Determining surface magnetization and local magnetic moments with atomic scale resolution

We propose a method to determine the direction of surface magnetization and local magnetic moments on the atomic scale. The method comprises high resolution scanning tunneling microscope experiments in conjunction with first principles simulations of the tunneling current. The potential of the method is demonstrated on a model system, antiferromagnetic Mn overlayers on W(110). We expect that it will ultimately allow to study the detailed changes of magnetic surface structures in the vicinity of dopants or impurities.Comment: Four pages (RevTeX) and five figures (EPS). For related papers see http://cmmp.phys.ucl.ac.uk/~wah

Local boron doping quantification in homoepitaxial diamond structures

The capability of transmission electronmicroscopy (TEM) using the high angle annular dark fieldmode (HAADF,also labelled Z-contrast) to quantify boron concentration, in the high doping range between 1019cm−3 and 1021cm−3, is demonstrated. Thanks to the large relative variation of atomic number Z between carbon and boron, doping concentration maps and profiles are obtained with a nanometer-scale resolution. A novel numerical simulation procedure allows the boron concentration quantification and demonstrates the high sensitivity and spatial resolution of the technique.4 page

Probing magnetic order in EELS of chromite spinels using both multiple scattering (FEFF8.2) and DFT (WIEN2k)

The electron energy loss near edge structure on the O K-edge from chromite spinels contains fine structure from the hybridisation of the O p-orbitals and the Cr d-orbitals. Unlike the aluminates, a non-spin polarised calculation of this fine structure differs significantly from experimental observations. This is due to the large magnetic moment on the Cr. Calculations using simplified collinear ordering of the spins and the local spin density approximation give much improved agreement. A real space multiple scattering formalism and a reciprocal space density functional formalism give results in substantial agreement. In general, the actual spin arrangement of these chromites is not known since they are typically frustrated magnetic systems with ordering temperatures in the 10–20 K range. The calculations are based on the hypothesis that dynamic short range order persists to room temperature over the time scale of the interaction with the fast electron. However, it is possible that the observed effects are due to the strong paramagnetism present at room temperatures but which it is not possible to simulate accurately at present

Spin state and phase competition in TbBaCo_{2}O_{5.5} and the lanthanide series LnBaCo_{2}O_{5+\delta} (0<=\delta<=1)

A clear physics picture of TbBaCo$_{2}$O$_{5.5}$ is revealed on the basis of density functional theory calculations. An antiferromagnetic (AFM) superexchange coupling between the almost high-spin Co$^{3+}$ ions competes with a ferromagnetic (FM) interaction mediated by both p-d exchange and double exchange, being responsible for the observed AFM-FM transition. And the metal-insulator transition is accompanied by an xy/xz orbital-ordering transition. Moreover, this picture can be generalized to the whole lanthanide series, and it is predicted that a few room-temperature magnetoresistance materials could be found in LnBa$_{1-x}$A$_{x}$Co$_{2}$O$_{5+\delta}$ (Ln=Ho,Er,Tm,Yb,Lu; A=Sr,Ca,Mg).Comment: 13 pages, 2 figures; to be published in Phys. Rev. B on 1st Sept. Title and Bylines are added to the revised versio

Optimization of inhomogeneous electron correlation factors in periodic solids

A method is presented for the optimization of one-body and inhomogeneous two-body terms in correlated electronic wave functions of Jastrow-Slater type. The most general form of inhomogeneous correlation term which is compatible with crystal symmetry is used and the energy is minimized with respect to all parameters using a rapidly convergent iterative approach, based on Monte Carlo sampling of the energy and fitting energy fluctuations. The energy minimization is performed exactly within statistical sampling error for the energy derivatives and the resulting one- and two-body terms of the wave function are found to be well-determined. The largest calculations performed require the optimization of over 3000 parameters. The inhomogeneous two-electron correlation terms are calculated for diamond and rhombohedral graphite. The optimal terms in diamond are found to be approximately homogeneous and isotropic over all ranges of electron separation, but exhibit some inhomogeneity at short- and intermediate-range, whereas those in graphite are found to be homogeneous at short-range, but inhomogeneous and anisotropic at intermediate- and long-range electron separation.Comment: 23 pages, 15 figures, 1 table, REVTeX4, submitted to PR

Repulsion-Sustained Supercurrent and Flux Quantization in Rings of Symmetric Hubbard Clusters

We test the response to a threading magnetic field of rings of 5-site $C_{4v}$-symmetric repulsive Hubbard clusters connected by weak intercell links; each 5-site unit has the topology of a CuO$_{4}$ cluster and a repulsive interaction is included on every site. In a numerical study of the three-unit ring with 8 particles, we take advantage of a novel exact-diagonalization technique which can be generally applied to many-fermion problems. For O-O hopping we find Superconducting Flux Quantization (SFQ), but for purely Cu-Cu links bound pair propagation is hindered by symmetry. The results agree with W=0 pairing theory.Comment: 4 pages, 2 figure

Electrical resistivity at large temperatures: Saturation and lack thereof

Many transition metal compounds show saturation of the resistivity at high temperatures, T, while the alkali-doped fullerenes and the high-Tc cuprates are usually considered to show no saturation. We present a model of transition metal compounds, showing saturation, and a model of alkali-doped fullerenes, showing no saturation. To analyze the results we use the f-sum rule, which leads to an approximate upper limit for the resistivity at large T. For some systems and at low T, the resistivity increases so rapidly that this upper limit is approached for experimental T. The resistivity then saturates. For a model of transition metal compounds with weakly interacting electrons, the upper limit corresponds to a mean free path consistent with the Ioffe-Regel condition. For a model of the high Tc cuprates with strongly interacting electrons, however, the upper limit is much larger than the Ioffe-Regel condition suggests. Since this limit is not exceeded by experimental data, the data are consistent with saturation also for the cuprates. After "saturation" the resistivity usually grows slowly. For the alkali-doped fullerenes, "saturation" can be considered to have happened already for T=0, due to orientational disorder. For these systems, however, the resistivity grows so rapidly after "saturation" that this concept is meaningless. This is due to the small band width and to the coupling to the level energies of the important phonons.Comment: 22 pages, RevTeX, 19 eps figures, additional material available at http://www.mpi-stuttgart.mpg.de/andersen/fullerene

Density-functional embedding using a plane-wave basis

The constrained electron density method of embedding a Kohn-Sham system in a substrate system (first described by P. Cortona, Phys. Rev. B {\bf 44}, 8454 (1991) and T.A. Wesolowski and A. Warshel, J. Phys. Chem {\bf 97}, 8050 (1993)) is applied with a plane-wave basis and both local and non-local pseudopotentials. This method divides the electron density of the system into substrate and embedded electron densities, the sum of which is the electron density of the system of interest. Coupling between the substrate and embedded systems is achieved via approximate kinetic energy functionals. Bulk aluminium is examined as a test case for which there is a strong interaction between the substrate and embedded systems. A number of approximations to the kinetic-energy functional, both semi-local and non-local, are investigated. It is found that Kohn-Sham results can be well reproduced using a non-local kinetic energy functional, with the total energy accurate to better than 0.1 eV per atom and good agreement between the electron densities.Comment: 11 pages, 4 figure

Electronic structure study of double perovskites A2A_{2}FeReO6_{6} (A=Ba,Sr,Ca) and Sr2M_{2}MMoO6_{6} (M=Cr,Mn,Fe,Co) by LSDA and LSDA+U

We have implemented a systematic LSDA and LSDA+U study of the double perovskites $A_{2}$FeReO$_{6}$ (A=Ba,Sr,Ca) and Sr$_{2}$$M$MoO$_{6}$ (M=Cr,Mn,Fe,Co) for understanding of their intriguing electronic and magnetic properties. The results suggest a ferrimagnetic (FiM) and half-metallic (HM) state of $A_{2}$FeReO$_{6}$ (A=Ba,Sr) due to a pdd-$\pi$ coupling between the down-spin Re$^{5+}$/Fe$^{3+}$ $t_{2g}$ orbitals via the intermediate O $2p_{\pi}$ ones, also a very similar FiM and HM state of Sr$_{2}$FeMoO$_{6}$. In contrast, a decreasing Fe $t_{2g}$ component at Fermi level ($E_{F}$) in the distorted Ca$_{2}$FeReO$_{6}$ partly accounts for its nonmetallic behavior, while a finite $pdd$-$\sigma$ coupling between the down-spin Re$^{5+}$/Fe$^{3+}$ $e_{g}$ orbitals being present at $E_{F}$ serves to stabilize its FiM state. For Sr$_{2}$CrMoO$_{6}$ compared with Sr$_{2}$FeMoO$_{6}$, the coupling between the down-spin Mo$^{5+}$/Cr$^{3+}$ $t_{2g}$ orbitals decreases as a noticeable shift up of the Cr$^{3+}$ 3d levels, which is likely responsible for the decreasing $T_{C}$ value and weak conductivity. Moreover, the calculated level distributions indicate a Mn$^{2+}$(Co$^{2+}$)/Mo$^{6+}$ ionic state in Sr$_{2}$MnMoO$_{6}$ (Sr$_{2}$CoMoO$_{6}$), in terms of which their antiferromagnetic insulating ground state can be interpreted. While orbital population analyses show that owing to strong intrinsic pd covalence effects, Sr$_{2}M$MoO$_{6}$ (M=Cr,Mn,Fe,Co) have nearly the same valence state combinations, as accounts for the similar M-independent spectral features observed in them.Comment: 21 pages, 3 figures. to be published in Phys. Rev. B on 15th Se