Using linear-response density-functional theory, we obtain the magnetic interactions in the several iron pnictides. The ground state has been found to be non-collinear in FeSe, with a large continuum of nearly degenerate states lying very close to the magnetic "striped" structure. The presence of non-collinearity also seems to be a generic feature of iron pnictides when the Fe moment is small. At small R_{Fe-Se} the system is itinerant: strong frustration give rise to excess of spin entropy, long ranged interactions create incommensurate orderings and strong biquadratic (or ring) couplings violate the applicability of Heisenberg model. There is a smooth transition to more localized behavior as R_{Fe-Se} increases: stable magnetic orbital order develops which favor long range AFM stripe ordering with strongly anisotropic in-plane exchange couplings. The stabilization of the stripe magnetic order is accompanied by the inversion of the exchange coupling.
The substitution of zinc for iron in YBaFe4O7 has allowed the oxide series YBaFe4-xZnxO7, with 0.40 < x < 1.50, belonging to the "114" structural family to be synthesized. These oxides crystallize in the hexagonal symmetry (P63mc), as opposed to the cubic symmetry (F-43m) of YBaFe4O7. Importantly, the d.c. magnetization shows that the zinc substitution induces ferrimagnetism, in contrast to the spin glass behaviour of YBaFe4O7. Moreover, a.c. susceptibility measurements demonstrate that concomitantly these oxides exhibit a spin glass or a cluster glass behaviour, which increases at the expense…
We consider a dynamical generalization of the Eshelby problem: the strain profile due to an inclusion or "defect" in an isotropic elastic medium. We show that the higher the oscillation frequency of the defect, the more localized is the strain field around the defect. We then demonstrate that the qualitative nature of the interaction between two defects is strongly dependent on separation, frequency and direction, changing from "ferromagnetic" to "antiferromagnetic" like behavior. We generalize to a finite density of defects and show that the interactions in assemblies of defects can be mapped…
The effects of electron doping and phonon vibrations on the magnetic properties of monolayer and bilayer FeSe epitaxial films on SrTiO$_3$ have been studied, respectively, using first-principles calculations with van der Waals correction. For monolayer FeSe epitaxial film, the combined effect of electron doping and phonon vibrations readily leads to magnetic frustration between the collinear antiferromagnetic state and the checkerboard antiferromagnetic Néel state. For bilayer FeSe epitaxial film, such magnetic frustration is much more easily induced by electron doping in its bottom layer than…
Frustration of magnetic systems which is caused by competing interactions is the driving force of several unusual phenomena such as plateaus and jumps of the magnetization curve as well as of unusual energy spectra with for instance many singlet levels below the first triplet state. The antiferromagnetic cuboctahedron can serve as a paradigmatic example of certain frustrated antiferromagnets. In addition it has the advantage that its complete energy spectrum can be obtained up to individual spin quantum numbers of s=3/2 (16,777,216 states).
We present a detailed investigation of the magnetic properties of complex vanadium phosphates M(VO)2(PO4)2 (M = Ca, Sr) by means of magnetization, specific heat, 31P NMR measurements, and band structure calculations. Experimental data evidence the presence of ferro- and antiferromagnetic interactions in M(VO)2(PO4)2 resulting in a nearly vanishing Curie-Weiss temperature θ_{CW} < 1 K that contrasts with the maximum of magnetic susceptibility at 3 K. Specific heat and NMR measurements also reveal weak exchange couplings with the thermodynamic energy scale J_c = 10-15 K. Additionally, the reduce…
We study the effects of frustration in an antiferromagnetic film of FCC lattice with Heisenberg spin model including an Ising-like anisotropy. Monte Carlo (MC) simulations have been used to study thermodynamic properties of the film. We show that the presence of the surface reduces the ground state (GS) degeneracy found in the bulk. The GS is shown to depend on the surface in-plane interaction $J_s$ with a critical value at which ordering of type I coexists with ordering of type II. Near this value a reentrant phase is found. Various physical quantities such as layer magnetizations and layer s…
We present an element selective resonant magnetic x-ray scattering study of NdFe3(BO3)4 as a function of temperature and applied magnetic field. Our measurements show that the magnetic order of the Nd sublattice is induced by the Fe spin order. When a magnetic field is applied parallel to the hexagonal basal plane, the helicoidal spin order is suppressed and a collinear ordering, where the moments are forced to align in a direction perpendicular to the applied magnetic field, is stabilized. This result excludes a non-collinear spin order as the origin of the magnetically induced electric polar…
Ultrasound velocity measurements of cubic spinel GeCo$_2$O$_4$ in single crystal were performed for the investigation of shear and compression moduli. The shear moduli in the paramagnetic state reveal an absence of Jahn-Teller activity despite the presence of orbital degeneracy in the Co$^{2+}$ ions. Such a Jahn-Teller inactivity indicates that the intersite orbital-orbital interaction is much stronger than the Jahn-Teller coupling. The compression moduli in the paramagnetic state near the N$\acute{e}$el temperature $T_N$ reveal that the most relevant exchange path for the antiferromagnetic tr…
In the triangular layered magnet PdCrO2 the intralayer magnetic interactions are strong, however the lattice structure frustrates interlayer interactions. In spite of this, long-range, 120$^\circ$ antiferromagnetic order condenses at $T_N = 38$~K. We show here through neutron scattering measurements under in-plane uniaxial stress and in-plane magnetic field that this occurs through a spontaneous lifting of the three-fold rotational symmetry of the nonmagnetic lattice, which relieves the interlayer frustration. We also show through resistivity measurements that uniaxial stress can suppress ther…
It is argued that the magnetic behavior of Sr$_2$MnMoO$_6$ is determined by the existence of two total energy minima corresponding to the metallic ferromagnetic and insulating antiferromagnetic states, which may be nearly degenerate depending on the magnitude of the breathing distortion.
The Cairo pentagonal lattice, consisting of an irregular pentagonal tiling of magnetic ions on two inequivalent sites (3- and 4-co-ordinated ones), represents a fascinating example for studying geometric frustration effects in two-dimensions. In this work, we investigate the spin $S$ = $1/2$ Cairo pentagonal lattice with respect to selective exchange coupling (which effectively corresponds to a virtual doping of $x$ = $0, 1/6, 1/3$), in a nearest-neighbour antiferromagnetic Ising model. We also develop a simple method to quantify geometric frustration in terms of a frustration index $ϕ(β,T)$, …
CrN is observed to undergo a paramagnetic to antiferromagnetic transition accompanied by a shear distortion from cubic NaCl-type to orthorhombic structure. Our first-principle plane wave and ultrasoft pseudopotential calculations confirm that the distorted antiferromagnetic phase with spin configuration arranged in double ferromagnetic sheets along [110] is the most stable. Antiferromagnetic ordering leads to a large depletion of states around Fermi level, but it does not open a gap. Simultaneous occurence of structural distortion and antiferromagnetic order is analyzed.
We have studied the magnetic configuration in ultrathin antiferromagnetic Mn films grown around monoatomic steps on an Fe(001) surface by spin-polarized scanning tunneling microscopy/spectroscopy and ab-initio-parametrized self-consistent real-space tight binding calculations in which the spin quantization axis is independent for each site thus allowing noncollinear magnetism. Mn grown on Fe(001) presents a layered antiferromagnetic structure. In the regions where the Mn films overgrows Fe steps the magnetization of the surface layer is reversed across the steps. Around these defects a frustra…
We study the electronic and magnetic structures of the newly-discovered compound KCr$_3$As$_3$. The non-magnetic state has five Fermi surface sheets involving respectively three quasi-one-dimensional and two three-dimensional energy bands. However, the ground state is magnetic, exhibiting a novel interlayer antiferromagnetic order where the basic block-spin state of a unit Cr triangle retains a high spin magnitude. Moreover, its Fermi surface involves three one-dimensional sheets only, providing evidence for local moments in this compound due to the reduced dimensionality. By fitting a twisted…
We systematically derive low-energy effective Hamiltonians for molecular solids $β^\prime$-$X$[Pd(dmit)$_{2}$]$_{2}$ ($X$ represents a cation) using ab initio density functional theory calculations and clarify how the cation controls the inter-dimer transfer integrals and the interaction parameters. The effective models are solved using the exact diagonalization method and the antiferromagnetic ordered moment is shown to be significantly suppressed around the spin-liquid candidate of $X$=EtMe$_{3}$Sb, which is reported in experiments. We also show that both the geometrical frustration and the …
A detailed study of poly- and single crystalline samples of the normal spinel HgCr2S4 is reported. The structural refinement reveals enhanced values of the atomic displacements suggesting closeness to a structural instability. Magnetization, electron-spin resonance and specific-heat studies document strong ferromagnetic fluctuations close to 50 K and the occurrence of complex antiferromagnetic order at TN = 22 K. We found highly unconventional behavior resembling properties of a non-collinear antiferromagnet and soft ferromagnet dependent on temperature and magnetic field. Even weak external m…
Based on experimental observations in A{x}MO{2} (A = Na, Li; M = Co, Ni), a model for suppression of magnetic frustration by electron doping in a nearest-neighbour antiferromagnetic triangular lattice is presented. It is found that frustration can be quantified, as determined by geometry and bond-counting, and its magnitude is a non-monotonic function of $x$. A mean-field calculation provides temperature-dependent magnetization, spin-entropy and heat capacity. Low-doping (x = 0.25, 0.33) results in a highly frustrated regime. A{0.5}MO{2} has strongest order and no frustration, while high dopin…
We present neutron diffraction, magnetic susceptibility and specific heat data for a single-crystal sample of the cubic (Cu3Au structure) compound Pr3In. This compound is believed to have a singlet (Gamma1) groundstate and a low-lying triplet (Gamma4) excited state. In addition, nearest-neighbor antiferromagnetic interactions are frustrated in this structure. Antiferromagnetic order occurs below T_N = 12K with propagation vector (0, 0, 0.5 +/-δ) where δ\approx 1/12. The neutron diffraction results can be approximated with the following model: ferromagnetic sheets from each of the three Pr site…
We report on the emergence of antiferromagnetic spin chains from two-dimensionally aligned spins on the anisotropic triangular lattice (ATL) in the insulating calcium rhenium oxychloride Ca3ReO5Cl2. The compound contains Re6+ ions each with one unpaired electron in the dxy orbital, which are arranged to form a spin-1/2 ATL with J'/J ~ 0.32 and J = 41 K, where J and J' are magnetic interactions in and between the chains, respectively. In spite of the apparent two dimensionality, we observe clear evidence of a gapless spin liquid that is characteristic of the spin-1/2 Heisenberg chain. This one-…
Polycrystalline Al7+xFe23Ge14-x-type orthorhombic Al8.5-xFe23Ge12.5+x (0<=x<=3) compounds were studied by X-ray diffraction measurement, metallographic examination, and magnetization and electrical resistivity measurements. The lattice parameters show anisotropic x dependences, reflecting a lower symmetry of rather complex crystal structure. In the x=0 sample, a ferromagnetic (FM) transition occurs at the Curie temperature TC of 255 K, which is systematically reduced with increasing x and disappears at x=2.5 where an antiferromagnetic (AFM) ground state is realized. The Neel temperature TN see…
Magnetic frustration, arising from the competition of exchange interactions, has received great attention because of its relevance to exotic quantum phenomena in materials. In the current work, we report an unusual checkerboard-shaped scattering anomaly in $\rm FeGe_2$, far from the known incommensurate magnetic satellite peaks, for the first time by inelastic neutron scattering. More surprisingly, such phenomenon appears as spin dynamics at low temperature, but it becomes prominent above Néel transition as elastic scattering. A new model Hamiltonian that includes an intraplane next-nearest ne…
Although the magnetic order is suppressed by a strong magnetic frustration, it is maintained but appears in complex order forms such as a cycloid or spin density wave in weakly frustrated systems. Herein, we report a weakly magnetic-frustrated two-dimensional van der Waals material CrPSe$_3$. Polycrystalline CrPSe$_3$ was synthesized at an optimized temperature of 700$^\circ$C to avoid the formation of any secondary phases (e.g., Cr$_2$Se$_3$). The antiferromagnetic transition appeared at $T_N\sim 126$ K with a large Curie-Weiss temperature $T_{\rm CW} \sim -371$ via magnetic susceptibility me…
Many technological applications of multiferroics are based on their ability to reconstruct the domain structure (DS) under the action of small external fields. In the present paper we analyze the different scenarios of the DS behavior in a multiferroic that shows simultaneously ferro- and antiferromagnetic ordering on the different systems of magnetic ions. We consider the way to control a composition of the DS and macroscopic properties of the sample by an appropriate field treatment. We found out that sensitivity of the DS to the external magnetic field and the magnetic susceptibility in a l…
Heat-capacity (C) and ac susceptibility measurements have been performed on the spin-chain compounds, Sr3ZnRhO6 and Ca3NiMnO6, to establish their magnetic behavior and to explore whether there are magnetic frustration effects due to antiferromagnetic coupling of the chains arranged in a triangular fashion. While the paramagnetic Curie temperatures have been known to be large with a negative sign, as though antiferromagnetic interaction is very strong, the results establish that (i) the former apparently undergoes inhomogeneous magnetic ordering only around 15 K, however without spin-glass anom…
The comparative study of the substitution of zinc and lithium for iron in the "114" ferrites, YBaFe4O7 and CaBaFe4O7, shows that these diamagnetic cations play a major role in tuning the competition between ferrimagnetism and magnetic frustration in these oxides. The substitution of Li or Zn for Fe in the cubic phase YBaFe4O7 leads to a structural transition to a hexagonal phase YBaFe4-xMxO7, for M = Li (0.30 < x < 0.75) and for M = Zn (0.40 < x < 1.50). It is seen that for low doping values i.e. x = 0.30 (for Li) and x = 0.40 (for Zn), these diamagnetic cations induce a strong ferrimagnetic c…
Frustration, or the competition between interacting components of a network, is often responsible for the complexity of many body systems, from social and neural networks to protein folding and magnetism. In quantum magnetic systems, frustration arises naturally from competing spin-spin interactions given by the geometry of the spin lattice or by the presence of long-range antiferromagnetic couplings. Frustrated magnetism is a hallmark of poorly understood systems such as quantum spin liquids, spin glasses and spin ices, whose ground states are massively degenerate and can carry high degrees o…
The macroscopic magnetic characterization of the Mn(II) - nitronyl nitroxide free radical chain (Mn(hfac)2(R)-3MLNN) evidenced its transition from a 1-dimensional behavior of ferrimagnetic chains to a 3-dimensional ferromagnetic long range order below 3 K. Neutron diffraction experiments, performed on a single crystal around the transition temperature, led to a different conclusion : the magnetic Bragg reflections detected below 3 K correspond to a canted antiferromagnet where the magnetic moments are mainly oriented along the chain axis. Surprisingly in the context of other compounds in this …
We present the crystal structure and magnetic properties of Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$, a stoichiometric frustrated quantum spin system with slightly distorted kagome layers. Single crystals of Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$ were grown under hydrothermal conditions. The structure was determined from single crystal X-ray diffraction and confirmed by neutron powder diffraction. The observed structure reveals two different Cu-positions leading to a slightly distored kagome layer in contrast to the closely related YCu$_{3}$(OH)$_{6}$Cl$_{3}$. Curie-Weiss behavior at high-temperatures w…
Macroscopic properties of multiferroics, the systems that show simultaneously two types of ordering, could be controlled by the external fields of different nature. We analyze the behavior of multiferroics with antiferro-(AFM) and ferromagnetic (FM) ordering under the action of external magnetic and stress fields. A combination of these two fields makes it possible to achieve macroscopic states with different domain structures. The two-domain state obtained in this way shows a linear dependence of macroscopic strain vs magnetic field which is unusual for AFMs. A small but nonzero stress applie…
How does magnetism behave when the physical dimension is reduced to the size of nanostructures? The multiplicity of magnetic states in these systems can be very rich, in that their properties depend on the atomic species, the cluster size, shape and symmetry or choice of the substrate. Small variations of the cluster parameters may change the properties dramatically. Research in this field has gained much by the many novel experimental methods and techniques exhibiting atomic resolution. Here I review the ab-initio approach, focusing on recent calculations on magnetic frustration and occurrenc…
Mechanical metamaterials present a promising platform for seemingly impossible mechanics. They often require incompatibility of their elementary building blocks, yet a comprehensive understanding of its role remains elusive. Relying on an analogy to ferromagnetic and antiferromagnetic binary spin interactions, we present a universal approach to identify and analyze topological mechanical defects for arbitrary building blocks. We underline differences between two- and three-dimensional metamaterials, and show how topological defects can steer stresses and strains in a controlled and non-trivial…
Ultrasound velocity measurements of the orbitally-frustrated GeCo$_2$O$_4$ reveal unusual elastic instabilities due to the phonon-spin coupling within the antiferromagnetic phase. Shear moduli exhibit anomalies arising from the coupling to short-range ferromagnetic excitations. Diplike anomalies in the magnetic-field dependence of elastic moduli reveal magnetic-field-induced orbital order-order transitions. These results strongly suggest the presence of geometrical orbital frustration which causes novel orbital phenomena within the antiferromagnetic phase.
