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The electronic structure and magnetic moment of dilute U impurity in metallic hosts have been calculated from first principles. The calculations have been performed within local density approximation of the density functional theory using Augmented plane wave+local orbital (APW+lo) technique, taking account of spin–orbit coupling and Coulomb correlation through LDA+U approach. We present here our results for the local density of states, magnetic moment and hyperfine field calculated for an isolated U impurity embedded in hosts with sp -, d - and f -type conduction electrons. The results of our systematic study provide a comprehensive insight on the pressure dependence of 5 f local magnetism in metallic systems. The unpolarized local density of states (LDOS), analyzed within the frame work of Stoner model suggest the occurrence of local moment for U in sp -elements, noble metals and f -block hosts like La, Ce, Lu and Th. In contrast, U is predicted to be nonmagnetic in most transition metal hosts except in Sc, Ti, Y, Zr, and Hf consistent with the results obtained from spin polarized calculation. The spin and orbital magnetic moments of U computed within the frame of LDA+U formalism show a scaling behavior with lattice compression. We have also computed the spin and orbital hyperfine fields and a detail analysis has been carried out. The host dependent trends for the magnetic moment, hyperfine field and 5 f occupation reflect pressure induced change of electronic structure with U valency changing from 3 + to 4 + under lattice compression. In addition, we have made a detailed analysis of the impurity induced host spin polarization suggesting qualitatively different roles of f -band electrons on moment stability. The results presented in this work would be helpful towards understanding magnetism and spin fluctuation in U based alloys. [ABSTRACT FROM AUTHOR]

Fluorite CeO2 doped with group IV elements is studied within the density functional theory ( DFT) and DFT + U framework. Concentration-dependent formation energies are calculated for Ce1− x Z x O2 (Z = C, Si, Ge, Sn, Pb, Ti, Zr, Hf) with 0 ≤ x ≤ 0.25 and a roughly decreasing trend with ionic radius is observed. The influence of the valence and near valence electronic configuration is discussed, indicating the importance of filled d and f shells near the Fermi level for all properties investigated. A clearly different behavior of group IVa and IVb dopants is observed: the former are more suitable for surface modifications and the latter are more suitable for bulk modifications. For the entire set of group IV dopants, there exists an inverse relation between the change, due to doping, of the bulk modulus, and the thermal expansion coefficients. Hirshfeld-I atomic charges show that charge-transfer effects due to doping are limited to the nearest-neighbor oxygen atoms. [ABSTRACT FROM AUTHOR]

The phase formation and crystallization processes of metastable [CsCl]Fe1-xSi phases were investigated by irradiating ℇ-FeSi/Si(111) thin films with a pulsed excimer laser in the energy density range 300–900 mJ/cm2. The samples were analysed by Rutherford backscattering and channeling spectrometry (RBS/C), cross-sectional transmission electron microscopy (TEM) and conversion electron Mössbauer spectroscopy (CEMS). Laser irradiation results in mixing of the FeSi with the Si substrate, with the final concentration depending on the laser energy density. Due to the extremely rapid quench of the melt, a non-uniform Fe concentration is obtained. Analysis by cross-sectional transmission electron microscopy confirmed that this phase, which exhibits epitaxial ordering, corresponds to the metastable [CsCl]Fe1-xSi phase, which converts into the semiconducting β-FeSi2 upon annealing at 600°C. CEMS indicates that no stable Fe-silicide phase nor a combination of stable phases have been formed. The CEM spectra consist of a distribution of quadrupole doublets and isomer shifts, in agreement with a [CsCl]Fe1-xSi phase that exhibits a (i) composition gradient and (ii) a random number of Fe vacancies in the neighbouring shells. These distributions make the CEM spectra hard to interpret. Full-Potential Linearized Augmented Plane Wave (FLAPW) calculations were performed to gain more insight in the hyperfine interaction parameters of the metastable [CsCl]Fe1-xSi phase and their dependence on a concentration variation. These calculations confirm the decreasing trend of the isomer shift with increasing number of laser pulses. [ABSTRACT FROM AUTHOR]

The functional properties of Mn-doped Ge depend to large extent on the lattice location of the Mn impurities. Here, we present a lattice location study of implanted diluted Mn by means of electron emission channeling. Surprisingly, in addition to the expected substitutional lattice position, a large fraction of the Mn impurities occupies the bond-centered site. Corroborated by ab initio calculations, the bond-centered Mn is related to Mn-vacancy complexes. These unexpected results call for a reassessment of the theoretical studies on the electrical and magnetic behavior of Mn-doped Ge, hereby including the possible role of Mn-vacancy complexes. [ABSTRACT FROM AUTHOR]

We present a lattice location study of the n-type dopant arsenic after ion implantation into germanium. By means of electron emission channeling experiments, we have observed that the implanted As atoms substitute the Ge host atoms and that, in contrast to several implanted metal impurities in Ge, no significant fraction of As is found on interstitial sites. The substitutional As impurities are found to be thermally stable up to 600 °C. After 700 °C annealing a strong reduction of emission channeling effects was observed, in full accordance with the expected diffusion-induced broadening of the As profile. [ABSTRACT FROM AUTHOR]

ZnAl2O4 (gahnite) is a ceramic which is considered a possible transparent conducting oxide (TCO) due to its wide band gap and transparency for UV. Defects play an important role in controlling the conductivity of a TCO material along with the dopant, which is the main source of conductivity in an otherwise insulating oxide. A comprehensive first-principles density functional theory study for point defects in ZnA2O4 spinel is presented using the Heyd, Scuseria, and Ernzerhof hybrid functional (HSE06) to overcome the band gap problem. We have investigated the formation energies of intrinsic defects which include the Zn, Al, and O vacancy and the antisite defects: Zn at the Al site (ZnAl) and Al at the Zn site (AlZn). The antisite defect Ala, has the lowest formation energy and acts as a shallow donor, indicating possible rc-type conductivity in ZnA2O4 spinel by Al doping. [ABSTRACT FROM AUTHOR]

The crystal structure of lanthanum cerium oxide (La2Ce2O7) is investigated using ab initio density functional theory calculations. The relative stability of fluorite- and pyrochlorelike structures is studied through comparison of their formation energies. These formation energies show the pyrochlore structure to be favored over the fluorite structure, apparently contradicting the conclusions based on experimental neutron and x-ray diffraction (XRD). By calculating and comparing XRD spectra for a set of differently ordered and random structures, we show that the pyrochlore structure is consistent with diffraction experiments. For these reasons, we suggest the pyrochlore structure as the ground-state crystal structure for La2Ce2O7. [ABSTRACT FROM AUTHOR]

We examine the electronic structure of the family of ternary zinc spinel oxides ZnX2O4 (X = Al, Ga and In). The band gap of ZnAl2O4 calculated using density functional theory (DFT) is 4.25 eV and is overestimated compared with the experimental value of 3.8-3.9 eV. The DFT band gap of ZnGa2O4 is 2.82 eV and is underestimated compared with the experimental value of 4.4-5.0 eV. Since DFT typically underestimates the band gap in the oxide system, the experimental measurements for ZnAl2O4 probably require a correction. We use two first-principles techniques capable of describing accurately the excited states of semiconductors, namely the GW approximation and the modified Becke-Johnson (MBJ) potential approximation, to calculate the band gap of ZnX2O4. The GW and MBJ band gaps are in good agreement with each other. In the case of ZnAl2O4, the predicted band gap values are >6 eV, i.e. ~2 eV larger than the only reported experimental value. We expect future experimental work to confirm our results. Our calculations of the electron effective masses and the second band gap indicate that these compounds are very good candidates to act as transparent conducting host materials. [ABSTRACT FROM AUTHOR]

The aim of this work is to investigate phase formation in the Fe–Si system upon pulsed laser annealing of an ϵ-FeSi layer on Si(111). The layers have been analysed with Rutherford backscattering spectrometry (RBS) and conversion electron Mo¨ssbauer spectroscopy (CEMS). Results of RBS indicate that layers are formed with an altered Fe/Si composition. Additionally, the Fe/Si composition within one layer is not homogeneous; a composition gradient is present throughout the layer. CEMS, a nuclear technique sensitive to the local environment of the 57Fe nucleus, indicates that no stable or combinations of stable Fe-silicide phases have been formed. The CEMS spectra observed point in the direction of the metastable [CsCl]Fe1−xSi phase. However, the CEMS spectra are hard to interpret, on one hand, due to the large amount of different local environments of the Fe nucleus in this [CsCl]Fe1−xSi phase giving rise to a distribution of electric field gradients and isomer shifts, and on the other hand the influence of the concentration gradient on this distribution of electric field gradients and isomer shifts. To gain more insight in the hyperfine interaction parameters of the metastable [CsCl]Fe1−xSi phase and their dependence on concentration variation, FLAPW calculations are performed. These are necessary for the confirmation of the CEMS results. [Copyright &y& Elsevier]

We examined the interaction between adatoms and graphene for Ag, Cd, In and Hg by density functional theory. We establish a relation between the binding energy and the electric-field gradient tensor (EFG) for each atom, which indicates that hyperfine interactions can be used to probe the binding and stability of adatoms on graphene. The EFG is also shown to be a fingerprint for the local configuration, even at the sub-Angstrom scale. This work demonstrates how suitable hyperfine methods, such as perturbed angular correlation spectroscopy, can be used to experimentally unravel details of atomic adsorption on graphene, and by extension on two-dimensional materials in general. [ABSTRACT FROM AUTHOR]

Epitaxially stabilized iron monosilicide films with the CsCl structure (B2-FeSi) have been investigated by conversion electron Mössbauer spectroscopy and x-ray diffraction. A detailed investigation of the elastic strain in these metastable layers is presented. Using hyperfine interaction information the tetragonal distortion of the silicide lattice could be quantified for layers as thin as 14 Å. A general tendency for strain relaxation with increasing layer thickness is observed. [ABSTRACT FROM AUTHOR]

We report Density Functional Theory calculations for the atomic positions and the electric-field gradients (EFG) at Zr sites in a series of Zr compounds, with the FP-LAPW and the GIPAW methods. These data are used to obtain a value for the nuclear quadrupole moments of 90Zr and 91Zr, of which the precision and reliability with respect to tabulated values is discussed. An error bar on our suggested values is provided. Good agreement is obtained between the (faster) GIPAW method and (slower yet established) FP-LAPW method, especially when identical atomic positions are imposed. This increases the confidence in GIPAW calculations for electric-field gradient and nuclear quadrupole moment determination. [ABSTRACT FROM AUTHOR]

Predictions of observable properties by density-functional theory calculations (DFT) are used increasingly often by experimental condensed-matter physicists and materials engineers as data. These predictions are used to analyze recent measurements, or to plan future experiments in a rational way. Increasingly more experimental scientists in these fields therefore face the natural question: what is the expected error for such a first-principles prediction? Information and experience about this question is implicitly available in the computational community, scattered over two decades of literature. The present review aims to summarize and quantify this implicit knowledge. This eventually leads to a practical protocol that allows any scientist—experimental or theoretical—to determine justifiable error estimates for many basic property predictions, without having to perform additional DFT calculations. A central role is played by a large and diverse test set of crystalline solids, containing all ground-state elemental crystals (except most lanthanides). For several properties of each crystal, the difference between DFT results and experimental values is assessed. We discuss trends in these deviations and review explanations suggested in the literature. A prerequisite for such an error analysis is that different implementations of the same first-principles formalism provide the same predictions. Therefore, the reproducibility of predictions across several mainstream methods and codes is discussed too. A quality factor Δ expresses the spread in predictions from two distinct DFT implementations by a single number. To compare the PAW method to the highly accurate APW+lo approach, a code assessment of VASP and GPAW (PAW) with respect to WIEN2k (APW+lo) yields Δ-values of 1.9 and 3.3 meV/atom, respectively. In both cases the PAW potentials recommended by the respective codes have been used. These differences are an order of magnitude smaller than the typical difference with experiment, and therefore predictions by APW+lo and PAW are for practical purposes identical. [ABSTRACT FROM AUTHOR]

We present an experimental lattice location study of Ga atoms in Ge after ion implantation at elevated temperature (250°C). Using extended x-ray absorption fine structure (EXAFS) experiments and a dedicated sample preparation method, we have studied the lattice location of Ga atoms in Ge with a concentration ranging from 0.5 at. % down to 0.005 at. %. At Ga concentrations ≤0.05 at.%, all Ga dopants are substitutional directly after ion implantation, without the need for post-implantation thermal annealing. At higher Ga concentrations, a reduction in the EXAFS amplitude is observed, indicating that a fraction of the Ga atoms is located in a defective environment. The local strain induced by the Ga atoms in the Ge matrix is independent of the Ga concentration and extends only to the first nearest neighbor Ge shell, where a 1% contraction in bond length has been measured, in agreement with density functional theory calculations. [ABSTRACT FROM AUTHOR]

We report on the spectroscopic quadrupole moment measurement of the 7/2¡" isomeric state in "JgS27 [E* = 320.5(5) keV, Tt/2 = 415(3) ns], using the time dependent perturbed angular distribution tech-nique at the RIKEN RIBF facility. Our value, | Qs |= 23(3)