Two kagome compounds, volborthite Cu3V2O7(OH)2-2H2O and herbertsmithite ZnCu3(OH)6Cl2, are compared in order to derive information about the intrinsic properties of the spin-1/2 kagome antiferromagnet. Volborthite shows a broad maximum at T ~ J / 4 and the approach at T = 0 to a large finite value of the bulk magnetic susceptibility chi_bulk as well as the local susceptibility chi_local from NMR measurements. These must be intrinsic properties for the spin-1/2 kagome antiferromagnet, as similar behavior has also been reported in chi_local for herbertsmithite [Olariu A et al. 2008 Phys. Rev. Lett., 100 087202]. Impurity effects that may significantly influence the bulk properties are discussed.
A novel cuprate Volborthite, Cu3V2O7(OH)2-2H2O, containing an S-1/2 (Cu 2+ spin) kagome-like lattice is studied by magnetic susceptibility, specific heat, and 51 V NMR measurements. Signs for neither long-range order nor spin-gapped singlet ground states are detected down to 1.8 K, in spite of large antiferromagnetic couplings of ~100 K between Cu spins forming a two-dimensional kagome-like network. It is suggested that Volborthite represents a system close to a quantum critical point between classical long-range ordered and quantum disordered phases.
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…
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 thr…
Volborthite compound is one of the very few realizations of S=1/2 quantum spins on a highly frustrated kagome-like lattice. Low-T SQUID measurements reveal a broad magnetic transition below 2K which is further confirmed by a peak in the 51V nuclear spin relaxation rate (1/T1) at 1.4K$\pm$0.2K. Through 51V NMR, the ground state (GS) appears to be a mixture of different spin configurations, among which 20% correspond to a well defined short range order, possibly of the $\sqrt{3} \times \sqrt{3}$ type. While the freezing involve all the Cu$^{2+}$ spins, only 40% of the copper moment is actually f…
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…
Thermodynamic properties such as magnetic susceptibility and specific heat have been computed for the Heisenberg Antiferromagnet with spatially anisotropic exchange on the kagome lattice on clusters up to N=24 spins from the full spectra obtained by exact diagonalization. This approach is shown to provide a good represention of these thermodynamic properties above temperatures of about $J_{\rm av}/5$ where $J_{\rm av}$ is an average of the coupling constants. Comparison with experimental Volborthite data obtained by Hiroi {\it {et al}} [J. Phys. Soc. Jpn. {\bf 70},3377 (2001)] shows that Volbo…
Recent evidence from magnetic torque, electron spin resonance, and second harmonic generation indicate that the prototypical quantum spin liquid candidate, herbertsmithite, has a symmetry lower than its x-ray refined trigonal space group. Here, we consider known and possible distortions of this mineral class, along with related copper kagome oxides and fluorides, relate these to possible valence bond patterns, and comment on their relevance to the physics of these interesting materials.
Employing complementary torque magnetometry and electron spin resonance on single crystals of herbertsmithite, the closest realization to date of a quantum kagome antiferromagnet featuring a spin-liquid ground state, we provide novel insight into different contributions to its magnetism. At low temperatures, two distinct types of defects with different magnetic couplings to the kagome spins are found. Surprisingly, their magnetic response contradicts the three-fold symmetry of the ideal kagome lattice, suggesting the presence of a global structural distortion that may be related to the establi…
Despite tremendous investigations, a quantum spin liquid state realized in spin-1/2 kagome Heisenberg antiferromagnet remains largely elusive. In herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$, a quantum spin liquid candidate on the perfect kagome lattice, precisely characterizing the intrinsic physics of the kagome layers is extremely challenging due to the presence of interlayer Cu/Zn antisite disorder within its crystal structure. Here we measured the specific heat and thermal conductivity of single crystal herbertsmithite in magnetic fields with high resolution. Our results are highlighted by the …
We investigate the lattice dynamics in the spin-1/2 frustrated kagome compound herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$ by a combination of infrared spectroscopy measurements and ab initio density functional theory calculations, and provide an unambiguous assignment of infrared-active lattice vibrations involving in-plane and out-of-plane atom displacements in the kagome layers. Upon cooling, non-thermal red-shifts and broadening appear specifically for modes that deform the kagome layer or affect the Cu-O-Cu bond angles, thus creating pronounced modifications of the antiferromagnetic exchange c…
Strongly correlated Fermi systems are among the most intriguing and fundamental systems in physics, whose realization in some compounds is still to be discovered. We show that herbertsmithite ZnCu_3(OH)_6Cl_2 can be viewed as a strongly correlated Fermi system whose low temperature thermodynamic in magnetic fields is defined by a quantum critical spin liquid. Our calculations of its thermodynamic properties are in good agreement with recent experimental facts and allow us to reveal their scaling behavior which strongly resembles that observed in HF metals and 2D 3He.
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 …
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 …
We present magnetization measurements on oriented powder of ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$ along and perpendicular to the orienting field. We find a dramatic difference in the magnetization between the two directions. It is biggest at low measurement fields $H$ or high temperatures. We show that the difference at high temperatures must emerge from Ising-like exchange anisotropy. This allows us to explain muon spin rotation data at $T\to 0$ in terms of an exotic ferromagnetic ground state.
The spin-1/2 kagome lattice antiferromagnet herbertsmithite, ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$, is a candidate material for a quantum spin liquid ground state. We show that the magnetic response of this material displays an unusual scaling relation in both the bulk ac susceptibility and the low energy dynamic susceptibility as measured by inelastic neutron scattering. The quantity $χT^α$ with $α\simeq 0.66$ can be expressed as a universal function of $H/T$ or $ω/T$. This scaling is discussed in relation to similar behavior seen in systems influenced by disorder or by the proximity to a quantum crit…
Low energy inelastic neutron scattering on single crystals of the kagome spin liquid compound ZnCu3(OD)6Cl2 (Herbertsmithite) reveals antiferromagnetic correlations between impurity spins for energy transfers E < 0.8 meV (~J/20). The momentum dependence differs significantly from higher energy scattering which arises from the intrinsic kagome spins. The low energy fluctuations are characterized by diffuse scattering near wavevectors (1 0 0) and (0 0 3/2), which is consistent with antiferromagnetic correlations between pairs of nearest neighbor Cu impurities on adjacent triangular (Zn) interlay…
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…
Recently Han et al. have provided an analysis of the observed behavior of $\rm ZnCu_{3}(OH)_6Cl_2$ Herbertsmithite based on a separation of the contributions to its thermodynamic properties due to impurities from those due to the kagome lattice. The authors developed an impurity model to account for the experimental data and claimed that it is compatible with the presence of a small spin gap in the kagome layers. We argue that the model they advocate is problematic, conflicting with the intrinsic properties of $\rm ZnCu_{3}(OH)_6Cl_2$ as observed and explained in recent experimental and theore…
Measuring the specific heat of herbertsmithite single crystals in high magnetic fields (up to $34$ T) allows us to isolate the low-temperature kagome contribution while shifting away extrinsic Schottky-like contributions. The kagome contribution follows an original power law $C_{p}(T\rightarrow0)\propto T^α$ with $α\sim1.5$ and is found field-independent between $28$ and $34$ T for temperatures $1\leq T\leq4$ K. These are serious constrains when it comes to replication using low-temperature extrapolations of high-temperature series expansions. We manage to reproduce the experimental observatio…
Neutron spectroscopy and diffuse neutron scattering on herbertsmithite [ZnCu3 (OH)6Cl2], a near-ideal realisation of the s = 1/2 kagome antiferromagnet, reveal the hallmark property of a quantum spin liquid; instantaneous short-ranged antiferromagnetic correlations in the absence of a time-averaged ordered moment. These dynamic antiferromagnetic correlations are only very weakly dependent of neutron-energy transfer and temperature, and persist up to 25 meV and 120 K. At low energy transfers a shift of the magnetic scattering to low Q is observed with increasing temperature, providing evidence …
The kagome Heisenberg antiferromagnet formed by frustrated spins arranged in a lattice of corner-sharing triangles is a prime candidate for hosting a quantum spin liquid (QSL) ground state consisting of entangled spin singlets. But the existence of various competing states makes a convincing theoretical prediction of the QSL ground state difficult, calling for experimental clues from model materials. The kagome lattice materials Zn-barlowite ZnCu$_{3}$(OD)$_{6}$FBr and herbertsmithite ZnCu$_{3}$(OD)$_{6}$Cl$_2$ do not exhibit long range order, and they are considered the best realizations of t…
We present transverse field muon spin rotation/relaxation measurements on single crystals of the spin-1/2 kagome antiferromagnet Herbertsmithite. We find that the spins are more easily polarized when the field is perpendicular to the kagome plane. We demonstrate that the difference in magnetization between the different directions cannot be accounted for by Dzyaloshinksii-Moriya type interactions alone, and that anisotropic axial interaction is present.
Optical conductivity measurements are combined with density functional theory calculations in order to understand the electrodynamic response of the frustrated Mott insulators Herbertsmithite $\mathrm{ZnCu_{3}(OH)_{6}Cl_{2}}$ and the closely-related kagome-lattice compound $\mathrm{Y_{3}Cu_{9}(OH)_{19}Cl_{8}}$. We identify these materials as charge-transfer rather than Mott-Hubbard insulators, similar to the high-$T_c$ cuprate parent compounds. The band edge is at 3.3 and 3.6 eV, respectively, establishing the insulating nature of these compounds. Inside the gap, we observe dipole-forbidden lo…
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…
In Volborthite, spin-1/2 moments form a distorted Kagomé lattice, of corner sharing isosceles triangles with exchange constants $J$ on two bonds and $J'$ on the third bond. We study the properties of such spin systems, and show that despite the distortion, the lattice retains a great deal of frustration. Although sub-extensive, the classical ground state degeneracy remains very large, growing exponentially with the system perimeter. We consider degeneracy lifting by thermal and quantum fluctuations. To linear (spin wave) order, the degeneracy is found to stay intact. Two complementary approach…
Local spectral functions and Nuclear Magnetic Relaxation (NMR) rates, 1/T1, for the spin-half Heisenberg antiferromagnet on the Kagome Lattice are calculated using Moriyas Gaussian approximation, as well as through an extrapolation of multiple frequency moments. The temperature dependence of the calculated rates is compared with the oxygen 1/T1 NMR data in Herbertsmithite. We find that the Gaussian approximation for 1/T1 shows behavior qualitatively similar to experiments with a sharp drop in rates at low temperatures, consistent with a spin-gapped behavior. However, this approximation signifi…
Nearest-neighbor interacting S = 1/2 spins on the ideal Kagomé lattice are predicted to form a variety of novel quantum entangled states, including quantum spin-liquid (SL) and valence bond solid (VBS) phases. In real materials, the presence of additional perturbative spin interactions may further expand the variety of entangled states, which recent theoretical analyses show are identifiable through the spontaneous loss of particular discrete point group symmetries. Here we comprehensively resolve the ground state point group symmetries of the prototypical Kagomé SL candidate ZnCu$_3$(OH)$_6$C…
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 on temperature dependence of the infrared reflectivity spectra of a single crystalline herbertsmithite in two polarizations --- parallel and perpendicular to the kagome plane of Cu atoms. We observe anomalous broadening of the low frequency phonons possibly caused by fluctuations in the exotic dynamical magnetic order of the spin liquid.
Herbertsmithite (ZnCu3(OH)6Cl2) is often discussed as the best realization of the highly frustrated antiferromagnetic kagome lattice known so far. We employ density functional theory calculations to determine eight exchange coupling constants of the underlying Heisenberg Hamiltonian. We find the nearest neighbour coupling J1 to exceed all other couplings by far. However, next-nearest neighbour kagome layer couplings of 0.019 J1 and interlayer couplings of up to -0.035 J1 slightly modify the perfect antiferromagnetic kagome Hamiltonian. Interestingly, the largest interlayer coupling is ferromag…
Quantum spin liquids form a novel class of matter where, despite the existence of strong exchange interactions, spins do not order down to the lowest measured temperature. Typically, these occur in lattices that act to frustrate the appearance of magnetism. In two dimensions, the classic example is the kagome lattice composed of corner sharing triangles. There are a variety of minerals whose transition metal ions form such a lattice. Hence, a number of them have been studied, and were then subsequently synthesized in order to obtain more pristine samples. Of particular note was the report in 2…
We study the properties of the Heisenberg antiferromagnet with spatially anisotropic nearest-neighbour exchange couplings on the kagome net, i.e. with coupling J in one lattice direction and couplings J' along the other two directions. For J/J' > 1, this model is believed to describe the magnetic properties of the mineral volborthite. In the classical limit, it exhibits two kinds of ground states: a ferrimagnetic state for J/J' < 1/2 and a large manifold of canted spin states for J/J' > 1/2. To include quantum effects self-consistently, we investigate the Sp(N) symmetric generalisation of the …
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…
We report 17O NMR measurements in the S=1/2 Cu2+ kagome antiferromagnet Herbertsmithite ZnCu3(OH)6Cl2 down to 45mK in magnetic fields ranging from 2T to 12T. While Herbertsmithite displays a gapless spin-liquid behavior in zero field, we uncover an instability toward a spin-solid phase at sub-kelvin temperature induced by an applied magnetic field. The latter phase shows largely suppressed moments $\lesssim 0.1\muB$ and gapped excitations. The H-T phase diagram suggests the existence of a quantum critical point at the small but finite magnetic field mu0 Hc=1.55(25)T. We discuss this finding in…
The ground state of the simple Heisenberg nearest-neighbor quantum kagome antiferromagnetic model is a magnetically disordered spin liquid, yet various perturbations may lead to fundamentally different states. Here we disclose the origin of magnetic ordering in the structurally-perfect kagome material YCu$_3$(OH)$_6$Cl$_3$, which is free of the widespread impurity problem. {\it Ab-initio} calculations and modeling of its magnetic susceptibility reveal that, similar to the archetypal case of herbertsmithite, the nearest-neighbor exchange is by far the dominant isotropic interaction. Dzyaloshins…
Recent neutron scattering experiments on the spin-1/2 kagome lattice antiferromagnet ZnCu3(OH)6Cl2 (Herbertsmithite) provide the first evidence of fractionalized excitations in a quantum spin liquid state in two spatial dimensions. In contrast to existing theoretical models of spin liquids, the measured dynamic structure factor reveals an excitation continuum which is remarkably flat as a function of frequency and has almost no momentum dependence along several high-symmetry directions. Here we show that many experimentally observed features can be explained by the presence of topological viso…
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.
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…
Recent terahertz conductivity measurements observed low-power-law frequency dependence of optical conduction within the Mott gap of the Kagome lattice spin-liquid candidate Herbertsmithite. We investigate mechanisms for this observed sub-gap conductivity for two possible scenarios in which the ground-state is described by: 1) a U(1) Dirac spin-liquid with emergent fermionic spinons or 2) a nearly critical Z2 spin-liquid in the vicinity of a continuous quantum phase transition to magnetic order. We identify new mechanisms for optical-absorption via magneto-elastic effects and spin- orbit coupli…
Herbertsmithite and Zn-doped barlowite are two compounds for experimental realization of twodimensional gapped kagome spin liquid. Theoretically, it has been proposed that charge doping a quantum spin liquid gives rise to exotic metallic states, such as high-temperature superconductivity. However, one recent experiment about herbertsmithite with successful Li-doping shows surprisingly the insulating state even under the heavy doped scenario, which can hardly be explained by many-body physics. Using first-principles calculation, we performed a comprehensive study about the Li intercalated dopin…
Recent discoveries in neutron scattering experiments for Kapellasite and Herbertsmithite as well as theoretical calculations of possible spin liquid phases have revived interest in magnetic phenomena on the kagome lattice. We study the quantum phase diagram of the S=1/2 Heisenberg kagome model as a function of nearest neighbor coupling J1 and second neighbor coupling J2. Employing the pseudofermion functional renormalization group, we find four types of magnetic quantum order (q=0 order, cuboc order, ferromagnetic order, and Sqrt{3}x\Sqrt{3} order) as well as extended magnetically disordered r…
Realizing a quantum spin liquid (QSL) ground state in a real material is a leading issue in condensed matter physics research. In this pursuit, it is crucial to fully characterize the structure and influence of defects, as these can significantly affect the fragile QSL physics. Here, we perform a variety of cutting-edge synchrotron X-ray scattering and spectroscopy techniques, and we advance new methodologies for site-specific diffraction and L-edge Zn absorption spectroscopy. The experimental results along with our first-principles calculations address outstanding questions about the local an…
We investigate the effects of Dzyaloshinsky-Moriya (DM) interactions on the frustrated $J_1$-$J_2$ kagome-Heisenberg model using the pseudo-fermion functional-renormalization-group (PFFRG) technique. In order to treat the off-diagonal nature of DM interactions, we develop an extended PFFRG scheme. We benchmark this approach in parameter regimes that have previously been studied with other methods and find good agreement of the magnetic phase diagram. Particularly, finite DM interactions are found to stabilize all types of non-collinear magnetic orders of the $J_1$-$J_2$ Heisenberg model ($\mat…
In the search for spin-1/2 kagome antiferromagnets, the mineral volborthite has recently been the subject of experimental studies [Hiroi et al.,2001]. It has been suggested that the magnetic properties of this material are described by a spin-1/2 Heisenberg model on the kagome lattice with spatially anisotropic exchange couplings. We report on investigations of the Sp(N) symmetric generalisation of this model in the large N limit. We obtain a detailed description of the dependence of possible ground states on the anisotropy and on the spin length S. A fairly rich phase diagram with a ferrimagn…
In recent work, we argued that a particular algebraic spin liquid (ASL) may be the ground state of the S = 1/2 kagome lattice Heisenberg antiferromagnet. This state, which lacks a spin gap, is appealing in light of recent experiments on herbertsmithite (ZnCu3(OH)6Cl2). Here, we study the properties of this ASL in more detail, using both the low-energy effective field theory and Gutzwiller-projected wavefunctions. We identify the competing orders of the ASL -- among them we find a set of magnetic orders lying at the M-points of the Brillouin zone, the q = 0 magnetic ordered state, the "Hastings…
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…
Quantifying the Phase Diagram and Hamiltonian of $S=1/2$ Kagome Antiferromagnets: Bridging Theory and Experiment
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（斯坦福材料能源科学研究所，SLAC国家加速器实验室）；Department of Applied Physics, Stanford University（斯坦福大学应用物理系）；Neutron Scattering Division, Oak Ridge National Laboratory（橡树岭国家实验室中子散射部）
Inspired by the recent theoretical suggestion that the random-bond $S=1/2$ antiferromagnetic Heisenberg model on the triangular and the kagome lattices might exhibit a randomness-induced quantum spin liquid (QSL) behavior when the strength of the randomness exceeds a critical value, and that this "random-singlet state" might be relevant to the QSL behaviors experimentally observed in triangular organic salts $κ{\rm -(ET)_2 Cu_2 (CN)_3}$and ${\rm EtMe_3 Sb[Pd(dmit)_2]_2}$ and in kagome herbertsmithite ${\rm CuZn_3(OH)_6Cl_2}$, we further investigate the nature of the static and the dynamical sp…
Synthetic barlowite, Cu4(OH)6BrF, has emerged as a new quantum spin liquid (QSL) host, containing kagome layers of S=1/2 Cu2+ ions separated by interlayer Cu2+ ions. Similar to synthetic herbertsmithite, ZnCu3(OH)6Cl2, it has been reported that Zn2+ substitution for the interlayer Cu2+ induces a QSL ground state. Here we report a scalable synthesis of single crystals of Cu4(OH)6BrF. Through x-ray, neutron, and electron diffraction measurements coupled with magic angle spinning 19F and 1H NMR spectroscopy, we resolve the previously reported positional disorder of the interlayer Cu2+ ions and fi…
We present a Raman spectroscopic investigation of the Herbertsmithite ZnCu3(OH)6Cl2, the first realization of a Heisenberg s=1/2 antiferromagnet on a perfect kagome lattice. The magnetic excitation spectrum of this compound is dominated by two components, a high temperature quasi elastic signal and a low temperature, broad maximum. The latter has a linear low energy slope and extends to high energy. We have investigated the temperature dependence and symmetry properties of both signals. Our data agree with previous calculations and point to a spin liquid ground state.
