Here, we present a detailed theoretical and experimental study on the pressure induced switching of anomalous Hall effect (AHE) in the triangular antiferromagnetic (AFM) compound Mn$_3$Sn. Our theoretical model suggests pressure driven significant splitting of the in-plane Mn bond lengths $i.e.$ an effective trimerization, which in turn stabilizes a helical AFM ground state by modifying the inter-plane exchange parameters in the system. We experimentally demonstrate that the AHE in Mn$_3$Sn reduces from 5$μΩ$ cm at ambient pressure to zero at an applied pressure of about 1.5 GPa. Furthermore, our pressure dependent magnetization study reveals that the conventional triangular AFM ground state of Mn$_3$Sn systematically transforms into the helical AFM phase where the symmetry does not support a non-vanishing Berry curvature required for the realization of a finite AHE. The pressure dependent x-ray diffraction (XRD) study rules out any role of structural phase transition in the observed phenomenon. In addition, the temperature dependent in-plane lattice parameter at ambient pressure is found to deviate from the monotonic behavior when the system enters into the helical AFM phase, thereby, supporting the proposed impact of trimerization in controlling the AHE. We believe that the present study makes an important contribution towards understanding the stabilization mechanism of different magnetic ground states in Mn$_3$Sn and related materials for their potential applications pertaining to AHE switching.
Hexagonal RMnO3 is a multiferroic compound with a giant spin-lattice coupling at an antiferromagnetic transition temperature [1]. Despite extensive studies over the past two decades, however, the origin and underlying microscopic mechanism of the strong spin-lattice coupling remain still very much elusive. In this study, we have tried to address this problem by measuring the thermal expansion and dielectric constant of doped single crystals Y1-xLuxMnO3 with x = 0, 0.25, 0.5, 0.75, and 1.0. From these measurements, we confirm that there is a progressive change in the physical properties with do…
The antiferromagnetic kagome material Na2Ti3Cl8 exhibits a first-order phase transition; the low-temperature phase is characterized by the trimerizations of Ti ions. In this work, we carry out first-principles calculations on the crystal and electronic structure of Na$_2$Ti$_3$Cl$_8$ at the high- and low-temperature phases. The crystal structures, including the lattice constant and the trimerization of Ti ions, are well reproduced by taking account a small Hubbard correction of 1 eV. The calculated total energy landscape reveals a first-order phase transition with the total energy barrier of 8…
We discuss the recent experimental data on various frustrated quasi-two-dimensional Heisenberg antiferromagnets from the viewpoint of the Z2-vortex order, which include S=3/2 triangular-lattice antiferromagnet NaCrO2, S=1 triangular-lattice antiferromagnet NiGa2S4, S=1/2 organic triangular-lattice antiferromagnets κ-(BEDT-TTF)2Cu2(CN)3 and EtMe3Sb[Pd(dmit)2]2, and S=1/2 kagome-lattice antiferromagnet volborthite Cu3V2O7(OH)22H2O, etc.
Resonant magnetic x-ray diffraction experiments were carried out on the stacked triangular lattice antiferromagnet GdPd2Al3. The experiments revealed an expected initial collinear c-axis order at TN1 followed by an additional in-plane order at TN2, while at the same time we found that the ground state is a helically ordered state of a very long incommensurate period of approximately 700A. The distribution of K-domains was highly anisotropic, and the domain with the modulation vector normal to the surface of the crystal was ascendant. Low-field magnetization is discussed on the basis of the obs…
Here, we report the synthesis and magnetic properties of a new triangular lattice antiferromagnet Ba$_3$CoTa$_2$O$_9$. The effective spin of Co$^{2+}$ is found to be $J=1/2$ at low temperatures due to the combined effect of crystal field and spin-orbit coupling. Ba$_3$CoTa$_2$O$_9$ undergoes two successive magnetic phase transitions at $T_{N1}\simeq0.70$~K and $T_{N2}\simeq0.57$~K in zero applied field, which is typical for triangular antiferromagnets with the easy-axis magnetic anisotropy. With increasing field, the transition anomalies are found to shift toward low temperatures, confirming t…
We found new two-dimensional (2D) quantum (S=1/2) antiferromagnetic systems: CuRE2Ge2O8 (RE=Y and La). According to our analysis of high-resolution X-ray and neutron diffraction experiments, the Cu-network of CuRE2Ge2O8 (RE=Y and La) exhibits a 2D triangular lattice linked via weak bonds along the perpendicular b-axis. Our bulk characterizations from 0.08 to 400 K show that they undergo a long-range order at 0.51(1) and 1.09(4) K for the Y and La systems, respectively. Interestingly, they also exhibit field induced phase transitions. For theoretical understanding, we carried out the density fu…
A new type of magnetically frustrated lattice is found in the layered fluoride NaBa2Mn3F11. A kagome-type array of regular triangles composed of Mn2+ ions (spin 5/2) deforms so as to generate the next-nearest-neighbor interaction J2 between three out of six spins in the hexagon of a normal kagome lattice, in addition to the nearest-neighbor interaction J1. As a function of |J2/J1|, this lattice can interconnect the kagome (J2 = 0) and the triangular (J2 = J1) lattices and thus is called the kagome-triangular (KT) lattice. Magnetic susceptibility and heat capacity measurements performed on a po…
The cradle of quantum spin liquids, triangular antiferromagnets show strong proclivity to magnetic order and require deliberate tuning to stabilize a spin-liquid state. In this brief review, we juxtapose recent theoretical developments that trace the parameter regime of the spin-liquid phase, with experimental results for Co-based and Yb-based triangular antiferromagnets. Unconventional spin dynamics arising from both ordered and disordered ground states is discussed, and the notion of a geometrically perfect triangular system is scrutinized to demonstrate non-trivial imperfections that may as…
The ordering of the classical Heisenberg antiferromagnet on the triangular lattice with the the bilinear-biquadratic interaction is studied by Monte Carlo simulations. It is shown that the model exhibits a topological phase transition at a finite-temperature driven by topologically stable vortices, while the spin correlation length remains finite even at and below the transition point. The relevant vortices could be of three different types, depending on the value of the biquadratic coupling. Implications to recent experiments on the triangular antiferromagnet NiGa$_2$S$_4$ is discussed.
We obtain the non-collinear ground states of a triangular-lattice antiferromagnet with exchange interactions up to third nearest neighbors as a function of the single-ion anisotropy $D$. At a critical value of $D$, the collinear $\uudd $ phase transforms into a complex non-collinear phase with odd-order harmonics of the fundamental ordering wavevector $\vQ $. The observed elastic peaks at $2π\vx -\vQ $ in both Al- and Ga- doped CuFeO$_2$ are explained by a "scalene" distortion of the triangular lattice produced by the repulsion of neighboring oxygen atoms.
We report the de Haas-van Alphen (dHvA) oscillations and first-principle calculations for triangular antiferromagnet PdCrO2 showing unconventional anomalous Hall effect (AHE). The dHvA oscillations in PdCrO2 reveal presence of several 2 dimensional Fermi surfaces of smaller size than found in nonmagnetic PdCoO2. This evidences Fermi surface reconstruction due to the non-collinear 120 antiferromagnetic ordering of the localized Cr, consistent with the first principle calculations. The temperature dependence of dHvA oscillations shows no signature of additional modification of Cr spin structure …
We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whereas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70\,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. …
We investigate the $S=1/2$ quantum spin antiferromagnets on the triangular and Kagome lattices in magnetic field, using the numerical exact diagonalization. Particularly we focus on an anomalous magnetization behavior of each system at 1/3 of the saturation magnetization. The critical exponent analyses suggest that it is a conventional magnetization plateau on the triangular lattice, while an unconventional phenomenon, called the magnetization ramp, on the Kagome lattice.
We report 7Li NMR studies of single crystals of triangular-lattice Heisenberg antiferromagnet Li7RuO6. Slow critical divergence with a wide critical region of |T/TN - 1|< 7 was observed in 7Li nuclear spin-lattice relaxation rate. The slowing down of staggered spin fluctuations was analyzed in a renormalized classical region of a two-dimensional triangular-lattice non-linear sigma model. A spin stiffness constant was found to reduce to about 20 % from the value in a spin-wave approximation. The effect of spin frustration, e.g., Z2 vortex excitations on the critical phenomena is suggested.
Spintronic devices using antiferromagnets (AFMs) are promising candidates for future applications. Recently, many interesting physical properties have been reported with AFM-based devices. Here we report a butterfly-shaped magnetoresistance (MR) in a micrometer-sized triangular-lattice antiferromagnet Ag$_2$CrO$_2$. The material consists of two-dimensional triangular-lattice CrO$_2$ layers with antiferromagnetically coupled $S$ = 3/2 spins and Ag$_2$ layers with high electrical conductivity. The butterfly-shaped MR appears only when the magnetic field is applied perpendicularly to the CrO$_2$ …
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…
The ground state of the spin-$1/2$ Heisenberg antiferromagnet on a distorted triangular lattice is studied using a numerical-diagonalization method. The network of interactions is the $\sqrt{3}\times\sqrt{3}$ type; the interactions are continuously controlled between the undistorted triangular lattice and the dice lattice. We find new states between the nonmagnetic 120-degree-structured state of the undistorted triangular case and the up-up-down state of the dice case. The intermediate states show spontaneous magnetizations that are smaller than one third of the saturated magntization correspo…
We perform high-field magnetization measurements on the triangular lattice antiferromagnet Fe$_{1/3}$NbS$_2$. We observe a plateau in the magnetization centered at approximately half the saturation magnetization over a wide range of temperature and magnetic field. From density functional theory calculations, we determine a likely set of magnetic exchange constants. Incorporating these constants into a minimal Hamiltonian model of our material, we find that the plateau and of the $Z_3$ symmetry breaking ground state both arise from interplane and intraplane antiferromagnetic interactions acting…
CuCrO2 is a manifestation of a two-dimensional triangular antiferromagnet which exhibits an incommensurate noncollinear magnetic structure similar to a classical 120 degree ordering. Using the inelastic neutron scattering technique, direct evidence of a magnon-phonon coupling in CuCrO2 is revealed via the mixed magnon-phonon character of the excitation mode at 12.5 meV as well as a minimum at the zone boundary. A simple model Hamiltonian that incorporates an exchange striction type magnon-phonon coupling reproduces the observed features accurately. Also, continuum excitations originating from …
Coupling between spin and lattice degrees of freedom are important in geometrically frustrated magnets where they can lead to degeneracy lifting and novel orders. We show that moderate spin-lattice couplings in triangular and Kagome antiferromagnets can induce complex colinear magnetic orders. When classical Heisenberg spins on the triangular lattice are coupled to Einstein phonons, a rich variety of phases emerge, including the experimentally observed four sublattice state and the five sublattice 1/5th plateau state seen in the magneto-electric material CuFeO$_2$. In addition we predict magne…
The spin wave excitations of the geometrically frustrated triangular lattice antiferromagnet (TLA) $\rm CuFeO_2$ have been measured using high resolution inelastic neutron scattering. Antiferromagnetic interactions up to third nearest neighbors in the ab plane (J_1, J_2, J_3, with $J_2/J_1 \approx 0.44$ and $J_3/J_1 \approx 0.57$), as well as out-of-plane coupling (J_z, with $J_z/J_1 \approx 0.29$) are required to describe the spin wave dispersion relations, indicating a three dimensional character of the magnetic interactions. Two energy dips in the spin wave dispersion occur at the incommens…
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-…
This work examines the critical anisotropy required for the local stability of the collinear ground states of a geometrically-frustrated triangular-lattice antiferromagnet (TLA). Using a Holstein-Primakoff expansion, we calculate the spin-wave frequencies for the 1, 2, 3, 4, and 8-sublattice (SL) ground states of a TLA with up to third neighbor interactions. Local stability requires that all spin-wave frequencies are real and positive. The 2, 4, and 8-SL phases break up into several regions where the critical anisotropy is a different function of the exchange parameters. We find that the criti…
We report the magnetic and electric properties of Ba$_3$NiNb$_2$O$_9$, which is a quasi-two-dimensional spin-1 triangular lattice antiferromagnet (TLAF) with trigonal structure. At low $T$ and with increasing magnetic field, the system evolves from a 120 degree magnetic ordering phase (A phase) to an up-up-down ($uud$) phase (B phase) with a change of slope at 1/3 of the saturation magnetization, and then to an "oblique" phase (C phase). Accordingly, the ferroelectricity switches on at each phase boundary with appearance of spontaneous polarization. Therefore, Ba$_3$NiNb$_2$O$_9$ is a unique T…
In this Letter, we report the results of ESR measurements in high magnetic fields up to about 53 T on single crystals of NiGa2S4 to clarify the spin dynamics in more detail. We have found that the dynamics of Z2 vortices affects the temperature dependence of the ESR absorption linewidth and the frequency dependence of the ESR resonance fields at 1.3 K is well explained by a conventional spin wave theory. These results suggest an occurrence of Z2 vortex-induced topological transition.
The magnetic ground state and the crystalline electric field level scheme of the triangular lattice antiferromagnet KCeO$_2$ are investigated. Below $T_N =$ 300 mK, KCeO$_2$ develops signatures of magnetic order in specific heat measurements and low energy inelastic neutron scattering data. Trivalent Ce$^{3+}$ ions in the $D_{3d}$ local environment of this compound exhibit large splittings among the lowest three $4f^1$ Kramers doublets defining for the free ion the $J = 5/2$ sextet and a ground state doublet with dipole character, consistent with recent theoretical predictions in M. S. Eldeeb …
Yb- and Ce-based delafossites were recently identified as effective spin-1/2 antiferromagnets on the triangular lattice. Several Yb-based systems, such as NaYbO2, NaYbS2, and NaYbSe2, exhibit no long-range order down to the lowest measured temperatures and therefore serve as putative candidates for the realization of a quantum spin liquid. However, their isostructural Ce-based counterpart KCeS2 exhibits magnetic order below TN = 400 mK, which was so far identified only in thermodynamic measurements. Here we reveal the magnetic structure of this long-range ordered phase using magnetic neutron d…
Frustrated Ising magnets host exotic excitations, such as magnetic monopoles in spin ice. The ground state (GS) in this case is characterized by an extensive degeneracy and associated residual entropy going back to the pioneering work by G. Wannier who established large residual entropy of nearly 50%Rln2 per mole spins in a triangular Ising antiferromagnet (TIAF) already in 1950. Here, we endeavor to verify this result experimentally using TmMgGaO4, a novel rare-earth-based frustrated antiferromagnet with Ising spins arranged on a perfect triangular lattice. Contrary to theoretical expectation…
Ordering of the frustrated classical Heisenberg model on the triangular-lattice with an incommensurate spiral spin structure is studied under magnetic fields by means of a mean-field analysis and a Monte Carlo simulation. Several types of multiple-q states including the "skyrmion-lattice" state is observed in addition to the standard single-q state. In contrast to the Dzyaloshinskii-Moriya interaction driven system, the present model allows both skyrmions and anti-skyrmions, together with a new thermodynamic phase where skyrmion and anti-skyrmion lattices form a domain state.
We present the ultralow-temperature specific heat and thermal conductivity measurements on single crystals of triangular-lattice antiferromagnet Na$_2$BaCo(PO$_4$)$_2$, which was recently argued to host itinerant fermionic excitations, like a quantum spin liquid, above its antiferromagnetic phase transition temperature $T_{\rm N}$ = 0.148 K. In specific heat measurements, we confirm the peaks due to antiferromagnetic ordering when magnetic field $μ_0 H \leq$ 1 T, roughly consistent with previous work [N. Li $et$ $al.$, Nat. Commun. 11, 4216 (2020)]. However, in thermal conductivity measurement…
