Helimagnetic State Research Articles

Chemical Trends of the Bulk and Surface Termination-Dependent Electronic Structure of Metal-Intercalated Transition Metal Dichalcogenides.

The addition of metal intercalants into the van der Waals gaps of transition metal dichalcogenides has shown great promise as a method for controlling their functional properties. For example, chiral helimagnetic states, current-induced magnetization switching, and a giant valley-Zeeman effect have all been demonstrated, generating significant renewed interest in this materials family. Here, we present a combined photoemission and density-functional theory study of three such compounds: , , and , to investigate chemical trends of the intercalant species on their bulk and surface electronic structure. Our resonant photoemission measurements indicate increased hybridization with the itinerant NbS2-derived conduction states with increasing atomic number of the intercalant, leading to pronounced mixing of the nominally localized intercalant states at the Fermi level. Using spatially and angle-resolved photoemission spectroscopy, we show how this impacts surface-termination-dependent charge transfers and leads to the formation of new dispersive states of mixed intercalant-Nb character at the Fermi level for the intercalant-terminated surfaces. This provides an explanation for the origin of anomalous states previously reported in this family of compounds and paves the way for tuning the nature of the magnetic interactions in these systems via control of the hybridization of the magnetic ions with the itinerant states.

Chirality reversal of magnetic solitons in chiral Cr1/3TaS2

Ferromagnetism in two-dimensional (2D) materials provides an ideal platform to study emergent electromagnetic phenomena in low dimensions for future spintronics. In magnetic-element intercalated transition metal dichalcogenides, topologically nontrivial spin textures, such as chiral helimagnetic spin states and chiral soliton lattices, are realized due to the chiral lattice distortions induced by intercalated magnetic ions. Consequently, the magnetic chirality is predictably determined by the sign of antisymmetric exchange interaction (or Dzyaloshinskii–Moriya interaction, DMI) vector that is coupled to the underlying crystal chirality. Here, using cryogenic Lorentz phase microscopy, we directly observed the chirality reversal behavior of the chiral soliton lattices in Cr1/3TaS2 across the structural defects. We show that a partial 1 T stacking in 2H-TaS2 locally reduces DMI, leading to magnetic chirality reversal with direct atomic resolution imaging. Our experimental results show that manipulation of stacking sequence provides a viable way to control the chirality of topologically nontrivial soliton lattices in 2D magnets.

Possible helimagnetic order in Co4+-containing perovskites Sr1−xCaxCoO3

We systematically synthesized perovskite-type oxides Sr1−xCaxCoO3 containing unusually high valence Co4+ ions by a high pressure technique and investigated the effect of systematic lattice change on the magnetic and electronic properties. As the Ca content x exceeds about 0.6, the structure changes from cubic to orthorhombic, which is supported by the first-principles calculations of enthalpy. Upon the orthorhombic distortion, the ground state remains to be apparently ferromagnetic, with a slight drop of the Curie temperature. Importantly, the compounds with x larger than 0.8 show antiferromagnetic behavior, with positive Weiss temperatures and nonlinear magnetization curves at the lowest temperature, implying that the ground state is non-collinear antiferromagnetic or helimagnetic. Considering the incoherent metallic behavior and the suppression of the electronic specific heat at the high x region, the possible emergence of a helimagnetic state in Sr1−xCaxCoO3 is discussed in terms of the bandwidth narrowing and the double-exchange mechanism with the negative charge transfer energy, as well as the spin frustration, owing to the next-nearest neighbor interaction.

Persistent exchange splitting in the chiral helimagnet Cr1/3NbS2

Using high-resolution angle-resolved photoemission spectroscopy (ARPES) and ab-initio calculation, we systematically investigate the electronic structure of the chiral helimagnet Cr1/3NbS2 and its temperature evolution. The comparison with NbS2 suggests that the electronic structure of Cr1/3NbS2 is strongly modified by the intercalation of Cr atoms. Our ab-initio calculation, consistent with experimental result, suggests strong hybridization between Nb- and Cr-derived states near the Fermi level. In the chiral helimagnetic state (below the Curie temperature Tc), we observe exchange splitting of the energy bands crossing EF, which follows the temperature evolution of the magnetic moment, suggesting an important role of the conduction electrons in the long-range magnetic ordering. Interestingly, the exchange splitting persists far above Tc with negligible temperature dependence, in drastic contrast to the itinerant ferromagnetism described by the Stoner model, indicating the existence of short-range magnetic order. Our results provide important insights into the microscopic mechanism of the chiral helimagnetic ordering in Cr1/3NbS2.

Electrical conductivity in helical and conical magnetic states

We theoretically study the electrical conductivity in a one-dimensional helimagnet whose spin texture changes from helimagnetic to conical magnetic, and to forced ferromagnetic state while increasing the magnetic field along the helical axis. We find that the conductivity in the helimagnetic state at zero field depends on the electron filling and the coefficient of the spin-charge coupling. We also find that the conductivity in the conical magnetic state changes nonlinearly to the applied field, and the magnetoresistance becomes negative and positive depending on the model parameters.

Microscopic origin of multiferroic order in monolayer NiI2

The discovery of multiferroic behavior in monolayer NiI2 provides a new symmetry-broken state in van der Waals monolayers, featuring the simultaneous emergence of helimagnetic order and ferroelectric order at a critical temperature of T = 21 K. However, the microscopic origin of multiferroic order in NiI2 monolayer has not been established, and in particular, the role of non-collinear magnetism and spin–orbit coupling in this compound remains an open problem. Here we reveal the origin of the two-dimensional multiferroicity in NiI2 using first-principles electronic structure methods. We show that the helimagnetic state appears as a consequence of the long-range magnetic exchange interactions, featuring sizable magnetic moments in the iodine atoms. We demonstrate that the electronic density reconstruction accounting for the ferroelectric order emerges from the interplay of non-collinear magnetism and spin–orbit coupling. We demonstrate that the ferroelectric order is controlled by the iodine spin–orbit coupling, and leads to an associated electronically-driven distortion in the lattice. Our results establish the microscopic origin of the multiferroic behavior in monolayer NiI2, putting forward the coexistence of helical magnetic order and ligand spin–orbit coupling as driving forces for multiferroic behavior in two-dimensional materials.

Spin excitation spectra in helimagnetic states: Proper-screw, cycloid, vortex-crystal, and hedgehog lattices

We investigate the spin excitation spectra in chiral and polar magnets by the linear spin-wave theory for an effective spin model with symmetric and antisymmetric long-range interactions. In one dimension, we obtain the analytic form of the dynamical spin structure factor for proper-screw and cycloidal helical spin states with uniform twists, which shows a gapless mode with strong intensity at the helical wave number. When introducing spin anisotropy in the symmetric interactions, we numerically show that the stable spin spirals become elliptically anisotropic with nonuniform twists and the spin excitation is gapped. In higher dimensions, we find that similar anisotropy stabilizes multiple-$Q$ spin states, such as vortex crystals and hedgehog lattices. We show that the anisotropy in these states manifests itself in the dynamical spin structure factor: a strong intensity in the transverse components to the wave number appears only when the helical wave vector and the corresponding easy axis are perpendicular to each other. Our findings could be useful not only to identify the spin structure but also to deduce the stabilization mechanism by inelastic neutron scattering measurements.

Enhanced electrical magnetochiral effect by spin-hedgehog lattice structural transition

Nonreciprocal resistance, depending on both directions of current ($j$) and magnetic-field ($H$) or magnetization ($M$), is generally expected to emerge in a chiral conductor, and be maximized for $j$ $\parallel$ $H$($M$). This phenomenon, electrical magnetochiral effect (eMChE), is empirically known to increase with $H$ in a paramagnetic or fully ferromagnetic state on chiral lattice or to depend on fluctuation properties of a helimagnetic state. We report here the eMChE over a wide temperature range in the chiral-lattice magnet MnGe in which the spin hedgehog lattice (HL) forms with the triple spin-helix modulation vectors. The magnitude of nonreciprocal resistivity is sharply enhanced in the course of the field-induced structural transition of HL from cubic to rhombohedral form. This is attributed to the enhanced asymmetric electron scatterings by vector spin chirality in association with the large thermal fluctuations of spin hedgehogs.

Strain-modulated helimagnetism and emergent magnetic phase diagrams in highly crystalline MnP nanorod films

We explore strain-modulated helimagnetism in highly crystalline MnP nanorod films grown on Si(100) substrates using molecular beam epitaxy. The strained MnP film exhibits a paramagnetic to ferromagnetic (FM) phase transition at ${T}_{C}\ensuremath{\sim}279\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, and the FM to helical phase transition at ${T}_{N}\ensuremath{\sim}110\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. The value of ${T}_{N}$ is greater than ${T}_{N}\ensuremath{\sim}47\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ for the MnP single crystal, indicating strong strain-modulated helimagnetic states in the MnP nanorod film. The presence of significant thermal hysteresis in the helical phase indicates the coexistence of competing magnetic interactions, leading to the first-order metamagnetic transition. Similar to its single-crystal counterpart, an anisotropic magnetic effect is observed in the MnP film, which is independently confirmed by magnetic hysteresis loop and radio-frequency transverse susceptibility (TS) measurements. The evolution of the screw to the cone and fan phases is precisely tracked from magnetization vs magnetic field/temperature measurements. The temperature dependence of the anisotropy fields, extracted from the TS spectra, yields further insight into the competing nature of the magnetic phases. Unfolding of the different helical phases at $T<120\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ $(\ensuremath{\sim}{T}_{\mathrm{N}})$ is analyzed by the temperature- and field-dependent magnetic entropy change. Based on these findings, the comprehensive magnetic phase diagrams of the MnP nanorod film are constructed for both the in-plane and out of plane magnetic field directions, revealing emergent strain/dimensionality-driven helical magnetic features that are absent in the magnetic phase diagram of the MnP single crystal.

Multiple quantum phase transitions of different nature in the topological kagome magnet Co3Sn2\u2212xInxS2

The exploration of topological electronic phases that result from strong electronic correlations is a frontier in condensed matter physics. One class of systems that is currently emerging as a platform for such studies are so-called kagome magnets based on transition metals. Using muon spin-rotation, we explore magnetic correlations in the kagome magnet Co3Sn2−xInxS2 as a function of In-doping, providing putative evidence for an intriguing incommensurate helimagnetic (HM) state. Our results show that, while the undoped sample exhibits an out-of-plane ferromagnetic (FM) ground state, at 5% of In-doping the system enters a state in which FM and in-plane antiferromagnetic (AFM) phases coexist. At higher doping, a HM state emerges and becomes dominant at the critical doping level of only xcr,1 ≃ 0.3. This indicates a zero temperature first order quantum phase transition from the FM, through a mixed state, to a helical phase at xcr,1. In addition, at xcr,2 ≃ 1, a zero temperature second order phase transition from helical to paramagnetic phase is observed, evidencing a HM quantum critical point (QCP) in the phase diagram of the topological magnet Co3Sn2−xInxS2. The observed diversity of interactions in the magnetic kagome lattice drives non-monotonous variations of the topological Hall response of this system.

Chirality Memory Stored in Magnetic Domain Walls in the Ferromagnetic State of MnP.

Chirality in a helimagnetic structure is determined by the sense of magnetic moment rotation. We found that the chiral information did not disappear even after the phase transition to the high-temperature ferromagnetic phase in a helimagnet MnP. The 2nd harmonic resistivity ρ^{2f}, which reflects the breaking down of mirror symmetry, was found to be almost unchanged after heating the sample above the ferromagnetic transition temperature and cooling it back to the helimagnetic state. The application of a magnetic field along the easy axis in the ferromagnetic state quenched the chirality-induced ρ^{2f}. This indicates that the chirality memory effect originated from the ferromagnetic domain walls.

Helical magnetic order and Fermi surface nesting in noncentrosymmetric ScFeGe

An investigation of the structural, magnetic, thermodynamic, and charge transport properties of noncentrosymmetric hexagonal ScFeGe reveals it to be an anisotropic metal with a transition to a weak itinerant incommensurate helimagnetic state below TN=36 K. Neutron diffraction measurements discovered a temperature and field independent helical wave vector k = (0 0 0.193) with magnetic moments of 0.53 μB per Fe confined to the ab plane. Density functional theory calculations are consistent with these measurements and find several bands that cross the Fermi level along the c axis with a nearly degenerate set of flat bands just above the Fermi energy. The anisotropy found in the electrical transport is reflected in the calculated Fermi surface, which consists of several warped flat sheets along the c axis with two regions of significant nesting, one of which has a wave vector that closely matches that found in the neutron diffraction. The electronic structure calculations, along with a strong anomaly in the c -axis conductivity at TN, signal a Fermi surface driven magnetic transition, similar to that found in spin density wave materials. Magnetic fields applied in the ab plane result in a metamagnetic transition with a threshold field of ≈6.7 T along with a sharp, strongly temperature dependent discontinuity and a change in sign of the magnetoresistance for in-plane currents. Thus, ScFeGe is an ideal system to investigate the effect of in-plane magnetic fields on a helimagnet with a c -axis propagation vector, where the relative strength of the magnetic interactions and anisotropies determine the topology and magnetic structure.6 MoreReceived 18 September 2020Revised 9 December 2020Accepted 11 January 2021DOI:https://doi.org/10.1103/PhysRevB.103.014443©2021 American Physical SocietyPhysics Subject Headings (PhySH)Physical SystemsNoncentrosymmetric materialsNoncollinear magnetsTechniquesDensity functional calculationsMagnetization measurementsNeutron diffractionResistivity measurementsCondensed Matter & Materials Physics

NMR study of magnetic structure and hyperfine interactions in the binary helimagnet FeP

We report a detailed study of the ground state helical magnetic structure in monophosphide FeP by means of ${}^{31}$P NMR spectroscopy. We show that the zero-field NMR spectrum of the polycrystalline sample provides strong evidence of an anisotropic distribution of local magnetic fields at the P site with substantially lower anharmonicity than that found at the Fe site by M\"{o}ssbauer spectroscopy. From field-sweep ${}^{31}$P NMR spectra we conclude that a continuous spin-reorientation transition occurs in an external magnetic field range of 4 - 7 T, which is also confirmed by specific-heat measurements. We observe two pairs of magnetically inequivalent phosphorus positions resulting in a pronounced four-peak structure of the single crystal ${}^{31}$P NMR spectra characteristic of an incommensurate helimagnetic ground state. We revealed a spatial redistribution of local fields at the P sites caused by Fe spin-reorientation transition in high fields and developed an effective approach to account for it. We demonstrate that all observed ${}^{31}$P spectra can be treated within a model of an isotropic helix of Fe magnetic moments in the ($ab$)-plane with a phase shift of 36$^{\circ}$ and 176$^{\circ}$ between Fe1-Fe3 (Fe2-Fe4) and Fe1-Fe2 (Fe3-Fe4) sites, respectively, in accordance with the neutron scattering data.

Robust nature of the chiral spin helix in CrNb3S6 nanostructures studied by off-axis electron holography

Magnetic soliton crystals with layered structures that host periodic chiral helimagnetic ordering are promising candidates for spintronic nanodevices. Among them, helimagnetic $\mathrm{Cr}{\mathrm{Nb}}_{3}{\mathrm{S}}_{6}$ is unique owing to its crystallographic chirality and monoaxial Dzyaloshinskii-Moriya interaction. It is crucial to explore its magnetic configurations and properties with respect to the temperature and thickness, especially in reduced dimensions. Here, the chiral helimagnetic ground state in $\mathrm{Cr}{\mathrm{Nb}}_{3}{\mathrm{S}}_{6}$ nanostructures is investigated using off-axis electron holography in the transmission electron microscope. The period of the helical state is found to be independent of both temperature and specimen thickness, while the temperature dependence of the saturation magnetization is shown to follow a classical Heisenberg spin model. Monte Carlo simulations based on a discrete classical Heisenberg model reproduce the experimental observations closely, confirming the applicability of a three-dimensional Heisenberg model even in a confined specimen geometry.

Jumplike Magnetic Disordering Processes Stimulated by a Magnetic Field in Systems with Structural Instability

A theoretical analysis of the features of first-order structural and magnetostructural transitions in magnetocaloric helimagnetic alloys of the Mn1 – xCrxNiGe system is performed. The observed structural transitions of the displacement type hex(P63/mmc) ↔ orth(Pnma) are described using the local soft mode model in the approximation of a displaced harmonic oscillator. In the absence of a magnetic field, the emergence of a helimagnetic order as a structurally induced second-order transition is described within the Heisenberg model with allowance for the dependence of the exchange integrals on the structural order parameters and elastic strains. In the presence of a magnetic field, it was found that the mutual approach of the characteristic temperatures for the helimagnetic state (HM(Pnma)) and the lability temperatures of the hexagonal paramagnetic state (PM(P63/mmc)), due to the action of the magnetic field, leads to the appearance of previously unexplored peripheral first-order magnetostructural transitions with insignificant magnetization jumps, increasing with increasing magnetic induction field. In this case, as the pressure increases to 4 kbar with a constant magnetic induction field, the peripheral transitions are transformed into reversible first-order magnetostructural transitions and, at even higher pressures (10–14 kbar), into full-scale first-order magnetostructural transitions with magnetization jumps comparable with the maximum magnetization. Experimental baric studies of the temperature dependences of the magnetization in static magnetic fields with an induction up to 1 T and pressure up to 14 kbar confirm the theoretical results.

Critical phenomenon of the layered chiral helimagnetic YbNi3Al9

Two-dimensional layered YbNi3Al9 exhibits a chiral helimagnetic ground state, which is a candidate for the field-modulated chiral magnetic soliton. In this work, the magnetism and critical phenomenon of YbNi3Al9 are investigated. As H ⊥ c, a magnetic step with loop can be observed in the field-dependent magnetization, which may be corresponding to the possible chiral magnetic soliton phase transition. Based on the analysis of isothermal magnetization around TC, the critical exponents are obtained as β = 0.1370(2), γ = 1.7955(4), and δ = 14.1043(7), which fulfill the Widom scaling relation and Rushbrooke’s law. Moreover, the obtained critical exponents are testified by the modified Arrott plot and scaling hypothesis. The critical exponents of YbNi3Al9 are close to the theoretically prediction of 2D-Ising model with the spatial-dimensionality n = 2 and spin-dimensionality d = 1, indicating one-dimensional magnetic coupling in the two-dimensional framework. Based on universality scaling, we construct the detailed H–T phase diagram around the phase transition with H ⊥ c, which reveals that the field-induced magnetic transition for H ⊥ c is of the first-order type.

Consequences of magnetic ordering in chiral Mn1/3NbS2

We have investigated the structural, magnetic, thermodynamic, and charge transport properties of Mn1/3NbS2 single crystals through x-ray and neutron diffraction, magnetization, specific heat, magnetoresistance, and Hall effect measurements. Mn1/3NbS2 displays a magnetic transition at TC ~ 45 K with highly anisotropic behavior expected for a hexagonal structured material. Below TC, neutron diffraction reveals increased scattering near the structural Bragg peaks having a wider Q-dependence along the c-axis than the nuclear Bragg peaks. This indicates helimagnetism with a long pitch length of ~250 nm (or a wavevector q~0.0025 {\AA}-1) along the c-axis. This q is substantially smaller than that found for the helimagnetic state in isostructural Cr1/3NbS2 (0.015 {\AA}-1). Specific heat capacity measurements confirm a second-order magnetic phase transition with a substantial magnetic contribution that persists to low temperature. The large low-temperature specific heat capacity is consistent with a large density of low-lying magnetic excitations that are likely associated with topologically interesting magnetic modes. Changes to the magnetoresistance, the magnetization, and the magnetic neutron diffraction, which become more apparent below 20 K, imply a modification in the character of the magnetic ordering corresponding to the magnetic contribution to the specific heat capacity. These observations signify a more complex magnetic structure both at zero and finite fields for Mn1/3NbS2 than for the well-investigated Cr1/3NbS2.

The Helical Magnet MnSi: Skyrmions and Magnons

Since the late 1970s, MnSi has played a major role in developing the theory of helical magnets in non-centrosymmetric materials showing the Dzyaloshinsky-Moriya interaction (DMI). With a long helimagnetic pitch of 175 Å as compared to the lattice d-spacing of 4.55 Å, it was ideal for performing neutron studies, especially as large single crystals could be grown. A (B-T)-phase diagram was measured, and in these studies, under the application of a field of about 180 mT perpendicular to the scattering vector Q, a so-called A-phase in the B-T phase diagram was found and first interpreted as a re-orientation of the magnetic helix. After the surprising discovery of the skyrmion lattice in the A-phase in 2009, much interest arose due to the rigidity of the skyrmionic lattice, which is only loosely bound to the crystal lattice, and therefore only relatively small current densities can already induce a motion of this lattice. A very interesting approach to even better understand the complex structures in the phase diagram is to measure and model the spin excitations in MnSi. As the helimagnetic state is characterized by a long pitch of about 175 Å, the associated characteristic excitations form a band structure due to Umklapp scattering and can only be observed at very small Q with energies below 1 meV. Similarly, the excitations of the skyrmion lattice are very soft and low-energetic. We investigated the magnons in MnSi in the whole (B,T)-phase diagram starting in the single-k helimagnetic state by applying a small magnetic field, B = 100 mT. This way, the complexity of the magnon spectrum is significantly reduced, allowing for a detailed comparison of the data with theory, resulting in a full theoretical understanding of the spin system of MnSi in all its different magnetic phases.

Extended exchange interactions stabilize long-period magnetic structures in Cr1∕3NbS2

The topologically protected, chiral soliton lattice is a unique state of matter offering intriguing functionality, and it may serve as a robust platform for storing and transporting information in future spintronic devices. While the monoaxial chiral magnet Cr1∕3NbS2 is known to host this exotic state in an applied magnetic field, its detailed microscopic origin has remained a matter of debate. Here, we work towards addressing this open question by measuring the spin wave spectrum of Cr1∕3NbS2 over the entire Brillouin zone with inelastic neutron scattering. The well-defined spin wave modes allow us to determine the values of several microscopic interactions for this system. The experimental data are well-explained by a Heisenberg Hamiltonian with exchange constants up to the third nearest neighbor and an easy plane magnetocrystalline anisotropy term. Our work shows that both the second and third nearest neighbor exchange interactions contribute to the formation of the helimagnetic and chiral soliton lattice states in this robust three-dimensional magnet.

Unusual stability of ground ferrimagnetic state in Tm2Fe17 under pressure

The magnetic properties of the near-stoichiometric Tm2Fe16 and Tm2Fe19 compounds under hydrostatic pressures up to 1 GPa were studied. We have revealed that the high-temperature ferrimagnetic state easily magnetized in the basal plane is very sensitive to the volume changes and even moderate pressure is sufficient to its complete suppression and transformation to a helimagnetic state. At the same time, the low-temperature ferrimagnetic state easily magnetized along the hexagonal axis does not disappear under pressure and the temperature of its transition to the high-temperature magnetic states increases under pressure. The remarkable stability of the ground ferrimagnetic state under external pressure can be attributed to the strengthening of the uniaxial magnetic anisotropy and to the mutual perpendicular orientation of the magnetic moments in the ground and the high-temperature magnetic states.