Relativistic energy, fine structure, and hyperfine-structure studies of the high-lying core-excited states P(n) (n = 1-3) and S(m) (m = 1-3) for the Be-like isoelectronic sequence

The variational method using a multiconfiguration interaction wavefunction is carried out on the high-lying core-excited states ⁵P(n) (n = 1-3) and ⁵S^o(m) (m = 1-3) for the Be-like isoelectronic sequence from Z = 7 to 10, including mass polarization and relativistic corrections. Relativistic energies, oscillator strengths, wavelengths, and lifetimes are reported. The results are compared with other theoretical and experimental data in the literature. The fine structure and hyperfine structure of core-excited states for this system are also investigated.     

Prolapse-free relativistic Gaussian basis sets for the superheavy elements up to Uuo (Z = 118) and Lr (Z = 103)

Prolapse-free basis sets suitable for four-component relativistic quantum chemical calculations are presented for the superheavy elements up to ₁₁₈Uuo (₁₀₄Rf, ₁₀₅Db, ₁₀₆Sg, ₁₀₇Bh, ₁₀₈Hs, ₁₀₉Mt, ₁₁₀Ds, ₁₁₁Rg, ₁₁₂Uub, ₁₁₃Uut, ₁₁₄Uuq, ₁₁₅Uup, ₁₁₆Uuh, ₁₁₇Uus, ₁₁₈Uuo) and ₁₀₃Lr. These basis sets were optimized by minimizing the absolute values of the energy difference between the Dirac-Fock-Roothaan total energy and the corresponding numerical value at a milli-Hartree order of magnitude, resulting in a good balance between cost and accuracy. Parameters for generating exponents and new numerical data for some superheavy elements are also presented.     

Wavelengths and transition probabilities for n = 4 → n′ = 4 transitions in heavy Cu-like ions (70 ? Z ? 92)

Wavelengths and transition probabilities have been calculated for the n = 4 → n′ = 4 allowed transitions in the heavy Cu-like ions with Z = 70-92. Fully relativistic multiconfiguration Dirac-Fock (MCDF) calculations were carried out. They take into account the correlations within the n = 4 complex, the core-valence n = 3 → n′ = 4 virtual excitations, and quantum electrodynamics effects. The present results are compared to and agree well with recent electron-beam ion-trap (EBIT) measurements in ytterbium, tungsten, osmium, gold, lead, bismuth, thorium, and uranium.     

Molybdenum L-shell X-ray production by 350-600 keV Xe (q = 25-30) ions

Molybdenum L-shell X-rays were produced by Xe^q+ (q = 25-30) bombardment at low energies from 2.65 to 4.55 keV/amu (350-600 keV). We observed a kinetic energy threshold of Mo L-shell ionization down to 2.65-3.03 keV/amu (350-400 keV). The charge state effect of the incident ions was not observed which shows that the ions were neutralized, reaching an equilibrium charge state and losing their initial charge state memory before production of L-shell vacancies resulted in X-ray production. The experimental ionization cross sections were compared with those from Binary Encounter Approximation theory. Taking into account projectile deflection in the target nuclear Coulomb field, the ionization cross section of Mo L-shell near the kinetic energy threshold was well described.     

K-shell absorption jump factors and jump ratios in elements between Tm (Z = 69) and Os (Z = 76) derived from new mass attenuation coefficient measurements

The K-shell absorption jump factors and jump ratios were derived from new mass attenuation coefficients measured using an energy dispersive X-ray fluorescence (EDXRF) spectrometer for Tm, Yb elements being Tm₂O₃, Yb₂O₃ compounds and pure Lu, Hf, Ta, W, Re and Os. The measurements, in the region 56-77 keV, were done in a transmission geometry utilizing the K_α1, K_α2, K_β1 and K_β2 X- rays from different secondary source targets (Yb, Ta, Os, W, Re and Ir, etc.) excited by the 123.6 keV γ-photons from an ⁵⁷Co annular source and detected by an Ultra-LEGe solid state detector with a resolution of 150 eV at 5.9 keV. Experimental results have been compared with theoretically calculated values. The measured values of Tm, Yb, Lu, Hf, Ta, W, Re and Os are reported here for the first time.     

Determination of K shell absorption jump factors and jump ratios in the elements between Tm(Z = 69) and Os(Z = 76) by measuring K shell fluorescence parameters

The K shell absorption jump factors and jump ratios have been measured in the elements between Tm (Z = 69) and Os(Z = 76) without having any mass attenuation coefficient at the upper and lower energy branch of the K absorption edge. The jump factors and jump ratios for these elements have been determined by measuring K shell fluorescence parameters such as the total atomic absorption cross-sections, the K_α X-ray production cross-sections, the intensity ratio of the K_β and K_α X-rays and the K shell fluorescence yields. We have performed the measurements for the calculations of these values in attenuation and direct excitation experimental geometry. The K X-ray photons are excited in the target using 123.6 keV gamma-rays from a strong ⁵⁷Co source, and detected with an Ultra-LEGe solid state detector with a resolution 0.15 keV at 5.9 keV. The measured values have been compared with theoretical and others’ experimental values. The results have been plotted versus atomic number.     

Non-dipole second order parameters of the photoelectron angular distribution for elements Z = 1-100 in the photoelectron energy range 1-10 keV

Presented here are the photoelectron angular distribution non-dipole parameters associated with the terms of the second order O [(kr)²] (k is the photon energy and r is the radius of the ionized atomic shell) for both unpolarized and linearly polarized radiation. The parameters are given for atomic shells with binding energies lower than 2 keV of all elements 1 ? Z ? 100 for four values of photoelectron energy in the range 1−10 keV. In this range, the second-order terms are shown to make a significant contribution (up to ∼30%) to the angular differential cross section. The inclusion of these terms becomes all the more important in calculations of the differential cross section ratio for the fixed geometry of angles which is measured experimentally in the case of linearly polarized radiation. The Dirac-Fock-Slater potential is used in the calculations. The hole left by the emitted electron is taken into account in the frozen orbital approximation.     

Rydberg and autoionizing triplet states in Helium up to the N = 5 threshold

Energy levels of highly excited bound Rydberg states, the position and widths of autoionizing states, and oscillator strengths are calculated for He ³S, ³P^e, ³P^o, ³D^e and ³D^o symmetries up to the N = 5 He⁺ excitation threshold. The calculations are performed with the K-matrix B-spline method with maximum orbital angular momentum ?_max = 8. Reliable doubly excited-state parameters up to the n = 20 multiplet below each ionization threshold are presented. One thousand and six hundred newly identified bound and metastable states, seven times those available in literature, fill many gaps, reveal a dozen intruder states, and allow new speculations on propensity rules and radiative decays of triplet Rydberg states.     

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%.     

Thermodynamic properties of ThxU1−xO2 (0 < x < 1) based on quantum-mechanical calculations and Monte-Carlo simulations

Th_xU_1−xO_2+y binary compositions occur in nature, uranothorianite, and as a mixed oxide nuclear fuel. As a nuclear fuel, important properties, such as the melting point, thermal conductivity, and the thermal expansion coefficient change as a function of composition. Additionally, for direct disposal of Th_xU_1−xO₂, the chemical durability changes as a function of composition, with the dissolution rate decreasing with increasing thoria content. UO₂ and ThO₂ have the same isometric structure, and the ionic radii of 8-fold coordinated U⁴⁺ and Th⁴⁺ are similar (1.14 nm and 1.19 nm, respectively). Thus, this binary is expected to form a complete solid solution. However, atomic-scale measurements or simulations of cation ordering and the associated thermodynamic properties of the Th_xU_1−xO₂ system have yet to be determined. A combination of density-functional theory, Monte-Carlo methods, and thermodynamic integration are used to calculate thermodynamic properties of the Th_xU_1−xO₂ binary (ΔH_mix, ΔG_mix, ΔS_mix, phase diagram). The Gibbs free energy of mixing (ΔG_mix) shows a miscibility gap at equilibration temperatures below 1000 K (e.g., E_exsoln = 0.13 kJ/(mol cations) at 750 K). Such a miscibility gap may indicate possible exsolution (i.e., phase separation upon cooling). A unique approach to evaluate the likelihood and kinetics of forming interfaces between U-rich and Th-rich has been chosen that compares the energy gain of forming separate phases with estimated energy losses of forming necessary interfaces. The result of such an approach is that the thermodynamic gain of phase separation does not overcome the increase in interface energy between exsolution lamellae for thin exsolution lamellae (10 Å). Lamella formation becomes energetically favorable with a reduction of the interface area and, thus, an increase in lamella thickness to >45 Å. However, this increase in lamellae thickness may be diffusion limited. Monte-Carlo simulations converge to an exsolved structure [lamellae || ] only for very low equilibration temperatures (below room temperature). In addition to the weak tendency to exsolve, there is an ordered arrangement of Th and U in the solid solution [alternating U and Th layers || {1 0 0}] that is energetically favored for the homogeneously mixed 50% Th configurations. Still, this tendency to order is so weak that ordering is seldom reached due to kinetic hindrances. The configurational entropy of mixing (ΔS_mix) is approximately equal to the point entropy at all temperatures, indicating that the system is not ordered.     

Maxwellian-averaged neutron-induced reaction cross sections and astrophysical reaction rates for kT = 1 keV to 1 MeV calculated from microscopic neutron cross section library JENDL-3.3

Maxwellian-averaged cross sections and astrophysical reaction rates were calculated for neutron capture, fission, (n,p), (n,α), and some threshold reactions based on a microscopic neutron cross section data library, the Japanese Evaluated Nuclear Data Library Version 3.3 (JENDL-3.3). The calculation was made for temperatures (kT) from 1 keV to 1 MeV including the most important range in astrophysical nucleosynthesis. Results are presented in the tables and graphs. The Maxwellian-averaged neutron capture cross sections are compared with recommendations of other authors. Implications of the differences between the present data and previous ones to s-process nucleosynthesis are discussed.     

Structural study of Pu1−xAmxO2 (x = 0.2; 0.5; 0.8) obtained by oxalate co-conversion

This study describes the synthesis and the characterisation of Pu_1−xAm_xO₂ (x = 0.2; 0.5; 0.8) mixed oxides obtained by oxalate co-conversion. We studied the self-irradiation effect in these compounds at the structural scale. We determined, for each composition, the initial lattice parameter and the equation describing its variation versus time and displacements per atom. Similarly to other α emitting compounds, it was observed a fast lattice parameter expansion rate, followed by a stabilisation at a maximum value. The observations also showed that the initial expansion rate varies according to the Am content and the maximum value to the Pu content. However, for all compositions, the lattice parameter relative variations are the same.     

Computer simulation of sputtering at the low index (1 0 0), (1 1 0) and (1 1 1) surfaces of Ni3Al in a STEM

The present study is relevant to the preferential Al sputtering and/or enhancement of the Ni/Al ratio in Ni₃Al observed by the scanning transmission electron microscopy fitted with a field emission gun (FEG STEM). Atomic recoil events at the low index (1 0 0), (1 1 0) and (1 1 1) surfaces of Ni₃Al through elastic collisions between electrons and atoms are simulated using molecular dynamics (MD) methods. The threshold energy for sputtering, E_sp, and adatom creation, E_ad, are determined as a function of recoil direction. Based on the MD determined E_sp, the sputtering cross-sections for Ni and Al atoms in these surfaces are calculated with the previous proposed model. It is found that the sputtering cross-section for Al atoms is about 7-8 times higher than that for Ni, indicating the preferential sputtering of Al in Ni₃Al, in good agreement with experiments. It is also found that the sputtering cross-sections for Ni atoms are almost the same in these three surfaces, suggesting that they are independent of surface orientation. Thus, the sputtering process is almost independent of the surface orientation in Ni₃Al, as it is controlled by the sputtering of Ni atoms with a lower sputtering rate.     

A special correcting winding for the l = 2 torsatron with split-type helical coils

A split-type special correcting winding (split-type SCW) for the l = 2 torsatron toroidal magnetic system with split-type helical coils is considered. The split-type SCW gives the possibility of controlling the position of the magnetic surface configuration in the direction perpendicular to the torus equatorial plane. Numerical simulations were carried out to investigate the influence of the split-type SCW magnetic field on centered and distant relative to the torus surface magnetic surface configuration with a plane magnetic axis, being promising for the fusion reactor. The configuration is realized in the l = 2 torsatron with split-type helical coils and with the coils of an additional toroidal magnetic field. The calculations show that the split-type SCW magnetic field influence on the initial magnetic surface configuration leads mainly to the magnetic surface configuration displacement along the straight z axis of torus rotation. The displacement of ∼0.1a, a is the minor radius of the torus, has no critical effect on the magnetic surface parameters. An idea on the split-type SCW magnetic field structure is obtained by numerical simulations of the effect of this field as a minority magnetic field imposed on the magnetic field of a well-known configuration. The split-type SCW magnetic field is directed, predominantly along the major radius of the torus within its volume. The displacement range of the closed magnetic surface configuration depends on the split-type SCW magnetic field value.     

Wavelengths and transition probabilities in heavy Ge-like ions (70 ? Z ? 92)

Wavelengths and transition probabilities have been calculated for the 4s²4p²-4s4p³ and 4s²4p²-4s²4p4d allowed transitions and for the forbidden (M1 and E2) transitions occurring within the ground configuration (4s²4p²) in the heavy Ge-like ions with Z = 70-92. The fully relativistic multiconfiguration Dirac-Fock method taking into account both the correlations within the n = 4 complex and the QED effects has been used for the calculations. The present results are compared to and agree well with recent electron-beam ion-trap measurements in tungsten, osmium, gold, bismuth, thorium, and uranium.     

Contribution of near-edge processes to attenuation of the characteristic X-rays in elements with 48 ≤ Z ≤ 83

Attenuation of the characteristic K X-rays in the ₄₈Cd, ₅₀Sn, ₅₂Te, ₆₄Gd, ₆₅Tb, ₆₆Dy, ₆₈Er, ₇₄Ta, ₇₅Re, ₇₉Au, ₈₂Pb and ₈₃Bi elements have been measured with especial emphasis for the X-ray energies (E_in) in the region of respective K-shell/L_i subshell (i = 1, 2, 3) ionization threshold (B_K/B_Li). The characteristic X-rays were obtained from different fluorescent target elements excited by the X-rays and γ-rays emitted from the ⁵⁵Fe and ²⁴¹Am radioisotopes, respectively. The measurements were performed using an energy-dispersive detection set up involving a low-energy Ge detector. The measured attenuation coefficients for the X-rays with energies away from ionization thresholds of the attenuator element are found to be in good agreement with the available theoretical coefficients, which incorporate contributions of the photoionization, and the Rayleigh and Compton scattering processes. However, the measured attenuation coefficients are found to deviate significantly from the theoretical values for the X-rays with energies in vicinity of B_K/Li. The observed alteration is attributed to the X-ray Absorption Fine Structure (XAFS) for negative B_K/Li − E_in values, and the K-shell/L_i subshell resonant Raman scattering (RRS) process for positive B_K/Li − E_in values. Systematic of the K-shell/L_i subshell RRS contribution to attenuation of the X-rays are discussed in terms of the respective oscillator density and fraction of electrons available in the K-shell/L_i subshell Lorentzian profile of the attenuation element below E_in.     

Temperature dependence of lattice disorder in Ar-irradiated (1 0 0), (1 1 0) and (1 1 1) MgO single crystals

To better appreciate dynamic annealing processes in ion irradiated MgO single crystals of three low-index crystallographic orientations, lattice damage variation with irradiation temperature was investigated. Irradiations were performed with 100 keV Ar ions to a fluence of 1 × 10¹⁵ Ar/cm² in a temperature interval from −150 to 1100 °C. Rutherford backscattering spectroscopy combined with ion channeling was used to analyze lattice damage. Damage recovery with increasing irradiation temperature proceeded via two characteristic stages separated by 200 °C. Strong radiation damage anisotropy was observed at temperatures below 200 °C, with (1 1 0) MgO being the most radiation damage tolerant. Above 200 °C damage recovery was isotropic and almost complete recovery was reached at 1100 °C. We attributed this orientation dependence to a variation of dynamic annealing mechanisms with irradiation temperature.     

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.     

Influence on the structural characteristic of defect solid solution GdxZr1−xO2−x/2 with 0.18 ? x ? 0.62 under longer term annealing studied by Gd Mössbauer spectroscopy

Three kinds of defect solid solution Gd_xZr_1−xO_2−x/2 with 0.18 ? x ? 0.62, including the three single crystal samples with x = 0.21, 0.26 and 0.30, were investigated by ¹⁵⁵Gd Mössbauer spectroscopy at 12 K. Difference in the structural characteristic under longer term annealing were confirmed by comparing the ¹⁵⁵Gd Mössbauer parameters of the polycrystalline samples sintered one time and twice at 1773 K for 16 h in air, respectively. The results indicated that the polycrystalline samples sintered twice have relatively equilibrated structure by comparing with the three single crystal samples. After being sintered twice, basically the local structure around the Gd³⁺ ions does not change, but the degree of the displacements of the six 48f oxygen ions from positions of cubic symmetry becomes slightly smaller, and distribution of the Gd³⁺ ions in the system becomes more homogeneous.