Defect-Induced Orbital Polarization and Collapse of Orbital Order in Doped Vanadium Perovskites.

We explore mechanisms of orbital-order decay in the doped Mott insulators R_{1-x}(Sr,Ca)_{x}VO_{3} (R=Pr,Y,La) caused by charged (Sr,Ca) defects. Our unrestricted Hartree-Fock analysis focuses on the combined effect of random charged impurities and associated doped holes up to x=0.5. The study is based on a generalized multiband Hubbard model for the relevant vanadium t_{2g} electrons and includes the long-range (i) Coulomb potentials of defects and (ii) electron-electron interactions. We show that the rotation of t_{2g} orbitals, induced by the electric field of defects, is a very efficient perturbation that largely controls the suppression of orbital order in these compounds. We investigate the inverse participation number spectra and find that electron states remain localized on few sites even in the regime where orbital order is collapsed. From the change of kinetic and superexchange energy, we can conclude that the motion of doped holes, which is the dominant effect for the reduction of magnetic order in high-T_{c} compounds, is of secondary importance here.

Defects, Disorder, and Strong Electron Correlations in Orbital Degenerate, Doped Mott Insulators.

We elucidate the effects of defect disorder and e-e interaction on the spectral density of the defect states emerging in the Mott-Hubbard gap of doped transition-metal oxides, such as Y(1-x)Ca(x)VO(3). A soft gap of kinetic origin develops in the defect band and survives defect disorder for e-e interaction strengths comparable to the defect potential and hopping integral values above a doping dependent threshold; otherwise only a pseudogap persists. These two regimes naturally emerge in the statistical distribution of gaps among different defect realizations, which turns out to be of Weibull type. Its shape parameter k determines the exponent of the power-law dependence of the density of states at the chemical potential (k-1) and hence distinguishes between the soft gap (k≥2) and the pseudogap (k<2) regimes. Both k and the effective gap scale with the hopping integral and the e-e interaction in a wide doping range. The motion of doped holes is confined by the closest defect potential and the overall spin-orbital structure. Such a generic behavior leads to complex nonhydrogenlike defect states that tend to preserve the underlying C-type spin and G-type orbital order and can be detected and analyzed via scanning tunneling microscopy.

Topological order in an entangled SU(2) ⊗ XY spin-orbital ring.

We present rigorous topological order which emerges in a one-dimensional spin-orbital model due to the ring topology. Although this model with SU(2) spin and XY orbital interactions is known to exactly separate spins from orbitals by means of a unitary transformation on the open chain, we find that they are not quite independent when the chain is closed, and the spins form two half-rings carrying opposite quasimomenta. We show that on changing the topology from an open to a periodic chain, the degeneracy of the ground state is partially lifted while the low-energy excitations have a quadratic dispersion as a function of the total quasimomentum. This novel type of topological order which emerges from changing the topology from an open to a periodic chain is reminiscent of the infinite-U Hubbard chain.

Hidden quasiparticles and incoherent photoemission spectra in Na2IrO3.

We study two Kitaev-Heisenberg t-J-like models on a honeycomb lattice, focusing on the zigzag magnetic phase of Na(2)IrO(3), and investigate hole motion by exact diagonalization and variational methods. The spectral functions are quite distinct from those of cuprates and are dominated by large incoherent spectral weight at high energy, almost independent of the microscopic parameters-a universal and generic feature for zigzag magnetic correlations. We explain why quasiparticles at low energy are strongly suppressed in the photoemission spectra and determine an analog of a pseudogap. We point out that the qualitative features of the predominantly incoherent spectra obtained within the two different models for the zigzag phase are similar, and they have a remarkable similarity to recently reported angular resolved photoemission spectra for Na(2)IrO(3).

Anharmonicity due to electron-phonon coupling in magnetite.

We present the results of inelastic x-ray scattering for magnetite and analyze the energies and widths of the phonon modes with different symmetries in a broad range of temperature 125 < T < 293 K. The phonon modes with X(4) and Δ(5) symmetries broaden in a nonlinear way with decreasing T when the Verwey transition is approached. It is found that the maxima of phonon widths occur away from high-symmetry points, which suggests the incommensurate character of critical fluctuations. Strong phonon anharmonicity induced by electron-phonon coupling is discovered by a combination of these experimental results with ab initio calculations which take into account local Coulomb interactions at Fe ions. It (i) explains observed anomalous phonon broadening and (ii) demonstrates that the Verwey transition is a cooperative phenomenon which involves a wide spectrum of phonons coupled to the electron charge fluctuations condensing in the low-symmetry phase.

Density functional theory study of Au-fcc/Ge and Au-hcp/Ge interfaces.

In recent years, nanostructures with hexagonal polytypes of gold have been synthesised, opening new possibilities in nanoscience and nanotechnology. As bulk gold crystallizes in the fcc phase, surface effects can play an important role in stabilizing hexagonal gold nanostructures. Here, we investigate several heterostructures with Ge substrates, including the fcc and hcp phases of gold that have been observed experimentally. We determine and discuss their interfacial energies and optimized atomic arrangements, comparing the theory results with available experimental data. Our DFT calculations for the Au-fcc(011)/Ge(001) junction show how the presence of defects in the interface layer can help to stabilize the atomic pattern, consistent with microscopic images. Although the Au-hcp/Ge interface is characterized by a similar interface energy, it reveals large atomic displacements due to significant mismatch. Finally, analyzing the electronic properties, we demonstrate that Au/Ge systems have metallic character, but covalent-like bonding states between interfacial Ge and Au atoms are also present.

Noncollinear magnetic order stabilized by entangled spin-orbital fluctuations.

Quantum phase transitions in the two-dimensional Kugel-Khomskii model on a square lattice are studied using the plaquette mean field theory and the entanglement renormalization Ansatz. When 3z(2)-r(2) orbitals are favored by the crystal field and Hund's exchange is finite, both methods give a noncollinear exotic magnetic order that consists of four sublattices with mutually orthogonal nearest-neighbor and antiferromagnetic second-neighbor spins. We derive an effective frustrated spin model with second- and third-neighbor spin interactions which stabilize this phase and follow from spin-orbital quantum fluctuations involving spin singlets entangled with orbital excitations.

Competing pairing symmetries in a generalized two-orbital model for the pnictide superconductors.

We introduce and study an extended "t-U-J" two-orbital model for the pnictides that includes Heisenberg terms deduced from the strong coupling expansion. Including these J terms explicitly allows us to enhance the strength of the (π,0)-(0,π) spin order which favors the presence of tightly bound pairing states even in the small clusters that are here exactly diagonalized. The A(1g) and B(2g) pairing symmetries are found to compete in the realistic spin-ordered and metallic regime. The dynamical pairing susceptibility additionally unveils low-lying B(1g) states, suggesting that small changes in parameters may render any of the three channels stable.

Ferro-orbitally ordered stripes in systems with alternating orbital order.

We establish a novel mechanism of stripe formation in doped systems with alternating t(2g) orbital order--the stripe takes the form of a ferro-orbitally ordered domain wall separating domains with staggered order and allowing for deconfined motion of holes along the stripe. At a finite level of hole concentration this gives rise to the stability of this solitonic type of stripes, while we show that the phase change of the staggered order by π plays a minor role in orbitally ordered systems. These results shed new light on the physics of doped materials in which orbital degeneracy is present.

Phonon confinement and spin-phonon coupling in tensile-strained ultrathin EuO films.

Reducing the material sizes to the nanometer length scale leads to drastic modifications of the propagating lattice excitations (phonons) and their interactions with electrons and magnons. In EuO, a promising material for spintronic applications in which a giant spin-phonon interaction is present, this might imply a reduction of the degree of spin polarization in thin films. Therefore, a comprehensive investigation of the lattice dynamics and spin-phonon interaction in EuO films is necessary for practical applications. We report a systematic lattice dynamics study of ultrathin EuO(001) films using nuclear inelastic scattering on the Mössbauer-active isotope 151Eu and first-principles theory. The films were epitaxially grown on YAlO3(110), which induces a tensile strain of ca. 2%. By reducing the EuO layer thickness from 8 nm to a sub-monolayer coverage, the Eu-partial phonon density of states (PDOS) reveals a gradual enhancement of the number of low-energy phonon states and simultaneous broadening and suppression of the peaks. These deviations from bulk features lead to significant anomalies in the vibrational thermodynamic and elastic properties calculated from the PDOS. The experimental results, supported by first-principles theory, unveil a reduction of the strength of the spin-phonon interaction in the tensile-strained EuO by a factor of four compared to a strain-free lattice.

Interplay between the orbital and magnetic order in monolayer La(1-x)Sr(1+x)MnO(4) manganites.

A two-dimensional model which describes e(g) electrons in a monolayer of an undoped and half doped manganite La(1-x)Sr(1+x)MnO(4) is studied using correlated wavefunctions. The effective Hamiltonian takes into account the kinetic energy, the crystal field splitting between x(2)-y(2) and 3z(2)-r(2) orbitals, and on-site Coulomb interactions for e(g) electrons. They interact with S = 3/2 spins due to t(2g) electrons, which are treated as frozen core spins. Furthermore, the model includes antiferromagnetic superexchange interaction between core spins, and the coupling between e(g) electrons and Jahn-Teller modes. The model reproduces the antiferromagnetic order in the undoped LaSrMnO(4) compound, with occupied 3z(2)-r(2) orbitals and elongated MnO(6) octahedra along the direction perpendicular to the Mn-O plane. In half doped La(0.5)Sr(1.5)MnO(4) manganite one finds robust chequerboard-like charge order using realistic parameters. However, the experimentally observed CE phase is more difficult to stabilize, and we discuss the necessary conditions to obtain it within the present model. Altogether, we conclude that the Jahn-Teller effect plays a crucial role in the entire regime of doping.

Magnetic Lifshitz transition and its consequences in multi-band iron-based superconductors.

In this paper we address Lifshitz transition induced by applied external magnetic field in a case of iron-based superconductors, in which a difference between the Fermi level and the edges of the bands is relatively small. We introduce and investigate a two-band model with intra-band pairing in the relevant parameters regime to address a generic behaviour of a system with hole-like and electron-like bands in external magnetic field. Our results show that two Lifshitz transitions can develop in analysed systems and the first one occurs in the superconducting phase and takes place at approximately constant magnetic field. The chosen sets of the model parameters can describe characteristic band structure of iron-based superconductors and thus the obtained results can explain the experimental observations in FeSe and Co-doped BaFe2As2 compounds.

A possibility of high spin hole states in doped CoO2 layered systems.

We introduce and investigate an effective five-band model for t2g and eg electrons to describe doped cobalt oxides with Co(3+) and Co(4+) ions in two-dimensional CoO2 triangular lattice layers, as in Na1-xCoO2. The effective Hamiltonian includes anisotropic kinetic energy (due to both direct Co-Co and indirect Co-O-Co hoppings), on-site Coulomb interactions parameterized by intraorbital Hubbard repulsion U and full Hund's exchange tensor, crystal field terms and Jahn-Teller static distortions. We study it using correlated wave functions on 6 × 6 clusters with periodic boundary conditions. The computations indicate a low S = 0 spin to high S = 2 spin abrupt transition in the undoped systems when increasing strength of the crystal field, while intermediate S = 1 spins are not found. Surprisingly, for the investigated realistic Hamiltonian parameters describing low-spin states in CoO2 planes, doping generates high S = 5/2 spins at Co(4+) ions that are pairwise bound into singlets, seen here as pairs of up and down spins. It is found that such singlet pairs self-organize at higher doping into lines of magnetic ions with coexisting antiferromagnetic and ferromagnetic bonds between them, forming stripe-like structures. The ground states are insulating within the investigated range of doping because computed HOMO-LUMO gaps are never small enough.

Fingerprints of spin-orbital entanglement in transition metal oxides.

The concept of spin-orbital entanglement on superexchange bonds in transition metal oxides is introduced and explained on several examples. It is shown that spin-orbital entanglement in superexchange models destabilizes the long-range (spin and orbital) order and may lead either to a disordered spin-liquid state or to novel phases at low temperature which arise from strongly frustrated interactions. Such novel ground states cannot be described within the conventionally used mean field theory which separates spin and orbital degrees of freedom. Even in cases where the ground states are disentangled, spin-orbital entanglement occurs in excited states and may become crucial for a correct description of physical properties at finite temperature. As an important example of this behaviour we present spin-orbital entanglement in the RV O(3) perovskites, with R = La,Pr,…,Y b,Lu, where the finite temperature properties of these compounds can be understood only using entangled states: (i) the thermal evolution of the optical spectral weights, (ii) the dependence of the transition temperatures for the onset of orbital and magnetic order on the ionic radius in the phase diagram of the RV O(3) perovskites, and (iii) the dimerization observed in the magnon spectra for the C-type antiferromagnetic phase of Y V O(3). Finally, it is shown that joint spin-orbital excitations in an ordered phase with coexisting antiferromagnetic and alternating orbital order introduce topological constraints for the hole propagation and will thus radically modify the transport properties in doped Mott insulators where hole motion implies simultaneous spin and orbital excitations.

Jahn-Teller mechanism of stripe formation in doped layered La(2-x)Sr(x)NiO4 nickelates.

We introduce an effective model for e(g) electrons to describe quasi-two-dimensional layered La(2-x)Sr(x)NiO(4) nickelates and study it using correlated wavefunctions on 8 × 8 and 6 × 6 clusters. The effective Hamiltonian includes the kinetic energy, on-site Coulomb interactions for e(g) electrons (intraorbital U and Hund's exchange J(H)) and the coupling between e(g) electrons and Jahn-Teller distortions (static modes). The experimental ground state phases with inhomogeneous charge, spin and orbital order at the dopings x = 1/3 and 1/2 are reproduced very well by the model. Although the Jahn-Teller distortions are weak, we show that they play a crucial role and stabilize the observed cooperative charge, magnetic and orbital order in the form of a diagonal stripe phase at x = 1/3 doping and a chequerboard phase at x = 1/2 doping.

Jahn-Teller distortions and the magnetic order in the perovskite manganites.

We introduce an effective model for e(g) electrons to describe three-dimensional perovskite (La(1 - x)Sr(x)MnO(3) and La(1 - x)Ca(x)MnO(3)) manganites and study the magnetic and orbital order on a 4 × 4 × 4 cluster using correlated wavefunctions. The model includes the kinetic energy, and on-site Coulomb interactions for e(g) electrons, antiferromagnetic superexchange interaction between S = 3/2 core spins, and the coupling between e(g) electrons and Jahn-Teller modes. The model reproduces the experimentally observed magnetic order: (i) an A-type antiferromagnetic phase in the undoped insulator LaMnO(3), with alternating e(g) orbitals and with small Jahn-Teller distortions, changing to a conducting phase at 32 GPa pressure, and (ii) ferromagnetic order in one-eighth-doped La(7/8)Sr(1/8)MnO(3) and in quarter-doped La(3/4)Sr(1/4)MnO(3) compounds. For half-doped La(1/2)Ca(1/2)MnO(3) one finds a competition between a ferromagnetic conductor and the CE insulating phase; the latter is stabilized by the Jahn-Teller coupling being two times larger than for the strontium-doped compound. Altogether, there is a subtle balance between all Hamiltonian parameters and the phase diagram is quite sensitive to the precise values they take.

Structure and elastic properties of Mg(OH)2 from density functional theory.

The structure, lattice dynamics and mechanical properties of magnesium hydroxide have been investigated by static density functional theory calculations as well as ab initio molecular dynamics. The hypothesis of a superstructure existing in the lattice formed by the hydrogen atoms has been tested. The elastic constants of the material have been calculated with a static deformations approach and are in fair agreement with the experimental data. The hydrogen subsystem structure exhibits signs of disordered behaviour while maintaining correlations between the angular positions of neighbouring atoms. We establish that the essential angular correlations between hydrogen positions are maintained to a temperature of at least 150 K and that they are well described by a physically motivated probabilistic model. The rotational degree of freedom appears to be decoupled from the lattice directions above 30 K.

Thermally activated Peierls dimerization in ferromagnetic spin chains.

We demonstrate that a Peierls dimerization can occur in ferromagnetic spin chains activated by thermal fluctuations. The dimer order parameter and entanglement measures are studied as functions of the modulation of the magnetic exchange interaction and temperature, using a spin-wave theory and the density-matrix renormalization group. We discuss the case where a periodic modulation is caused by spin-phonon coupling and the case where electronic states effectively induce such a modulation. The importance of the latter for a number of transition metal oxides is highlighted.

Absence of hole confinement in transition-metal oxides with orbital degeneracy.

We investigate the spectral properties of a hole moving in a two-dimensional Hubbard model for strongly correlated t(2g) electrons. Although superexchange interactions are Ising-like, a quasi-one-dimensional coherent hole motion arises due to effective three-site terms. This mechanism is fundamentally different from the hole motion via quantum fluctuations in the conventional spin model with SU(2) symmetry. The orbital model describes also propagation of a hole in some e(g) compounds, and we argue that orbital degeneracy alone does not lead to hole self-localization.

Evolution of spin-orbital-lattice coupling in the RVO3 perovskites.

We introduce a microscopic model which unravels the physical mechanisms responsible for the observed phase diagram of the RVO3 perovskites. It reveals a nontrivial interplay between superexchange, the orbital-lattice coupling due to the GdFeO3-like rotations of the VO6 octahedra, and orthorhombic lattice distortions. We find that the lattice strain affects the onset of the magnetic and orbital order by partial suppression of orbital fluctuations. The present approach also provides a natural explanation of the observed reduction of magnon energies from LaVO3 to YVO3.