用高质量的多晶样品研究了自旋为1/2kagome的类化合物伏硼硫石的磁性。磁化强度和比热测量表明，可果美晶格上的自旋在低温下仍然波动，低至T = 60 mK，对应于最近邻反铁磁相互作用的1/1500，既不表现出传统的长程序，也不表现出自旋间隙。与此相反，51 V NMR实验揭示了一个尖锐的峰在1 K的弛豫速率，这表明一定的奇异秩序发生。令人惊讶的是，我们已经观察到三个“步骤”的磁化作为磁场的函数，这表明至少有四个类液体或其他量子态存在于磁场。
英文摘要：
Magnetic properties of the spin-1/2 kagome-like compound volborthite are studied using a high-quality polycrystalline sample. It is evidenced from magnetization and specific heat measurements that the spins on the kagome lattice still fluctuate at low temperature, down to T = 60 mK that corresponds to 1/1500 of the nearest-neighbor antiferromagnetic interaction, exhibiting neither a conventional long-range order nor a spin gap. In contrast, 51V NMR experiments revealed a sharp peak at 1 K in relaxation rate, which indicates that a certain exotic order occurs. Surprisingly, we have observed three "steps" in magnetization as a function of magnetic field, suggesting that at least four liquid-like or other quantum states exist under magnetic fields.
The magnetization of two spin-1/2 kagome antiferromagnets, volborthite and vesignieite, has been measured in pulsed magnetic fields up to 68 T. A magnetization plateau is observed for each compound near the highest magnetic field. Magnetizations at saturation are approximately equal to 0.40Ms for both compounds, where Ms is the fully saturated magnetization, irrespective of a difference in the distortion of the kagome lattice between the two compounds. It should be noted that these values of magnetizations are significantly larger than Ms/3 predicted theoretically for the one-third magnetizati…
In this Letter, we identify a noncoplanar chiral spin texture on the distorted kagomé-lattice antiferromagnets induced by the presence of a magnetic field applied perpendicular to the distorted kagomé plane. The noncoplanar chiral spin texture has a nonzero scalar spin chirality similar to a chiral quantum spin liquid with broken time-reversal symmetry. In the noncoplanar regime we observe nontrivial topological magnetic excitations and thermal Hall response through the emergent field-induced scalar spin chirality in contrast to collinear ferromagnets in which the Dzyaloshinskii-Moriya (DM) sp…
Thermodynamic investigations on volborthite (Cu3V2O7(OH)2 2H2O), which possesses a two-dimensional kagome structure of S-1/2 spins, are presented. The low-temperature heat capacities of volborthite and its Zn analogue compound were measured by the relaxation calorimetry technique between 0.8 and 45 K. The magnetic heat capacity of volborthite is characterized by two contributions of T-linear and T2 dependences, the former of which is large above 1 K, giving evidence of dense gapless excitations. We find a distinct kink in Cp T-1 at T* = 1 K, which demonstrates a thermodynamic phase transition …
We report 51V-NMR study on a high-quality powder sample of volborthite Cu3V2O7(OH)2/2H2O, a spin-1/2 Heisenberg antiferromagnet on a distorted kagome lattice formed by isosceles triangles. In the magnetic fields below 4.5 T, a sharp peak in the nuclear spin-lattice relaxation rate 1/T1 accompanied with line broadening revealed a magnetic transition near 1 K. The low temperature phase shows anomalies such as a Lorentzian line shape, a 1/T1 propto T behavior indicating dense low energy excitations, and a large spin-echo decay rate 1/T2 pointing to unusually slow fluctuations. Another magnetic ph…
We present spatial and dynamic information on the s=1/2 distorted kagome antiferromagnet volborthite, Cu3V2O7(OD)2.2D2O, obtained by polarized and inelastic neutron scattering. The instantaneous structure factor, S(Q), is dominated by nearest neighbor pair correlations, with short range order at wave vectors Q1=0.65(3) Å^-1 and Q2=1.15(5) Å^-1 emerging below 5 K. The excitation spectrum, S(Q,ω), reveals two steep branches dispersing from Q1 and Q2, and a flat mode at ω=5.0(2) meV. The results allow us to identify the cross-over at T*=1 K in 51V NMR and specific heat measurements as the build-u…
The Kagome-lattice-based material, Volborthite, $\mathrm{Cu_3 V_2 O_7 (OH)_2 \cdot 2 H_2 O}$, has been considered as a promising platform for discovery of unusual quantum ground states due to the frustrated nature of spin interactions. Here we explore possible quantum spin liquid and magnetically ordered phases in a two-dimensional non-symmorphic lattice described by $p2gg$ layer space group, which is consistent with the spatial anisotropy of the spin model derived from density functional theory (DFT) for Volborthite. Using the projective symmetry group (PSG) analysis and Schwinger boson mean …
Microscopic spin interactions on a deformed Kagomé lattice of volborthite are investigated through magnetoelastic couplings. A negative longitudinal magnetostriction $ΔL<0$ in the $b$ axis is observed, which depends on the magnetization $M$ with a peculiar relation of $ΔL/L \propto M^{1.3}$. Based on the exchange striction model, it is argued that the negative magnetostriction originates from a pantograph-like lattice change of the Cu-O-Cu chain in the $b$ axis, and that the peculiar dependence arises from the local spin correlation. This idea is supported by DFT+$U$ calculations simulating th…
We determined the spin exchanges between the Cu2+ ions in the kagome layers of volborthite, Cu3V2O7(OH)2x2H2O, by performing the energy-mapping analysis based on DFT+U calculations, to find that the kagomé layers of Cu2+ ions are hardly spin-frustrated, and the magnetic properties of volborthite below ~75 K should be described by very weakly interacting antiferromagnetic uniform chains made up of effective S=1/2 pseudospin units. This conclusion was verified by synthesizing single crystals of not only Cu3V2O7(OH)2x2H2O but also its deuterated analogue Cu3V2O7(OD)2x2D2O and then by investigatin…
When quantum fluctuations destroy underlying long-range ordered states, novel quantum states emerge. Spin-liquid (SL) states of frustrated quantum antiferromagnets, in which highly-correlated spins keep to fluctuate down to very low temperatures, are prominent examples of such quantum states. SL states often exhibit exotic physical properties, but the precise nature of the elementary excitations behind such phenomena remains entirely elusive. Here we utilize thermal Hall measurements that can capture the unexplored property of the elementary excitations in SL states, and report on the observat…
We have synthesized high-quality single crystals of volborthite, a seemingly distorted kagome antiferromagnet, and carried out high-field magnetization measurements up to 74 T and 51V NMR measurements up to 30 T. An extremely wide 1/3 magnetization plateau appears above 28 T and continues over 74 T at 1.4 K, which has not been observed in previous study using polycrystalline samples. NMR spectra reveal an incommensurate order (most likely a spin-density wave order) below 22 T and a simple spin structure in the plateau phase. Moreover, a novel intermediate phase is found between 23 and 26 T, wh…
Recently, thermal Hall effect has been observed in the paramagnetic state of Volborthite, which consists of distorted Kagome layers with $S=1/2$ local moments. Despite the appearance of a magnetic order below $1 \, \mathrm{K}$, the response to external magnetic field and unusual properties of the paramagnetic state above $1 \, \mathrm{K}$ suggest possible realization of exotic quantum phases. Motivated by these discoveries, we investigate possible spin liquid phases with fermionic spinon excitations in a non-symmorphic version of the Kagome lattice, which belongs to the two-dimensional crystal…
We report results of 51V NMR in the field-induced phase of volborthite Cu3V2O7(OH)dot2H2O, a spin-1/2 antiferromagnet on a distorted kagome lattice. In magnetic fields above 4.5 T, two types of V sites with different spin-echo decay rates are observed. The hyperfine field at the fast decaying sites has a distribution, while it is more homogeneous at the slowly decaying sites. Our results indicate a heterogeneous state consisting of two spatially alternating Cu spin systems, one of which exhibits anomalous spin fluctuations contrasting with the other showing a conventional static order.
Motivated by a recent experiment on volborthite, a typical spin-$1/2$ antiferromagnet with a kagomé lattice structure, we study the magnetization process of a classical Heisenberg model on a spatially distorted kagomé lattice using the Monte Carlo (MC) method. We find a distortion-induced magnetization step at low temperatures and low magnetic fields. The magnitude of this step is given by $Δm_z=\left|1-α\right|/3α$ at zero temperature, where $α$ denotes the spatial anisotropy in exchange constants. The magnetization step signals a first-order transition at low temperatures, between two phases…
We report single-crystal 51V NMR studies on volborthite Cu3V2O7(OH)2 2H2O, which is regarded as a quasi-two-dimensional frustrated magnet with competing ferromagnetic and antiferromagnetic interactions. In the 1/3 magnetization plateau above 28 T, the nuclear spin-lattice relaxation rate 1/T1 indicates an excitation gap with a large effective g factor in the range of 4.6-5.9, pointing to magnon bound states. Below 26 T where the gap has closed, the NMR spectra indicate small internal fields with a Gaussian-like distribution, whereas 1/T1 shows a power-law-like temperature dependence in the par…
Volborthite offers an interesting example of a highly frustrated quantum magnet in which ferromagnetic and antiferromagnetic interactions compete on anisotropic kagome lattices. A recent density functional theory calculation has provided a magnetic model based on coupled trimers, which is consistent with a broad 1/3-magnetization plateau observed experimentally. Here we study the effects of Dzyaloshinskii-Moriya (DM) interactions in volborthite. We derive an effective model in which pseudospin-1/2 moments emerging on trimers form a network of an anisotropic triangular lattice. Using the effect…
We present a microscopic magnetic model for the spin-liquid candidate volborthite Cu3V2O7(OH)2(H2O)2. The essentials of this DFT-based model are (i) the orbital ordering of Cu(1) 3d 3z2-r2 and Cu(2) 3d 3x2-y2, (ii) three relevant couplings J_ic, J_1 and J_2, (iii) the ferromagnetic nature of J_1 and (iv) frustration governed by the next-nearest-neighbor exchange interaction J_2. Our model implies magnetism of frustrated coupled chains in contrast to the previously proposed anisotropic kagome model. Exact diagonalization studies reveal agreement with experiments.
We report results of 51V NMR experiments on a high-quality powder sample of volborthite Cu3V2O7(OH)2/2H2O, a spin-1/2 Heisenberg antiferromagnet on a distorted kagome lattice. Following the previous experiments in magnetic fields $B$ below 12 T, the NMR measurements have been extended to higher fields up to 31 T. In addition to the two already known ordered phases (phases I and II), we found a new high-field phase (phase III) above 25 T, at which a second magnetization step has been observed. The transition from the paramagnetic phase to the antiferromagnetic phase III occurs at 26 K, which is…
Motivated by recent experiments on volborthite single crystals showing a wide 1/3-magnetization plateau, we perform microscopic modeling by means of density functional theory (DFT) with the single-crystal structural data as a starting point. Using DFT+U, we find four leading magnetic exchanges: antiferromagnetic J and J2, as well as ferromagnetic J' and J1. Simulations of the derived spin Hamiltonian show good agreement with the experimental low-field magnetic susceptibility and high-field magnetization data. The 1/3-plateau phase pertains to polarized magnetic trimers formed by strong J bonds…
Despite the conceptional importance of realizing spin liquids in solid states only few compounds are known. On the other side the effect of lattice distortions and anisotropies on the magnetic exchange topology and the fluctuation spectrum are an interesting problem. We compare the excitation spectra of the two s=1/2 kagome lattice compounds volborthite and vesignieite using Raman scattering. We demonstrate that even small modifications of the crystal structure may have a huge effect on the phonon spectrum and low temperature properties.
The magnetization process of the isotropic Heisenberg antiferromagnet on the kagome lattice is studied. Data obtained from the numerical-diagonalization method are reexamined from the viewpoint of the derivative of the magnetization with respect to the magnetic field. We find that the behavior of the derivative at approximately one-third of the height of the magnetization saturation is markedly different from that for the cases of typical magnetization plateaux. The magnetization process of the kagome-lattice antiferromagnet reveals a new phenomenon, which we call the "magnetization ramp".
Unconventional features of the magnetization curve at zero temperature such as plateaus or jumps are a hallmark of frustrated spin systems. Very little is known about their behavior at non-zero temperatures. Here we investigate the temperature dependence of the magnetization curve of the kagome lattice antiferromagnet in particular at 1/3 of the saturation magnetization for large lattice sizes of up to N=48 spins. We discuss the phenomenon of asymmetric melting and trace it back to a combined effect of unbalanced magnetization steps on either side of the investigated plateau as well as on the …
Magnetization plateaus in quantum spin systems emerges in two-dimensional frustrated systems such as kagome lattice. The spin-1/2 antiferromagnetic Heisenberg model on square-kagome lattice is also appropriate for the study of magnetization plateau. Motivated by recent experimental finding of such a square-kagome lattice with nonequivalent three bonds, we investigate the phase diagrams and magnetization plateaus of the lattice by the exact diagonalization method. In addition to previously reported the 1/3 and 2/3 plateaus in the model with two equivalent bonds, we find a new 2/3 plateau whose …
We clarify the existence of several magnetization plateaux for the kagome $S=1/2$ antiferromagnetic Heisenberg model in a magnetic field. Using approximate or exact localized magnon eigenstates, we are able to describe in a similar manner the plateau states that occur for magnetization per site $m=1/3$, $5/9$, and $7/9$ of the saturation value. These results are confirmed using large-scale Exact Diagonalization on lattices up to 63 sites.
Spin-1/2 Heisenberg model on kagome lattice is a typical frustrated quantum spin system. A basic structure of kagome lattice is also present in kagome-strip lattice in one dimension, where a similar type of frustration is expected. We thus study the magnetization plateaus of the spin-1/2 Heisenberg model on a kagome-strip chain with three-independent antiferromagnetic exchange interactions by the density-matrix renormalization group method. In a certain range of exchange parameters, we find twelve kinds of magnetization plateaus, nine of which have magnetic structures breaking either translati…
To capture the high-field magnetization process of herbertsmithite (ZnCu3(OH)6Cl2), Faraday rotation (FR) measurements were carried out on a single crystal in magnetic fields of up to 190 T. The magnetization data evaluated from the FR angle exhibited a saturation behavior above 150 T at low temperatures, which was attributed to the 1/3 magnetization plateau. The overall behavior of the magnetization process was reproduced by theoretical models based on the nearest-neighbor Heisenberg model. This suggests that herbertsmithite is a proximate kagome antiferromagnet hosting an ideal quantum spin …
Highly frustrated spin systems such as the kagome lattice (KL) are a treasure trove of new quantum states with large entanglements. We thus study the spin-$\frac{1}{2}$ Heisenberg model on a kagome-strip chain (KSC), which is one-dimensional KL, using the density-matrix renormalization group (DMRG) method. Calculating central charge and entanglement spectrum for the KSC, we find a novel gapless spin liquid state with doubly degenerate entanglement spectra in a 1/5 magnetization plateau. We also obtain a gapless low-lying continuum in the dynamic spin structure calculated by dynamical DMRG meth…
We propose a modified spin-wave theory to study the 1/3 magnetization plateau of the antiferromagnetic Heisenberg model on the kagome lattice. By the self-consistent inclusion of quantum corrections, the 1/3 plateau is stabilized over a broad range of magnetic fields for all spin quantum numbers, S. The values of the critical magnetic fields and the widths of the magnetization plateaus are fully consistent with recent numerical results from exact diagonalization and infinite projected entangled paired states.
Materials with zero energy band gap display intriguing properties including high sensitivity of the electronic band structure to external stimulus such as pressure or magnetic field. An interesting candidate for zero energy band gap are Weyl nodes at the Fermi level EF. A prerequisite for the existence of Weyl nodes is to either have inversion or time reversal symmetry broken. Weyl nodes in systems with broken time reversal symmetry are ideal to realize the tunability of the electronic band structure by magnetic field. Theoretically, it has been shown that in ferromagnetic Weyl materials, the …
In order to clarify why the experimental magnetization curve of the spherical kagome cluster in {W72V30} at 0.5 K shows no sign of staircase behavior up to 50 T, we study the effects of Dzyaloshinsky-Moriya (DM) interactions and tilts of the g tensors, both of which lead to the breaking of the total-S z conservation, by using the exact diagonalization method. It is found that the D vector component parallel to the radiation direction of the polyhedron cancels out the staircase in a low magnetic field region efficiently. The tilts of the g tensors are inherent to systems defined on the poly- he…
Frustrated spin systems on Kagome lattices have long been considered to be a promising candidate for realizing exotic spin liquid phases. Recently, there has been a lot of renewed interest in these systems with the discovery of materials such as Volborthite and Herbertsmithite that have Kagome like structures. In the presence of an external magnetic field, these frustrated systems can give rise to magnetization plateaus of which the plateau at $m=\frac{1}{3}$ is considered to be the most prominent. Here we study the problem of the antiferromagnetic spin-1/2 quantum XXZ Heisenberg model on a Ka…
Kagome magnets provide a fascinating platform for a plethora of topological quantum phenomena. Here, utilizing angle-resolved photoemission spectroscopy, we demonstrate Weyl lines with strong out-of-plane dispersion in an A-A stacked kagome magnet TbxGd1-xMn6Sn6. On the Gd rich side, the Weyl line remains nearly spin-orbit-gapless due to a remarkable cooperative interplay between Kane-Mele spin-orbit-coupling, low site symmetry and in-plane magnetic order. Under Tb substitution, the kagome Weyl line gaps due to a magnetic reorientation to out-of-plane order. Our results illustrate the magnetic…
We investigate the effect of spin-lattice coupling (SLC) on the magnetic properties of the classical kagome-lattice Heisenberg antiferromagnet (KHAF) using improved Monte Carlo updates. The lattice modes are represented by Einstein site phonons, which introduce effective further-neighbor spin interactions in addition to the nearest-neighbor biquadratic interactions. In the weak SLC, the macroscopically degenerate coplanar ground state remains at zero field, while a $\sqrt{3} \times \sqrt{3}$ ordered phase accompanied by a 1/3-magnetization plateau appears in external magnetic fields. In the st…
We investigate the properties in finite magnetic field of an extended anisotropic XXZ spin-1/2 model on the Kagome lattice, originally introduced by Balents, Fisher, and Girvin [Phys. Rev. B, 65, 224412 (2002)]. The magnetization curve displays plateaus at magnetization m=1/6 and 1/3 when the anisotropy is large. Using low-energy effective constrained models (quantum loop and quantum dimer models), we discuss the nature of the plateau phases, found to be crystals that break discrete rotation and/or translation symmetries. Large-scale quantum Monte-Carlo simulations were carried out in particul…
We use a semiclassical large-$S$ expansion to study a plateau at $1/3$ saturation in the magnetization curve of a frustrated ferrimagnet on a spatially anisotropic kagomé lattice. The spins have both ferromagnetic and antiferromagnetic nearest-neighbor Heisenberg couplings, and a frustrating next-nearest-neighbor coupling in one lattice direction. The magnetization plateau appears at the classical level for a certain range of couplings, and quantum fluctuations significantly broaden it at both ends. Near the region of the phase diagram where the classical plateau destabilizes, we find an exoti…
A spin-1/2 Heisenberg model on honeycomb lattice is investigated by doing triplon analysis and quantum Monte Carlo calculations. This model, inspired by Cu$_2$(pymca)$_3$(ClO$_4$), has three different antiferromagnetic exchange interactions ($J_A$, $J_B$, $J_C$) on three different sets of nearest-neighbour bonds which form a kagome superlattice. While the model is bipartite and unfrustrated, its quantum phase diagram is found to be dominated by a quantum paramagnetic phase that is best described as a spin-gapped hexagonal-singlet state. The Néel antiferromagnetic order survives only in a small…
Variational study of the magnetization plateaus in the spin-1/2 kagome Heisenberg antiferromagnet: An approach from vision transformer neural quantum states
Université de Toulouse, CNRS, Laboratoire de Physique Théorique（图卢兹大学，法国国家科学研究中心，理论物理实验室）
We perform an exact diagonalization study of the spin-$1/2$ XXZ Heisenberg antiferromagnet on the kagome lattice at finite magnetization $m = \frac{2}{3}$ with an emphasis on the XY point ($J_z = 0$), and in the presence of a small chiral term. Recent analytic work by Kumar, Sun and Fradkin [Phys. Rev. B 90, 174409 (2014)] on the same model, using a newly developed flux attachment transformation, predicts a plateau at this value of the magnetization described by a chiral spin liquid (CSL) with a spin Hall conductance of $σ_{xy} = \frac{1}{2}$. Such a state is topological in nature, has a groun…
There is a growing family of rare-earth kagome materials with dominant nearest-neighbor interactions and strong spin orbit coupling. The low symmetry of these materials makes theoretical description complicated, with six distinct nearest-neighbor coupling parameters allowed. In this Article, we ask what kinds of classical, ordered, ground states can be expected to occur in these materials, assuming generic (i.e. non-fine-tuned) sets of exchange parameters. We use symmetry analysis to show that there are only five distinct classical ground state phases occurring for generic parameters. The five…
Gapped 1/9 Magnetization Plateau in the Anisotropic Kagome Antiferromagnet Y-kapellasite
Université Paris-Saclay（巴黎萨克雷大学）；CNRS（法国国家科学研究中心）；Laboratoire de Physique des Solides（固体物理实验室）；Clarendon Laboratory, Department of Physics, University of Oxford（牛津大学克拉伦登实验室物理系）；Department of Physics, University of Warwick（华威大学物理系）；Physikalisches Institut, Goethe-Universität Frankfurt（法兰克福歌德大学物理研究所）；Laboratoire National des Champs Magnétiques Intenses, LNCMI-CNRS (UPR3228), EMFL, Univ. Grenoble Alpes, Univ. Toulouse, INSA-T（强磁场国家实验室，LNCMI-CNRS (UPR3228)，欧洲强磁场联合实验室，格勒诺布尔阿尔卑斯大学，图卢兹大学，INSA-T）；Max-Planck-Institute for So（马克斯·普朗克研究所）
The magnetization and specific heat measurements have been performed on single-crystalline Gd_3_Ru_4_Al_12_ with a distorted Kagome lattice structure. This spin system is regarded as an antiferromagnetic triangular lattice of XY like Heisenberg model at low temperatures. The magnetic phase diagrams indicate the existence of frustration and Z_2_ degeneracy. The magnetization and specific heat imply the successive phase transitions with partial disorder and a T-shaped spin structure in the ground state.
