as a surrogate to extract (n, f) cross sections in the 10-20 MeV equivalent neutron energy range is found to be suitable.