First-principles calculations of magnetic and electronic structures around surfaces and interfaces of magnetic multi-layered structure

Electronic and magnetic structures of ferromagnetic (FM)/non-magnetic (NM) and FM/antiferromagnetic (AF) bi-layer systems are calculated by the first principles approach. For the FM/NM system, we focus on the Co/Cu multi-layered structure whose interfacial layer is assumed to have a mixed composition of Co and Cu atoms, and show a possibility that Co atoms at the interface play a significant role as the spin-dependent scattering potentials. In the FM/AF system, we consider Fe or Co monolayer as FM layer and MnNi as AF layers. It is predicted that the Mn moments adjacent to FM layer are forced to align the FM moments, and those of under layer go gradually to anti-parallel alignment as in the bulk MnNi.     

Spin–orbit induced magnetic phenomena in bulk metals and their surfaces and interfaces

First-principles electronic structure studies based on local spin density functional theory and performed on extremely complex simulations of ever increasingly realistic systems, play a very important role in explaining and predicting surface and interface magnetism. This review deals with what is a major issue for first-principles theory, namely the theoretical/computational treatment of the weak spin–orbit coupling in magnetic transition metals and their alloys and its important physical consequences: magneto-crystalline anisotropy, magnetostriction, magneto-optical Kerr effects and X-ray magnetic circular dichroism. As is demonstrated, extensive first-principles calculations and model analyses now provide simple physical insights and guidelines to search for new magnetic recording and sensor materials.     

Surface and near-surface passivation, chemical reaction, and Schottky barrier formation at ZnO surfaces and interfaces

Using a combination of depth-resolved cathodoluminescence spectroscopy, electronic transport, and surface science techniques, we have demonstrated the primary role of native defects within ZnO single crystals as well as native defects created by metallization on metal-ZnO Schottky barrier heights and their ideality factors. Native defects and impurities resident within the ZnO depletion region as well as defects extending into the bulk from the intimate metal-ZnO interface contribute to barrier thinning of, carrier hopping across, and tunneling through these Schottky barriers. Chemical reactions at clean ZnO-metal interfaces lead to metal-specific eutectic or oxide formation with pronounced transport effects. These results highlight the importance of bulk crystal quality, surface cleaning, metal interaction, and post-metallization annealing for controlling Schottky barriers.     

X-ray absorption spectra: K-edges of 3d transition metals,L-edges of 3d and 4d metals,and M-edges of palladium

The X-ray absorption spectra of the 3d and 4d transition metals have been calculated within the single-particle approximation by a new linearized augmented plane wave method. The spectra, calculated with sharp atomic and band-structure single-particle levels, have been convoluted with a Lorentzian broadening function whose width is the sum of that of the core hole and the excited electrons. Plots are shown for (i) the K-edge fine structures up to at least 100 eV above the edge for Ca, Ti, Cr, Co, Cu, and Zn, (ii) the L_{2, 3} white lines for Ca, Ti, Cr, Co, and Cu, (iii) the L₃ white lines for Sr, Zr, Nb, Ru, Rh, and Pd, and (iv) the M_{2, 3} and M_4,5 spectrum of Pd. Systematic features which depend on the crystal structure and the placement of the Fermi level with conduction band are briefly discussed.     

Radioactive ions for solid-state investigations at magnetic surfaces and interfaces

Hyperfine interactions observed at isomeric states of radioactive probe nuclei are used as a tool for solid-state investigations. This method is sensitive to atomic-scale properties. In recent years surface and interface investigations using radioactive probes delivered many results which can hardly be achieved by any other method. Several groups, e.g., from Konstanz, Leuven, Groningen, Aarhus, Uppsala, Tel Aviv, Pennsylvania, contributed to this field. Our group studies magnetic properties at surfaces and interfaces performing perturbed angular correlation (PAC) measurements in the UHV chamber ASPIC (Apparatus for Surface Physics and Interfaces at CERN). We take advantage of the enhanced variety of PAC probes delivered by the on-line mass separator ISOLDE. First, we report on measurements of magnetic hyperfine fields ( B _hf) at Se adatoms on a ferromagnetic substrate using ⁷⁷Se as a PAC probe. The investigation of induced magnetic interactions in nonmagnetic materials is a further subject of our studies. Here the nonmagnetic 4d element Pd is investigated, when it is in contact with ferromagnetic nickel. An outlook will be given on studies to be done in the future. The experiments were performed at the HMI, Berlin, and at CERN, Geneva. Received: 1 May 2001 / Accepted: 4 December 2001     

Microscopic structure and structuring of perovskite surfaces and interfaces: SrTiO3, RBa2Cu3O7-δ

3 surfaces and bicrystal interfaces and the growth of YBa₂Cu₃O_7-δ thin films on such substrates using scanning tunneling microscopy and X-ray diffraction. Proper annealing of SrTiO₃ in oxygen and/or ultrahigh vacuum produces uniformly terminated, atomically flat and well-ordered surfaces. For vicinal SrTiO₃(001) surfaces the particular annealing sequence and miscut angle sensitively determines the resulting step structure and thus the microscopic surface morphology. Steps of SrTiO₃(001) surfaces can be adjusted to a height of one, two, or multiple times the unit-cell height (a_STO=0.3905 nm). The growth of YBa₂Cu₃O_7-δ films on these substrates by pulsed laser deposition was traced from the initial nucleation to a thickness of about 300 nm. The morphology, texture, and defect structure of the films is determined by the specific structure and morphology of the pristine substrate. Anisotropic, planar defects, originating from substrate step edges, strongly modify the electronic transport properties of the film leading to critical currents up to ≈9×10⁷ A/cm² at 4 K as well as pronounced transport anisotropies. Surfaces and interface energy terms are discussed, which also determine the observed structure of bicrystal boundaries. Received: 16 April 1998/Accepted: 21 August 1998     

Electronic structure and magnetism of surfaces,interfaces and modulated structures (superlattices)

Recent developments in the study of surfaces and interfaces of metals and of artificial materials such as bimetallic sandwiches and modulated structures are described. Key questions include the effects on magnetism of reduced dimensionality and the possibility of magnetically dead layers. These developments have stimulated an intensified theoretical effort to investigate and describe the electronic and magnetic structure of surfaces and interfaces. One notable success has been the development of a highly accurate full-potential all-electron method (the FLAPW method) for solving the local spin density equations self-consistently for a single slab geometry. We describe here this advanced state of ab initio calculations in determining the magnetic properties of transition metal surfaces such as those of the ferromagnetic metals Ni(001) and Fe(001) and the Ni/Cu(001) interface. For both clean Fe and Ni(001) we find an enhancement of the magnetic moments in the surface layer. The magnetism of surface and interface Ni layers on Cu(001) (no dead layers are found) is described and compared to the clean Ni(001) results. Finally, the role ofSR experiments in answering some of the questions raised in these studies will be discussed.     

Analysis of the liquid structure of 3d transition metals from the Wills-Harrison model

Calculations of the liquid structure of 3d transition metals from the effective pair interactions of Wills and Harrison are performed by using the optimized random phase approximation in order to point out the influence of thes-electron pseudopotential on the repulsive and attractive forces governing the liquid structure. Our results are compared to those obtained in the Weeks, Chandler Andersen approximation and in the thermodynamic variational method.     

A theoretical study of the structure and stability of borohydride on 3d transition metals

The adsorption of borohydride on 3d transition metals (Cr, Mn, Fe, Co, Ni and Cu) was studied using first principles calculations within spin-polarized density functional theory. Magnetic effect on the stability of borohydride is noted. Molecular adsorption is favorable on Co, Ni and Cu, which is characterized by the strong s–d_zz hybridization of the adsorbate-substrate states. Dissociated adsorption structure yielding one or two H adatom fragments on the surface is observed for Cr, Mn and Fe.     

Density-functional calculation of subband structure on semiconductor surfaces

The Hohenberg-Kohn-Sham theory of an inhomogeneous electron gas is applied to the calculation of subband structures of n-channel accumulation and inversion layers on a Si(100) surface. The exchange-correlation effect is shown to be very important and lower the subband energies considerably. In case of accumulation layers it changes the subband structure. The first excited subband becomes really a bound state in contrast to a result of the Hartree approximation. The agreement between the theory and experimental results of intersubband optical transitions is satisfactory. The effective mass and the g factor are also calculated.     

The electronic structure of alkali-metal layers on semiconductor surfaces

Alkali-metal layers on semiconductor surfaces are model systems for metal-semiconductor contacts, Schottky barriers, and metallization processes. The strong decrease of the work function as a function of alkali-metal coverage is also technically made use of. Recently, however, interest in these systems is growing owing to ongoing controversial discussions about questions like: Is the adsorbate system at monolayer coverage metallic or semiconducting, and does the metallization take place in the alkali overlayer or in the top layer of the semiconductor? Is the bonding ionic or covalent? What ist the absolute coverage at saturation? What are the adsorption sites? Do all alkali metals behave similar on the same semiconductor surface? We try to answer some of the questions for Li, Na, K and Cs on Si(111)(2×1), K and Cs on Si(111)(7×7) and on GaAs(110), and Na and K on Si(100)(2×1) employing the techniques of direct and inverse photoemission.     

Temperature-induced local magnetic moments (TILMM) in monosilicides of 3d transition metals

Features of the formation of temperature-induced local magnetic moments (TILMM) and their influence on the magnetic and thermophysical characteristics of iron, cobalt, and manganese monosilicides are investigated. The results obtained for magnetic susceptibility and specific heat measurements are discussed within the framework of spin-fluctuation theory. Temperature-concentration dependences are established for the TILMM absolute value for mutual solid solutions Fe_1–xCo_xSi and Fe_1–yMn_ySi. It is shown that for a number of the alloys studied the saturation of the TILMM absolute value does not occur, while the anomalous behavior of the polytherm of their physical properties is associated with features of the band structure.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 4, pp. 18–23, April, 1988.     

Atomistic and electronic structure calculation of defects at the surfaces of oxides

We present the results of simulations using both atomistic and density functional theory (DFT) approaches that illustrate the uses of these techniques for investigating the structure and electronic structure of defects at the surfaces of oxides. Atomistic simulation studies of the low index surfaces of spinel (MgAl 2 O 4 ) will show the role of vacancy configuration and surface rearrangement. Atomistic and DFT studies on Li doped MgO illustrate the importance of both the defect structure and its effect of morphology. We will also illustrate using DFT electronic defects at the surface of CeO 2 , which are of great importance in redox reactions and catalytic activity. Finally we will present a novel atomistic approach for predicting the structure of supported oxide nanoclusters giving rise to a wide range of defects including a range of surface terminations, grain formation, mixed screw edge dislocations and misfit dislocations. We will illustrate this using the structure of a BaO supported MgO nanocluster.