Distorted Kagome Lattice Research Articles

Magnetic coupled electronic landscape in bilayer-distorted titanium-based kagome metals

Quantum materials whose atoms are arranged on a lattice of corner-sharing triangles, i.e., the kagome lattice, have recently emerged as a captivating platform for investigating exotic correlated and topological electronic phenomena. Here, we combine ultralow temperature angle-resolved photoemission spectroscopy (ARPES) with scanning tunneling microscopy and density functional theory calculations to reveal the fascinating electronic structure of the bilayer-distorted kagome material LnTi3Bi4, where stands for Nd and Yb. Distinct from other kagome materials, LnTi3Bi4 exhibits twofold, rather than sixfold, symmetries, stemming from the distorted kagome lattice, which leads to a unique electronic structure. Combining experiment and theory we map out the electronic structure and discover double flat bands as well as multiple Van Hove singularities (VHSs), with one VHS exhibiting higher-order characteristics near the Fermi level. Notably, in the magnetic version NdTi3Bi4, the ultralow base temperature ARPES measurements unveil an unconventional band splitting in the band dispersions which is induced by the ferromagnetic ordering. These findings reveal the potential of bilayer-distorted kagome metals LnTi3Bi4 as a promising platform for exploring novel emergent phases of matter at the intersection of strong correlation and magnetism. Published by the American Physical Society 2024

Observation of Thermally Induced Piezomagnetic Switching in Cu2OSeO3 Polymorph Synthesized under High‐Pressure

AbstractA polymorph of Cu2OSeO3 with the distorted kagome lattice is successfully obtained using the high‐pressure synthesis technique (Cu2OSeO3‐HP). The structural analysis using X‐ray and neutron powder diffraction suggests that the tetrahedral Cu2+ clusters [similar to those in Cu2OSeO3 ambient‐pressure phase (Cu2OSeO3‐AP)] exist in Cu2OSeO3‐HP but with three symmetry inequivalent sites. No structural change is observed between 1.5 K and the room temperature. The complex magnetic H‐T phase diagram is established based on the temperature‐ and field‐dependent magnetization data, indicating two distinct antiferromagnetic phases at low and intermediate temperatures, in addition to the higher‐temperature spin‐glass‐like phase. The low temperature phase is identified by neutron powder diffraction refinements as a canted noncollinear antiferromagnetic order with a weak ferromagnetic component along the b‐axis. Size of the refined ordered moment is ≈1.00(4) µB in Cu2OSeO3‐HP, indicating a large enhancement compared to that of Cu2OSeO3‐AP (≈0.61 µB). By applying a uniaxial stress, finite enhancement of weak ferromagnetic component in the noncollinear antiferromagnetic phase in Cu2OSeO3‐HP is observed, which is the clear evidence of the piezomagnetic effect. Interestingly, the sign of the induced magnetization changes on heating from the low‐temperature to the intermediate‐temperature phases, indicating a novel piezomagnetic switching effect in this compound.

Lifshitz Transition in a Single-Atom-Thick GdxYb1-xPb3 Kagome Compound on Si(111).

Lanthanide (Ln) elements Gd and Yb alloyed with a Pb monolayer on the Si(111) substrate form LnPb3 compounds having the same crystal structure. They comprise a single-atom-thick Pb layer arranged in a slightly distorted kagome lattice with Ln atoms filling the hexagonal voids. They have similar electronic band structures except for the Fermi level position, which varies between the divalent Yb- and trivalent Gd-containing compounds by ∼0.47 eV. The ability to create a 2D solid solution with the unified continuous Pb layer and hexagonal voids randomly filled with either Gd or Yb atoms allows precise control of the Fermi level position. Small alteration of the Fermi level triggers drastic changes in the Fermi surface topology due to the Lifshitz transition, hence in the physical properties. In particular, the sheet resistance of the GdxYb1-xPb3/Si(111) system can be controllably varied over an order of magnitude range.

Enhancement of the anomalous Hall effect by distorting the Kagome lattice in an antiferromagnetic material

In topological magnetic materials, the topology of the electronic wave function is strongly coupled to the structure of the magnetic order. In general, ferromagnetic Weyl semimetals generate a strong anomalous Hall conductivity (AHC) due to a large Berry curvature that scales with their magnetization. In contrast, a comparatively small AHC is observed in noncollinear antiferromagnets. We investigated HoAgGe, an antiferromagnetic (AFM) Kagome spin-ice compound, which crystallizes in a hexagonal ZrNiAl-type structure in which Ho atoms are arranged in a distorted Kagome lattice, forming an intermetallic Kagome spin-ice state in the ab-plane. It exhibits a large topological Hall resistivity of ~1.6 µΩ-cm at 2.0 K in a field of ~3 T owing to the noncoplanar structure. Interestingly, a total AHC of 2,800 Ω-1 cm-1 is observed at ~45 K, i.e., 4 TN, which is quite unusual and goes beyond the normal expectation considering HoAgGe as an AFM Kagome spin-ice compound with a TN of ~11 K. We demonstrate further that the AHC below TN results from the nonvanishing Berry curvature generated by the formation of Weyl points under the influence of the external magnetic field, while the skew scattering led by Kagome spins dominates above the TN. These results offer a unique opportunity to study frustration in AFM Kagome lattice compounds.

Higher‐Order Topological Corner States in a Specially Distorted Photonic Kagome Lattice

AbstractKagome lattices have garnered significant interest over the decades due to their rich physics and implications for exotic superconductors and topological materials. In particular, the so‐called “breathing Kagome lattice” (BKL) is often used as a prototypical model to understand higher‐order topological insulators. Here it is demonstrated that higher‐order corner states exist in a specially distorted Kagome lattice, resembling the “Inverse Hexagram” lattice distortion originally introduced in the study of charge density waves in Kagome metals. Importantly, it is found that such an Inverse Hexagram‐like Kagome lattice with C6 rotational symmetry hosts two types of in‐gap corner states, in contrast to a flat‐cutting BKL of C3 symmetry that supports only one type of corner state under the tight‐binding condition. It is shown that the nontrivial corner states exhibit a fractional corner anomaly, revealing the feature of higher‐order topology. Using laser‐written waveguide lattices as a photonic platform, these two types of corner states are experimentally observed, along with a direct comparison with the corner excitation at their trivial counterparts. Experimental observations are further corroborated by numerical simulations and stability analysis under random perturbation. These results may prove relevant and applicable to similar phenomena in other Kagome platforms beyond photonics.

Controlled Frustration Release on the Kagome Lattice by Uniaxial-Strain Tuning.

It is predicted that strongly interacting spins on a frustrated lattice may lead to a quantum disordered ground state or even form a quantum spin liquid with exotic low-energy excitations. However, a controlled tuning of the frustration strength, separating its effects from those of disorder and other factors, is pending. Here, we perform comprehensive ^{1}H NMR measurements on Y_{3}Cu_{9}(OH)_{19}Cl_{8} single crystals revealing an unusual Q[over →]=(1/3×1/3) antiferromagnetic state below T_{N}=2.2 K. By applying insitu uniaxial stress, we break the symmetry of this disorder-free, frustrated kagome system in a controlled manner yielding a linear increase of T_{N} with strain, in line with theoretical predictions for a distorted kagome lattice. In-plane strain of ≈1% triggers a sizable enhancement ΔT_{N}/T_{N}≈10% due to a release of frustration, demonstrating its pivotal role for magnetic order.

Magnetic structure of the S = ½ staircase kagome lattice PbCu3TeO7

The crystal and magnetic structure characterization of geometrically distorted PbCu3TeO7 with S=1/2 Cu2+ spins forming a staircase kagome lattice was investigated using x-ray and neutron diffraction on a powder sample. The distorted kagome lattice of antiferromagnet PbCu3TeO7 exhibits a quasi-two-dimensional spin network. The x-ray diffraction data show that PbCu3TeO7 crystallizes in the orthorhombic system in the space group Pnma (No. 62). The lattice parameters a = 10.488(1) Å, b = 6.353(1) Å, and c = 8.814(2) Å. Our temperature-dependent x-ray diffraction data show that there is no structure phase transition between 12 and 298 K. From our powder neutron diffraction data at 2 K, we observed two distinct magnetic Bragg peaks at low angles, confirming the magnetic transition to the ordered state at low temperatures. In previous work, the ordering vector for the magnetic structure was determined using simulations to be (0,1/3,0). However, in this work, we found that based on the neutron diffraction data the ordering vector is in fact (0,1/3,1/3). The magnetic structure of PbCu3TeO7 exhibiting an antiferromagnet with noncollinear spin order is proposed.

Constructing Two-Dimensional Distorted Kagome Lattices on Ag(111).

Two-dimensional (2D) tessellation of organic species acquired increased interest recently because of their potential applications in physics, biology, and chemistry. Herein, we successfully synthesized the chiral distorted Kagome lattice p3 (333) with bicomponent precursors on Ag(111). Scanning tunneling microscopy and density functional calculation studies reveal that the networks are formed by multiple intermolecular hydrogen bonds. The network structures can be rationally tuned by adjusting the stoichiometric ratio of the reaction precursors. Our study provides new strategies to synthesize complex low-dimensional nanostructures on metal surfaces.

Magnetic field induced reentrant multipolar ordering in the distorted kagome-lattice antiferromagnet Dy3Ru4Al12

We report on ultrasonic and magnetocaloric-effect measurements of the hexagonal antiferromagnet ${\mathrm{Dy}}_{3}{\mathrm{Ru}}_{4}{\mathrm{Al}}_{12}$ having a distorted kagome lattice. We observed a pronounced softening of the transverse modulus, ${C}_{44}$, above 30 T applied along [100], indicating an as-yet-unidentified magnetic field induced phase transition. We determined the field-temperature phase diagrams using pulsed magnetic fields up to 55.2 T, applied along [100] and [001]. Optimizing crystal-electric-field parameters within the mean-field approximation, we conclude that the enhancement of the field induced phase-transition temperature is due to electric quadrupolar and magnetic octupolar mediated interactions. We propose that the order parameter of the magnetic field induced phase transitions is the electric quadrupole ${O}_{zx}$, facilitated by octupole-mediated interactions.

Magnetic phases of the frustrated ferromagnetic spin-trimer system Gd3Ru4Al12 with a distorted kagome lattice structure

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.

New two-dimensional flat band materials: B3C11O6 and B3C15O6.

Recently, there has been growing interest in the field of flat-band physics due to its attractive properties and wide range of practical applications. In this study, we introduce two novel two-dimensional monolayers, namely B3C11O6 and B3C15O6, which exhibit a flat band near the Fermi level. These monolayers have been found to be energetically favorable, dynamically stable, and thermodynamically stable based on formation energies, phonon spectra, and molecular dynamics simulations. The nearly flat band (NFB) in B3C11O6 arises from the extended kagome sublattice of carbon atoms. Due to the strong interaction between carbon atoms beyond their nearest neighbors, the bandwidth of the initial flat band is extended to approximately 0.5 eV. Nevertheless, there is still a prominent peak in the density of states near the Fermi level. On the other hand, the NFB in B3C15O6 originates from the localized states of the carbon five-ring structure, which forms a distorted kagome lattice. The presence and characteristics of the NFB strongly depend on the interactions between next-nearest neighbors. Interestingly, the partially occupied NFB in B3C11O6 leads to spin splitting, resulting in a transformation of the system into a ferromagnetic metal. Our research not only presents two types of lattices capable of hosting flat bands or NFBs, but also provides two monolayers that can be employed to investigate various intriguing quantum phases.

Incommensurate Magnetic Order in Sm3BWO9 with Distorted Kagome Lattice

We investigate the magnetic ground state of Sm3BWO9 with a distorted kagome lattice. A magnetic phase transition is identified at T N = 0.75 K from the temperature dependence of specific heat. From 11B nuclear magnetic resonance measurements, an incommensurate magnetic order is shown by the double-horn type spectra under a c-axis magnetic field, and absence of line splitting is observed for field oriented within the ab-plane, indicating the incommensurate modulation of the internal field strictly along c-axis. From the spin dynamics, the critical slowing-down behavior is observed in the temperature dependence of 1/T 1 with μ 0 H⊥c-axis, which is completely absent in the case with μ 0 H||c-axis. Based on the local symmetry of 11B sites, we analyze the hyperfine coupling tensors and propose two constraints on the possible magnetic structure. The single ion anisotropy should play an important role in determination of contrasting ground states of Sm3BWO9 and Pr3BWO9.

Second-Harmonic-Generation Effect and Giant Optical Birefringence in the Weyl Material CaAgAs.

Nonlinear-optical (NLO) materials suitable for the "8-14 μm" atmospheric transparent window are in urgent need. Arsenide is one of the most promising material systems for such an application. However, the second-harmonic-generation (SHG) effect of arsenide is difficult to characterize using the conventional powder SHG technique with a 2 μm fundamental laser. To overcome this problem, we focused on a novel arsenide Weyl material, CaAgAs, with a zero band gap and proposed a modified powder SHG measurement method for narrow-band-gap materials. We successfully observed the SHG signal of CaAgAs, which was approximately 0.7 times that of CdGeAs2. Moreover, on the basis of first-principles calculations, the largest SHG coefficient for CaAgAs is equal to 236 pm/V, and the ionic bonds in the [Ca3As13] motif play an indispensable role for the SHG effect because of the distorted Kagome lattice pattern. CaAgAs is predicted to have strong optical anisotropy with a giant optical birefringence of 0.52.

Cluster quantum Monte Carlo study of two-dimensional weakly coupled frustrated trimer antiferromagnets

We report results from spin trimer-based cluster quantum Monte Carlo simulations for the thermodynamic properties of two-dimensional frustrated quantum antiferromagnets that are composed of weakly-coupled three-spin (trimer) clusters. In particular, we consider the spin-1/2 kagome lattice with a strong breathing distortion, and the triangle-square lattice model proposed previously for the cuprate La${}_4$Cu${}_3$MoO${}_{12}$. For both cases, we demonstrate that an appropriately chosen trimer-based computational basis allows us to significantly reduce the quantum Monte Carlo sign problem down to the low-temperature regime. Besides exploring the thermodynamic behavior for the triangle-square lattice model we also assess a mean field theory-based prediction for the onset of chiral order. For the breathing distorted kagome lattice model, we observe a robust two-peak structure in the specific heat, both in the quantum spin liquid and the lattice-nematic regimes.

Multi‐Center Magnon Excitations Open the Entire Brillouin Zone to Terahertz Magnetometry of Quantum Magnets

AbstractDue to the small photon momentum, optical spectroscopy commonly probes magnetic excitations only at the center of the Brillouin zone; however, there are ways to override this restriction. In case of the distorted kagome quantum magnet Y‐kapellasite, Y3Cu9(OH)19Cl8, under scrutiny here, the spin (magnon) density of states (SDOS) can be accessed over the entire Brillouin zone through three‐center magnon excitations. This mechanism is aided by the three different magnetic sublattices and strong short‐range correlations in the distorted kagome lattice. The results of THz time‐domain experiments agree remarkably well with linear spin‐wave theory (LSWT). Relaxing the conventional zone‐center constraint of photons gives a new aspect to probe magnetism in matter.

Supramolecular Tiling of a Conformationally Flexible Precursor.

Supramolecular self-assembly offers a possible pathway for nanopatterning and functionality. In particular, molecular tiling such as trihexagonal tiling (also known as the Kagome lattice) has promising chemical and physical properties. Distorted Kagome lattices are not well understood due to their complexity, and studies of their controllable fabrication are few. Here, by employing a conformationally flexible precursor, 2,4,6-tris(3-bromophenyl)-1,3,5-triazine (mTBPT), we demonstrate two-dimensional distorted Kagome lattice p3, (333) by supramolecular self-assembly and achieve tuning of the metastable phases, including the homochiral porous network and distorted Kagome lattice p3, (333) by steering deposition rates on a cold Ag(111) substrate. By a combination of scanning tunneling microscopy and density functional theory calculations, the distorted Kagome lattice is energetically unfavorable but can be trapped at a high deposition rate, and the process mainly depends on surface kinetics. This work using conformationally flexible mTBPT molecules provides a pathway for the controllable growth of different phases, including metastable Kagome lattices.

Local evidence for collective spin excitations in the distorted kagome antiferromagnet Pr3BWO9

We report the local probe investigation of a frustrated antiferromagnet Pr$_3$BWO$_9$ with the distorted kagome lattice. Absence of magnetic order or spin freezing is indicated by the spectral analysis down to 0.3 K and specific heat measurements down to 0.09 K. The Knight shifts show an upturn behavior with the sample cooling down, which is further suppressed by external field. For the spin dynamics, gapped spin excitation is observed from the temperature dependence of spin-lattice relaxation rates, with the gap size proportional to the applied magnetic field intensity. Comparatively, an unexpected sharp peak is observed in the nuclear spin-spin relaxation rate data at $T^*\sim 4-5$ K. These results indicate an unconventional persistent fluctuating paramagnetic ground state with antiferromagnetic collective spin excitations in the strongly frustrated spin system.

Pressure-induced tuning of quantum spin liquid state in ZnCu3(OH)6Cl2

Mineral Herbertsmithite, ${\mathrm{ZnCu}}_{3}{(\mathrm{OH})}_{6}{\mathrm{Cl}}_{2}$, is an excellent candidate for S = 1/2 Heisenberg kagome antiferromagnet supporting quantum spin liquid (QSL) ground state at low temperature and ambient pressure. The pressure-induced structural evolution of the kagome lattice in Herbertsmithite has been investigated up to 16 GPa using x-ray diffraction and Raman scattering measurements. The system develops a distorted kagome lattice structure (clinoatacamite-like) beyond 8 GPa. This is accompanied by gradual suppression of the quasi-elastic Raman scattering intensity. Our high pressure magnetic susceptibility measurements indicate the emergence of a weak magnetic ordering in the distorted kagome lattice. Pressure-induced enhancement of the magnetic ordering temperature supports a gapped topological QSL rather than gapless ground state close to a quantum critical point. High-pressure optical absorption measurements support the structural evolution.

Synthesis of a New Ruthenate Ba26Ru12O57

Single crystals of Ba 26 Ru 12 O 57 were grown by the floating zone method. The crystal structure is formed by an alternating stacking of pseudo-hexagonal Ru single layers and double layers. The Ru ions within the double layers are dimerized (Ru 2 O 9 ) whereas the Ru ions within the single layers arrange in a distorted Kagome lattice of trigonal bipyramidally coordinated RuO 5 polyhedra. Additionally, this Kagome lattice is “decorated” with RuO 6 octahedra that are situated in the central free spaces within this Kagome lattice. According to the composition, the oxidation state of most of the Ru ions should be formally close to 5+.

Crystal-field effects in Er3Ru4Al12 with a distorted kagome lattice

Crystal-field effects in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>Er</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:msub><mml:mi>Ru</mml:mi><mml:mn>4</mml:mn></mml:msub><mml:msub><mml:mi>Al</mml:mi><mml:mn>12</mml:mn></mml:msub></mml:mrow></mml:math> with a distorted kagome lattice