We theoretically study electric quadrupole orders in f-electron systems on the fcc lattice. Qudrupole degrees of freedom $O_{20}$ and $O_{22}$ originate in the non-Kramers doublet ground state $Γ_3$ of ion with $f^2$ electron configuration. For discussing quadrupole orders, we use a minimal model with isotropic ($J$) and anisotropic ($K$) nearest-neighbor interactions, and determine the phase diagram using a four-site mean-field approximation at zero and finite temperatures. Quadrupoles couple the $Γ_3$ doublet to the singlet excited state $Γ_1$, and its effects on canting antiferro orders are examined in detail. We found that this coupling leads to a rich phase diagram including two- and four-sublattice antiferro phases, and that two phases show a partial order of quadrupoles at finite temperatures.
The Heisenberg model on a face center cubic (fcc) lattice is a typical three-dimensional frustrated spin system expected to have magnetization plateaus and supersolid phases. There are model compounds $A_2$CoTeO$_6$ ($A$ = Ca, Sr, Pb) for the fcc lattice but with lattice distortions. Motivated by the presence of the compounds, we investigate the ground state of the spin-1/2 antiferromagnetic Heisenberg model on a tetragonally distorted fcc lattice in the magnetic field using a large-size cluster mean-field method for the sake of finding new supersolid phases. We find five supersolid phases in …
The Berry phase due to the spin wavefunction gives rise to the orbital ferromagnetism and anomalous Hall effect in the non-coplanar antiferromagnetic ordered state on face centered cubic (fcc) lattice once the crystal is distorted perpendicular to (1,1,1) or (1,1,0)- plane. The relevance to the real systems $γ$-FeMn and NiS$_2$ is also discussed.
The Hubbard model on fcc-type lattices is studied in the dynamical mean-field theory of infinite spatial dimensions. At intermediate interaction strength finite temperature Quantum Monte Carlo calculations yield a second order phase transition to a highly polarized, metallic ferromagnetic state. The Curie temperatures are calculated as a function of electronic density and interaction strength. A necessary condition for ferromagnetism is a density of state with large spectral weight near one of the band edges.
Spin waves in the type-III ordered antiferromagnetic state of the frustrated $t$-$t'$ Hubbard model on the fcc lattice are calculated to investigate finite-$U$-induced competing interaction and frustration effects on magnetic excitations and instabilities. Particularly strong competing interactions generated due to interplay of fcc lattice geometry and magnetic order result in significant spin wave softening. The calculated spin wave dispersion is found to be in qualitative agreement with the measured spin wave dispersion in the pyrite mineral $\rm Mn S_2$ obtained from inelastic neutron scatt…
The classical ground states of the SU(4) Heisenberg model on the face centered cubic lattice constitute a highly degenerate manifold. We explicitly construct all the classical ground states of the model. To describe quantum fluctuations above these classical states, we apply linear flavor-wave theory. At zero temperature, the bosonic flavor waves select the simplest of these SU(4) symmetry breaking states, the four-sublattice ordered state defined by the cubic unit cell of the fcc lattice. Due to geometrical constraints, flavor waves interact along specific planes only, thus rendering the syst…
We find evidence for long-range and short-range ($ζ$ $=$ 70 Å~at 4 K) incommensurate magnetic order on the quasi-face-centered-cubic (FCC) lattices of the monoclinic double perovskites La$_2$NaRuO$_6$ and La$_2$NaOsO$_6$ respectively. Incommensurate magnetic order on the FCC lattice has not been predicted by mean field theory, but may arise via a delicate balance of inequivalent nearest neighbour and next nearest neighbour exchange interactions. In the Ru system with long-range order, inelastic neutron scattering also reveals a spin gap $Δ$ $\sim$ 2.75 meV. Magnetic anisotropy is generally min…
We investigate magnetic properties of a frustrated Heisenberg antiferromagnet with a face-centered cubic (FCC) lattice and exchange interactions between the nearest- and next-nearest neighbours, J1 and J2. In a collinear phase with the wave vector Q = (pi,pi,pi) the equations of the self-consistent spin-wave theory for the sublattice magnetization and the average short range order parameter are obtained and numerically solved. The dependence of the Neel temperature T_N on the ratio J2/J1 is obtained. It is shown, that at strong enough frustration there is a wide temperature region above T_N wi…
We have performed inelastic neutron scattering experiments to investigate the magnetic excitations in the quasi-face-centered-cubic (fcc) iridate double perovskites La2ZnIrO6 and La2MgIrO6, which are characterized by A-type antiferromagnetic ground states. The neutron scattering data, which reveal gapped spin wave excitations with a very weak dispersion, are shown to be well-described by theoretical calculations on a model Hamiltonian with dominant Kitaev interactions. Our surprising finding shows that in contrast to honeycomb materials, where the Kitaev interaction manifests itself via comple…
We report on the unconventional magnetism in the cubic B-site ordered double perovskite Ba2YMoO6, using AC and DC magnetic susceptibility, heat capacity and muSR. No magnetic order is observed down to 2 K while the Weiss temperature is ~ -160 K. This is ascribed to the geometric frustration in the lattice of edge-sharing tetrahedra with orbitally degenerate Mo5+ s=1/2 spins. Our experimental results point to a gradual freezing of the spins into a disordered pattern of spin-singlets, quenching the orbital degeneracy while leaving the global cubic symmetry unaffected, and providing a rare exampl…
Electronic frustration and strong correlations may lead to large Seebeck coefficients. To understand this physics on general grounds, we compute the thermopower of the one-band Hubbard model on the 3-dimensional fcc lattice over the whole range of fillings for intermediate and large interaction strength. Dynamical mean-field theory shows that when the density approaches half-filling, the fcc lattice at strong coupling exhibits a large low temperature Seebeck coefficient $S$. The largest effect occurs as one approaches $n=1$ from dopings where electronic frustration is maximized. The high-frequ…
Magnetic frustration in metals is scarce and hard to pinpoint, but exciting due to the possibility of the emergence of fascinating novel phases. The cubic intermetallic compound HoInCu$_4$ with all holmium atoms on an fcc lattice, exhibits partial magnetic frustration, yielding a ground state where half of the Ho moments remain without long-range order, as evidenced by our neutron scattering experiments. The substitution of In with Cd results in HoCdCu$_4$ in a full breakdown of magnetic frustration. Consequently we found a fully ordered magnetic structure in our neutron diffraction experiment…
We have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites La$_2$ZnIrO$_6$ and La$_2$MgIrO$_6$, which are characterized by A-type antiferromagnetic ground states. The powder inelastic neutron scattering data on these geometrically frustrated $j_{\rm eff}=1/2$ Mott insulators provide clear evidence for gapped spin wave excitations with very weak dispersion. The INS results and thermodynamic data on these materials can be reproduced by conventional Heisenberg-Ising models wi…
Motivated by experiments on the double perovskites La2ZnIrO6 and La2MgIrO6, we study the magnetism of spin-orbit coupled j=1/2 iridium moments on the three-dimensional, geometrically frustrated, face-centered cubic lattice. The symmetry-allowed nearest-neighbor interaction includes Heisenberg, Kitaev, and symmetric off-diagonal exchange. A Luttinger-Tisza analysis shows a rich variety of orders, including collinear A-type antiferromagnetism, stripe order with moments along the [111]-direction, and incommensurate non-coplanar spirals, and we use Monte Carlo simulations to determine their magnet…
The Kitaev-Heisenberg (KH) model has been proposed to capture magnetic interactions in iridate Mott insulators on the honeycomb lattice. We show that analogous interactions arise in many other geometries built from edge-sharing IrO_6 octahedra, including the pyrochlore and hyperkagome lattices relevant to Ir2O4 and Na4Ir3O8 respectively. The Kitaev spin liquid exact solution does not generalize to these lattices. However, a different exactly soluble point of the honeycomb lattice KH model, obtained by a four-sublattice transformation to a ferromagnet, generalizes to all these lattices. A Klein…
The Dynamical Mean-Field theory (DMFT) approach to the Hubbard model requires a method to solve the problem of a quantum impurity in a bath of non-interacting electrons. Iterated Perturbation Theory (IPT) has proven its effectiveness as a solver in many cases of interest. Based on general principles and on comparisons with an essentially exact Continuous-Time Quantum Monte Carlo (CTQMC) solver, here we show that the standard implementation of IPT fails away from half-filling when the interaction strength is much larger than the bandwidth. We propose a slight modification to the IPT algorithm t…
We report the characterisation of natural samples of the cubic pyrite mineral MnS2 using very high resolution synchrotron X-ray diffraction techniques. At low temperatures we find a new low temperature polymorph, which results from coupling between magnetic and lattice degrees of freedom. Below the magnetic ordering temperature T_N= 48 K, we detect a pseudo-tetragonal distortion with a tiny c/a ratio of 1.0006. The structure can be refined in the space group Pbca. The symmetry lowering reduces magnetic frustration in the fcc Mn2+ lattice and is likely responsible for the previously reported lo…
The ground-state magnetic phase diagram (including collinear and spiral states) of the single-band Hubbard model for the face-centered cubic lattice and related metal-insulator transition (MIT) are investigated within the slave-boson approach by Kotliar and Ruckenstein. The correlation induced electronic spectrum narrowing and a comparison with a generalized Hartree-Fock approximation allow one to estimate the strength of correlation effects. This, as well as the MIT scenario, depends dramatically on the ratio of the next-nearest and nearest electron hopping integrals $t'/t$. In contrast with …
We study the intrinsic orbital magnetization (OM) in antiferromagnets on the distorted face-centered-cubic lattice. The combined lattice distortion and spin frustration induce nontrivial $k$-space Chern invariant, which turns to result in profound effects on the OM properties. We derive a specific relation between the OM and the Hall conductivity, according to which it is found that the intrinsic OM vanishes when the electron chemical potential lies in the Mott gap. The distinct behavior of the intrinsic OM in the metallic and insulating regions is shown. The Berry phase effects on the thermoe…
In order to investigate multipole ordering in f-electron systems from a microscopic viewpoint, we study the so-called Γ_8 models on three kinds of lattices, simple cubic (sc), bcc, and fcc, based on a j-j coupling scheme with f-electron hopping integrals through (ffσ) bonding. From the Γ_8 model, we derive an effective model for each lattice structure by using the second-order perturbation theory with respect to (ffσ). By further applying mean-field theory to the effective model, we find a Γ_{3g} antiferro-quadrupole transition for the sc lattice, a Γ_{2u} antiferro-octupole transition for the…
Based on a generalized one-band Hubbard model, we study magnetic properties of Mott insulating states for ultracold spin-3/2 fermionic atoms in optical lattices. When the \textit{s}-wave scattering lengths for the total spin $S=2,0$ satisfy conditions $a_{2}>a_{0}>0$, we apply a functional integral approach to the half filled case, where the spin-quadrupole fluctuations dominate. On a 2D square lattice, the saddle point solution yields a staggered spin-quadrupole ordering at zero temperature with symmetry breaking from SO(5) to SO(4). Both spin and spin-quadrupole static structure factors are …
Neutron scattering experiment on NiS2 single crystal revealed a honeycomb pattern of the intensity distribution in reciprocal lattice space (continuous-line structure along the fcc zone boundary) providing the first direct evidence for nearly frustrated antiferromagnetism (AF) on the face centered cubic (fcc) lattice. A small but finite lattice distortion below 30.9 K lifts the degeneracy of the magnetic ground state due to the frustration and eventually result in the coexistence of the type I and the type II AF long range orderings, which are mutually incompatible in the fcc symmetry at highe…
Cubic crystal structure and regular octahedral environment of Ir$^{4+}$ render antifluorite-type K$_2$IrCl$_6$ a model fcc antiferromagnet with a combination of Heisenberg and Kitaev exchange interactions. High-resolution synchrotron powder diffraction confirms cubic symmetry down to at least 20 K, with a low-energy rotary mode gradually suppressed upon cooling. Using thermodynamic and transport measurements, we estimate the activation energy of $Δ\simeq 0.7$ eV for charge transport, the antiferromagnetic Curie-Weiss temperature of $θ_{\rm CW}\simeq -43$ K, and the extrapolated saturation fiel…
We investigate the possibility of ferromagnetic ordering in the non-degenerate Hubbard model on the face-centered cubic lattice within the functional renormalization group technique using temperature as a scale parameter. We assume the relations between nearest, next-nearest, and next-next-nearest hopping parameters providing higher order (giant) van Hove singularity of the density of states. The ferromagnetic instability formation with lowering temperature is described consistently in the one-loop approximation for a one-particle irreducible vertex of two-particle electron interaction. The ch…
Monte Carlo simulation results are reported on magnetic ordering in ABC stacked Kagomé layers with fcc symmetry for both XY and Heisenberg models which include exchange interactions with the eight near-neighbors. Well known degeneracies of the 2D system persist in the 3D case and analysis of the numerical data provides strong evidence for a fluctuation-driven first-order transition to well-defined long-range order characterized as the layered $q=0$ (120-degree) spin structure. Effects of varying the inter-layer coupling are also examined. The results are relevant to understanding the role of f…
The synthesis and characterization of the previously unknown material LaCaScIrO$_6$ is reported. LaCaScIrO$_6$ presents a new example of the rare case of a double perovskite with the strongly spin-orbit coupled 5\textit{d}-ion Ir$^{4+}$ as its only magnetic species, forming a monoclinically distorted version of the frustrated fcc lattice. Magnetization measurements show a weak anomaly at 8~K. The Curie-Weiss temperature Θ$_{CW}$ and effective magnetic moment μ$_{eff}$ of LaCaScIrO$_6$ are in close proximity to the related compound La$_2$MgIrO$_6$ but differ from La$_2$ZnIrO$_6$. This suggests …
We provide numerical evidence that a spin-flux phase exists as a ground state of the Kondo lattice model with classical local spins on a square lattice. This state manifests itself as a double-Q magnetic order in the classical spins with spin density at both $(0,π)$ and $(π,0)$ and further exhibits fermionic spin currents around an elementary plaquette of the square lattice. We examine the spin-wave spectrum of this phase. We further discus an extension to a face centered cubic (FCC) lattice where a spin-flux phase may also exist. On the FCC lattice the spin-flux phase manifests itself as a tr…
To clarify a key role of $f$ orbitals in the emergence of antiferro-quadrupole structure in PrPb$_{3}$, we investigate the ground-state property of an orbital-degenerate Kondo lattice model by numerical diagonalization techniques. In PrPb$_{3}$, Pr$^{3+}$ has a $4f^{2}$ configuration and the crystalline-electric-field ground state is a non-Kramers doublet $Γ_{3}$. In a $j$-$j$ coupling scheme, the $Γ_{3}$ state is described by two local singlets, each of which consists of two $f$ electrons with one in $Γ_{7}$ and another in $Γ_{8}$ orbitals. Since in a cubic structure, $Γ_{7}$ has localized na…
We study the multipole interactions between $f^2$ ions with the $Γ_3$ non-Kramers doublet ground state under a cubic crystalline electric field. We construct the $Γ_3$ doublet state of the electrons with the total angular momentum $j=5/2$. By applying the second-order perturbation theory with respect to the intersite hopping, we derive the multipole interactions. We obtain a quadrupole interaction for a simple cubic lattice, an octupole interaction for a bcc lattice, and both quadrupole and octupole interactions for an fcc lattice. We also discuss general tendencies of the multipole interactio…
Electronic structure and electron correlations of the Hubbard model on the Beta-Mn lattice have been investigated on the basis of the momentum dependent local ansatz wavefunction method. It is found that the electrons on the Beta-Mn lattice are significantly correlated as compared with those on the face centered cubic (fcc) and the body centered cubic (bcc) lattices; the correlation energy gain of the Beta-Mn lattice structure is the largest among the Beta-Mn, the fcc, and the bcc structures, and the charge fluctuations show a significant suppression. In particular, it is found that the mass e…
We consider XY-spin degrees of freedom on an FCC lattice, such that the system respects some subsystem global symmetry. We then gauge this global symmetry and study the corresponding $U(1)$ gauge theory on the FCC lattice. Surprisingly, this $U(1)$ gauge theory is dual to the original spin system. We also analyze a similar $\mathbb{Z}_N$ gauge theory on that lattice. All these systems are fractonic. The $U(1)$ theories are gapless and the $\mathbb{Z}_N$ theories are gapped. We analyze the continuum limits of all these systems and present free continuum Lagrangians for their low-energy physics.…
The majority of fulleride superconductors with unusually high transition-temperature to kinetic-energy ratios have a face-centred-cubic (FCC) structure. We demonstrate that, within extended Hubbard models with strong Coulomb repulsion, paired fermions in FCC lattices have qualitatively different properties than pairs in other three-dimensional cubic lattices. Our results show that strongly bound, light, and small pairs can be generated in FCC lattices across a wide range of the parameter space. We estimate that such pairs can Bose condense at high temperatures even if the lattice constant is l…
We study the half-filled Hubbard model on the geometrically frustrated face centered cubic (FCC) lattice, using an auxiliary field based real space technique. The low temperature state is a paramagnetic metal at weak interaction, an antiferromagnetic insulator (AFI) with flux like order at intermediate interaction, and an AFI with `C type' order at very strong interaction. Remarkably, there is a narrow window between the paramagnetic metal and the AFI where the system exhibits spin glass behaviour arising from the presence of disordered but `frozen' local moments. The spin glass state is metal…
Geometrically Frustrated Quadrupoles on the Pyrochlore Lattice and Generalized Spin Liquids
Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Laboratoire Léon Brillouin, CEA, CNRS, Université Paris-Saclay（里昂·布里渊实验室，法国原子能和替代能源委员会，法国国家科学研究中心，巴黎萨克雷大学）；Université Grenoble Alpes, CNRS, Institut Néel（格勒诺布尔阿尔卑斯大学，法国国家科学研究中心，尼尔研究所）
Spin-orbit-entangled frustrated magnetism in fcc Ba$_2$(Yb,Nd)NbO$_6$ double perovskites
Shiv Nadar Institution of Eminence（Shiv Nadar卓越学院）；Bennett University（贝内特大学）；UGC-DAE Consortium for Scientific Research（UGC-DAE科学研究联盟）；Indian Institute of Science Education and Research, Thiruvananthapuram（印度科学教育与研究研究所，特里凡得琅）；Japan Atomic Energy Agency（日本原子能机构）
We establish the double perovskite Ba$_2$CeIrO$_6$ as a nearly ideal model system for j=1/2 moments, with resonant inelastic x-ray scattering indicating a deviation of less than 1% from the ideally cubic j=1/2 state. The local j=1/2 moments form an fcc lattice and are found to order antiferromagnetically at $T_N$=14K, more than an order of magnitude below the Curie-Weiss temperature. Model calculations show that the geometric frustration of the fcc Heisenberg antiferromagnet is further enhanced by a next-nearest neighbor exchange, indicated by ab initio theory. Magnetic order is driven by a bo…
We have studied long range orders of electric quadrupole moments described by an effective pseudospin-$\frac{1}{2}$ Hamiltonian representing pyrochlore magnets with non-Kramers ions under [111] magnetic field, in relevance to Tb$_{2}$Ti$_{2}$O$_{7}$. Order parameters and phase transitions of this frustrated system are investigated using classical Monte-Carlo simulations. In zero field, the model undergoes a first-order phase transition from a paramagnetic state to an ordered state with an antiparallel arrangement of pseudospins. This pseudospin order is characterized by the wavevector $\boldsy…
Possible order parameters of the phase IV in CexLa1-xB6 are discussed with special attention to the lattice distortion recently observed. A Γ_{5u}-type octupole order with finite wave number is proposed as the origin of the distortion along the [111] direction. The Γ_8 crystalline electric field (CEF) level splits into three levels by a mean field with the Γ_{5u} symmetry. The ground and highest singlets have the same quadrupole moment, while the intermediate doublet has an opposite sign. It is shown that any collinear order of Γ_{5u}-type octupole moment accompanies the Γ_{5g}-type ferro-quad…
DyB4 has a two-dimensional Shastry-Sutherland (Sh-S) lattice with strong Ising character of the Dy ions. Despite the intrinsic frustrations, surprisingly, it undergoes two successive transitions: a magnetic ordering at TN = 20K, and a quadrupole ordering at TQ=12.5 K. From high-resolution neutron and synchrotron X-ray powder diffraction studies, we have obtained full structural information on this material in all phases, and demonstrate that structural modifications occurring at quadrupolar transition lead to the lifting of frustrations inherent in the Sh-S model. Our study thus provides a com…
We report first principles calculations of the structural parameters and phonon dispersion of the tetragonal non-centrosymmetric heavy fermion compound CeAuAl$_3$. Taking into account weak magnetoelastic interactions of the rare-earth (RE) ions with the spectrum of phonons, we obtain an analytical expression for the hybridization of quadrupole excitations and phonons from the poles of the one-phonon Green-function. In the paramagnetic phase, we predict the formation of mixed modes that may be observed by inelastic neutron scattering. Our results show that magnetoelastic interactions, albeit be…
Nearest-neighbor Heisenberg antiferromagnet on a face-centered cubic lattice is studied by extensive Monte Carlo simulations in zero magnetic field. The parallel tempering algorithm is utilized, which allows to overcome a slow relaxation of the magnetic order parameter and fully equilibrate moderate size clusters with up to N ~ 7*10^3 spins. By collecting energy and order parameter histograms on clusters with up to N ~ 2*10^4 sites we accurately locate the first-order transition point at T_c=0.4459(1)J.
The Properties of the Mott insulator to superfluid phase transition are obtained through the fermionic approximation in the Jaynes-Cummings-Hubbard model on linear, square, SC, FCC, and BCC Bravais lattices. For varying excitation number and atom-cavity frequency detuning. We find that the Mott lobes and the critical hopping are not scalable only for the FCC lattice. At the large excitation number regime, the critical hopping is scalable for all the lattices and it does not depend on the detuning.
We investigate antiferro quadrupole orders in a diamond lattice under magnetic fields by Monte Carlo simulations for two types of classical effective models. One is an XY model with Z_3 anisotropy, and the other is a two-component phi^4 model with a third-order anisotropy. We confirm that the universality class of the zero-field transition is that for the three-dimensional XY model. Magnetic field corresponds to a Z_3 field in the effective model, and under this field, we find that collinear and canted antiferro-quadrupole orders compete. Each phase is characterized by symmetry breaking in the…
Magnetic Anisotropies and Skyrmion Lattice Related to Magnetic Quadrupole Interactions of the RKKY Mechanism in Frustrated Spin-Trimer System Gd$_{3}$Ru$_{4}$Al$_{12}$ with a Breathing Kagome Structure
In frustrated magnetic systems with competing interactions fluctuations can lift the residual accidental degeneracy. We argue that the state selection may have different outcomes for quantum and thermal order by disorder. As an example, we consider the semiclassical Heisenberg fcc antiferromagnet with only the nearest-neighbor interactions. Zero-point oscillations select the type 3 collinear antiferromagnetic state at T=0. Thermal fluctuations favor instead the type 1 antiferromagnetic structure. The opposite tendencies result in a finite-temperature transition between the two collinear states…
Huge deformations of the crystal lattice can be achieved in materials with inherent structural instability by epitaxial straining. By coherent growth on seven different substrates the in-plane lattice constants of 50 nm thick Fe70Pd30 films are continuously varied. The maximum epitaxial strain reaches 8,3 % relative to the fcc lattice. The in-plane lattice strain results in a remarkable tetragonal distortion ranging from c/abct = 1.09 to 1.39, covering most of the Bain transformation path from fcc to bcc crystal structure. This has dramatic consequences for the magnetic key properties. Magneto…
We report a study of the Mott insulator La$_2$O$_3$Fe$_2$Se$_2$ by means of $^{139}$La nuclear quadrupole resonance (NQR). The NQR spectra evidence a single La site in the paramagnetic phase and two inequivalent La sites, La1 and La2, in the antiferromagnetically-ordered phase (Néel temperature $T_{\rm{N}} \simeq 90$ K). These two sites are characterized by different quadrupole couplings, indicative of distinct lattice and/or charge configurations likely segregated in domains. The dependence of the quadrupole coupling for La2 on temperature suggests that the magnetic order parameter drives the…
