In experiments, the ternary Eu pnictide EuRh2P2 shows an unusual coexistence of a non-integral Eu valence of about 2.2 and a rather high Neel temperature of 50 K. In this paper, we present a model which explains the non-integral Eu valence via covalent bonding of the Eu 4f-orbitals to P2 molecular orbitals. In contrast to intermediate valence models where the hybridization with delocalized conduction band electrons is known to suppress magnetic ordering temperatures to at most a few Kelvin, covalent hybridization to the localized P2 orbitals avoids this suppression. Using perturbation theory we calculate the valence, the high temperature susceptibility, the Eu single-ion anisotropy and the superexchange couplings of nearest and next-nearest neighbouring Eu ions. The model predicts a tetragonal anisotropy of the Curie constants. We suggest an experimental investigation of this anisotropy using single crystals. From experimental values of the valence and the two Curie constants, the three free parameters of our model can be determined.
Periodic and cluster density-functional theory (DFT) calculations, including DFT+U and hybrid functionals, are applied to study magnetostructural correlations in spin-1/2 frustrated chain compounds CuX2: CuCl2, CuBr2, and a fictitious chain structure of CuF2. The nearest-neighbor and second-neighbor exchange integrals, J1 and J2, are evaluated as a function of the Cu-X-Cu bridging angle, theta, in the physically relevant range 80-110deg. In the ionic CuF2, J1 is ferromagnetic for theta smaller 100deg. For larger angles, the antiferromagnetic superexchange contribution becomes dominant, in acco…
We investigate an effective Hamiltonian for Na0.5CoO2 that includes the electrostatic potential due to the ordered Na ions and strong electronic correlations. This model displays a subtle interplay between metallic and insulating phases and between charge and magnetic order. For realistic parameters, the model predicts an insulating phase with similarities to a covalent insulator. We show that this interpretation gives a consistent explanation of experiments on Na0.5CoO2, including the small degree of charge ordering, the small charge gap, the large moment, and the optical conductivity.
We report a first-principles Wannier function study of the electronic structure of PdTe. Its electronic structure is found to be a broad three-dimensional Fermi surface with highly reduced correlations effects. In addition, the higher filling of the Pd $d$-shell, its stronger covalency resulting from the closer energy of the Pd-$d$ and Te-$p$ shells, and the larger crystal field effects of the Pd ion due to its near octahedral coordination all serve to weaken significantly electronic correlations in the particle-hole (spin, charge, and orbital) channel. In comparison to the Fe Chalcogenide e.g…
The electronic and magnetic properties of Ba$_5$AlIr$_2$O$_{11}$ containing Ir-Ir dimers are investigated using the GGA and GGA+SOC calculations. We found that strong suppression of the magnetic moment in this compound recently found in [J. Terzic {\it et al.}, Phys. Rev. B {\bf 91}, 235147 (2015)] is not due to charge-ordering, but is related to the joint effect of the spin-orbit interaction and strong covalency, resulting in the formation of metal-metal bonds. They conspire and act against the intra-atomic Hund's rule exchange interaction to reduce total magnetic moment of the dimer. We argu…
We calculate the effective trigonal crystal field Delta which splits the t2g levels of effective models for NaxCoO2 as the local symmetry around a Co ion is reduced from Oh to D3d. To this end we solve numerically a CoO6 cluster containing a Co ion with all 3d states and their interactions included, and its six nearest-neighbor O atoms, with the geometry of the system, in which the CoO6 octahedron is compressed along a C3 axis. We obtain Delta near 130 meV, with the sign that agrees with previous quantum chemistry calculations, but disagrees with first-principles results in the local density a…
Magnetism of ruthernium pyrochlore oxides A2Ru2O7 (A = Hg, Cd, Ca), whose electronic properties within a localized ion picture are characterized by non-degenerate t2g orbitals (Ru5+, 4d3) and thereby subject to geometrical frustration, has been investigated by muon spin rotation/relaxation (muSR) technique. The A cation (mostly divalent) was varied to examine the effect of covalency (Hg > Cd > Ca) on their electronic property. In a sample with A = Hg that exhibits a clear metal-insulator (MI) transition below >> 100 K (which is associated with a weak structural transition), a nearly commensura…
Chlorine covalently bonded to an open shell metal is present in many materials with desirable or intriguing physical properties. Materials include highly luminescent nontoxic alternatives to lead halide perovskites for optoelectronic applications K2CuCl3 and Rb2CuCl3, enantiomorphic CsCuCl3 that presents magneto-chiral dichroism at a low temperature, and cubic K2RuCl6 that possesses a singlet ground state generated by antiparallel spin and orbital angular momenta. Structural chirality of CsCuCl3 has been confirmed by resonant x-ray Bragg diffraction. We explore likely benefits of the technique…
The importance of covalent bonding for the magnetism of 3d metal complexes was first noted by Pauling in 1931. His point became moot, however, with the success of the ionic picture of Van Vleck, where ligands influence magnetic electrons of 3d ions mainly through electrostatic fields. Anderson's theory of spin superexchange later established that covalency is at the heart of cooperative magnetism in insulators, but its energy scale was believed to be small compared to other inter-ionic interactions and therefore it was considered a small perturbation of the ionic picture. This assertion fails …
Magnetism in transition metal compounds is usually considered starting from a description of isolated ions, as exact as possible, and treating their (exchange) interaction at a later stage. We show that this standard approach may break down in many cases, especially in $4d$ and $5d$ compounds. We argue that there is an important intersite effect -- an orbital-selective formation of covalent metal-metal bonds, which leads to an "exclusion" of corresponding electrons from the magnetic subsystem, and thus strongly affects magnetic properties of the system. This effect is especially prominent for …
We have investigated the shifts of the core-level photoemission spectra of La$_{0.6}$Sr$_{0.4}$MnO$_3$ thin films grown on three kinds of substrates, SrTiO$_3$, (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$, and LaAlO$_3$. The experimental shifts of the La 4d and Sr 3d core levels are almost the same as the calculation, which we attribute to the absence of covalency effects on the Madelung potentials at these atomic sites due to the nearly ionic character of these atoms. On the other hand, the experimental shifts of the O $1s$ and Mn $2p$ core levels are negligibly small, in disagr…
In order to explore the effects of structural geometry on properties of correlated metals we investigate the magnetic properties of cubic (3C) and hexagonal (4H) BaRuO$_3$. While the 3C variant of BaRuO$_3$ is ferromagnetic below 60K, the 4H phase does not show any long-range magnetic order, however, there is experimental evidence of short-range antiferromagnetic correlations. Employing a combination of computational tools, namely density-functional theory and dynamical mean-field theory calculations, we probe the origin of contrasting magnetic properties of BaRuO$_3$ in the 3C and 4H structur…
Single-crystal sample of chromium doped with ca.0.2 at.%119Sn was studied by means of a transmission Mössbauer spectroscopy in the temperature range of 310-315 K. An anomaly in the temperature behavior of the center shift was found at ca. 313 K, a temperature that coincides well with the Néel temperature of chromium. The anomaly gives evidence that the vibrations of atoms in the studied system are affected by the magnetism.
Inter-band effects of magnetic field on orbital magnetic susceptibility and Hall effect in weak magnetic field have been studied theoretically at absolute zero for the model of massless Fermions in two dimension described by Weyl equation similar to graphenes, which are simplified version of newly found one in molecular solids, arfa-ET2I3 described by "tilted Weyl" equation. The dependences on the Fermi energy of both orbital susceptibility and Hall conductivity near the zero-gap region scale with elastic scattering time and then are very singular.
Based on the available literature reviewed are results pertinent to the effect of magnetism on lattice dynamics obtained by Mössbauer spectroscopy at 57Fe and 119Sn probe atoms. Presented and discussed are sigma-phase Fe-Cr, Fe-V, Fe-Cr-Ni and lambda-phase (C14 Laves) NbFe2 compounds that belong to the Frank-Kasper family of phases, metallic chromium and iron mono-arsenide, FeAs. The common feature of all these metallic systems is itinerant character of their magnetism. Two spectral parameters relevant to the lattice dynamics viz. the center shift, CS, and/or the recoil-free fraction, f, are c…
We report the effect of hydrostatic pressure on the electronic state of the antiferromagnet UIrGe, which is isostructural and isoelectronic with the ferromagnetic superconductors UCoGe and URhGe. The Neel temperature decreases with increasing pressure. We constructed a p-T phase diagram and estimated the critical pressure pc, where the antiferromagnetism vanishes, as 12 GPa. The antiferromagnetic/paramagnetic transition appears to be first order.
We employ a combination of density functional theory and dynamical mean-field theory to investigate the electronic structure of the recently synthesized insulator BaCrO$_3$. Our calculations show that Hund's coupling is responsible for strong correlation effects, which are however not sufficient to turn the system insulating. A finite Jahn-Teller distortion lifting the orbital degeneracy is necessary to stabilize an insulating state with orbital ordering and consequent magnetic ordering.
Sigma-phase Fe0.525Cr0.455Ni0.020 alloy was studied by means of Mössbauer spectrometry in the temperature range of 5-293 K. The average center shift, <CS>, determined from the recorded Mössbauer spectra was shown to significantly deviate from the Debye model in the temperature range below ca. 50 K i.e. in the magnetic state of the sample. The deviation is obviously due to the effect of magnetism on the lattice dynamics of the studied sample. Analysis of the <CS>-data in the paramagnetic phase in terms of the Debye model yielded the value of 437(7) K for the Debye temperature.
Orbital magnetization is known empirically to play an important role in several magnetic phenomena, such as permanent magnetism and ferromagnetic superconductivity. Within the recently developed ''modern theory of orbital magnetization'', theoretical insight has been gained into the nature of this often neglected contribution to magnetism, but is based on an underlying mean-field approximation. From this theory, a few treatments have emerged which also take into account correlations beyond the mean-field approximation. Here, we apply the scheme developed in a previous work [Phys. Rev. B ${\bf …
The unusual electronic and magnetic properties of the systems Ce$_3$Pd$_{20}$T$_6$ (T = Ge, Si) with two non-equivalent Ce positions are discussed. The logarithmic growth of resistance for both the systems confirms the presence of the Kondo effect in the two respective temperature ranges. The two-scale behavior is explained by consecutive splitting of Ce ion levels in the crystal field. The effects of the frustration caused by the coexistence of the different positions of cerium are treated, which may also significantly enhance the observed values of specific heat. A model of "molecular magnet…
We present the results of muon-spin relaxation (muSR) measurements on the hexagonal manganite HoMnO3. Features in the temperature-dependent relaxation rate, lambda, correlate with the magnetic transitions at 76 K, 38 K and 34 K. The highest temperature transition, associated with the ordering of Mn3+ moments has the largest effect on lambda. The application of a static electric field of E=10^4 Vm^-1 below T=50 K causes a small reduction in lambda which is suggestive of coupling between ferroelectric and magnetic domain walls in the ordered state of the material.
We present here the first-principles dynamical CPA (coherent potential approximation) combined with the tight-binding LMTO LDA+U method towards quantitative calculations of the electronic structure and magnetism at finite temperatures in transition metals and compounds. The theory takes into account the single-site dynamical charge and spin fluctuations using the functional integral technique as well as an effective medium. Numerical results for Fe, Co, and Ni show that the theory explains quantitatively the high-temperature properties such as the effective Bohr magneton numbers and the excita…
The influence of correlation effects on the orbital moments for transition metals and their alloys is studied by first-principle relativistic Density Functional Theory in combination with the Dynamical Mean-Field Theory. In contrast to the previous studies based on the orbital polarization corrections we obtain an improved description of the orbital moments for wide range of studied systems as bulk Fe, Co and Ni, Fe-Co disordered alloys and 3$d$ impurities in Au. The proposed scheme can give simultaneously a correct dynamical description of the spectral function as well as static magnetic prop…
The magnetic properties of the diluted magnetic semiconductor Ga_{1-x}Mn_{x}As are studied within the dynamical cluster approximation. We use the k-dot-p Hamiltonian to describe the electronic structure of GaAs with spin-orbit coupling and strain effects. We show that nonlocal effects are essential for explaining the experimentally observed transition temperature and saturation magnetization. We also demonstrate that the cluster anisotropy is very strong and induces rotational frustration and a cube-edge direction magnetic anisotropy at low temperature. With this, we explain the temperature-dr…
We have used a combination of resonant magnetic x-ray scattering (RMXS) and x-ray absorption spectroscopy (XAS) to investigate the properties of the doped spin-orbital Mott insulator Sr2Ir(1-x)Rh(x)O4 (0.07 < x < 0.70). We show that Sr2Ir(1-x)Rh(x)O4 represents a unique model system for the study of dilute magnetism in the presence of strong spin-orbit coupling, and provide evidence of a doping-induced change in magnetic structure and a suppression of magnetic order at x_c ~ 0.17. We demonstrate that Rh-doping introduces Rh3+/Ir5+ ions which effectively hole-dope this material. We propose that…
We illustrate the magnetoelectric effect conditioned by the Katsura-Nagaosa-Balatsky (KNB) mechanism within the frames of exactly solvable spin-1/2 $XY$ chains. Due to three-spin interactions which are present in our consideration, the magnetization (polarization) is influenced by the electric (magnetic) field even in the absence of the magnetic (electric) field. We also discuss a magnetoelectrocaloric effect examining the entropy changes under the isothermal varying of the magnetic or/and electric field.
In magnetism, of which molecular magnetism is a part, the term frustration is used rather sloppily. Sometimes one gains the impression that if the reason for some phenomenon is not quite clear then it is attributed to frustration. In this paper I discuss the effects of frustration that I feel are relevant for the field of molecular magnetism. As will become clear later they indeed lead to a variety of unusual magnetic properties.
The local magnetism induced by vacancies in the presence of the spin-orbital interaction is investigated based on the half-filled Kane-Mele-Hubbard model on the honeycomb lattice. Using the self-consistent mean-field theory, we find that the spin-orbital coupling will enhance the localization of the spin moments near a single vacancy. We further study the magnetic structures along the zigzag edges formed by a chain of vacancies. We find that the spin-orbital coupling tends to suppress the counter-polarized ferrimagnetic order on the upper and lower edges, because of the open of the spin-orbita…
The t-t' Hubbard model for the Fermi level near the Van Hove singularity is considered within the renormalization group and parquet approaches. The interplay of ferromagnetic, antiferromagnetic, and superconducting channels is investigated, and the phase diagram of the model is constructed. In comparison with previous approaches, the account of ferromagnetic fluctuations suppresses superconducting pairing and, vice versa, the influence of the Cooper channel decreases the Curie temperature, so that the Stoner criterion is inapplicable even qualitatively.
The cooperative behavior of quantum impurities on 2D materials, such as graphene and bilayer graphene, is characterized by a non-trivial competition between screening (Kondo effect), and Ruderman-Kittel-Kasuya-Yosida (RKKY) magnetism. In addition, due to the small density of states at the Fermi level, impurities may not couple to the conduction electrons at all, behaving as free moments. Employing a recently developed {\em{exact}} numerical method to study multi-impurity lattice systems, we obtain non-perturbative results that dramatically depart from expectations based on the conventional RKK…
We report the normal-state transport and magnetic properties of a pressure-induced superconductor CeTe$_{1.82}$. We found that the applied pressure is required to increase the Kondo temperature scale ($T^*_{\rm K} \sim$ 170 K), associated with the two-dimensional motion of the carriers confined within the Te plane. Both the short-range ferromagnetic ordering temperature ($T_{\rm SRF} \sim$ 6 K) and the long-range antiferromagnetic transition temperature ($T_{\rm N} \sim$ 4.3 K) are slightly increased with pressure. We suggest that the application of pressure enhances a coupling between the 4$f…
Effect of level statistics on local electronic states and local magnetism in nanoscale metallic grains with transition-metal impurity in the ballistic regime is studied. It is shown that the mean occupation of local electron and the local magnetic moment in nanoscale metallic grains with odd conduction electrons are larger than those with even conduction electrons. The effect of even-odd parity on the condition for the occurrence of local magnetic moment is also discussed, it is found that the critical value $ρ_{d}(0)U_{c}$ for the formation of local moment in nanoscale metallic grains is much…
The discovery of EuFeAs2, currently the only charge-neutral parent phase of the 112-type iron-pnictide system, provides a new platform for the study of elemental doping effects on magnetism and superconductivity (SC). In this study, a series of polycrystalline EuFe1-yCoyAs2 and Eu0.9Pr0.1Fe1-yCoyAs2 samples are synthesized through solid-state reaction, and the evolutions of SC and magnetism with Co doping in EuFeAs2 and Eu0.9Pr0.1FeAs2 are investigated by electrical transport and magnetic susceptibility measurements. For EuFe1-yCoyAs2, the Eu-related antiferromagnetic (AFM) transition around 4…
We calculate the effect of local magnetic moments on the electron-phonon coupling in BaFe$_{2}$As$_{2}+δ$ using the density functional perturbation theory. We show that the magnetism enhances the total electron-phonon coupling by $\sim 50%$, up to $λ\lesssim 0.35$, still not enough to explain the high critical temperature, but strong enough to have a non-negligible effect on superconductivity, for instance, by frustrating the coupling with spin fluctuations and inducing order parameter nodes. The enhancement comes mostly from a renormalization of the electron-phonon matrix elements. We also in…
We have explored Pauli paramagnetism, Landau diamagnetism and de Haas-van Alphen effect in a single framework, and unified these three effects for all temperatures as well as for all strengths of magnetic field. Our result goes beyond Pauli-Landau result on the magnetism of the 3-D ideal gas of electrons, and is able to describe crossover of the de Haas-van Alphen oscillation to the saturation of magnetization. We also have obtained a novel asymptotic series expansion for the low temperature properties of the system.
Single wall carbon nanotubes grown entirely from 13-C form an ideal system to study the effect of electron interaction on nuclear magnetism in one dimension. If the electrons are in the metallic, Luttinger liquid regime, we show that even a very weak hyperfine coupling to the 13-C nuclear spins has a striking effect: The system is driven into an ordered phase, which combines electron and nuclear degrees of freedom, and which persists up into the millikelvin range. In this phase the conductance is reduced by a universal factor of 2, allowing for detection by standard transport experiments.
It have been demonstrated that the zigzag honeycomb nanoribbons exhibit an intriguing edge magnetism. Here the effect of the anisotropy on the edge magnetism in zigzag honeycomb nanoribbons is investigated by using two kinds of large-scale quantum Monte Carlo simulations. The anisotropy in zigzag honeycomb nanoribbons is characterized by the ratios of nearest-neighboring hopping integrals $t_{1}$ in one direction and $t_{2}$ in another direction. Considering the electron-electron correlation, it is shown that the edge ferromagnetism could be enhanced greatly as $t_{2}/|t_{1}|$ increase from $1…
We discuss the orbital magnetism and the Hall effect in the weak magnetic field in two dimensional Dirac fermion systems with energy gap. This model is related to the graphene sheet, organic conductors, and $d$-density wave superconductors. We found the strong diamagnetism and finite Hall conductivity even in gapped systems. We also discuss the relation between the weak-magnetic field formalism and the Landau quantization with the Euler-Maclaurin expansion.
We study the effects of short-range correlated disorder arising from chemical dopants or local lattice distortions, on the ferromagnetism of 3d double exchange systems. For this, we integrate out the carriers and treat the resulting disordered spin Hamiltonian within local random phase approximation, whose reliability is shown by direct comparison with Monte Carlo simulations. We find large scale inhomogeneities in the charge, couplings and spin densities. Compared with the homogeneous case, we obtain larger Curie temperatures ($T_{C}$) and very small spin stiffnesses ($D$). As a result, large…
Among the members of the series R2PdSi3 (R= Rare-earths), the magnetic behavior of the Nd compound is interesting in some respects. This compound is considered to order ferromagnetically (below 16 K), unlike other members of this series which order antiferromagnetically. In addition, magnetic ordering temperature (To) is significantly enhanced with respect to de Gennes scaled value. In order to understand the magnetism of this compound better, we have investigated the magnetic behavior in detail (under external pressure as well) and also of its solid solutions based on substitutions at Nd and …
Electronic and magnetic properties of DNA structures doped by simple and transition d- and f-metal ions (Gd, La, Cu, Zn, Au) are reviewed. Both one- and two dimensional systems are considered. A particular attention is paid to gadolinium and copper doped DNA systems, their unusual magnetism being treated. The problem of classical and quantum transport (including transfer of genetic information during replication and transcription) and electron localization in biological systems is discussed.
The effect of differently oriented magnetic field on chiral incommensurate helimagnet UPtGe is studied both experimentally and theoretically. The magnetization measurements up to the field above the saturation have revealed an isotropic magnetic response below 20 T and a remarkable nonmonotonic anisotropy in high fields. Moreover, the two principally different phase transitions from the noncollinear incommensurate to the field-induced ferromagnetic state have been observed. These properties are successfully explained by density-functional theory calculations taking into account the noncollinea…
Impurity effects on the triangular antiferromagnets Ni$_{1-x}M_x$Ga$_2$S$_4$ ($M=$ Mn, Fe, Co and Zn) are studied. The 2D frozen spin-disordered state of NiGa$_2$S$_4$ is stable against the substitution of Zn$^{2+}$ ($S=0$) and Heisenberg Fe$^{2+}$ ($S=2$) spins, and exhibits a $T^2$-dependent magnetic specific heat, scaled by the Weiss temperature. In contrast, the substitutions with Co$^{2+}$ ($S=3/2$) spin with Ising-like anisotropy and Heisenberg Mn$^{2+}$ ($S=5/2$) spin induce a conventional spin glass phase. From these comparisons, it is suggested that integer size of Heisenberg spins is…
We present a detailed study on the microscopic origin of magnetism in suspended and dielectrically embedded CrI$_3$ monolayer. To this end, we down-fold two distinct minimal generalized Hubbard models with different orbital basis sets from \emph{ab initio} calculations using the constrained random phase approximation. Within mean-field approximation, we show that these models are capable of describing the formation of localized magnetic moments in CrI$_3$ and of reproducing electronic properties of full \emph{ab initio} calculations. We utilize the magnetic force theorem to study microscopic m…
Despite extensive researches on manganites owing to widespread use in modern electronics, this class of metal oxides does not cease to surprise with its unique properties and new phenomena. Here we have studied structural and magnetic properties of non-Heisenberg manganite nanoparticles with a strong spin-electron coupling. During transition from low temperature ferromagnetic to high temperature paramagnetic state, the change in charge, valence and spin (magnetic moment) with the localization of eg-electrons on the manganese ions have been detected. With decrease in a temperature, the overstat…
