The inability of systems of interacting objects to satisfy all constraints simultaneously leads to frustration. A particularly important consequence of frustration is the ability to access certain protected parts of a system without disturbing the others. For magnets such "protectorates" have been inferred from theory and from neutron scattering, but their practical consequences have been unclear. We show that a magnetic analogue of optical hole-burning can address these protected spin clusters in a well-known, geometrically frustrated Heisenberg system, gadolinium gallium garnet. Our measurements additionally provide a resolution of a famous discrepancy between the bulk magnetometry and neutron diffraction results for this magnetic compound.
Frustrated magnetism plays a central role in the phenomenology of exotic quantum states. However, because the magnetic structures of frustrated systems are aperiodic, there has always been the problem that they cannot be determined using traditional crystallographic techniques. Here we show that the magnetic component of powder neutron scattering data is actually sufficiently information-rich to drive magnetic structure solution for frustrated systems, including spin ices, spin liquids, and molecular magnets. Consequently, single-crystal samples are not prerequisite for detailed characterisati…
By neutron scattering, we have studied the spin correlations and spin fluctuations in frustrated Laves hydrides, where magnetic disorder sets in the topologically frustrated Mn lattice. Below the transition towards short range magnetic order, static spin clusters coexist with fluctuating and alsmost uncorrelated spins. The magnetic response shows a complexe lineshape, connected with the presence of the magnetic inhomogeneities. Its analysis shows the existence of two different processes, relaxation and local excitations, for the spin fluctuations below the transition. The paramagnetic fluctuat…
The triangular lattice compound TlYbS$_2$ was prepared as large single crystals via a molten flux growth technique using sodium chloride. Anisotropic magnetic susceptibility measurements down to 0.4 K indicate a complete absence of long-range magnetic order. Despite this lack of long-range order, short-range antiferromagnetic interactions are evidenced through broad transitions, suggesting frustrated behavior. Variable magnetic field measurements reveal metamagnetic behavior at temperatures less than 2 K. Complex low temperature field-tunable magnetic behavior, in addition to no observable lon…
Based on measurements of soft x-ray magnetic scattering and symmetry considerations, we demonstrate that the magnetoelectric effect in TbMn$_2$O$_5$ arises from an internal field determined by $\vec{S}_{\vec{q}} \times {\vec{S}_{-\vec{q}}}$ with $\vec{S}_{\vec{q}}$ being the magnetization at modulation vector $\vec{q}$, whereas the magneto-elastic effect in the exchange energy governs the response to external electric fields. Our results set fundamental symmetry constraints on the microscopic mechanism of multiferroicity in frustrated magnets.
We study the spin-1 honeycomb lattice magnets with frustrated exchange interactions. The proposed microscopic spin model contains first and second neighbor Heisenberg interactions as well as the single-ion anisotropy. We establish a rich phase diagram that includes a featureless quantum paramagnet and various spin spiral states induced by the mechanism of order by quantum disorder. Although the quantum paramagnet is dubbed featureless, it is shown that, the magnetic excitations develop a contour degeneracy in the reciprocal space at the band minima. These contour degenerate excitations are res…
Spin wave dispersion in the frustrated fcc type-III antiferromagnet MnS$_2$ has been determined by inelastic neutron scattering using a triple-axis spectrometer. Existence of multiple spin wave branches, with significant separation between high-energy and low-energy modes highlighting the intrinsic magnetic frustration effect on the fcc lattice, is explained in terms of a spin wave analysis carried out for the antiferromagnetic Heisenberg model for this $S=5/2$ system with nearest and next-nearest-neighbor exchange interactions. Comparison of the calculated dispersion with spin wave measuremen…
Frustrated magnetic systems exhibit extraordinary physical properties but quantification of their magnetic correlations poses a serious challenge to experiment and theory. Current insight into frustrated magnetic correlations relies on modelling techniques such as reverse Monte Carlo methods, which require knowledge about the exact ordered atomic structure. Here we present a method for direct reconstruction of magnetic correlations in frustrated magnets by three-dimensional difference pair distribution function analysis of neutron total scattering data. The methodology is applied to the disord…
Dielectric and magnetic phenomena in spin and charge frustrated system RFe2O4 (R is a rare-earth metal ion) are studied. An electronic model for charge, spin and orbital degrees in a pair of triangular-lattice planes is derived. We analyze this model by utilizing the mean-field approximation and the Monte-Carlo simulation in a finite size cluster. A three fold-type charge ordered structure with charge imbalance between the planes is stabilized in finite temperatures. This polar charge order is reinforced by spin ordering of Fe ions. This novel magneto-dielectric phenomenon is caused by spin fr…
We have measured extremely large coercive magnetic fields of up to 55~T in Sr$_3$NiIrO$_6$, with a switched magnetic moment $\approx 0.8~μ_{\rm B}$ per formula unit. As far as we are aware, this is the largest coercive field observed thus far. This extraordinarily hard magnetism has a completely different origin from that found in conventional ferromagnets. Instead, it is due to the evolution of a frustrated antiferromagnetic state in the presence of strong magnetocrystalline anisotropy due to the overlap of spatially-extended Ir$^{4+}$ 5$d$ orbitals with oxygen 2$p$ and Ni$^{2+}$ 3$d$ orbital…
We have investigated the magnetic, dielectric and magnetodielectric (MDE) behavior of a geometrically frustrated spin-chain system, Ca3Co1.4Rh0.6O6, in the single crystalline form for different orientations. The results bring out that the magnetic behavior of this compound is by itself interesting in the sense that this compound exhibits an anisotropic glassy-like magnetic behavior with a huge frequency dependence of ac susceptibility peak for an orientation along the spin-chain in the range 30-60 K; this behavior is robust to applications of large external magnetic fields (H) unlike in canoni…
Noncollinear frustrated magnets are proposed as a new class of spintronic materials with high magnetoresistance which can be controlled with relatively small applied voltages. It is demonstrated that their magnetic configuration strongly depends on position of the Fermi energy and applied voltage. The voltage induced control of noncollinear frustrated materials (VCFM) can be seen as a way to intrinsic control of colossal magnetoresistance (CMR) and is the bulk material counterpart of spin transfer torque concept used to control giant magnetoresistance in layered spin-valve structures.
We study the impact of geometry on magnetostatically frustrated single-domain nanomagnet arrays. We examine square and hexagonal lattice arrays, as well as a brickwork geometry that combines the anisotropy of the square lattice and the topology of the hexagonal lattice. We find that the more highly frustrated hexagonal lattice allows for the most thorough minimization of the magnetostatic energy, and that the pair-wise correlations between moments differ qualitatively between hexagonal and brickwork lattices, although they share the same lattice topology. The results indicate that the symmetry…
We study the phase diagram of a frustrated spin-1/2 ferromagnetic chain with anisotropic exchange interactions in an external magnetic field, using the density matrix renormalization group method. We show that an easy-axis anisotropy enhances the tendency towards multimagnon bound states, while an easy-plane anisotropy favors chirally ordered phases. In particular, a moderate easy-plane anisotropy gives rise to a quantum phase transition at intermediate magnetization. We argue that this transition is related to the finite-field phase transition experimentally observed in the spin-1/2 compound …
The correct stacking of hexagonal layers is used to obtain accurate estimates for the exchange and anisotropy parameters of the geometrically-frustrated antiferromagnet CuFeO$_2$. Those parameters are highly constrained by the stability of a collinear metamagnetic phase between fields of 13.5 and 20 T. Constrained fits of the spin-wave frequencies of the collinear $\uudd $ phase below 7 T are used to identify the magnetic unit cell of the metamagnetic $\uuudd $ phase, which contains two hexagonal layers and 10 Fe$^{3+}$ spins.
Frustrated magnets are one class of fascinating materials that host many intriguing phases such as spin ice, spin liquid and complex long-range magnetic orderings at low temperatures. In this work we use first-principles calculations to find that in a wide range of magnetically frustrated oxides, at zero temperature a number of non-collinear magnetic orderings are more stable than the type-I collinear ordering that is observed at finite temperatures. The emergence of non-collinear orderings in those complex oxides is due to higher-order exchange interactions that originate from second-row and …
We report on the observation of a large topological Hall effect (THE) over a wide temperature region in a geometrically frustrated Fe3Sn2 magnet with a kagome-bilayer structure. We found that the magnitude of the THE resistivity increases with temperature and reaches -0.875 μΩ.cm at 380 K. Moreover, the critical magnetic fields with the change of THE are consistent with the magnetic structure transformation, which indicates that the real-space fictitious magnetic field is proportional to the formation of magnetic skyrmions in Fe3Sn2. The results strongly suggest that the large THE originates f…
We report magnetization and specific heat measurements on polycrystalline samples of BaCdVO(PO_4)_2 and show that this compound is a S=1/2 frustrated square lattice with ferromagnetic nearest-neighbor (J_1) and antiferromagnetic next-nearest-neighbor (J_2) interactions. The coupling constants J_1\simeq -3.6 K and J_2\simeq 3.2 K are determined from a fitting of the susceptibility data and confirmed by an analysis of the saturation field (H_s=4.2 T), the specific heat, and the magnetic entropy. BaCdVO(PO_4)_2 undergoes magnetic ordering at about 1 K, likely towards a columnar antiferromagnetic …
We report the low-temperature properties of SrNd$_2$O$_4$, a geometrically frustrated magnet. Magnetisation and heat capacity measurements performed on polycrystalline samples indicate the appearance of a magnetically ordered state at $T_{\rm N}=2.28(4)$~K. Powder neutron diffraction measurements reveal that an \afm\ state with the propagation vector \QV\ is stabilised below this temperature. The magnetic order is incomplete, as only one of the two Nd$^{3+}$ sites carries a significant magnetic moment while the other site remains largely disordered. The presence of a disordered magnetic compon…
Partially-ordered magnets are distinct from both spin liquids and conventional ordered magnets because order and disorder coexist in the same magnetic phase. Here, we determine the nature of partial order in the canonical frustrated pyrochlore antiferromagnet Gd$_2$Ti$_{2}$O$_{7}$. Using single-crystal neutron-diffraction measurements in applied magnetic field, magnetic symmetry analysis, inelastic neutron-scattering measurements, and spin-wave modeling, we show that its low-temperature magnetic structure involves two propagation vectors (2-$\mathbf{k}$ structure) with suppressed ordered magne…
Magnetism in single-side hydrogenated (C$_2$H) and fluorinated (C$_2$F) graphene is analyzed in terms of the Heisenberg model with parameters determined from first principles. We predict a frustrated ground state for both systems, which means the instability of collinear spin structures and sheds light on the absence of a conventional magnetic ordering in defective graphene demonstrated in recent experiments. Moreover, our findings suggest a highly correlated magnetic behavior at low temperatures offering the possibility of a spin-liquid state.
Competing magnetic interactions in geometrically frustrated magnets give rise to new forms of correlated matter, such as spin liquids and spin ices. Characterizing the magnetic structure of these states has been difficult due to the absence of long-range order. Here, we demonstrate that the spin Seebeck effect (SSE) is a sensitive probe of magnetic short-range order (SRO) in geometrically frustrated magnets. In low temperature (2 - 5 K) SSE measurements on a model frustrated magnet \mathrm{Gd_{3}Ga_{5}O_{12}}, we observe modulations in the spin current on top of a smooth background. By compari…
The structurally simplest high-temperature superconductor FeSe exhibits an intriguing superconducting nematic paramagnetic phase with unusual spin excitation spectra that are different from typical spin waves; thus, determining its effective magnetic exchange interactions is challenging. Here we report neutron scattering measurements of spin fluctuations of FeSe in the tetragonal paramagnetic phase. We show that the equal-time magnetic structure factor, $\mathcal{S}(\textbf{Q})$, can be effectively modeled using the self-consistent Gaussian approximation calculation with highly frustrated near…
We measured two magnetic modes with finite and discrete energies in an antiferromagnetic ordered phase of a geometrically frustrated magnet MgCr2O4 by single-crystal inelastic neutron scattering, and clarified the spatial spin correlations of the two levels: one is an antiferromagnetic hexamer and the other is an antiferromagnetic heptamer. Since these correlation types are emblematic of quasielastic scattering with geometric frustration, our results indicate instantaneous suppression of lattice distortion in an ordered phase by spin-lattice coupling, probably also supported by orbital and cha…
The skyrmions generated by frustration in centrosymmetric structures host extra internal degrees of freedom: vorticity and helicity, resulting in distinctive properties and potential functionality, which are not shared by the skyrmions stemming from the Dzyaloshinskii-Moriya interaction in noncentrosymmetric structures. The present work indicates that the magnetism-driven electric polarization carried by skyrmions provides a direct handle for tuning helicity. Especially for the in-plane magnetized skyrmions, the helicity can be continuously rotated and exactly picked by applying an external el…
The study of skyrmion/antiskyrmion motion in magnetic materials is very important in particular for the spintronics applications. In this work, we study the dynamics of isolated skyrmions and antiskyrmions in frustrated magnets driven by magnetic field gradient, using the Landau-Lifshitz-Gilbert simulations on the frustrated classical Heisenberg model on the triangular lattice. A Hall-like motion induced by the gradient is revealed in bulk system, similar to that in the well-studied chiral magnets. More interestingly, our work suggests that the lateral confinement in nano-stripes of the frustr…
Some strongly frustrated magnets such as the "spin-ice" compounds fail to produce any magnetic order at finite temperatures even in the presence of magnetic field. Still they have very unusual low-temperature thermodynamic properties related to the field-induced ground state transitions. Here we show that general qualitative picture of such peculiar thermodynamics can be obtained in the antiferromagnetic Ising model on the triangular Husimi lattice. The analytical results for this model show magnetic plateaus, entropy spikes, crossing points and peculiarities in magnetic susceptibility and spe…
Various and spontaneous magnetic skyrmionic bubbles are experimentally observed for the first time, at room temperature in a frustrated kagome magnet Fe3Sn2 with unixial magnetic anisotropy. The magnetization dynamics were investigated using in-situ Lorentz transmission electron microscopy, revealing that the transformation between different magnetic bubbles and domains are via the motion of Bloch lines driven by applied external magnetic field. The results demonstrate that Fe3Sn2 facilitates a unique magnetic control of topological spin textures at room temperature, making it a promising cand…
A magneto-optical survey was conducted for HgCr$_2$O$_4$ powder samples under pulsed high magnetic fields of up to 55 T. Intensity changes in magnetic fields observed for the exciton-magnon-phonon optical transition spectra coincide well with those of magnetization, lattice distortion from X-ray diffraction, and electron-magnetic resonances. The last-ordered phase was detected prior to the fully polarized magnetic phase, similarly to the other chromium spinel oxide, ZnCr$_2$O$_4$ and CdCr$_2$O$_4$.
Below its Néel temperature, the frustrated magnet CdCr$_2$O$_4$ exhibits an antiferromagnetic spin-spiral ground state. Such states can give rise to a sizable magnetoelectric coupling. In this report, we measure the electric polarization induced in single-crystalline CdCr$_2$O$_4$ by a large applied magnetic field. Because the detection of a macroscopic polarization is hindered by the structural domains in the tetragonal spin-spiral phase, we have pioneered an alternative method of measuring polarization induced by high magnetic fields, using electrostatic force microscopy. This method enables…
We have performed a combined study of magnetization hysteresis loops and time dependence of the magnetization in a broad temperature range for the ferrimagnetic La2Ni(Ni1/3Sb2/3)O6 double perovskite. This material has a ferrimagnetic order transition at ~100 K and at lower temperatures (~ 20 K) shows the signature of a frustrated state due to the presence of two competing magnetic exchange interactions. The temperature dependence of the coercive field shows an important upturn below the point where the frustrated state sets in. The use of the magnetization vs. applied magnetic field hysteresis…
We have searched nearly 40,000 inorganic solids in the Inorganic Crystal Structural Database to identify compounds containing a transition metal or rare earth kagomé sublattice, a geometrically magnetically frustrated lattice, ultimately identifying $\sim$500 materials. A broad analysis of the chemical and structural trends of these materials shows three types of kagomé sheet stacking and several classes of magnetic complexity. Following the search and classification, we rapidly screen the magnetic properties of a subset of the materials using density functional theory to eliminate those that …
We report the magnetic features of a new one-dimensional stack of antiferromagnetically coupled equilateral copper(II) triangles. High-field magnetization measurements show that the interaction between the copper triangles is of the same order of magnitude as the intra-triangle exchange although only coupled via hydrogen bonds. The infinite chain turns out to be an interesting example of a frustrated cylindrical three-leg ladder with competing intra- and inter-triangle interactions. We demonstrate that the ground state is a spin singlet which is gaped from the triplet excitation.
Helicity indicates the in-plane magnetic-moment swirling direction of a skyrmionic configuration. The ability to reverse the helicity of a skyrmionic bubble via purely electrical means has been predicted in frustrated magnetic systems, however its experimental observation has remained challenging. Here, we experimentally demonstrate the current-driven helicity reversal of the skyrmionic bubble in a nanostructured frustrated Fe3Sn2 magnet. The critical current density required to trigger the helicity reversal is 109 - 1010 A/m2, with a corresponding pulse-width varying from 1 μs to 100 ns. Comp…
A magnetic Skyrmion is a stable two-dimensional nanoparticle describing a localized winding of the magnetization in certain magnetic materials. Skyrmions are the subject of intense experimental and theoretical investigation and have potential technological spintronic applications. Here we show that numerical computations of frustrated magnets predict that Skyrmions can be tied into knots to form new stable three-dimensional nanoparticles. These stable equilibria of twisted loops of Skyrmion strings have an integer-valued topological charge, known as the Hopf charge, that counts the number of p…
