Decoupling method for dynamical mean field theory calculations

In this paper we explore the use of an equation of motion decoupling method as an impurity solver to be used in conjunction with the dynamical mean field self-consistency condition for the solution of lattice models. We benchmark the impurity solver against exact diagonalization, and apply the method to study the infinite $U$ Hubbard model, the periodic Anderson model and the $pd$ model. This simple and numerically efficient approach yields the spectra expected for strongly correlated materials, with a quasiparticle peak and a Hubbard band. It works in a large range of parameters, and therefore can be used for the exploration of real materials using LDA+DMFT.Comment: 30 pages, 7 figure

Time-dependent energy absorption changes during ultrafast lattice deformation

The ultrafast time-dependence of the energy absorption of covalent solids upon excitation with femtosecond laser pulses is theoretically analyzed. We use a microscopic theory to describe laser induced structural changes and their influence on the electronic properties. We show that from the time evolution of the energy absorbed by the system important information on the electronic and atomic structure during ultrafast phase transitions can be gained. Our results reflect how structural changes affect the capability of the system to absorb external energy.Comment: 7 pages RevTeX, 8 ps figures, submitted to Journal of Appl. Physic

Electronic properties of Fabre charge-transfer salts under various temperature and pressure conditions

Using density functional theory, we determine parameters of tight-binding Hamiltonians for a variety of Fabre charge transfer salts, focusing in particular on the effects of temperature and pressure. Besides relying on previously published crystal structures, we experimentally determine two new sets of structures; (TMTTF)$_2$SbF$_6$ at different temperatures and (TMTTF)$_2$PF$_6$ at various pressures. We find that a few trends in the electronic behavior can be connected to the complex phase diagram shown by these materials. Decreasing temperature and increasing pressure cause the systems to become more two-dimensional. We analyze the importance of correlations by considering an extended Hubbard model parameterized using Wannier orbital overlaps and show that while charge order is strongly activated by the inter-site Coulomb interaction, the magnetic order is only weakly enhanced. Both orders are suppressed when the effective pressure is increased.Comment: 12 pages, 16 figure

Comparative investigation of the coupled-tetrahedra quantum spin systems Cu2Te2O5X2, X=Cl, Br and Cu4Te5O12Cl4

We present a comparative study of the coupled-tetrahedra quantum spin systems Cu2Te2O5X2, X=Cl, Br (Cu-2252(X)) and the newly synthesized Cu4Te5O12Cl4 (Cu-45124(Cl)) based on ab initio Density Functional Theory calculations. The magnetic behavior of Cu-45124(Cl) with a phase transition to an ordered state at a lower critical temperature T$_c$=13.6K than in Cu-2252(Cl) (T$_c$=18K) can be well understood in terms of the modified interaction paths. We identify the relevant structural changes between the two systems and discuss the hypothetical behavior of the not yet synthesized Cu-45124(Br) with an ab initio relaxed structure using Car-Parrinello Molecular Dynamics.Comment: 2 pages, 1 figure; submitted to Proceedings of M2S-HTSC VIII, Dresden 200

Multiferroic FeTe2_2O5_5Br: Alternating spin chains with frustrated interchain interactions

A combination of density functional theory calculations, many-body model considerations, magnetization and electron spin resonance measurements shows that the multiferroic FeTe$_2$O$_5$Br should be described as a system of alternating antiferromagnetic $S=5/2$ chains with strong Fe-O-Te-O-Fe bridges weakly coupled by two-dimensional frustrated interactions, rather than the previously reported tetramer models. The peculiar temperature dependence of the incommensurate magnetic vector can be explained in terms of interchain exchange striction being responsible for the emergent net electric polarization.Comment: 7 pages, 6 figure

Na2IrO3 as a molecular orbital crystal

Contrary to previous studies that classify Na2IrO3 as a realization of the Heisenberg-Kitaev model with dominant spin-orbit coupling, we show that this system represents a highly unusual case in which the electronic structure is dominated by the formation of quasi-molecular orbitals (QMOs), with substantial quenching of the orbital moments. The QMOs consist of six atomic orbitals on an Ir hexagon, but each Ir atom belongs to three different QMOs. The concept of such QMOs in solids invokes very different physics compared to the models considered previously. Employing density functional theory calculations and model considerations we find that both the insulating behavior and the experimentally observed zigzag antiferromagnetism in Na2IrO3 naturally follow from the QMO model.Comment: Final version, accepted by PR

Local moments and symmetry breaking in metallic PrMnSbO

We report a combined experimental and theoretical investigation of the layered antimonide PrMnSbO which is isostructural to the parent phase of the iron pnictide superconductors. We find linear resistivity near room temperature and Fermi liquid-like T^{2} behaviour below 150 K. Neutron powder diffraction shows that unfrustrated C-type Mn magnetic order develops below \sim 230 K, followed by a spin-flop coupled to induced Pr order. At T \sim 35 K, we find a tetragonal to orthorhombic (T-O) transition. First principles calculations show that the large magnetic moments observed in this metallic compound are of local origin. Our results are thus inconsistent with either the itinerant or frustrated models proposed for symmetry breaking in the iron pnictides. We show that PrMnSbO is instead a rare example of a metal where structural distortions are driven by f-electron degrees of freedom

The monoclinic crystal structure of α\alpha-RuCl3_3 and the zigzag antiferromagnetic ground state

The layered honeycomb magnet alpha-RuCl3 has been proposed as a candidate to realize a Kitaev spin model with strongly frustrated, bond-dependent, anisotropic interactions between spin-orbit entangled jeff=1/2 Ru4+ magnetic moments. Here we report a detailed study of the three-dimensional crystal structure using x-ray diffraction on untwinned crystals combined with structural relaxation calculations. We consider several models for the stacking of honeycomb layers and find evidence for a crystal structure with a monoclinic unit cell corresponding to a stacking of layers with a unidirectional in-plane offset, with occasional in-plane sliding stacking faults, in contrast with the currently-assumed trigonal 3-layer stacking periodicity. We report electronic band structure calculations for the monoclinic structure, which find support for the applicability of the jeff=1/2 picture once spin orbit coupling and electron correlations are included. We propose that differences in the magnitude of anisotropic exchange along symmetry inequivalent bonds in the monoclinic cell could provide a natural mechanism to explain the spin gap observed in powder inelastic neutron scattering, in contrast to spin models based on the three-fold symmetric trigonal structure, which predict a gapless spectrum within linear spin wave theory. Our susceptibility measurements on both powders and stacked crystals, as well as neutron powder diffraction show a single magnetic transition at TN ~ 13K. The analysis of the neutron data provides evidence for zigzag magnetic order in the honeycomb layers with an antiferromagnetic stacking between layers. Magnetization measurements on stacked single crystals in pulsed field up to 60T show a single transition around 8T for in-plane fields followed by a gradual, asymptotic approach to magnetization saturation, as characteristic of strongly anisotropic exchange interactions.Comment: 13 pages, 9 figures, published in Physical Review

Theory for the ultrafast ablation of graphite films

The physical mechanisms for damage formation in graphite films induced by femtosecond laser pulses are analyzed using a microscopic electronic theory. We describe the nonequilibrium dynamics of electrons and lattice by performing molecular dynamics simulations on time-dependent potential energy surfaces. We show that graphite has the unique property of exhibiting two distinct laser induced structural instabilities. For high absorbed energies (> 3.3 eV/atom) we find nonequilibrium melting followed by fast evaporation. For low intensities above the damage threshold (> 2.0 eV/atom) ablation occurs via removal of intact graphite sheets.Comment: 5 pages RevTeX, 3 PostScript figures, submitted to Phys. Re