arXiv subjects

W. E. Pickett

Publications and source records attributed to W. E. Pickett.

At least 73 records · Page 4Linked to original sources

arXiv2007

Half Semimetallic Antiferromagnetism in the Sr$_2$CrTO$_6$ System, T=Os, Ru

Double perovskite Sr$_2$CrOsO$_6$ is (or is very close to) a realization of a spin-asymmetric semimetallic compensated ferrimagnet, according to first principles calculations. This type of near-half metallic antiferromagnet is an unusual occurrence, and more so in this compound because the zero gap is accidental rather than being symmetry determined. The large spin-orbit coupling (SOC) of osmium upsets the spin balance (no net spin moment without SOC): it reduces the Os spin moment by 0.27 $μ_B$ and induces an Os orbital moment of 0.17 $μ_B$ in the opposite direction. The effects combine (with small oxygen contributions) to give a net total moment of 0.54 $μ_B$ per cell in \scoo, reflecting a large impact of SOC in this compound. This value is in moderately good agreement with the measured saturation moment of 0.75 $μ_B$. The value of the net moment on the Os ion obtained from neutron diffraction (0.73 $μ_B$ at low temperature) differs from the calculated value (1.14 $μ_B$). Rather surprisingly, in isovalent Sr$_2$CrRuO$_6$ the smaller SOC-induced spin changes and orbital moments (mostly on Ru) almost exactly cancel. This makes Sr$_2$CrRuO$_6$ a "half (semi)metallic antiferromagnet" (practically vanishing net total moment) even when SOC is included, with the metallic channel being a small-band-overlap semimetal. Fixed spin moment (FSM) calculations are presented for each compound, illustrating how they provide different information than in the case of a nonmagnetic material. These FSM results indicate that the Cr moment is an order of magnitude stiffer against longitudinal fluctuations than is the Os moment.

cond-mat.mtrl-sci↗

arXiv2007

s-wave Superconductivity Phase Diagram in the Inhomogeneous Two-Dimensional Attractive Hubbard Model

We study s-wave superconductivity in the two-dimensional square lattice attractive Hubbard Hamiltonian for various inhomogeneous patterns of interacting sites. Using the Bogoliubov-de Gennes (BdG) mean field approximation, we obtain the phase diagram for inhomogeneous patterns in which the on-site attractive interaction U_i between the electrons takes on two values, U_i=0 and -U/(1-f) (with f the concentration of non-interacting sites) as a function of average electron occupation per site n, and study the evolution of the phase diagram as f varies. In certain regions of the phase diagram, inhomogeneity results in a larger zero temperature average pairing amplitude (order parameter) and also a higher superconducting (SC) critical temperature T_c, relative to a uniform system with the same mean interaction strength (U_i=-U on all sites). These effects are observed for stripes, checkerboard, and even random patterns of the attractive centers, suggesting that the pattern of inhomogeneity is unimportant. The phase diagrams also include regions where superconductivity is obliterated due to the formation of various charge ordered phases. The enhancement of T_{c} due to inhomogeneity is robust as long as the electron doping per site n is less than twice the fraction of interacting sites [2(1-f)] regardless of the pattern. We also show that for certain inhomogeneous patterns, when n = 2(1-f), increasing temperature can work against the stability of existing charge ordered phases for large f and as a result, enhance T_{c}.

cond-mat.supr-con↗

arXiv2007

Orbital-quenching-induced magnetism in Ba_2NaOsO_6

The double perovskite \bnoo with heptavalent Os ($d^1$) is observed to remain in the ideal cubic structure ({\it i.e.} without orbital ordering) despite single occupation of the $t_{2g}$ orbitals, even in the ferromagnetically ordered phase below 6.8 K. Analysis based on the {\it ab initio} dispersion expressed in terms of an Os $t_{2g}$-based Wannier function picture, spin-orbit coupling, Hund's coupling, and strong Coulomb repulsion shows that the magnetic OsO$_6$ cluster is near a moment-less condition due to spin and orbital compensation. Quenching (hybridization) then drives the emergence of the small moment. This compensation, unprecedented in transition metals, arises in a unified picture that accounts for the observed Mott insulating behavior.

cond-mat.str-el↗

arXiv2007

Static versus dynamic fluctuations in the one-dimensional extended Hubbard model

The extended Hubbard Hamiltonian is a widely accepted model for uncovering the effects of strong correlations on the phase diagram of low-dimensional systems, and a variety of theoretical techniques have been applied to it. In this paper the world-line quantum Monte Carlo method is used to study spin, charge, and bond order correlations of the one-dimensional extended Hubbard model in the presence of coupling to the lattice. A static alternating lattice distortion (the ionic Hubbard model) leads to enhanced charge density wave correlations at the expense of antiferromagnetic order. When the lattice degrees of freedom are dynamic (the Hubbard-Holstein model), we show that a similar effect occurs even though the charge asymmetry must arise spontaneously. Although the evolution of the total energy with lattice coupling is smooth, the individual components exhibit sharp crossovers at the phase boundaries. Finally, we observe a tendency for bond order in the region between the charge and spin density wave phases.

cond-mat.str-el↗

arXiv2007

Correlation Effects in the Triangular Lattice Single-band System Li_xNbO_2

Superconductivity in hole-doped Li_xNbO_2 has been reported with T_c ~ 5 K in the range 0.45 < x < 0.8. The electronic structure is based on a two-dimensional triangular Nb lattice. The strong trigonal crystal field results in a single Nb d(z^2) band isolated within a wide gap, leading to a single-band triangular lattice system. The isolated, partially filled band has a width W=1.5 eV with dominant second neighbor hopping. To identify possible correlation effects, we apply DMFT(QMC) using on-site Coulomb repulsion U=0-3 eV, and check selected results using determinant QMC. For U as small as 1 eV, the single particle spectrum displays a robust lower Hubbard band, suggesting the importance of correlation effects in Li_xNbO_2 even for U < W. At half-filling (x=0), a Mott transition occurs at U_c ~ 1.5 eV. Coupling between the O A_g phonon displacement and correlation effects is assessed.

cond-mat.supr-con↗

arXiv2007

Rare-Earth Tetraborides RB$_4$: Analysis of Trends in the Electronic Structure

Both the basic electronic structure of tetraborides, and the changes across the lanthanide series in $R$B$_4$ ($R$ = rare earth) compounds, are studied using the correlated band theory LDA+U method in the all-electron Full Potential Local Orbital (FPLO) code. A set of boron bonding bands can be identified that are well separated from the antibonding bands. Separately, the ``dimer B'' $2p_z$ orbital is non-bonding ({\it viz.} graphite and MgB$_2$), and mixes strongly with the metal 4d or $5d$ states that form the conduction states. The bonding bands are not entirely filled even for the trivalent compounds (thus the cation $d$ bands have some filling), which accounts for the lack of stability of this structure when the cations are divalent (with more bonding states unfilled). The trends in the mean $4f$ level for both majority and minority, and occupied and unoccupied, states are presented and interpreted.

cond-mat.mtrl-sci↗

arXiv2007

Chemical Differences between K and Na in Alkali Cobaltates

K$_x$CoO$_2$ shares many similarities with Na$_x$CoO$_2$, as well as some important differences (no hydration-induced superconductivity has been reported). At $T_{c2}$=20 K, K$_{0.5}$CoO$_2$ becomes an insulator with a tiny optical gap as happens in Na$_{0.5}$CoO$_2$ at 52 K. This similarity, with a known common structure, enables direct comparisons to be made. Using the K-zigzag structure recently reported and the local density approximation, we compare and contrast these cobaltates at x=0.5. Although the electronic structures are quite similar as expected, substantial differences are observed near the Fermi level. These differences are found to be attributable mostly to the chemical, rather than structural difference: although Na is normally considered to be fully ion, K has somewhat more highly ionic character than does Na in these cobaltates.

cond-mat.str-el↗

arXiv2007

Linear response separation of a solid into atomic constituents: Li, Al, and their evolution under pressure

We present the first realization of the generalized pseudoatom concept introduced by Ball, and adopt the name enatom to minimize confusion. This enatom, which consists of a unique decomposition of the total charge density (or potential) of any solid into a sum of overlapping atomiclike contributions that move rigidly with the nuclei to first order, is calculated using (numerical) linear response methods, and is analyzed for both fcc Li and Al at pressures of 0, 35, and 50 GPa. These two simple fcc metals (Li is fcc and a good superconductor in the 20-40 GPa range) show different physical behaviors under pressure, which reflects the increasing covalency in Li and the lack of it in Al. The nonrigid (deformation) parts of the enatom charge and potential have opposite signs in Li and Al; they become larger under pressure only in Li. These results establish a method of construction of the enatom, whose potential can be used to obtain a real-space understanding of the vibrational properties and electron-phonon interaction in solids.

cond-mat.mtrl-sci↗

arXiv2006

Mott Transition of MnO under Pressure: Comparison of Correlated Band Theories

The electronic structure, magnetic moment, and volume collapse of MnO under pressure are obtained from four different correlated band theory methods; local density approximation + Hubbard U (LDA+U), pseudopotential self-interaction correction (pseudo-SIC), the hybrid functional (combined local exchange plus Hartree-Fock exchange), and the local spin density SIC (SIC-LSD) method. Each method treats correlation among the five Mn 3d orbitals (per spin), including their hybridization with three O $2p$ orbitals in the valence bands and their changes with pressure. The focus is on comparison of the methods for rocksalt MnO (neglecting the observed transition to the NiAs structure in the 90-100 GPa range). Each method predicts a first-order volume collapse, but with variation in the predicted volume and critical pressure. Accompanying the volume collapse is a moment collapse, which for all methods is from high-spin to low-spin (5/2 to 1/2), not to nonmagnetic as the simplest scenario would have. The specific manner in which the transition occurs varies considerably among the methods: pseudo-SIC and SIC-LSD give insulator-to-metal, while LDA+U gives insulator-to-insulator and the hybrid method gives an insulator-to-semimetal transition. Projected densities of states above and below the transition are presented for each of the methods and used to analyze the character of each transition. In some cases the rhombohedral symmetry of the antiferromagnetically ordered phase clearly influences the character of the transition.

cond-mat.str-el↗

arXiv2006

Dynamical mean field study of the Mott transition in the half-filled Hubbard model on a triangular lattice

We employ dynamical mean field theory (DMFT) with a Quantum Monte Carlo (QMC) atomic solver to investigate the finite temperature Mott transition in the Hubbard model with the nearest neighbor hopping on a triangular lattice at half-filling. We estimate the value of the critical interaction to be $U_c=12.0 \pm 0.5$ in units of the hopping amplitude $t$ through the evolution of the magnetic moment, spectral function, internal energy and specific heat as the interaction $U$ and temperature $T$ are varied. This work also presents a comparison between DMFT and finite size determinant Quantum Monte Carlo (DQMC) and a discussion of the advantages and limitations of both methods.

cond-mat.str-el↗

arXiv2006

Origin of Strong Coupling in Lithium under Pressure

In an attempt to provide a clearer understanding of the impressive increase in T_c under pressure in elemental Li, linear response calculation of the phonon dispersion curves, electron-phonon matrix elements, phonon linewidths and mode lambda's have been carried out on a finer mesh (24^3 in the Brillouin zone) than done previously, for the volume corresponding to 20 GPa pressure. The result illustrates the great need for a fine mesh (even finer than this) for converged results of lambda and the spectral function alpha^2 F. Although the initial pressure-induced transverse T_1 phonon instability (in harmonic approximation) near the symmetry point K has dominated attention, the current results show that the high value of T_c gets strong contributions from elsewhere in the zone, particularly from the longitudinal mode along (100).

cond-mat.supr-con↗

arXiv2006

Stability of the Gd Magnetic Moment to the 500 GPa Regime

The evolution of the magnetic moment and various features of the electronic structure of fcc Gd are followed to reduced volume V/Vo = 0.125 using the LDA+U correlated band method. The stability of the moment is substantial; crude estimates of this signature of a possible ``Mott transition'' in the 4f system suggest a critical pressure Pc 500 GPa. The $4f$ occupation is found to increase under pressure due to broadening and lowering of the minority states. This trend is consistent with the interpretation of x-ray spectra of Maddox et al. across the volume collapse transition at 59 GPa, and tends to support their suggestion that the delocalization of the 4f states in Gd differs from the original abrupt picture, being instead a process that occurs over an extended range of pressure.

cond-mat.str-el↗

arXiv2006

Strong Electron-Phonon Coupling in Yttrium under Pressure

Linear response methods are applied to identify the increase in electron-phonon coupling in elemental yttrium that is responsible for its high superconducting critical temperature Tc, which reaches nearly 20 K at 115 GPa. While the evolution of the band structure and density of states is smooth and seemingly modest, there is strong increase in the 4d content of the occupied conduction states under pressure. We find that the transverse mode near the L point of the fcc Brillouin zone, already soft at ambient pressure, becomes unstable (in harmonic approximation) at a relative volume V/Vo=0.60 (P ~ 42 GPa). The coupling to transverse branches is relatively strong at all high symmetry zone boundary points X, K, and L. Coupling to the longitudinal branches is not as strong, but extends over more regions of the Brillouin zone and involves higher frequencies. Evaluation of the electron-phonon spectral function $α^2F(ω)$ shows a very strong increase with pressure of coupling in the 2-7 meV range, with a steady increase also in the 7-20 meV range. These results demonstrates strong electron-phonon coupling in this system that can account for the observed range of Tc.

cond-mat.supr-con↗

arXiv2006

Frustration in Coupled Rattler System: KOs2O6

The phenomenon of frustration, which gives rise to many fascinating phenomena, is conventionally associated with the topology of non-bipartite lattices, where nearest-neighbor (nn) interactions and global connectivity compete in the lowering of energy. The issue of rattling atoms in spacious lattice sites is a separate occurrence that can also lead to a high density of low energy states (unusual low temperature thermodynamics) and to practical applications such as in improved thermoelectric materials. In this letter we address a unique situation where both phenomena arise: a four-fold single-site instability leads to rattling of cations on a diamond structure sublattice where nn interactions frustrate simple ordering of the displacements. The system deals with this coupling of rattling+frustration by commensurate ordering. Such a disorder-order transition may account for the second phase transition seen in KOs2O6 within the superconducting state, and the unusual low-energy dynamics and associated electron-phonon coupling can account for the qualitative differences in physical properties of KOs2O6 compared to RbOs2O6 and CsOs2O6, all of which have essentially identical average crystal and electronic structures.

cond-mat.str-el↗

arXiv2006

Effect of inhomogeneity on s-wave superconductivity in the attractive Hubbard model

Inhomogeneous s-wave superconductivity is studied in the two-dimensional, square lattice attractive Hubbard Hamiltonian using the Bogoliubov-de Gennes (BdG) mean field approximation. We find that at weak coupling, and for densities mainly below half-filling, an inhomogeneous interaction in which the on-site interaction $U_i$ takes on two values, $U_i=0, 2U$ results in a larger zero temperature pairing amplitude, and that the superconducting $T_c$ can also be significantly increased, relative to a uniform system with $U_i=U$ on all sites. These effects are observed for stripe, checkerboard, and even random patterns of the attractive centers, suggesting that the pattern of inhomogeneity is unimportant. Monte Carlo calculations which reintroduce some of the fluctuations neglected within the BdG approach see the same effect, both for the attractive Hubbard model and a Hamiltonian with d-wave pairing symmetry.

cond-mat.supr-con↗

arXiv2006

Charge and Spin Ordering in Insulating Na$_{0.5}$CoO$_2$: Effects of Correlation and Symmetry

Ab initio band theory including correlations due to intra-atomic repulsion is applied to study charge disproportionation and charge- and spin-ordering in insulating Na$_{0.5}$CoO$_2$. Various ordering patterns (zigzag and two striped) for four-Co supercells are analyzed before focusing on the observed "out-of-phase stripe" pattern of antiferromagnetic Co$^{4+}$ spins along charge-ordered stripes. This pattern relieves frustration and shows distinct analogies with the cuprate layers: a bipartite lattice of antialigned spins, with axes at 90 degree angles. Substantial distinctions with cuprates are also discussed, including the tiny gap of a new variant of "charge transfer" type within the Co 3d system.

cond-mat.str-el↗

arXiv2006

Study of Correlation Effects in the High Formal Oxidation State Compound Sr$_2$CoO$_4$

Two recent reports confirm that the newly synthesized Sr$_2$CoO$_4$ (formal oxidation state Co$^{4+}$) shows a high Curie temperature (~ 250 K), but they report different moments of 1.8 $μ_B$ and 1 $μ_B$ per Co. Using both commonly used functionals in the correlated band approach (LDA+U) as well as the local density approximation (LDA),the combined effects of correlation and hybridization with O 2p states are calculated and analyzed. Sr$_2$CoO$_2$ is already ferromagnetic within LDA (M=1.95 $μ_B$). Increasing U from zero, the two LDA+U schemes affect the moment oppositely out to a critical value $U_c$=2.5 eV, at which point they transform discontinuously from different states to the same large U state. Fixing U at $U_c$, fixed spin moment calculations show similar behavior out to a minimum at 1$μ_B$ (a half metallic state), beyond which the fully-localized-limit scheme jumps to a state with energy minimum very near 2$μ_B$ very close to the LDA moment). Although the energy minima occur very near integer values of the moment/Co (1$μ_B, 2$μ_B$), the strong 3d-2p mixing and resulting 3d orbital occupations seem to preclude any meaningful S=1/2 or S=1 assignment to the Co ion.

cond-mat.str-el↗

arXiv2006

Boron Spectral Density and Disorder Broadening in B-doped Diamond

Comparison of periodic B dopants with a random alloy of substitional boron in diamond is carried out using several supercells and the coherent potential approximation (CPA) for the random alloy case. The main peak in the B local density of states is shifted to lower binding energy compared to the corresponding C peak in intrinsic diamond. In supercells, this shows up as strongly B-character bands split from bulk C bands away from the zone center,in an energy region around -1 eV. Even for a 4*4*4 supercell (BC$_{127}$), effects of the dopant order are evident in the form of primarily B-character bands just below the Fermi level at the supercell zone boundary. The bands resulting from the CPA are of continuous mixed C-B character. They resemble virtual crystal bands, but broadened somewhat reflecting the disorder-induced lifetime, and are consistent with angle-resolved photoemission band maps. The B character is 1.7 times larger than for C (per atom) near the top of the valence bands for CPA, and roughly the same for supercells. CPA results are particularly useful since they characterize the wavevector and energy dependence of disorder broadening.

cond-mat.supr-con↗