Connection between charge transfer and alloying core-level shifts based on density-functional calculations

The measurement of alloying core-level binding energy (CLBE) shifts has been used to give a precise meaning to the fundamental concept of charge transfer. Here, ab-initio density-functional calculations for the intermetallic compound MgAu are used to investigate models which try to make a connection between the core levels shifts and charge transfer. The calculated CLBE shifts agree well with experiment, and permit an unambiguous separation into initial-state and screening contributions. Interestingly, the screening contribution is large and cannot be neglected in any reasonable description. Comparison of the calculated results with the predictions of simple models show that these models are not adequate to describe the realistic situation. On the positive side, the accuracy of the density-functional calculations indicates that the combination of experiments with such calculations is a powerful tool to investigate unknown systems.Comment: RevTeX 10 pages incl 8 figure

Extracting convergent surface energies from slab calculations

The formation energy of a solid surface can be extracted from slab calculations if the bulk energy per atom is known. It has been pointed out previously that the resulting surface energy will diverge with slab thickness if the bulk energy is in error, in the context of calculations which used different methods to study the bulk and slab systems. We show here that this result is equally relevant for state-of-the-art computational methods which carefully treat bulk and slab systems in the same way. Here we compare different approaches, and present a solution to the problem that eliminates the divergence and leads to rapidly convergent and accurate surface energies.Comment: 3 revtex pages, 1 figure, in print on J. Phys. Cond. Mat

Reconstruction Mechanism of FCC Transition-Metal (001) Surfaces

The reconstruction mechanism of (001) fcc transition metal surfaces is investigated using a full-potential all-electron electronic structure method within density-functional theory. Total-energy supercell calculations confirm the experimental finding that a close-packed quasi-hexagonal overlayer reconstruction is possible for the late 5$d$-metals Ir, Pt, and Au, while it is disfavoured in the isovalent 4$d$ metals (Rh, Pd, Ag). The reconstructive behaviour is driven by the tensile surface stress of the unreconstructed surfaces; the stress is significantly larger in the 5$d$ metals than in 4$d$ ones, and only in the former case it overcomes the substrate resistance to the required geometric rearrangement. It is shown that the surface stress for these systems is due to $d$ charge depletion from the surface layer, and that the cause of the 4th-to-5th row stress difference is the importance of relativistic effects in the 5$d$ series.Comment: RevTeX 3.0, 12 pages, 1 PostScript figure available upon request] 23 May 199

Screened Coulomb interaction in the maximally localized Wannier basis

We discuss a maximally localized Wannier function approach for constructing lattice models from first-principles electronic structure calculations, where the effective Coulomb interactions are calculated in the constrained random-phase-approximation. The method is applied to the 3d transition metals and a perovskite (SrVO_3). We also optimize the Wannier functions by unitary transformation so that U is maximized. Such Wannier functions unexpectedly turned out to be very close to the maximally localized ones.Comment: 22 pages, 6 figure

Fingerprints of the Magnetic Polaron in Nonequilibrium Electron Transport through a Quantum Wire Coupled to a Ferromagnetic Spin Chain

We study nonequilibrium quantum transport through a mesoscopic wire coupled via local exchange to a ferromagnetic spin chain. Using the Keldysh formalism in the self-consistent Born approximation, we identify fingerprints of the magnetic polaron state formed by hybridization of electronic and magnon states. Because of its low decoherence rate, we find coherent transport signals. Both elastic and inelastic peaks of the differential conductance are discussed as a function of external magnetic fields, the polarization of the leads and the electronic level spacing of the wire.Comment: 5 pages, 4 figure

Quasiparticles in the Kondo lattice model at partial fillings of the conduction band

We study the spectral properties of the one-dimensional Kondo lattice model as function of the exchange coupling, the band filling, and the quasimomentum in the ferromagnetic and paramagnetic phase. Using the density-matrix renormalization group method, we compute the dispersion relation of the quasiparticles, their lifetimes, and the Z-factor. As a main result, we provide evidence for the existence of the spinpolaron at partial band fillings. We find that the quasiparticle lifetime differs by orders of magnitude between the ferromagnetic and paramagnetic phase and depends strongly on the quasimomentum.Comment: 9 pages, 9 figure

Charge redistribution at Pd surfaces: ab initio grounds for tight-binding interatomic potentials

A simplified tight-binding description of the electronic structure is often necessary for complex studies of surfaces of transition metal compounds. This requires a self-consistent parametrization of the charge redistribution, which is not obvious for late transition series elements (such as Pd, Cu, Au), for which not only d but also s-p electrons have to be taken into account. We show here, with the help of an ab initio FP-LMTO approach, that for these elements the electronic charge is unchanged from bulk to the surface, not only per site but also per orbital. This implies different level shifts for each orbital in order to achieve this orbital neutrality rule. Our results invalidate any neutrality rule which would allow charge redistribution between orbitals to ensure a common rigid shift for all of them. Moreover, in the case of Pd, the power law which governs the variation of band energy with respect to coordination number, is found to differ significantly from the usual tight-binding square root.Comment: 6 pages, 2 figures, Latex; Phys.Rev. B 56 (1997

Electric excitation of spin resonance in antiferromagnetic conductors

Antiferromagnetism couples electron spin to its orbital motion, thus allowing excitation of electron-spin transitions by an ac electric rather than magnetic field - with absorption, exceeding that of common electron spin resonance at least by four orders of magnitude. In addition to potential applications in spin electronics, this phenomenon may be used as a spectroscopy to study antiferromagnetic materials of interest - from chromium to borocarbides, cuprates, iron pnictides, and organic and heavy fermion conductors.Comment: the journal print versio

Exact results on the Kondo-lattice magnetic polaron

In this work we revise the theory of one electron in a ferromagnetically saturated local moment system interacting via a Kondo-like exchange interaction. The complete eigenstates for the finite lattice are derived. It is then shown, that parts of these states lose their norm in the limit of an infinite lattice. The correct (scattering) eigenstates are calculated in this limit. The time-dependent Schr\"odinger equation is solved for arbitrary initial conditions and the connection to the down-electron Green's function and the scattering states is worked out. A detailed analysis of the down-electron decay dynamics is given.Comment: 13 pages, 9 figures, accepted for publication in PR

Electronic Structure and Lattice Relaxation Related to Fe in Mgo

The electronic structure of Fe impurity in MgO was calculated by the linear muffin-tin orbital--full-potential method within the conventional local-density approximation (LDA) and making use of the LDA+$U$ formalism. The importance of introducing different potentials, depending on the screened Coulomb integral $U$, is emphasized for obtaining a physically reasonable ground state of the Fe$^{2+}$ ion configuration. The symmetry lowering of the ion electrostatic field leads to the observed Jahn--Teller effect; related ligand relaxation confined to tetragonal symmetry has been optimized based on the full-potential total energy results. The electronic structure of the Fe$^{3+}$ ion is also calculated and compared with that of Fe$^{2+}$.Comment: 13 pages + 4 PostScript figures, Revtex 3.0, SISSA-CM-94-00