The electronic and magnetic properties of K$_{2}$CuP$_{2}$O$_{7}$ were investigated by means of susceptibility, specific heat and $^{31}$P nuclear magnetic resonance (NMR) measurements and by LDA band structure calculations. The temperature dependence of the NMR shift $K(T)$ is well described by the $S=1/2$ Heisenberg antiferromagnetic chain (HAF) model with nearest neighbor exchange $J_{1}$ $\simeq $ $(141\pm 5)$ K. The corresponding mapping of an LDA-derived tight-binding model leads to $J_{1}^{LDA}$ $\simeq$ 196 K. The spin lattice relaxation rate $1/T_{1}$ decreases with temperature below 300 K but becomes nearly temperature independent between 30 K and 2 K as theoretically expected for an $S = {1/2}$ HAF chain. None of the investigated properties give any evidence for long range magnetic order above 2K, in agreement with the results of the band structure calculation, which yield extremely weak exchange to the next nearest neighbor (NNN) and a very small and frustrated inter-chain exchange. Thus, K$_{2}$CuP$_{2}$O$_{7}$ seems to be a better realization of a nearest neighbor $S = {1/2}$ HAF chain than the compounds reported so far.
The magnetization curves and magnetocaloric effect during the adiabatic demagnetization of antiferromagnetic spin-1/2 $XXZ$ Heisenberg clusters with the shape of Johnson's solids (triangular cupola, square cupola and pentagonal cupola) are investigated using the exact numerical diagonalization for different values of the exchange anisotropy ranging in between the Ising and fully isotropic limit. It is demonstrated that spin-1/2 $XXZ$ Heisenberg cupolae display, in comparison with their Ising counterparts, at least one more magnetization plateau. The novel magnetization plateaux extends over a …
From thermodynamics, LSDA+U calculations and exact diagonalization studies of a five-band Hubbard (Cu 3d, O 2p) model on CuO2 stripes we found that Li2ZrCuO4 (Li2CuZrO4 in traditional notation) is close to a ferromagnetic critical point. Analyzing its measured susceptibility chi(T) and specific heat cp(T,H) within a Heisenberg model, we show that the ratio of the 2nd to the 1st neighbor exchange integrals alpha=-J2/J1 of the order of 0.3, i.e. it is close to the critical value alpha_c=1/4. Comparing with related chain cuprates we explain the rather strong field dependence of cp, the monotonous…
We examine two-spin (2S) and cyclic four-spin (4S) magnetic interactions in insulating ladder and two-dimensional (2D) cuprates. By a comparison of eigenstates between d-p and Heisenberg models, we evaluate magnitudes of these interactions. We find that the 4S interaction is $\sim$10% of nearest neighboring 2S interaction, and a diagonal 2S interaction is considerably small. The 4S interaction for a ladder cuprate is larger than that for 2D one, and plays an important role in the low-energy excitation. The Heisenberg ladder with the obtained 2S and 4S interactions reproduces very well the expe…
We calculate the Heisenberg exchange J in the quasi-2D antiferromagnetic cuprates La2CuO4, YBa2Cu3O6, Nd2CuO4 and Sr2CuO2Cl2. We apply all-electron (MC)SCF and non-orthogonal CI calculations to [Cu2O11]18-, [Cu2O9]14-, [Cu2O7]10- and [Cu2O7Cl4]14- clusters in a model charge embedding. The (MC)SCF triplet and singlet ground states are well characterized by Cu2+ (dx2-y2) and O2-. The antiferromagnetic exchange is strongly enhanced by admixing relaxed (MC)SCF triplet and singlet excited states, in which a single electron is transferred from the central O ion to Cu. We ascribe this effect to orbit…
High temperature superconductivity in cuprates arises from an electronic state that remains poorly understood. We report the observation of a related electronic state in a non-cuprate material Sr2IrO4 in which the unique cuprate Fermiology is largely reproduced. Upon surface electron doping through in situ deposition of alkali-metal atoms, angle-resolved photoemission spectra of Sr2IrO4 display disconnected segments of zero-energy states, known as Fermi arcs, and a gap as large as 80 meV. Its evolution toward a normal metal phase with a closed Fermi surface as a function of doping and temperat…
We have investigated the thermal conductivity κ_mag of high-purity single crystals of the spin chain compound Sr2CuO3 which is considered an excellent realization of the one-dimensional spin-1/2 antiferromagnetic Heisenberg model. We find that the spinon heat conductivity κ_mag is strongly enhanced as compared to previous results obtained on samples with lower chemical purity. The analysis of κ_mag allows to compute the spinon mean free path l_mag as a function of temperature. At low-temperature we find l_mag\sim0.5\mum, corresponding to more than 1200 chain unit cells. Upon increasing the tem…
We report on a comprehensive characterization of the newly synthesized Cu$^{2+}$-based molecular magnet [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ (CuPOF), where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, $μ^+$SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the 2D square-lattice $S=1/2$ antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of $J/k_\mathrm{B} = 6.80(5)$ K, and an extremely small interlayer interaction of a…
We study the electronic structure of the ladder compounds (SrCa)CuO 14-24-41 and SrCuO 123. LDA calculations for both give similar Cu 3d-bands near the Fermi energy. The hopping parameters estimated by fitting LDA energy bands show a strong anisotropy between the t_perp t_par intra-ladder hopping and small inter-ladder hopping. A downfolding method shows that this anisotropy arises from the ladder structure.The conductivity perpendicular to the ladders is computed assuming incoherent tunneling giving a value close to experiment.
We report a detailed examination the magnetic structure of anhydrous cupric chloride CuCl2 carried out by powder neutron diffraction, magnetic susceptibility and specific heat measurements on polycrystalline and single crystal samples as well as an evaluation of the spin exchange interactions by first principles density functional theory (DFT) calculations. Anhydrous CuCl2 shows one dimensional antiferromagnetic behavior and long range antiferromagnetic ordering below a Neel temperature of 23.9 K. Neutron powder and single crystal diffraction reveal that, below 23.9K, CuCl2 undergoes a phase t…
We theoretically analyze some of the anomalies of the optical sumrules in the high-temperature superconductors. In particular we address the particularly strong dependence on temperature of the sumrule in the normal state. Both electron-electron correlations and the presence of a Van-Hove singularity have been shown to enhance such a dependence. Here we consider both effects simultaneously by means of Dynamical Mean-Field Theory for a two dimensional Hubbard model with realistic parameters for different cuprates, and we find that the two effects are not cooperative, as they appear to compete o…
Using low-energy projection of the one-band t-t'-t"-Hubbard model we derive an effective spin-Hamiltonian and its spin-wave expansion to order 1/S. We fit the spin-wave dispersion of several parent compounds to the high-temperature superconducting cuprates: La2CuO4, Sr2CuO2Cl2 and Bi2Sr2YCu2O8. Our accurate quantitative determination of the one-band Hubbard model parameters allows prediction and comparison to experimental results of measurable quantities such as staggered moment, double occupancy density, spin-wave velocity and bimagnon excitation spectrum and density of states, which is discu…
We report a comparative study of 63Cu Nuclear Magnetic Resonance spin lattice relaxation rates, T_1^{-1}, on undoped SrCuO_2 and Ca doped Sr_{0.9}Ca_{0.1}CuO_2 spin chain compounds. A temperature independent T_1^{-1} is observed for SrCuO_2 as expected for an S=1/2 Heisenberg chain. Surprisingly, we observe an exponential decrease of T_1^{-1} for T < 90,K in the Ca-doped sample evidencing the opening of a spin gap. The data analysis within the J_1-J_2 Heisenberg model employing density-matrix renormalization group calculations suggests an impurity driven small alternation of the J_2-exchange c…
A microscopic theory for electronic spectrum of the CuO2 plane within an effective p-d Hubbard model is proposed. Dyson equation for the single-electron Green function in terms of the Hubbard operators is derived which is solved self-consistently for the self-energy evaluated in the noncrossing approximation. Electron scattering on spin fluctuations induced by kinematic interaction is described by a dynamical spin susceptibility with a continuous spectrum. Doping and temperature dependence of electron dispersions, spectral functions, the Fermi surface and the coupling constant are studied in t…
High resolution resonant inelastic x-ray scattering has been performed to reveal the role of lattice-coupling in a family of quasi-1D insulating cuprates, Ca$_{2+5x}$Y$_{2-5x}$Cu$_5$O$_{10}$. Site-dependent low energy excitations arising from progressive emissions of a 70 meV lattice vibrational mode are resolved for the first time, providing a direct measurement of electron-lattice coupling strength. We show that such electron-lattice coupling causes doping-dependent distortions of the Cu-O-Cu bond angle, which sets the intra-chain spin exchange interactions. Our results indicate that the lat…
It is widely accepted that the low-energy physics in edge-sharing cuprate materials has one-dimensional (1D) character. The relevant model to study such systems is believed to be the 1D extended Heisenberg model with ferromagnetic nearest-neighbor (NN) interaction and antiferromagnetic next-nearest-neighbor one. Thus far, however, theoretical studies of such materials have been confined to the case of isotropic interactions. In the present work, we compare the spin susceptibility of the 1D extended Heisenberg model with anisotropy in the NN channel, obtained by means of the Transfer Matrix Ren…
On the basis of an analysis of theoretical and numerical studies of model systems, and of experiments on superconductivity in doped C$_{60}$, polyacenes, and the cuprate high temperature superconductors, we propose that a purely electronic mechanism of superconductivity requires structures at an intermediate or mesoscale. Specifically, we address the crucial question of how high temperature superconducting pairing on the mesoscale can arise from purely repulsive electronic interactions.
Correlation effects in CuO$_2$ layers give rise to a complicated landscape of collective excitations in high-T$_{\rm c}$ cuprates. Their description requires an accurate account for electronic fluctuations at a very broad energy range and remains a challenge for the theory. Particularly, there is no conventional explanation of the experimentally observed `resonant' antiferromagnetic mode, which is often considered to be a mediator of superconductivity. Here we model spin excitations of the hole-doped cuprates in the paramagnetic regime and show that this antiferromagnetic mode is associated wi…
Sr$_2$CuTeO$_6$ presents an opportunity for exploring low-dimensional magnetism on a square lattice of $S=1/2$ Cu$^{2+}$ ions. We employ ab initio multi-reference configuration interaction calculations to unravel the Cu$^{2+}$ electronic structure and to evaluate exchange interactions in Sr$_2$CuTeO$_6$. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr$_2$CuTeO$_6$ is an almost realization …
We describe here a minimal theory of tight binding electrons moving on the square planar Cu lattice of the hole-doped cuprates and mixed quantum mechanically with pairs of them (Cooper pairs). Superconductivity occurring at the transition temperature T_c is the long-range, d-wave symmetry phase coherence of these Cooper pairs. Fluctuations necessarily associated with incipient long-range superconducting order have a generic large distance behaviour near T_c. We calculate the spectral density of electrons coupled to such Cooper pair fluctuations and show that features observed in Angle Resolved…
Doping and strain dependences of the electronic structure of the CuO6-octahedra layer within LDA+GTB method in the frameworks of six-band p-d model are calculated. Band structure and Fermi surface of the quasiparticle excitations in the effective Hubbard model are characterized by inhomogeneous distribution of the k-dependent spectral weight. Doping results in reconstruction of the band structure, redistribution of the spectral weight over dispersion surface and reconstruction of Fermi surface from small hole pockets in the underdoped region to large hole contour in the overdoped region throug…
It is shown that a quasi two dimensional (layered) Heisenberg antiferromagnet with fully frustrated interplane couplings ({\it e.g.} on a body-centered tetragonal lattice) generically exhibits two thermal phase transitions with lowering temperature -- an upper transition at $T_{TO}$ (``order from disorder without order'') in which the lattice point-group symmetry is spontaneously broken, and a lower Néel transition at $T_{N}$ at which spin-rotation symmetry is broken. Although this is the same sequence of transitions observed in La$_2$CuO$_4$, in the Heisenberg model (without additional lattic…
During the last decade, translational and rotational symmetry-breaking phases -- density wave order and electronic nematicity -- have been established as generic and distinct features of many correlated electron systems, including pnictide and cuprate superconductors. However, in cuprates, the relationship between these electronic symmetry-breaking phases and the enigmatic pseudogap phase remains unclear. Here, we employ resonant x-ray scattering in a cuprate high-temperature superconductor La$_{1.6-x}$Nd$_{0.4}$Sr$_{x}$CuO$_{4}$ (Nd-LSCO) to navigate the cuprate phase diagram, probing the rel…
New electronic Raman and I.R. spectroscopy results from optimally and overdoped high temperature superconducting (HTSC) cuprate systems are interpreted in terms of the negative-U, boson-fermion crossover model. Distinction is made between those features which follow the condensate gap, 2Delta(p), and those that are set by the local-pair binding energy, cursive U(p). The critical role of doping level psubc = 0.185 is highlighted in conjunction with the matter of developing quasiparticle incoherence, making connection here with recent transport and related results. E//c IR results in magnetic fi…
We show that the mean-field resonating valence bond approximation proposed in 1987 by Baskaran, Zou, and Anderson describes gapless charge pair excitations confined to the boundaries of the spinon Brillouin zone. The existence of such pairs accounts for all the essential anomalous electronic properties of cuprates, with superconductivity arising due to the charge drag by the spinon superflow. This mechanism may be relevant to other unconventional superconductors.
Removing electrons from the CuO2 plane of cuprates alters the electronic correlations sufficiently to produce high-temperature superconductivity. Associated with these changes are spectral weight transfers from the high energy states of the insulator to low energies. In theory, these should be detectable as an imbalance between the tunneling rate for electron injection and extraction - a tunneling asymmetry. We introduce atomic-resolution tunneling-asymmetry imaging, finding virtually identical phenomena in two lightly hole-doped cuprates: Ca1.88Na0.12CuO2Cl2 and Bi2Sr2Dy0.2Ca0.8Cu2O8+d. Inten…
The doping and temperature dependence of the electronic Raman response in cuprate superconductors is studied within the framework of the kinetic energy driven superconducting mechanism for the t-J model. It is shown that the temperature dependent depletion at low-energy shifts is faster in B_{1g} symmetry than in B_{2g} symmetry. In analogy to the domelike shape of the doping dependent superconducting transition temperature, the pair-breaking peak energy in B_{2g} channel increases with increasing doping in the underdoped regime, and reaches a maximum in the optimal doping, then decreases in t…
We calculate electronic single-particle properties of short-range ordered stripe states, using Monte-Carlo simulations of collective charge-density wave (CDW) order parameters coupled to fermions on a 2d square lattice. For superconducting bond-centered stripes with a d-wave form factor, we find a valence-bond "glass" which coexists with low-energy quasiparticles featuring interference phenomena, in agreement with recent scanning-tunneling-microscopy (STM) measurements on underdoped BSCCO and CaNaCuOCl. Together with earlier work, our calculations provide a link between CDW features seen in ST…
The low-frequency dielectric response of hole-doped insulators La_{2}Cu_{1-x}Li_{x}O_{4} and La_{2-x}Sr_{x}NiO_{4} shows a large dielectric constant ε^{'} at high temperature and a step-like drop by a factor of 100 at a material-dependent low temperature T_{f}. T_{f} increases with frequency and the dielectric response shows universal scaling in a Cole-Cole plot, suggesting that a charge glass state is realized both in the cuprates and in the nickelates.
After an extended introduction, the thesis considers the electronic properties of BSCCO and the recent progress in understanding the electronic structure of this material. The main result of this part of the work is a model of the Green's function that is later used for calculating the two-particle excitation spectrum. Then, the matrix element effects in the photoemission spectra of cuprates are discussed with a focus on the recently discovered anomalous behavior of the ARPES spectra that partially originates from the momentum-dependent photoemission matrix element. The momentum- and excitatio…
We have studied the electronic structure of the two-dimensional Heisenberg antiferromagnet VOCl using photoemission spectroscopy and density functional theory including local Coulomb repulsion. From calculated exchange integrals and the observed energy dispersions we argue that the degree of one-dimensionality regarding both the magnetic and electronic properties is noticeably reduced compared to the isostructural compounds TiOCl and TiOBr. Also, our analysis provides conclusive justification to classify VOCl as a multi-orbital Mott insulator. In contrast to the titanium based compounds densit…
We show that important anomalous features of the normal-state thermoelectric power S of high-Tc materials can be understood as being caused by doping dependent short-range antiferromagnetic correlations. The theory is based on the fluctuation-exchange approximation applied to Hubbard model in the framework of the Kubo formalism. Firstly, the characteristic maximum of S as function of temperature can be explained by the anomalous momentum dependence of the single-particle scattering rate. Secondly, we discuss the role of the actual Fermi surface shape for the occurrence of a sign change of S as…
The mixed manganite-cuprate CaCu3Mn4O12 is found, using density functional methods, to be a narrow gap (90 meV calculated) ferrimagnetic semiconductor. Cu (formally S=1/2) antialigns with Mn (formally S=3/2), and the net spin moment is 9 μ_B consistent with the formal spins. Holes have Cu d_{xy}-O p_σ (i.e. antibonding dpσ) character with spins aligned antiparallel to the net magnetization; electrons have the opposite spin and have mixed Cu d_{xy} - Mn e_g character. Thermally excited electrons and holes will each be fully spin polarized, but in opposite directions. The properties of this mate…
In complex transition metal oxide heterostructures of physically dissimilar perovskite compounds, interface phenomena can lead to novel physical properties not observed in either of their constituents. This remarkable feature opens new prospects for technological applications in oxide electronic devices based on nm-thin oxide films. Here we report on a significant electronic charge and orbital reconstruction at interfaces between YBa2Cu3O6 and SrTiO3 studied using local spin density approximation (LSDA) with intra-atomic Coulomb repulsion (LSDA+U). We show that the interface polarity results i…
Hall effect and quantum oscillation measurements on high temperature cuprate superconductors show that underdoped compositions have a small Fermi surface pocket whereas when heavily overdoped, the pocket increases dramatically in size. The origin of this change in electronic structure has been unclear, but may be related to the high temperature superconductivity. Here we show that the clean overdoped single-layer cuprate Tl2Ba2CuO6+x (Tl2201) displays CDW order with a remarkably long correlation length $ξ\approx 200$ Å which disappears above a hole concentration p_CDW ~ 0.265. We show that the…
In this review article, we show our recent results relating to the undoped (Ce-free) superconductivity in the electron-doped high-Tc cuprates with the so-called T' structure. For an introduction, we briefly mention the characteristics of the electron-doped T'-cuprates, including the reduction annealing, conventional phase diagram and undoped superconductivity. Then, our transport and magnetic results and results relating to the superconducting pairing symmetry of the undoped and underdoped T'-cuprates are shown. Collaborating spectroscopic and nuclear magnetic resonance results are also shown …
We report ab initio quantum chemical cluster calculations of the chain (J_a) and the largest interchain (J_b) Heisenberg exchange of the chain cuprates Ca_2CuO_3 and Sr_2CuO_3. We find that J_a is comparable to the in-plane J in layered cuprates and J_a/J_b ~250-400. Using recent theory we obtain close agreement with experiment for the staggered moments and the critical temperatures. This implies that T_N does not depend on the third parameter J_c << J_b, and cannot be calculated using spin-wave theory. We propose an explanation for this interms of a 1D->2D cross-over.
The real part of the optical in-plane conductivity of p-- and n--type cuprates thin films at various doping levels was deduced from highly accurate reflectivity measurements. We present here a comprehensive set of optical spectral weight data as a function of the temperature $T (> T_c$), for underdoped and overdoped samples. The temperature dependence of the spectral weight is not universal. Using various cut-off frequencies for the spectral weight, we show that n--type Pr$_{2-x}$Ce$_x$CuO$_4$ and p--type Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ exhibit both similarities and striking differences. The Fer…
This article is devoted to a discussion of stripe and electron-nematic order and their connection to electronic properties in the pseudogap regime of copper-oxide superconductors. We review basic properties of these symmetry-breaking ordering phenomena as well as proposals which connect them to quantum-oscillation measurements. Experimental data indicate that these orders are unlikely to be the cause of the pseudogap phenomenon, implying that they occur on top of the pseudogap state which itself is of different origin. Specifically, we discuss the idea that the non-superconducting pseudogap gr…
Despite decades of progress, an understanding of unconventional superconductivity still remains elusive. An important open question is about the material dependence of the superconducting properties. Using the quasiparticle self-consistent GW method, we re-examine the electronic structure of copper oxide high-Tc materials. We show that QSGW captures several important features, distinctive from the conventional LDA results. The energy level splitting between dx2-y2 and d3z2-r2 is significantly enlarged and the van Hove singularity point is lowered. The calculated results compare better than LDA…
We investigate the high-energy magnetic excitation spectrum of the high-$T_c$ cuprate superconductor Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi-2212) using Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS). Broad, dispersive magnetic excitations are observed, with a zone boundary energy of $\sim$300 meV and a weak dependence on doping. These excitations are strikingly similar to the bosons proposed to explain the high-energy `kink' observed in photoemission. A calculation of the spin-response based on the ARPES-derived electronic structure and YRZ-quasi-particles reproduces the key features of t…
Sr_2CuO_3 and Ca_2CuO_3 are considered to be model systems of strongly anisotropic, spin-1/2 Heisenberg antiferromagnets. We report on the basis of a band-structure analysis within the local density approximation and on the basis of available experimental data a careful analysis of model parameters for extended Hubbard and Heisenberg models. Both insulating compounds show half-filled nearly one-dimensional antibonding bands within the LDA. That indicates the importance of strong on-site correlation effects. The bonding bands of Ca_2CuO_3 are shifted downwards by 0.7 eV compared with Sr_2CuO_3,…
This article summarizes and extends the recent developments in the microscopic modeling of the magnetic excitations in cuprate two-leg ladder systems. The microscopic Hamiltonian comprises dominant Heisenberg exchange terms plus an additional four-spin interaction which is about five times smaller. We give an overview over the relevant energies like the one-triplon dispersion, the energies of two-triplon bound states and the positions of multi-triplon continua and over relevant spectral properties like spectral weights and spectral densities in the parameter regime appropriate for cuprate syst…
Many recently discovered advanced materials, such as high-Tc cuprates, iron pnictides and several heavy-fermions, exhibit a rich phase diagram suggesting the presence of different competing interactions that would lead to various types of ordering. Nevertheless, there is not yet a clear unifying picture allowing the understanding of the detailed mechanisms that generate such competing interactions. Having such a picture, however, could quite well be at the very roots of the requirements for understanding high-Tc superconductivity in cuprates and pnictides, for instance. In this work we conside…
The S=1/2 Heisenberg bilayer antiferromagnet with randomly removed inter-layer dimers is studied using quantum Monte Carlo simulations. A zero-temperature multi-critical point (p*,g*) at the classical percolation density p=p* and inter-layer coupling g* approximately 0.16 is demonstrated. The quantum critical exponents of the percolating cluster are determined using finite-size scaling. It is argued that the associated finite-temperature quantum critical regime extends to zero inter-layer coupling and could be relevant for antiferromagnetic cuprates doped with non-magnetic impurities.
