Positron lifetime spectroscopy was used to study native vacancy defects in semi-insulating silicon carbide. The material is shown to contain (i) vacancy clusters consisting of four to five missing atoms and (ii) Si-vacancy-related negatively charged defects. The total open volume bound to the clusters anticorrelates with the electrical resistivity in both as-grown and annealed materials. Our results suggest that Si-vacancy-related complexes electrically compensate the as-grown material, but migrate to increase the size of the clusters during annealing, leading to loss of resistivity. © 2007 The American Physical Society.
We report on the results of a systematic ab initio study of the magnetic structure of Fe rich fcc FeNi binary alloys for Ni concentrations up to 50 at. %. Calculations are carried out within density-functional theory using two complementary techniques, one based on the exact muffin-tin orbital theory within the coherent potential approximation and another one based on the projector augmented-wave method. We observe that the evolution of the magnetic structure of the alloy with increasing Ni concentration is determined by a competition between a large number of magnetic states, collinear as well as noncollinear, all close in energy. We emphasize a series of transitions between these magnetic structures, in particular we have investigated a competition between disordered local moment configurations, spin spiral states, the double layer antiferromagnetic state, and the ferromagnetic phase, as well as the ferrimagnetic phase with a single spin flipped with respect to all others. We show that the latter should be particularly important for the understanding of the magnetic structure of the Invar alloys.
We employ multibillion time step embedded-atom molecular dynamics simulations to investigate the homoepitaxial growth of Pt(111) from hyperthermal Pt atoms (EPt=0.2–50eV) using deposition fluxes approaching experimental conditions. Calculated antiphase diffraction intensity oscillations, based on adatom coverages as a function of time, reveal a transition from a three-dimensional multilayer growth mode with EPt<20eV to a layer-by-layer growth with EPt≥20eV. We isolate the effects of irradiation-induced processes and thermally activated mass transport during deposition in order to identify the mechanisms responsible for promoting layer-by-layer growth. Direct evidence is provided to show that the observed transition in growth modes is primarily due to irradiation-induced processes which occur during the 10ps following the arrival of each hyperthermal atom. The kinetic pathways leading to the transition involve both enhanced intralayer and interlayer adatom transport, direct incorporation of energetic atoms into clusters, and cluster disruption leading to increased terrace supersaturation.
A normal incidence photodetector operating at 8-14 μm is demonstrated using p-type δ-doped SiGe dot multilayer structures grown by molecular beam epitaxy on Si(001) substrates. Based on the experimental results of photoluminescence and photoluminescence excitation spectroscopies together with numerical analysis, the origin of the measured photocurrent was attributed to intersubband optical transitions between the heavy hole and light hole states of the valence band of the self-assembled SiGe dots and subsequent lateral transport of photo-excited carriers in the conduction channels formed by Ge wetting layers.
We present calculations of structural and magnetic properties of the iron-pnictide superconductor LaFeAsO including electron-electron correlations. For this purpose we apply a fully charge self-consistent combination of density-functional theory with the dynamical mean-field theory, allowing for the calculation of total energies. We find that the inclusion of correlation effects gives a good agreement of the arsenic z position with experimental data even in the paramagnetic (high-temperature) phase. Going to low temperatures, we study the formation of the ordered moment in the striped spin-density-wave phase, yielding an ordered moment of about 0.60 mu(B), again in good agreement with experiments. This shows that the inclusion of correlation effects improves both structural and magnetic properties of LaFeAsO at the same time.
Titanium nitride based materials are applied in several technological applications owing to their stability at high temperatures, mechanical and optical properties, as well as good electrical conductivity. Here, I use theoretical first-principles methods to investigate the possibilities for a semiconducting state as well as the phase stability of Ti1-x MgxNy ternary alloys and compounds. I demonstrate that B1 (NaCl) solid solutions of Ti1-xMgxN with x less than= 0.5 are thermodynamically stable with respect to all previously reported phases in the Ti-Mg-N system. For the composition x = 0.5, an ordered TiMgN2 phase with an L1(1)-type order of Ti and Mg on the metal sublattice is predicted to be the configurational ground state at low temperatures. Other ordered phases present in neighboring materials systems are considered but are found to be unstable. The electronic origin of the stability of the B1 structure solid solutions is identified. A metal to semiconductor transition is observed as the Mg content is increased to x = 0.5. TiMgN2 as well as disordered Ti0.5Mg0.5N solid solution are investigated with hybrid functional calculations and predicted to be semiconductors with band gaps of 1.1 eV and around 1.3 eV, respectively, the latter depending on the details of the Ti and Mg configuration.
First-principles calculations are used to investigate the magnetic properties of Ti_{1‑x}Cr_{x}N solid solutions. We show that the magnetic interactions between Cr spins that favor antiferromagnetism in CrN is changed upon alloying with TiN leading to the appearance of ferromagnetism in the system at approximately x≤0.50 in agreement with experimental reports. Furthermore we suggest that this effect originates in an electron density redistribution from Ti to Cr that decreases the polarization of Crd states with t_{2g} symmetry while it increases the polarization of Crd states with e_{g} symmetry, both changes working in favor of ferromagnetism.
The phenomenon of superhardening in TiN/SiNx nanocomposites and the prediction of extreme hardness in bulk gamma-Si3N4 have attracted a large interest to this material system. Attempts to explain the experimental findings by means of first-principles calculations have so far been limited to static calculations. The dynamical stability of suggested structures of the SiNx tissue phase critical for the understanding of the nanocomposites is thus unknown. Here, we present a theoretical study of the phonon-dispersion relations of B1 and B3 SiN. We show that both phases previously considered as metastable are dynamically unstable. Instead, two pseudo-B3 Si3N4 phases derived from a L1(2)- or D0(22)-type distribution of Si vacancies are dynamically stable and might explain recent experimental findings of epitaxial SiNx in TiN/SiNx multilayers.
Two different methods for the modeling of a magnetically disordered CrN stateusing a supercell approach are investigated. They are found to give equivalentresults of the total energy, being also similar to results obtained with an effectivemedium approach. Furthermore, CrN is shown to be better described using aLDA+U framework for the treatment of electron-electron correlations as comparedto GGA or LDA calculations. Modeling the cubic paramagnetic phase with ourmodels for magnetic disorder and considering the strong electron correlations, thetemperature and pressure induced phase transitions in CrN can be explained.
We demonstrate the importance of thermal effects such as temperature-induced electronic, magnetic and vibrational excitations, as well as structural defects in the first-principles calculations of the magnetic critical temperature of complex alloys using half-Heusler Ni1-xCuxMnSb alloys as a case study. The thermal lattice expansion and one-electron excitations have been accounted for self-consistently in the Curie temperature calculations. In the Ni-rich region, electronic excitations, thermal expansion, and structural defects substantially decrease the calculated Curie temperature. At the same time, some defects are shown to increase T-C in Cu-rich samples.
We use a study of the cubic Ti1−xAlxN system to illustrate a practical way of combining the major methodologies within alloy theory, the Connolly-Williams cluster expansion and the generalized perturbation method, in order to solve difficult alloy problems. The configurational, concentration dependent, Hamiltonian is separated into a fixed-lattice and a local lattice relaxation part. The effective cluster interactions of the first part is obtained primarily with a GPM-based approach while the later is obtained using cluster expansion. In our case the impact on the isostructural phase diagram of considering short range clustering beyond the mean field approximation, obtained from the mixing enthalpy and entropy of the random alloy, is rather small, especially in the composition region x ≤ 0.66, within reach of thin film growth techniques.
Wedescribe an efficient first-principles method that can be used tocalculate mixing enthalpies of transition metal nitrides with B1 structureand substitutional disorder at the metal sublattice. The technique isbased on the density functional theory. The independent sublattice modelis suggested for the treatment of disorder-induced local lattice relaxationeffects. It supplements the description of the substitutional disorder withinthe coherent potential approximation. We demonstrate the excellent accuracy ofthe method by comparison with calculations performed by means ofthe projector augumented wave method on supercells constructed as specialquasirandom structures. At the same time, the efficiency of thetechnique allows for total energy calculations on a very finemesh of concentrations which enables a reliable calculation of thesecond concentration derivative of the alloy total energy. This isa first step towards first-principles predictions of concentrations and temperatureintervals where the alloy decomposition proceeds via the spinodal mechanism.We thus calculate electronic structure, lattice parameter, and mixing enthalpiesof the quasibinary alloy c-Ti_{1−x}Al_{x}N. The lattice parameter follows Vegard'slaw at low fractions of AlN but deviates increasingly withincreasing Al content. We show that the asymmetry of themixing enthalpy and its second concentration derivative is associated withsubstantial variations of the electronic structure with alloy composition. Thephase diagram is constructed within the mean-field approximation.
The first material to be predicted from first-principles calculations as half-metallic was NiMnSb, and the research on this material has been intense due to its possible applications in spintronics devices. The failure of many experiments to measure spin polarization to more than a fraction of the predicted 100% has partly been blamed on structural defects. In this work a complete first-principles treatise of point defects, including nonstoichiometric antisites, interstitial and vacancy defects, as well as stoichiometric atomic swap defects in NiMnSb, is presented. We find that the formation energies of the defects span a large scale from 0.2 to 14.4 eV. The defects with low formation energies preserve the half-metallic character of the material. We also find that some of the defects increase the magnetic moment and thus can explain the experimentally observed increase of magnetic moments in some samples of NiMnSb. Most interesting in this respect are Mn interstitials which increase the magnetic moment, have a low formation energy, and keep the half-metallic character of the material.
We use metastable NaCl-structure Ti_{0.5}Al_{0.5}N alloys to probe effects of configurational disorder on adatom surface diffusion dynamics which control phase stability and nanostructural evolution during film growth. First-principles calculations were employed to obtain energy potential maps of Ti and Al adsorption on an ordered TiN(001) reference surface and a disordered Ti_{0.5}Al_{0.5}N(001) solid-solution surface. The energetics of adatom migration on these surfaces are determined and compared to isolate effects of configurational disorder. The results show that alloy surface disorder dramatically reduces Ti adatom mobilities. Al adatoms, in sharp contrast, experience only small disorder-induced differences in migration dynamics.
Based on ab initio density-functional calculations in supercells of 3C-SiC, the stable configurations of hydrogen and dihydrogen defects have been established. The calculated formation energies are used to give semiquantitative estimates for the concentration of hydrogen in SiC after chemical vapor deposition, low temperature H-plasma anneal, or heat treatment in high temperature hydrogen gas. Vibration frequencies, spin distributions, and occupation levels were also calculated in order to facilitate spectroscopic identification of these defects. (V+nH) complexes are suggested as the origin of some of the signals assigned earlier to pure vacancies. Qualitative extrapolation of our results to hexagonal polytypes explains observed electrical passivation effects of hydrogen.
We have performed a numerical study of the process of electron localization in reduced ceria. Our results show that different localized charge distributions can be attained in a bulk system by varying the lattice parameter. We demonstrate that the effect of electron localization is mainly determined by lattice relaxation and an accurate account for the effects of electronic correlation is necessary to achieve localized charge distribution.
We present a large-scale density functional theory (DFT) investigation of the ABO(3) chemical space in the perovskite crystal structure, with the aim of identifying those that are relevant for forming piezoelectric materials. Screening criteria on the DFT results are used to select 49 compositions, which can be seen as the fundamental building blocks from which to create alloys with potentially good piezoelectric performance. This screening finds all the alloy end points used in three well-known high-performance piezoelectrics. The energy differences between different structural distortions, deformation, coupling between the displacement of the A and B sites, spontaneous polarization, Born effective charges, and stability is analyzed in each composition. We discuss the features that cause the high piezoelectric performance of the well-known piezoelectric lead zirconate titanate (PZT), and investigate to what extent these features occur in other compositions. We demonstrate how our results can be useful in the design of isovalent alloys with high piezoelectric performance.
We screen a large chemical space of perovskite alloys for systems with optimal properties to accommodate a morphotropic phase boundary (MPB) in their composition-temperature phase diagram, a crucial feature for high piezoelectric performance. We start from alloy end points previously identified in a high-throughput computational search. An interpolation scheme is used to estimate the relative energies between different perovskite distortions for alloy compositions with a minimum of computational effort. Suggested alloys are further screened for thermodynamic stability. The screening identifies alloy systems already known to host an MPB and suggests a few others that may be promising candidates for future experiments. Our method of investigation may be extended to other perovskite systems, e.g., (oxy-)nitrides, and provides a useful methodology for any application of high-throughput screening of isovalent alloy systems.
An exchange potential functional is constructed from semi-local quantities and is shown to reproduce hydrogen chain polarizabilities with the same accuracy as exact exchange methods. We discuss the exchange potential features that are essential for accurate polarizability calculations, i.e., derivative discontinuities and the potential step structure. The possibility of a future generalization of the methods into a complete semi-local exchange-correlation functional is discussed.
It has recently been shown that local values of the conventional exchange energy per particle cannot be described by an analytic expansion in the density variation. Yet, it is known that the total exchange-correlation (XC) energy per particle does not show any corresponding nonanalyticity. Indeed, the nonanalyticity is here shown to be an effect of the separation into conventional exchange and correlation. We construct an alternative separation in which the exchange part is made well behaved by screening its long-ranged contributions, and the correlation part is adjusted accordingly. This alternative separation is as valid as the conventional one, and introduces no new approximations to the total XC energy. We demonstrate functional development based on this approach by creating and deploying a local-density-approximation-type XC functional. Hence, this work includes both the theory and the practical calculations needed to provide a starting point for an alternative approach towards improved approximations of the total XC energy.
We design a density-functional-theory (DFT) exchange-correlation functional that enables an accurate treatment of systems with electronic surfaces. Surface-specific approximations for both exchange and correlation energies are developed. A subsystem functional approach is then used: an interpolation index combines the surface functional with a functional for interior regions. When the local density approximation is used in the interior, the result is a straightforward functional for use in self-consistent DFT. The functional is validated for two metals (Al, Pt) and one semiconductor (Si) by calculations of (i) established bulk properties (lattice constants and bulk moduli) and (ii) a property where surface effects exist (the vacancy formation energy). Good and coherent results indicate that this functional may serve well as a universal first choice for solid-state systems and that yet improved functionals can be constructed by this approach.
A viable way of extending the successful use of density-functional theory into studies of even more complex systems than are addressed today has been suggested by Kohn and Mattsson [W. Kohn and A. E. Mattsson, Phys. Rev. Lett. 81, 3487 (1998); A. E. Mattsson and W. Kohn, J. Chem. Phys. 115, 3441 (2001)], and is further developed in this work. The scheme consists of dividing a system into subsystems and applying different approximations for the unknown (but general) exchange-correlation energy functional to the different subsystems. We discuss a basic requirement on approximative functionals used in this scheme; they must all adhere to a single explicit choice of the exchange-correlation energy per particle. From a numerical study of a model system with a cosine effective potential, the Mathieu gas, and one of its limiting cases, the harmonic oscillator model, we show that the conventional definition of the exchange energy per particle cannot be described by an analytical series expansion in the limit of slowly varying densities. This indicates that the conventional definition is not suitable in the context of subsystem functionals. We suggest alternative definitions and approaches to subsystem functionals for slowly varying densities and discuss the implications of our findings on the future of functional development.
We present a multilayer model for analysis of Hall effect data of semiconductor structures composed of sublayers with different thicknesses and contacts placed on the top surface. Based on the circuit theory we analyze the contributions of the conductivity of every sublayer and derive general expressions for the conductivity and carrier mobility of a multilayer planar sample. The circuit analysis is performed taking into account the fact that the sample sublayers are partially connected in parallel to each other by series resistances formed in areas lying below the contacts from each upper layer. In order to solve the inverse problem of determining the electrical parameters of one of the sublayers, a procedure for analysis of the Hall effect data is proposed. The model is simplified for a structure composed of two layers with the same type of conductivity, and is used to determine the electrical parameters of GaN films grown on relatively thick GaN buffers.
We simulate the spectral distribution of the free-electron recombination band in optical emission spectra of GaN with a free-carrier concentration in the range of 5 x 10(17)-1 x 10(20) cm(-3). The influence of several factors, such as nonparabolicity, electron-electron interaction. and electron-impurity interaction on both the spectral and energy position and the effective gap narrowing are taken into account. The calculated properties of the free-electron-related emission bands are used to interpret the experimental photoluminescence and cathodoluminescence spectra of GaN epitaxial layers.
We studied the shape and energy position of near-band-edge photoluminescence spectra of InN epitaxial layers with different doping levels. We found that the experimental spectra of InN layers with moderate doping level can be nicely interpreted in the frames of the "free-to-bound" recombination model in degenerate semiconductors. For carrier concentrations above n>5x10(18) cm(-3) the emission spectra can also be modeled satisfactorily, but a contribution due to a pushing up of nonequilibrium holes over the thermal delocalization level in the valence band tails should be considered in the model. The emission spectra of samples with low doping level were instead explained as a recombination from the bottom of the conduction band to a shallow acceptor assuming the same value of the acceptor binding energy estimated from the spectra of highly doped samples. Analyzing the shape and energy position of the free-electron recombination spectra we determined the carrier concentrations responsible for the emissions and found that the fundamental band gap energy of InN is E-g=692+/-2 meV for an effective mass at the conduction-band minimum m(n0)=0.042m(0).
The single-crystal and polycrystalline elastic constants and the elastic anisotropy in face-centered cubic and hexagonal close-packed FeNi alloys have been investigated at ultrahigh pressures by means of first-principles calculations using the exact muffin-tin orbitals method and the coherent-potential approximation. Comparisons with earlier calculations for pure Fe and experimental results are presented and discussed. We show that Ni alloying into Fe increases slightly the density and has very little effect on bulk moduli. Moreover, the relative decrease in c(44) elastic constant is much stronger in the hcp phase than in the fcc one. It is found that the elastic anisotropy is higher for face-centered cubic than for the hexagonal close-packed structure of FeNi, even though the face-centered cubic phase has a higher degree of symmetry. The anisotropy in face-centered cubic structure decreases with increasing nickel concentration while a very weak increase is observed for the hexagonal close-packed structure.
The energy differences between the ground state body-centered structure and closed-packed face-centered structure for transition metals in the middle of the series show unusually large disagreements when they are obtained by the thermochemical approach based on the analysis of experimental data or by first-principles electronic structure calculations. Considering a typical example, the lattice stability of Mo, we present a solution to this long-standing problem. We carry out ab initio molecular dynamics simulations for the two phases at high temperature and show that the configurational energy difference approaches the value derived by means of the thermochemical approach. The main contribution to the effect comes from the modification of the canonical band structure due to anharmonic thermal motion at high temperature.
Weak localization in graphene is studied as a function of carrier density in the range from 1 x 10(11) cm(-2) to 1.43 x 10(13) cm(-2) using devices produced by epitaxial growth onto SiC and CVD growth on thin metal film. The magnetic field dependent weak localization is found to be well fitted by theory, which is then used to analyze the dependence of the scattering lengths L-phi, L-i, and L-* on carrier density. We find no significant carrier dependence for L-phi, a weak decrease for L-i with increasing carrier density just beyond a large standard error, and a n(-1/4) dependence for L-*. We demonstrate that currents as low as 0.01 nA are required in smaller devices to avoid hot-electron artifacts in measurements of the quantum corrections to conductivity. DOI: 10.1103/PhysRevB.86.235441
Energy loss rates for hot carriers in graphene have been measured using graphene produced by epitaxial growth on SiC, exfoliation, and chemical vapor deposition (CVD). It is shown that the temperature dependence of the energy loss rates measured with high-field damped Shubnikov-de Haas oscillations and the temperature dependence of the weak localization peak close to zero field correlate well, with the high-field measurements understating the energy loss rates by similar to 40% compared to the low-field results. The energy loss rates for all graphene samples follow a universal scaling of T-e(4) at low temperatures and depend weakly on carrier density proportional to n(-1/2), evidence for enhancement of the energy loss rate due to disorder in CVD samples.
We report angle-resolved photoemission measurements of the dispersion of the shallow surface state around (A)overbar and the surface electron-phonon mass-enhancement parameter lambda(s) at the Be(1010) surface. The eccentricity of the elliptical Fermi line formed by the surface state is found to be epsilon=0.684. We obtain lambda(s)=0.672 +/- 0.027 along the major axis and lambda(s)= 0.642+/-0.031 along the minor axis of the Fermi line. The lambda(s) values are about three times larger than the bulk lambda(b) = 0.24.
The surface electronic band structure of the Be(10(1) over bar 0) surface is experimentally determined by angle-resolved photoemission and calculated by using density-functional theory. The experimental results agree well with the calculations, except for the fact that we were only able to resolve three surface states in the gap at (L) over bar, instead of four as predicted by the calculations. Through the temperature-dependent study, the phonon contribution subtracted width (h times inverse lifetime) of the shallow surface state at (A) over bar is found to be 51 +/- 8 meV. This is compared with the electron-electron interaction contribution to the width (53 meV) of the shallow surface state at A obtained from model potential calculations.
The spontaneous magnetization of a quantum point contact (QPC) formed between two large quantum dots by a lateral confinement of a high-mobility two-dimensional electron gas is studied for a realistic GaAs/AlxGa1-xAs heterostructure. The model of the device incorporates the contributions from a patterned gate, doping, surface states, and mirror charges. To explore the magnetic properties, the Kohn-Sham local spin-density formalism is used with exchange and correlation potentials that allows for local spin polarization. Exchange is the dominant mechanism behind local magnetization within the QPC, while the correlation part is less prominent. However, the correlation potential gives rise to an important correction in the QPC potential. Below the first conduction plateau we thus find a magnetized regime corresponding approximately to a single electron spin. Using an approximate separable saddle potential we compute the conductance and recover the so-called similar to0.7 (2e(2)/h) conduction anomaly plus an additional anomaly at similar to0.4 (2e(2)/h) below which the magnetization collapses.
The conductance through open quantum dots, or quantum billiards, shows fluctuations that can be explained as interference between waves following different paths between the leads of the billiard. We examine such systems by the use of a semiclassical Greens functions. In this paper we examine how the choice of boundary conditions at the lead mouths affects the diffraction. We derive a superior formula for the S-matrix element. Finally, we compare semiclassical simulations to quantum mechanical ones, and show that this formula yields superior results.
We utilize a semiclassical (SC) approach to calculate the conductance and weak-locatization (WL) corrections in a triangular billiard of a given shape in the presence of nonzero magnetic field. The semiclassical conductance is given as a sum of all classical trajectories between the leads, each of them carrying the quantum-mechanical phase. The present SC approach is numerically exact (i.e., free from any approximations), explicitly includes diffractive effects in the leads, and is valid for arbitrary (low) mode numbers in the leads. We find however that the symmetry of the SC conductance/reflectance with respect to the direction of magnetic field or direction of the current is not satisfied, as well as that the WL corrections for the conductance and reflectance are inconsistent with each other, the SC approach does not satisfy the current conservation requirements and does not reproduce the corresponding exact quantum-mechanical results. The reason for that is traced to the topological difference in the sets of classical trajectories between the leads for different current or magnetic field directions which determine the conductance in the SC approximation. Our findings raise a question as to what extent one can rely on numerous predictions for statistical properties of the conductance oscillations of ballistic cavities including the WL line shapes and fractal conductance which were essentially based on the standard SC approach.
We provide a semiclassical interpretation of the conductance oscillations in a square billiard and outline its relation to a commonly used picture of periodic orbits. We demonstrate that the characteristic frequencies in the conductance arise as a result of interference of pairs of long trajectories that typically bounce in a vicinity of the corresponding periodic orbits in the phase space. We present an unambiguous identification of the specific pairs of trajectories causing the pronounced peaks in the observed length spectrum of the conductance. This allows us to extract directly the phase coherence length from the frequency of the observed oscillations.
Stable junctions between a single carbon chain and two single-wall carbon nanotubes were produced via coalescence of functionalized fullerenes filled into a single-wall carbon nanotube and directly imaged by in situ transmission electron microscopy. First principles quantum chemical calculations support the observed stability of such molecular junctions. They also show that short carbon chains bound to other carbon structures are cumulenes and stable semiconductors due to Peierls-like distortion. Junctions like this can be regarded as archetypical building blocks for all-carbon molecular electronics.
The van der Waals (vdW) interaction between thin metallic films varies with separation as the separation to a fractional power. This is in contrast to the usual integer-power separation dependence between objects such as atoms, dielectric films, or thick metallic films. We have calculated the free energy of attraction between sheets of gold, silver, copper, beryllium, and tungsten numerically using experimentally found dielectric functions. The results are compared with the corresponding analytical results obtained using simple model dielectric functions. We have investigated how thin the metallic films must be in order for the fractional vdW interaction to be present. To our knowledge, fractional vdW interaction has not yet been confirmed experimentally.
We recently investigated the van der Waals force between thin metal films. Under certain conditions this force decrease with separation to a fractional power. In the present work we use optical data of metals and the zero-temperature Lifshitz formalism to demonstrate a retardation effect. The retarded attraction between thin metal films may be larger than the nonretarded attraction. This property is related to a comparatively weak retardation dependence of the energy that originates from the transverse magnetic modes. At separations where the transverse electric modes give a significant contribution, the net effect can actually be an increased attraction. This effect vanishes with increasing film thickness and with increasing dissipation.
The orbital and spin magnetic properties of iron inside metallic and semiconducting carbon nanotubes are studied by means of local x-ray magnetic circular dichroism (XMCD) and bulk superconducting quantum interference device (SQUID). The iron-nanotube hybrids are initially ferrocene filled single-walled carbon nanotubes (SWCNT) of different metallicities. We show that the ferrocene's molecular orbitals interact differently with the SWCNT of different metallicities with no significant XMCD response. At elevated temperatures the ferrocene molecules react with each other to form cementite nanoclusters. The XMCD at various magnetic fields reveal that the orbital and/or spin magnetic moments of the encapsulated iron are altered drastically as the transformation to the 1D clusters takes place. The orbital and spin magnetic moments are both found to be larger in filled semiconducting nanotubes than in the metallic sample. This could mean that the magnetic polarization of the encapsulated material depends on the metallicity of the tubes. From a comparison between the iron 3d magnetic moments and the bulk magnetism measured by SQUID, we conclude that the delocalized magnetisms dominate the magnetic properties of these 1D hybrid nanostructures.
We study bound states of the two-dimensional Helmholtz equations with Dirichlet boundary conditions in an open geometry given by two straight leads of the same width which cross at an angle theta. Such a four-terminal junction with a tunable theta can realized experimentally if a right-angle structure is filled by a ferrite. It is known that for theta=90degrees there is one proper bound state and one eigenvalue embedded in the continuum. We show that the number of eigenvalues becomes larger with increasing asymmetry and the bound-state energies are increasing as functions of theta in the interval (0,90degrees). Moreover, states which are sufficiently strongly bound exist in pairs with a small energy difference and opposite parities. Finally, we discuss how the bound states transform with increasing theta into quasibound states with a complex wave vector.
We study spin-dependent electron transmission through one- and two-dimensional curved waveguides and quantum dots with account of spin-orbit interaction. We prove that for a transmission through an arbitrary structure there is no spin polarization provided the electron transmits in an isolated energy subband and only two leads are attached to the structure. In particular there is no spin polarization in the one-dimensional wire, for which a spin-dependent solution is found analytically. The solution demonstrates the spin evolution as dependent on a length of wire. The numerical solution for transmission of electrons through the two-dimensional curved waveguides coincides with the solution for the one-dimensional wire if the energy of electron is within the first energy subband. In the vicinity of edges of the energy subbands there are sharp anomalies of spin flipping.
The magnetic anisotropy energy (MAE) of Fe, Co, and Ni is presented for tetragonal and trigonal structures along two paths of structural distortion connecting the bcc and the fcc structure. The MAE was calculated from first principles with the full-potential linear muffin-tin orbital method and the force theorem. As is expected from symmetry considerations, the MAE increases by orders of magnitude when the cubic symmetry is broken. For tetragonal structures of Co and Ni a regular behavior of the MAE is observed, i.e., only the symmetry dictated nodes at the cubic structures appear along this path of distortion. In the case of tetragonal Fe, additional reorientations of the easy axis occur that are attributed to a topological change of the Fermi surface upon distortion. For the trigonal structures of all three elements the strain dependence of the MAE is more complicated, with additional reorientations of the easy axis and an unexpectedly large MAE for certain distortions of Ni, and a strongly nonlinear behavior for trigonal structures of Co close to fcc. Furthermore, the linear magnetoelastic coupling coefficients are calculated from the MAE at small distortions from the cubic equilibrium structure of the three elements. Two different Brillouin-zone integration techniques were used to calculate the MAE. Since the Gaussian broadening method smears out details of the Fermi surface, it results in a different MAE as compared to the tetrahedron method in some cases.
The uniaxial magnetic anisotropy energy (MAE) of L 10 FePt and Fe1-x Mnx Pt, x=0-0.25, was studied from first principles using two fully relativistic computational methods, the full-potential linear muffin-tin orbitals method and the exact muffin-tin orbitals method. It was found that the large MAE of 2.8 meV/f.u. is caused by a delicate interaction between the Fe and Pt atoms, where the large spin-orbit coupling of the Pt site and the hybridization between Fe 3d and Pt 5d states is crucial. The effect of random order on the MAE was modeled by mutual alloying of the sublattices within the coherent potential approximation (CPA), and a strong dependence of the MAE on the degree of chemical long-range order was found. The alloying of FePt with Mn was investigated with the virtual crystal approximation and the CPA as well as supercell calculations. The MAE increases up to 33% within the concentration range studied here, an effect that is attributed to band filling. Furthermore, the dependence of the MAE on the structural properties was studied. © 2005 The American Physical Society.
We measured the Mn L_{α,β} x-ray fluorescence spectra of MnO excited by selected photon energies near the L_{2,3} absorption edges. The resulting resonant inelastic x-ray scattering spectra probe low-lying electronic excited states, due to dd and charge-transfer excitations. Using a two-step model and a purely atomic approximation, we reproduce both energies and varying intensities of dd excitations relative to the electronic recombination peak. Our results show that strongly varying line shapes in resonant x-ray emission need not be due to channel interference effects.
Ti and Mn L_{α,Β} x-ray fluorescence spectra of FeTiO_{3} and KMnO_{4} were measured with monochromatic photon excitation on selected energies across the L_{2,3} absorption edges. The resulting inelastic x-ray-scattering structures and their changes with varying excitation energies are interpreted within the framework of a localized, many-body approach based on the Anderson impurity model, where the radiative process is characterized by transitions to low-energy interionic-charge-transfer excited states. Sweeping the excitation energy through the metal 2p threshold enhances the fluorescence transitions to the antibonding states pushed out of the band of continuous states due to strong metal 3d–ligand 2p hybridization and matching the low-photon-energy satellites in the spectra. Based on the energy position of these charge-transfer satellites with respect to the recombination peak the effective metal 3d–ligand 2p hybridization strength in the ground state of the system can be estimated directly from the experiment.
cw hot photoluminescence (PL) complemented by transient PL measurements is employed to evaluate momentum and spin relaxation of heavy hole (HH) excitons in ZnMnSe CdSe superlattices. The rate of acoustic-phonon assisted momentum relaxation is concluded to be comparable to the total rate of exciton decay processes, about (2-3) × 1010 s-1, independent of applied magnetic fields. In magnetic fields when the Zeeman splitting ? of the exciton states is below the energy of the longitudinal optical (LO) phonon (?LO), a surprisingly strong suppression of spin relaxation rate from the bottom of the upper spin band is observed, which becomes comparable to that of momentum scattering via acoustic phonons. On the other hand, dramatic acceleration of the spin relaxation process by more than one order of magnitude is found for the excitons with a high momentum K. The findings are interpreted as being due to electron and hole spin flip processes via exchange interaction with isolated Mn2+ ions. Experimental evidence for the efficient interaction between the hot excitons and Mn impurities is also provided by the observation of spin flip transitions within Mn2+ - Mn2+ pairs that accompany the momentum relaxation of the hot HH excitons. In higher magnetic fields ?= ?LO, abrupt shortening of the spin flip time is observed. It indicates involvement of a new and more efficient spin relaxation process and is attributed to direct LO-assisted exciton spin relaxation with a subpicosecond spin relaxation time. © 2005 The American Physical Society.
Three independent experimental techniques, namely, time-resolved photoluminescence (PL) spectroscopy, PL polarization, and optically detected cyclotron resonance, are employed to determine the band alignment of GaNxAS1-x/GaAs quantum structures with a low-N composition. It is concluded that band lineup is type I based on the following experimental results: (i) comparable radiative decay time of the GaNAs-related emission measured from single GaNAs epilayers and from GaNAs/GaAs quantum well (QW) structures, (ii) polarization of the GaNAs-related emission, and (iii) spatial confinement of the photoexcited holes within the GaNAs layers under resonant excitation of the GaNAs QW's.
The solid state of free radicals of bis(9-cyclohexylimino-1-oxyphenalenyl) boron is one of few neutral molecular systems which exhibit high conductivity at room temperature. The system is crystalline but highly anistotropic. We have performed band structure calculations based on the density functional theory on this system. It is evident from these studies that the system is quasi-one-dimensional with strong intermolecular interactions along one crystal direction. The bandwidth is 0.424 eV along this direction as compared to 0.055 eV perpendicular to it. Despite the quasi-one-dimensional character of the system, no signature of a Peierls distortion towards a dimerized state is observed. We argue that this is due to the fact that the Fermi energy lies slightly below the middle of the conduction band. In this case the electronic driving force for the distortion to occur is weakened and overcome by the restoring force of the lattice. Also the optical properties of the system have been investigated and the origin of the low lying excitations in the system has been clarified.
An investigation of defect generation at the interface during growth of epitaxial (100) oriented Mo/W superlattices by ion-assisted deposition has been carried out using molecular-dynamics simulations. The influence of the impact parameter within the irreducible bcc unit cell [001] surface and the incident ion energy on the energy accommodation, the dynamics of energy transfer, and energy dissipation are discussed. A detailed model of the generation of point defects is presented and the influence of materials upon the type and the number of defects as well as the energy accommodation of the superlattice is revealed. It is shown that the behavior of the superlattice as a whole is largely dominated by the material in the surface monolayer.
V(TCNE)_{x}, with TCNE=tetracyanoethylene and x~2, is an organic-based molecular magnet with potential to be used in spintronic devices. With the aim of shedding light on the unoccupied frontier electronic structure of V(TCNE)_{x} we have studied pristine TCNE and sodium-intercalated TCNE by near edge x-ray absorption fine structure (NEXAFS) spectroscopy as well as with theoretical calculations. Sodium-intercalated TCNE was used as a model system of the more complex V(TCNE)_{x} and both experimental and theoretical results of the model compound have been used to interpret the NEXAFS spectra of V(TCNE)_{x}. By comparing the experimental and theoretical C K-edge of pristine TCNE, the contributions from the various carbon species (cyano and vinyl) could be disentangled. Upon fully sodium intercalation, TCNE is n doped with one electron per molecule and the features in the C and N K-edge spectra of pristine TCNE undergo strong modification caused by partially filling the TCNE lowest unoccupied molecular orbital (LUMO). When comparing the C and N K-edge NEXAFS spectra of fully sodium-doped TCNE with V(TCNE)_{x}, the spectra are similar except for broadening of the features which originates from structural disorder of the V(TCNE)_{x} films. The combined results from the model system and V(TCNE)_{x} suggest that the lowest unoccupied molecular orbital with density on the nitrogen atoms in V(TCNE)_{x} has no significant hybridization with vanadium and is similar to the so-called singly occupied molecular orbital of the TCNE anion. This suggests that the LUMO of V(TCNE)_{x} is TCNE^{−} or vanadiumlike, in contrast to the frontier occupied electronic structure where the highest occupied molecular orbital is a hybridization between V(3d) and cyano carbons. The completely different nature of the unoccupied and occupied frontier electronic structure of the material will most likely affect both charge injection and transport properties of a spintronic device featuring V(TCNE)_{x}.