A new family of disorder-free Rare-Earth-based kagomé lattice magnets: structure and magnetic characterizations of RE3BWO9 (RE=Pr, Nd, Gd-Ho) Boratotungstates
Malik Ashtar, Jinjin Guo, Zongtang Wan, Yongqiang Wang, Gaoshang Gong, Yong Liu, Yuling Su, Zhaoming Tian
Exploration of rare-earth (RE)-based Kagome lattice magnets with spin-orbital entangled jeff=1/2 moments will provide new platform for investigating the exotic magnetic phases. Here, we report a new family of RE3BWO9 (RE=Pr,Nd,Gd-Ho) boratotungstates with magnetic RE3+ ions arranged on Kagome lattice, and perform its structure and magnetic characterizations. This serial compounds crystallize in hexagonal coordinated structure with space group P63 (No.173), where magnetic RE3+ ions have distorted Kagomé lattice connections within the ab plane and stacked in a AB-type fashion along c axis. The interlayer RE-RE separation is comparable with that of intralayer distance, forming 3-dimensional (3D) exchange coupled magnetic framework of RE3+ ions. The magnetic susceptibility data of RE3BWO9 (RE=Pr, Nd, Gd-Ho) reveal dominant antiferromagnetic interactions between magnetic RE3+ ions, but without visible magnetic ordering down to 2 K. The magnetization analyses for different RE3+ ions show diverse anisotropic behaviors, make RE3BWO9 as an appealing Kagome-lattice antiferromagnet to explore exotic magnetic phases.
Kagome lattices host flat bands due to their frustrated lattice geometry, which leads to destructive quantum interference of electron wave functions. Here, we report imaging of the kagome flat band localization in real-space using scanning tunneling microscopy. We identify both the Fe3Sn kagome lattice layer and the Sn2 honeycomb layer with atomic resolution in kagome antiferromagnet FeSn. On the Fe3Sn lattice, at the flat band energy determined by the angle resolved photoemission spectroscopy, tunneling spectroscopy detects an unusual state localized uniquely at the Fe kagome lattice network.…
Electronic properties of the single crystal of GdV6Sn6, where non-magnetic V-kagome layers are separated by magnetic Gd-triangular lattice, are investigated. GdV6Sn6 exhibits unique magnetotransport properties at low-temperature such as non-linear Hall resistivity and increase of resistance R in magnetic field H as R ~ H^0.75 up to 56 T with Shubnikov-De Haas oscillations. Investigation of the non-magnetic analogue YV6Sn6 and the first principles calculations reveal these properties are relevant to the bands arising from the V-kagome layer. A magnetic transition at 5 K in GdV6Sn6 modifies the …
We prepared a powder sample of edwardsite Cd2Cu3(SO4)2(OH)6 4H2O, which is a new candidate compound for the spin-1/2 kagome antiferromagnet, and studied its magnetic properties by magnetic susceptibility and heat capacity measurements. Edwardsite has a deformed kagome lattice with an average antiferromagnetic interaction of 51 K between nearby spins and shows an antiferromagnetic order accompanied by a small ferromagnetic moment below 4.3 K. The weak ferromagnetism is likely due to spin canting caused by sizable Dzyaloshinsky-Moriya interactions, which may stabilize the long-range magnetic ord…
We investigate the electronic and magnetic properties of the kagome mineral averievite (CsCl)Cu$_5$V$_2$O$_{10}$ and its phosphate analog (CsCl)Cu$_5$P$_2$O$_{10}$ using first-principles calculations. The crystal structure of these compounds features Cu$^{2+}$ kagome layers sandwiched between Cu$^{2+}$-P$^{5+}$/Cu$^{2+}$-V$^{5+}$ honeycomb planes, with pyrochlore slabs made of corner-sharing Cu-tetrahedra being formed. The induced chemical pressure effect upon substitution of V by P causes significant changes in the structure and magnetic properties. Even though the in-plane antiferromagnetic …
Strongly correlated Kagome magnets are promising candidates for achieving controllable topological devices owing to the rich interplay between inherent Dirac fermions and correlation-driven magnetism. Here we report tunable local magnetism and its intriguing control of topological electronic response near room temperature in the Kagome magnet Fe3Sn2 using small angle neutron scattering, muon spin rotation, and magnetoresistivity measurement techniques. The average bulk spin direction and magnetic domain texture can be tuned effectively by small magnetic fields. Magnetoresistivity, in response,…
We report on the observation of a large topological Hall effect (THE) over a wide temperature region in a geometrically frustrated Fe3Sn2 magnet with a kagome-bilayer structure. We found that the magnitude of the THE resistivity increases with temperature and reaches -0.875 μΩ.cm at 380 K. Moreover, the critical magnetic fields with the change of THE are consistent with the magnetic structure transformation, which indicates that the real-space fictitious magnetic field is proportional to the formation of magnetic skyrmions in Fe3Sn2. The results strongly suggest that the large THE originates f…
The magnetization process of single crystals of the metallic kagomé ferromagnet Co3Sn2S2 was carefully measured via magnetization and AC susceptibility. Field-dependent anomalous transitions in the magnetization indicate a low-field unconventionally ordered phase stabilized just below TC. The magnetic phase diagrams in applied fields along different crystallographic directions were determined. The magnetic relaxation process studied in frequencies covering five orders of magnitude from 0.01 to 1000 Hz indicates characteristic relaxation times of several seconds at the boarders of the anomalous…
This study examines the effect of distorted triangular magnetic interactions in the Kagome lattice. Using a Holstein-Primakoff expansion, we determine the analytical solutions for classical energies and the spin-wave modes for various magnetic configurations. By understanding the magnetic phase diagram, we characterize the changes in the spin waves and examine the spin distortions of the ferromagnetic (FM), Antiferrimagnetic (AfM), and 120$^{\circ}$ phases that are produced by variable exchange interactions and lead to various non-collinear phases, which provides a deeper understanding of the …
We report magnetic and electrical properties for single crystals of NdMn$_6$Sn$_6$ and SmMn$_6$Sn$_6$. They crystallize into a structure which has distorted, Mn-based kagome lattices, compared to the pristine kagome lattices in heavy-rare-earth-bearing RMn$_6$Sn$_6$ compounds. They are hightemperature ferromagnets of which the R moment is parallel with the Mn moment. We observed a large intrinsic anomalous Hall effect (AHE) that is comparable to the ferrimagnetic, heavy-R siblings in a wide range of temperature. We conclude that their intrinsic AHE is stemming from the Mn-based kagome lattice,…
The search for two dimensional quantum spin liquids, exotic magnetic states with an entangled ground state remaining disordered down to zero temperature, has been a great challenge in frustrated magnetism during the last decades. Recently, fractionalized excitations, called spinons, emerging from these states, have been evidenced in kagome and triangular antiferromagnets. In contrast, quantum ferromagnetic spin liquids in two dimensions, namely quantum kagome ices, have been less investigated, yet their classical counterparts exhibit amazing properties, magnetic monopole crystals as well as ma…
The structural-magnetic models of 25 AFM kagome cuprates similar to herbertsmithite (ZnCu3(OH)6Cl2) - a perspective spin liquid - have been calculated and analyzed. Main correlations between the structure and magnetic properties of these compounds were revealed. It has been demonstrated that, in all AFM kagome cuprates, including herbertsmithite, there exists the competition between the exchange interaction and the antisymmetric anisotropic exchange one (the Dzyaloshinskii-Moriya interaction), as magnetic ions are not linked to the center of inversion in the kagome lattice. This competition is…
The competition between interactions in frustrated magnets allows a wide variety of new ground states, often exhibiting emergent physics and unique excitations. Expanding the suite of lattices available for study enhances our chances of finding exotic physics. Mn$_2$Sb$_2$O$_7$ forms in a chiral, kagome-based structure in which a fourth member is added to the kagome-plane triangles to form an armchair unit and link adjacent kagome planes. This structural motif may be viewed as intermediate between the triangles of the kagome network and the tetrahedra in the pyrochlore lattice. Mn$_2$Sb$_2$O$_…
Exploration of the topological quantum materials with electron correlation is at the frontier of physics, as the strong interaction may give rise to new topological phases and transitions. Here we report that a family of kagome magnets RMn$_6$Sn$_6$ manifest the quantum transport properties analogical to those in the quantum-limit Chern magnet TbMn$_6$Sn$_6$. The topological transport in the family, including quantum oscillations with nontrivial Berry phase and large anomalous Hall effect arising from Berry curvature field, points to the existence of massive Dirac fermions. Our observation dem…
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…
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.
Compounds with a Kagome type lattice are known to exhibit magnetic frustration. Large single crystals of two compounds Ni3V2O8 and Co3V2O8, which are variants of a Kagome net lattice, have been grown successfully by the floating zone technique using an optical image furnace. The single crystals are of high quality and exhibit intriguing magnetic properties.
We investigate the connection between highly frustrated kagome based Hamiltonians and a recently synthesized family of materials containing Ti3+ S=1/2 ions. Employing a combination of all electron density functional theory and numerical diagonalization techniques, we establish the Heisenberg Hamiltonians for the distorted kagome antiferromagnets Rb2NaTi3F12, Cs2NaTi3F12 and Cs2KTi3F12. We determine magnetization curves in excellent agreement with experimental observations. Our calculations successfully clarify the relationship between the experimental observations and the magnetization-plateau…
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 present the crystal structures and magnetic properties of RE3Sb3Mg2O14 (La3Sb3Mg2O14, Pr3Sb3Mg2O14, Sm3Sb3Mg2O14, Eu3Sb3Mg2O14, Tb3Sb3Mg2O14, and Ho3Sb3Mg2O14), a family of novel materials based on a perfect geometry 2D rare earth Kagome lattice. Structure refinements were performed by the Rietveld method using X-ray diffraction data, indicating that the layered compounds are fully structurally ordered. The compounds crystallize in a rhombohedral supercell of the cubic pyrochlore structure, in the space group R-3m. As indicated by magnetic susceptibility measurements, they exhibit predomina…
We investigate the low temperature magnetic properties of a $S=\frac{5}{2}$ Heisenberg kagomé antiferromagnet, the layered monodiphosphate Li$_9$Fe$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$, using magnetization measurements and $^{31}$P nuclear magnetic resonance. An antiferromagnetic-type order sets in at $T_{\rm N}=1.3$ K and a characteristic magnetization plateau is observed at 1/3 of the saturation magnetization below $T^* \sim 5$ K. A moderate $^{31}$P NMR line broadening reveals the development of anisotropic short-range correlations within the plateau phase concomitantly with a gapless spin-latti…
Low temperature magnetic and structural behavior of the extended Kagome system YBaCo4O7 has been studied by single crystal neutron diffraction and high-resolution powder X-ray diffraction. Long-range magnetic ordering associated with a structural transition from orthorhombic Pbn2_1 to monoclinic P2_1 symmetry has been found at T_1 ~ 100 K. The interplay between the structural and magnetic degrees of freedom testifies that the degeneracy of the magnetic ground state, present in the orthorhombic phase, is lifted through a strong magnetoelastic coupling, as observed in other frustrated systems. A…
The kagome lattice, consisting of interconnected triangles and hexagons uniquely, is an excellent model system for study frustrated magnetism, electronic correlation and topological electronic structure. After an intensive investigation on frustrated magnetism in insulating magnetic kagome lattices, the interplay between charge and spin degrees of freedom via spin-orbital coupling in metallic systems (kagome metals) has become an attractive topic recently. Here, we study centrosymmetric YMn6Sn6 with Mn kagome lattice. We discover that it exhibits giant topological Hall effect near room tempera…
The magnetization process of the spin-S Heisenberg antiferromagnet on the kagome lattice is studied by the numerical-diagonalization method. Our numerical-diagonalization data for small finite-size clusters with S=1, 3/2, 2, and 5/2 suggest that a magnetization plateau appears at one-third of the height of the saturation in the magnetization process irrespective of S. We discuss the S dependences of the edge fields and the width of the plateau in comparison with recent results obtained by real-space perturbation theory.
Recently, kagome materials have become an engrossing platform to study the interplay among symmetry, magnetism, topology, and electron correlation. The latest works on RMn6Sn6 (R = rare earth metal) compounds have illustrated that this family could be intriguing to investigate various physical phenomena due to large spin-orbit coupling and strong magnetic ordering. However, combined transport and spectroscopic studies in RMn6Sn6 materials are still limited. Here, we report magnetic, magneto-transport, and angle-resolved photoemission spectroscopy measurements of a kagome magnet ErMn6Sn6 that u…
The kagome lattice -- a two-dimensional (2D) arrangement of corner-sharing triangles -- is at the forefront of the search for exotic states generated by magnetic frustration. Such states have been observed experimentally for Heisenberg and planar spins. In contrast, frustration of Ising spins on the kagome lattice has previously been restricted to nano-fabricated systems and spin-ice materials under applied magnetic field. Here, we show that the layered Ising magnet Dy3Mg2Sb3O14 hosts an emergent order predicted theoretically for individual kagome layers of in-plane Ising spins. Neutron-scatte…
YBaCo4O7 belongs to a new class of geometrically frustrated magnets like the pyrochlores, in which Co-spins occupy corners of tetrahedra. The structure can be viewed as an alternating stacking of Kagome and triangular layers. Exactly half of the triangular units of the Kagome plane are capped by Co ions to form columns running perpendicular to the Kagome sheets. Neutron powder diffraction reveals a broad temperature range of diffuse magnetic scattering, followed by long range magnetic ordering below 110K. A unique low-temperature magnetic structure simultaneously satisfies an S=0 arrangement i…
The magnetization process of the S=1/2 Heisenberg antiferromagnet on the kagome lattice is studied by the numerical-diagonalization method. We successfully obtain a new result of the magnetization process of a 42-site cluster in the entire range. Our analysis clarifies that the critical behavior around one-third of the height of the saturation is different from the typical behavior of the well-known magnetization plateau in two-dimensional systems. We also examine the effect of the $\sqrt{3}\times\sqrt{3}$-type distortion added to the kagome lattice. We find at one-third of the height of the s…
Quantum materials, particularly Dirac materials with linearly dispersing bands, can be effectively tuned by strain-induced lattice distortions leading to a pseudo-magnetic field that strongly modulates their electronic properties. Here, we grow kagome magnet FeSn films, consisting of alternatingly stacked Sn$_2$ honeycomb (stanene) and Fe$_3$Sn kagome layers, on SrTiO$_3$(111) substrates by molecular beam epitaxy. Using scanning tunneling microscopy/spectroscopy, we show that the Sn honeycomb layer can be periodically deformed by epitaxial strain for film thickness below 10 nm, resulting in di…
Magnetic materials with kagome crystal structure exhibit rich physics such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here we report the synthesis of high-quality epitaxial films of topological kagome magnet Fe$_3$Sn$_2$ by atomic layer molecular beam epitaxy. Structural and magnetic characterization of Fe$_3$Sn$_2$ on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies o…
We obtain a classical spin liquid (CSL) phase by applying a magnetic field in $J_1$-$J_2$-$J_3$ Ising model on a kagome lattice. As we proved in the previous study [Phys. Rev. Lett. {\bf 119}, 077207 (2017)], this model realizes one species of CSL, the hexamer CSL, at zero magnetic field, which consists of macroscopically degenerate spin configurations with mixed total magnetization, $M$. The magnetic field selects its subset, which can be mapped to a trimer covering of the dual lattice, and forms a magnetization plateau of $M=1/9$. In addition to this CSL, we find two other magnetization plat…
Anomalous magnetotransport in a non-collinear correlated kagome ferromagnet MgMn6Sn6
S. N. Bose National Centre for Basic Sciences（S.N. 玻色基础科学国家中心）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；ISIS Neutron and Muon Source, Science and Technology Facilities Council, Rutherford Appleton Laboratory（ISIS中子与μ子源，科学与技术设施委员会，拉瑟福德阿普尔顿实验室）；School of Physical Sciences, Indian Institute of Technology Goa（印度果阿理工学院物理科学学院）
We study the magnetization process of the spin-$1/2$ Heisenberg antiferromagnet on a distorted square-kagome lattice by the numerical-diagonalization method. The magnetization jump at one-third of the height of the saturation is examined in detail; we find that the jump becomes larger when a small distortion is switched on and that it is accompanied by an abrupt change in lines along microscopic spin directions. Our finite-size results successfully confirm that the magnetization jump in a spin-isotropic system is a macroscopic jump that survives in the thermodynamic limit and that the changes …
We have successfully synthesized S = 1/2 kagome antiferromagnets MCu3(OH)6Cl2 (M = Ni and Co) by hydrothermal method with rotating pressure vessel. Structural characterization shows that both compounds have the similar crystal structure as ZnCu3(OH)6Cl2 with R-3m symmetry. Similar to ZnCu3(OH)6Cl2, the compounds show no obvious hysteresis at 2 K. A spin glass transition is found in both NiCu3(OH)6Cl2 and CoCu3(OH)6Cl2 at low temperatures (6.0 and 3.5 K respectively) by AC susceptibility measurements. It indicates no long-range magnetic order and a strong spin frustration. The substitution of Z…
The study of quantum spin-liquid states (QSL) with lattice dimension $>1$ has proven an enduring problem in solid state physics. Key candidate materials are the $S=\frac{1}{2}$ kagome magnets due to their ability to host quantum fluctuations within the high degeneracy of their frustrated geometries. Studies of an increasing library of known $S=\frac{1}{2}$ kagome magnetic materials has challenged our understanding of the possible QSL states, for example, the recent discovery of a chiral spin-liquid ground state in kapellasite showed that even magnets with ferromagnetic nearest-neighbour exchan…
The dielectric constant of the Kagome staircase-like Co3V2O8 polycrystalline compound has been measured as function of temperature and magnetic field up to 14T. It is found that the application of an external magnetic field suppresses the anomaly for the dielectric constant beyond 6.1K. Furthermore, its magnetic field dependence reveals a negative magnetocapacitance which is proportional to the magnetic susceptibility, suggesting a common magnetostrictive origin for the magnetic field dependence of the two quantities. This result is very different from that obtained from the isostructural comp…
The kagome-lattice crystal hosts various intriguing properties including the frustrated magnetism, charge order, topological state, superconductivity and correlated phenomena. To achieve high-performance kagome-lattice compounds for electronic and spintronic applications, careful tuning of the band structure would be desired. Here, the electronic structures of kagome-lattice crystal Ni3In2S2 were investigated by transport measurements, angle-resolved photoemission spectroscopy as well as ab initio calculations. The transport measurements reveal Ni3In2S2 as a compensated semimetal with record-h…
Co3Sn2S2 is a ferromagnetic Weyl semimetal that has been the subject of intense scientific interest due to its large anomalous Hall effect. We show that the coupling of this material's topological properties to its magnetic texture leads to a strongly exchange biased anomalous Hall effect. We argue that this is likely caused by the coexistence of ferromagnetism and spin glass phases, the latter being driven by the geometric frustration intrinsic to the Kagome network of magnetic ions.
An extensive low temperature magnetisation study of high quality single crystals of the Kagome staircase compounds Ni3V2O8 and Co3V2O8 has been performed, and the H-T phase diagrams have been determined from these measurements. The magnetisation and susceptibility curves for Co3V2O8 are analysed in terms of their compatibility with the different ferromagnetic and antiferromagnetic structures proposed for this compound. For Ni3V2O8, the phase diagram is extended to magnetic fields higher than previously reported; for a field applied along the a-axis, the low temperature incommensurate phase is …
We have searched nearly 40,000 inorganic solids in the Inorganic Crystal Structural Database to identify compounds containing a transition metal or rare earth kagomé sublattice, a geometrically magnetically frustrated lattice, ultimately identifying $\sim$500 materials. A broad analysis of the chemical and structural trends of these materials shows three types of kagomé sheet stacking and several classes of magnetic complexity. Following the search and classification, we rapidly screen the magnetic properties of a subset of the materials using density functional theory to eliminate those that …
Inelastic neutron scattering measurements have been performed on single crystal samples of Co3V2O8 and Ni3V2O8. The magnetic system in these compounds is believed to be frustrated, as the magnetic ions Co2+ with S=3/2 and Ni2+ with S=1 adopt a buckled version of the Kagome lattice. Magnetic excitations have been observed in both samples using a time-of-flight neutron spectrometer. The excitation spectrum is dispersive for both samples and has a considerable gap in the low temperature phases, while the intermediate temperature phases are marked by a significant softening of the excitations ener…
Various and spontaneous magnetic skyrmionic bubbles are experimentally observed for the first time, at room temperature in a frustrated kagome magnet Fe3Sn2 with unixial magnetic anisotropy. The magnetization dynamics were investigated using in-situ Lorentz transmission electron microscopy, revealing that the transformation between different magnetic bubbles and domains are via the motion of Bloch lines driven by applied external magnetic field. The results demonstrate that Fe3Sn2 facilitates a unique magnetic control of topological spin textures at room temperature, making it a promising cand…
Nature of magnetic exchange interactions in kagome antiferromagnets FeGe and FeSn
Institute of High Pressure Physics, School of Physical Science and Technology, Ningbo University（宁波大学物理科学与技术学院高压物理研究所）；College of Science, Nanjing University of Aeronautics and Astronautics（南京航空航天大学理学院）
Materials with a layered Kagome lattice are expected to give rise to novel physics arising from band structures with topological properties, spin liquid behavior and the formation of skyrmions. Until now, most work on Kagome materials has been performed on bulk samples due to difficulties in thin film synthesis. Here, by using molecular beam epitaxy, layered Kagome-structured FeSn films are synthesized on (111) oriented LaAlO3 substrate. Both in-situ and ex-situ characterizations indicate these films are highly crystalline and c-axis oriented, with atomically smooth surfaces. However, the film…
Here we report crystallographic and magnetic studies on high quality samples of the magnetically frustrated S = 1/2 kagome antiferromagnet vesignieite, BaCu3V2O8(OD)2. Powder neutron diffraction data collected from samples obtained by a new hydrothermal synthetic route reveal a previously unobserved trigonal P3121 structure, similar to the isoelectronic mineral SrCu3V2O8(OH)2. The refined structure is consistent with orbital frustration of the eg d-orbitals in a sublattice of the Cu2+ kagome network due to a dynamic Jahn-Teller effect, which persists below the magnetic transition at TN = 9K an…
We theoretically study the carrier doping effect for magnetism in a stacked-kagome system $\rm{{Co}_3{Sn}_2{S}_2}$ based on an effective model and the Hartree-Fock method. We show the electron filling and temperature dependences of the magnetic order parameter. The perpendicular ferromagnetic ordering is suppressed by hole doping, wheres undoped $\rm{{Co}_3{Sn}_2{S}_2}$ shows magnetic Weyl semimetal state. Additionally, in the electron-doped regime, we find a non-collinear antiferromagnetic ordering. Especially, in the non-collinear antiferromagnetic state, by considering a certain spin-orbit …
