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At least 19 records

Codimension-two spiral spin liquid in the effective honeycomb-lattice compound Cs 3 ⁢Fe 2 ⁢Cl 9

A codimension-two spiral spin liquid is a correlated paramagnetic state with one-dimensional ground state degeneracy hosted within a three-dimensional lattice. Here, in this work, via neutron scattering experiments and numerical simulations, we establish the existence of a codimension-two spiral spin liquid in the effective honeycomb-lattice compound Cs 3 ⁢Fe 2⁢ Cl 9 , which demonstrates an alternate path to spiral spin liquids by overcoming the long-standing impediment of weak further-neighbor interactions. In the long-range ordered regime, competing spiral and spin density wave orders emerge as a function of applied magnetic field, among which a possible order-by-disorder transition is identified.

Monte Carlo methods↗

Line-Graph Approach to Spiral Spin Liquids

Competition among exchange interactions is able to induce novel spin correlations on a bipartite lattice without geometrical frustration. A prototype example is the spiral spin liquid, which is a correlated paramagnetic state characterized by subdimensional degenerate propagation vectors. Here, using spectral graph theory, we show that spiral spin liquids on a bipartite lattice can be approximated by a further-neighbor model on the corresponding line-graph lattice that is nonbipartite, thus broadening the space of candidate materials that may support the spiral spin liquid phases. As examples, we examine neutron scattering experiments performed on two spinel compounds, ZnCr 2 Se 4 and CuInCr 4 Se 8 , to demonstrate the feasibility of this new approach and expose its possible limitations in experimental realizations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Observation of the spiral spin liquid in a triangular-lattice material

The spiral spin liquid (SSL) is a highly degenerate state characterized by a continuous contour or surface in reciprocal space spanned by a spiral propagation vector. Although the SSL state has been predicted in a number of various theoretical models, very few materials are so far experimentally identified to host such a state. Via combined single-crystal wide-angle and small-angle neutron scattering, we report observation of the SSL in the quasi-two-dimensional delafossite-like AgCrSe 2 . We show that it is a very close realization of the ideal Heisenberg J 1 –J 2 –J 3 frustrated model on the triangular lattice. By supplementing our experimental results with microscopic spin-dynamics simulations, we demonstrate how such exotic magnetic states are driven by thermal fluctuations and exchange frustration.

36 MATERIALS SCIENCE↗

Incommensurate Spiral Spin Order in CaMn 2 Bi 2 Observed via High-Pressure Neutron Diffraction

Here, high-pressure neutron diffraction is employed to investigate the magnetic behavior of CaMn 2 Bi 2 in extreme conditions. In contrast to antiferromagnetic ordering on Mn atoms reported at ambient pressure, our results reveal that at high pressure, incommensurate spiral spin order emerges due to the interplay between magnetism on the Mn atoms and strong spin–orbit coupling on the Bi atoms: sinusoidal spin order is observed at pressures as high as 7.4 GPa. First-principles calculations with a noncollinear spin orientation demonstrate band crossing behavior near the Fermi level as a result of strong hybridization between the d orbitals of Mn and the p orbitals of Bi atoms. Competing antiferromagnetic order is observed at different temperatures in the partially frustrated lattice. Theoretical models have been developed to investigate spin dynamics. This research provides a unique toolbox for conducting experimental and theoretical magnetic and spin dynamics studies of magnetic quantum materials via high-pressure neutron diffraction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spiral spin cluster in the hyperkagome antiferromagnet Mn 3 RhSi

Local spin correlation orders emerge in a paramagnetic state, with notable examples such as the partial order, cooperative paramagnetism, and soliton spin liquid. The noncentrosymmetric intermetallic antiferromagnet Mn 3 RhSi also exhibits the local spin correlation order in the paramagnetic state as magnetic short-range order in a wide temperature range. Here, we show that the local spin correlation order has a spiral structure by neutron scattering measurement of a Mn 3 RhSi single crystal. The possible origins of the magnetic cluster formation are discussed in terms of the Lifshitz invariant and the Griffiths phase, and compared with the room-temperature skyrmion phase of Co 7 Zn 7 Mn 6 and non-Fermi liquid behavior of β-Mn.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Shear–Mediated Stabilization of Spin Spiral Order in Multiferroic NiI 2

Type-II multiferroicity from non-collinear spin order is recently explored in the van der Waals material NiI 2 . Despite the importance for improper ferroelectricity, the microscopic mechanism of the helimagnetic order remains poorly understood. Here, the magneto-structural phases of NiI 2 are investigated using resonant magnetic X-ray scattering (RXS) and X-ray diffraction. Two competing magnetic phases are identified. Below 60 K, an incommensurate magnetic reflection (q ≈ [0.143,0,1.49] reciprocal lattice units) is observed which exhibits finite circular dichroism in RXS, signaling the inversion symmetry-breaking helimagnetic ground state. At elevated temperature, in the non-polar phase (60 K < T < 75 K), a distinct q ≈ [0.087,0.087,1.5] magnetic order is observed, attributed to a collinear incommensurate (CI) state. The first-order CI-helix transition is concomitant with a structural transition characterized by a significant interlayer shear, which drives the helimagnetic ground state as evidenced by a mean-field Heisenberg model including interlayer exchange and its coupling to the structural distortion. Furthermore, these findings identify interlayer magneto-structural coupling as the key driver behind multiferroicity in NiI 2 .

36 MATERIALS SCIENCE↗

Signatures of polarized chiral spin disproportionation in rare earth nickelates

In rare earth nickelates (RENiO 3 ), electron-lattice coupling drives a concurrent metal-to-insulator and bond disproportionation phase transition whose microscopic origin has long been the subject of active debate. Of several proposed mechanisms, here we test the hypothesis that pairs of self-doped ligand holes spatially condense to provide local spin moments that are antiferromagnetically coupled to Ni spins. These singlet-like states provide a basis for long-range bond and spiral spin order. Using magnetic resonant X-ray scattering on NdNiO 3 thin films, we observe the chiral nature of the spin disproportionated state, with spin spirals propagating along the crystallographic (101) ortho direction. These spin spirals are found to preferentially couple to X-ray helicity, establishing the presence of a hitherto-unobserved macroscopic chirality. The presence of this chiral magnetic configuration suggests a potential multiferroic coupling between the noncollinear magnetic arrangement and improper ferroelectric behavior as observed in prior studies on NdNiO 3 (101) ortho films and RENiO 3 single crystals. Experimentally constrained theoretical double-cluster calculations confirm the presence of an energetically stable spin-disproportionated state with Zhang-Rice singlet-like combinations of Ni and ligand moments

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Atomic-Scale Modulation of Synthetic Magnetic Order in Oxide Superlattices

We report atomic-scale precision control of magnetic interactions facilitates a synthetic spin order useful for spintronics, including advanced memory and quantum logic devices. Conventional modulation of synthetic spin order has been limited to metallic heterostructures that exploit Ruderman–Kittel–Kasuya–Yosida interaction through a nonmagnetic metallic spacer; however, they face issues arising from Joule heating and/or electric breakdown. The practical realization and observation of a synthetic spin order across a nonmagnetic insulating spacer will lead to the development of spin-related devices with a completely different concept. Herein, the atomic-scale modulation of the synthetic spiral spin order in oxide superlattices composed of ferromagnetic metal and nonmagnetic insulator layers is reported. The atomically controlled superlattice exhibits an oscillatory magnetic behavior, representing the existence of a spiral spin structure. Depth-sensitive polarized neutron reflectometry evidences modulated spiral spin structures as a function of the nonmagnetic insulator layer thickness. Atomic-scale customization of the spin state can move the field one step further to actual spintronic applications.

74 ATOMIC AND MOLECULAR PHYSICS↗

Electrical switching of a p-wave magnet

Magnetic states with zero magnetization but non-relativistic spin splitting are outstanding candidates for the next generation of spintronic devices. Their electronvolt (eV)-scale spin splitting, ultrafast spin dynamics and nearly vanishing stray fields make them particularly promising for several applications. A variety of such magnetic states with non-trivial spin textures have been identified recently, including even-parity d-wave, g-wave or i-wave altermagnets and odd-parity p-wave magnets. Achieving voltage-based control of the non-uniform spin polarization of these magnetic states is of great interest for realizing energy-efficient and compact devices for information storage and processing. Spin-spiral type II multiferroics are optimal candidates for such voltage-based control, as they exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization, allowing for symmetry-protected cross-control between spin chirality and polar order. Here we combine photocurrent measurements, first-principles calculations and group-theory analysis to provide direct evidence that the spin polarization of the spin-spiral type II multiferroic NiI 2 exhibits odd-parity character connected to the spiral chirality. The symmetry-protected coupling between chirality and polar order enables electrical control of a primarily non-relativistic spin polarization. Our findings represent an observation of p-wave magnetism in a spin-spiral type II multiferroic, which may lead to the development of voltage-based switching of non-relativistic spin polarization in compensated magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Self-selecting vapor growth of transition-metal-halide single crystals

Transition-metal halides can host a large variety of novel phenomena, such as magnetism in the monolayer limit, quantum spin liquid and spiral spin liquid states, topological magnons, and chiral phonons. Sizable high-quality single crystals are necessary for investigations of magnetic and lattice excitations by, for example, inelastic neutron scattering. In this paper, we review a less well-known vapor transport technique, self-selecting vapor growth, and report our growths of transition-metal halides using this technique. We report the growth and characterizations of sizable single crystals of α–RuCl 3 , CrCl 3 , Ru 1–x Cr x Cl 3 , and CrBr 3 . In order to expedite the conversion of starting powder to single crystals, we modified the technique by cooling the growth ampoule through an appropriate temperature range. Our work shows that the self-selecting vapor transport technique can provide large single crystals of transition-metal halides, demonstrating its potential for providing high-quality single crystals of quantum materials.

2-dimensional systems↗

Anomalous Hall effect in conical helimagnetic crystals

Spin-spiral texture can substantially change charge transport properties in helimagnets. Here we find the anomalous Hall effect (AHE) exhibiting the dramatic behavior with respect to chemical potential μ in conical magnetic structures. The direct conductivity demonstrates kinks, and the anomalous Hall current exhibits minima and maxima changing the sign. We analytically derive the expression for energy bands and eigenstates in the most general case. Because of the conical potential, the energy bands are split into two nonparabolic bands where the lower band can have one- or two-minima shapes in the k z direction ($\hat{z}$ is a direction of the spiral axis). We prove that the origin of the anomalous Hall effect is not topological and is due to the interplay between the asymmetry of energy bands in the x and z directions and spin restrictions in the phase space due to the conical potential. We also investigate the dependence of transport properties on cone half- angle θ, and find that the effects are most pronounced at θ=π/2 (a helical state). Electric current is calculated using the Boltzmann equation where the relaxation is caused by electron-acoustic phonon interaction. The transition probability is found to be a 2×2 matrix with nonvanishing off-diagonal elements indicating the strong interband transitions. The origin of interband transitions is because of the nature of the conical potential where conduction electron spins interact with localized magnetic moments. To verify the proposed theory, we calculate the temperature dependence of resistivity for MnSi crystals and find the discontinuity at the phase transition between conical and paramagnetic phases. The calculations are in the excellent agreement with the experimental data. In addition, we predict the discontinuity behavior for the anomalous Hall resistivity at the phase transition where the resistivity exhibits the abrupt change at T=T C , (a) to zero if the relativistic effects for the conduction electrons are small or (b) to a nonzero value if Rashba/Dresselhaus effects are taken into account.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Competing magnetic phases in Li-Fe-Ge kagome systems

Competing interlayer magnetic interactions in kagome magnets can lead to diverse magnetic phases, which enable promising topological or quantum material properties. In this work, the electronic structure and magnetic properties are studied using first-principles calculations for the Li⁢Fe6⁢G⁡e6, Li⁢Fe6⁢G⁡e4, and Li⁢Fe6⁢G⁡e5 compounds sharing the kagome F⁡e3⁢Ge layer motif but with different interlayer arrangements. For Li⁢Fe6⁢G⁡e4 and Li⁢Fe6⁢G⁡e5, the predicted magnetic ground states are collinear antiferromagnetic (AFM) states involving a mix of ferromagnetic (FM) and AFM interlayer orientations. In contrast, for Li⁢Fe6⁢G⁡e6, an incommensurate cycloidal spin spiral ground state is stabilized, although its energy is close to a collinear A-type AFM state. The analysis of magnetic RKKY exchange coupling confirms the results of calculations. The values of atomic magnetic moments are in good agreement with existing experimental estimations. Our experiments on Li⁢Fe6⁢G⁡e6 single crystals reveals AFM ordering at ∼540 K and transition to another magnetic phase with a small FM component, possibly with spin canting, below ∼270 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The theory of transport in helical spin-structure crystals

Abstract We study helical structures in spin-spiral single crystals. In the continuum approach for the helicity potential energy the simple electronic band splits into two non-parabolic bands. For low exchange integrals, the lower band is described by a surface with a saddle shape in the direction of the helicity axis. Using the Boltzmann equation with the relaxation due to acoustic phonons, we discover the dependence of the current on the angle between the electric field and helicity axis leading to the both parallel and perpendicular to the electric field components in the electroconductivity. The latter can be interpreted as a planar Hall effect. In addition, we find that the transition rates depend on an electron spin allowing the transition between the bands. The electric conductivities exhibit nonlinear behaviors with respect to chemical potential µ . We explain this effect as the interference of the band anisotropy, spin conservation, and interband transitions. The proposed theory with the spherical model in the effective mass approximation for conduction electrons can elucidate nonlinear dependencies that can be identified in experiments. We find the excellent agreement between the theoretical and experimental data for parallel resistivity depending on temperature at the phase transition from helical to ferromagnetic state in a M n P single crystal. In addition, we predict that the perpendicular resistivity abruptly drops to zero in the ferromagnetic phase.

Physics↗

Switching the spin cycloid in BiFeO3 with an electric field

Abstract Bismuth ferrite (BiFeO 3 ) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO 3 are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements. Using nitrogen vacancy-based diamond magnetometry, we observe the magnetic spin cycloid structure of BiFeO 3 in real space. This structure is magnetoelectrically coupled through symmetry to the ferroelectric polarization and this relationship is maintained through electric field switching. Through a combination of in-plane and out-of-plane electrical switching, coupled with ab initio studies, we have discovered that the epitaxy from the substrate imposes a magnetoelastic anisotropy on the spin cycloid, which establishes preferred cycloid propagation directions. The energy landscape of the cycloid is shaped by both the ferroelectric degree of freedom and strain-induced anisotropy, restricting the spin spiral propagation vector to changes to specific switching events.

36 MATERIALS SCIENCE↗

CrRhAs: a member of a large family of metallic kagome antiferromagnets

Abstract Kagome lattice materials are an important platform for highly frustrated magnetism as well as for a plethora of phenomena resulting from flat bands, Dirac cones and van Hove singularities in their electronic structures. We study the little known metallic magnet CrRhAs, which belongs to a vast family of materials that includes 3 d , 4 f , and 5 f magnetic elements, as well as numerous nonmagnetic metals and insulators. Using noncollinear spin density functional calculations (mostly spin spirals), we extract a model magnetic Hamiltonian for CrRhAs. While it is dominated by an antiferromagnetic second nearest neighbor coupling in the kagome plane, the metallic nature of the compound leads to numerous nonzero longer range couplings and to important ring exchange terms. We analyze this Hamiltonian and find unusual ground states which are dominated by nearly isolated antiferromagnetic triangles that adopt 120 ∘ order either with positive or with negative vector chirality. We discuss the connection to the few known experimental facts about CrRhAs. Finally, we give a brief survey of other interesting magnetic members of this family of kagome compounds.

36 MATERIALS SCIENCE↗

Small Co-doping induced magnetic and electrical transitions in single crystal CaF⁢e 0.95 ⁢C⁢o 0.05 ⁢O 3

CaFe⁢O 3 and CaF⁢e 0.95 ⁢C⁢o 0.05 ⁢O 3 single crystals were grown by combing floating-zone method with high oxygen pressure treatment. Both crystals show charge disproportionation of Fe (F⁡e 4+ → F⁡e 3+ + F⁡e 5+ ) accompanied by a metal-to-insulator transition as well as a crystal structural transformation from Pbnm to 𝑃⁢2 1 /𝑛. However, the slight introduction of Co significantly suppresses the critical temperature of charge disproportionation from 290 K in CaFe⁢O 3 to 260 K in CaF⁢e 0.95 ⁢C⁢o 0.05 ⁢O 3 . Different from the single antiferromagnetic phase transition as observed in the polycrystalline CaFe⁢O 3 , two sequential antiferromagnetic transitions are found to occur in these two single crystals with the Néel temperatures around 119 and 112 K for CaFe⁢O 3 crystal and 109 and 98 K for CaF⁢e 0.95 ⁢C⁢o 0.05 ⁢O 3 crystal, respectively. Neutron diffraction illustrates the formation of a spiral antiferromagnetic structure. Moreover, as the temperature further decreases to 65 K, a third magnetic transition accompanied by a second electrical transition is observed in the slightly Co-doped CaF⁢e 0.95 ⁢C⁢o 0.05 ⁢O 3 crystal. In conclusion, first-principles calculations suggest that the introduction of a moderate amount of Co and the peculiar spiral spin texture play an important role in the presence of such new magnetic and electrical transitions.

Xia, Hailiang [Chinese Academy of Sciences (CAS), ↗

Breakdown of helical edge state topologically protected conductance in time-reversal-breaking excitonic insulators

Gapless helical edge modes are a hallmark of the quantum spin Hall effect. Protected by time-reversal symmetry, each edge contributes a quantized zero-temperature conductance quantum G 0 ≡ e 2 /h. However, the experimentally observed conductance in WT e2 decreases below G 0 per edge already at edge lengths around 100 nm, even in the absence of explicit time-reversal breaking due to an external field or magnetic impurities. Here we show how a time-reversal breaking excitonic condensate with a spin-spiral order that can form in WT e2 leads to the breakdown of conductance quantization. We perform Hartree-Fock calculations to compare time-reversal breaking and preserving excitonic insulators. Using these mean-field models we demonstrate via quantum transport simulations that weak nonmagnetic disorder reproduces the edge length scaling of resistance observed in the experiments. We complement this by analysis in the Luttinger liquid picture, shedding additional light on the mechanism behind the quantization breakdown.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗