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.
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.
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. Le…
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.
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 …
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…
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.
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…
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 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…
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…
Is Herbertsmithite far from an ideal antiferromagnet? Ab-initio answer including in-plane Dzyaloshinskii-Moriya interactions and coupling with extra-plane impurities
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…
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 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…
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…
New physics can emerge in magnetic materials where quantum fluctuations are enhanced due to reduced dimensionality and strong frustration. One long sought example is the resonating-valence-bond (RVB) state, where atomic magnetic moments are strongly correlated but do not order or freeze even in the limit of T -> 0. The RVB ground state does not break conventional symmetries, such as lattice translation or spin-rotation. The realization of such a quantum spin liquid in two-dimensions would represent a new state of matter. It is believed that spin liquid physics plays a role in the phenomenon of…
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…
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…
The dc-magnetization of the unique S=1/2 kagome antiferromagnet Herbertsmithite has been measured down to 0.1K. No sign of spin freezing is observed in agreement with former muSR and ac-susceptibility results. The low temperature magnetic response is dominated by a defect contribution which exhibits a new energy scale $\simeq 1$ K, likely reflecting the coupling of the defects. The defect component is saturated at low temperature by H>8T applied magnetic fields which enables us to estimate an upper bound for the non saturated intrinsic kagome susceptibility at T=1.7K.
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.
Herbertsmithite, ZnCu3(OH)6Cl2, is the prototype candidate for a spin liquid behavior on a geometrically perfect kagome lattice. Its discovery and the absence of any evidence for spin-freezing down to the lowest probed temperature to-date enable one to explore the properties of kagome-related physics in an unprecedented temperature range. We review its properties and discuss some open issues. A tentative comparison to models is also performed.
We compute the real-space spin correlations and frquency and wave-vector resolved dynamic structure factors $S(\vec q,ω)$ for the nearest-neighbor Kagome-Lattice Heisenberg Antiferromagnet (KLHM) at finite temperatures using Numerical Linked Cluster Expansion (NLCE) method. A triangle-based NLCE is used to calculate frequency moments of the dynamic structure factors in the thermodynamic limit, which show excellent convergence for $T> J/4$. A Gaussian approximation and the fluctuation-dissipation relation are used to to reconstruct the frequency dependence. We find that some features of the low…
A quantum spin liquid (QSL) is a state of matter in which magnetic spins interact strongly, but quantum fluctuations inhibit long-range magnetic order even at zero temperature. A QSL has been predicted to have a host of exotic properties, including fractionalized excitations and long-range quantum entanglement. Despite the numerous theoretical studies, experimental realization of a QSL has proved to be challenging due to the lack of candidate materials. The triangular organic salts EtMe3Sb[Pd(dmit)2]2 and κ-(BEDT-TTF)2Cu2(CN)3, and kagome ZnCu3(OH)6Cl2 (Herbertsmithite) have recently emerged a…
It has been suggested that the nearest-neighbour (NN) antiferromagnetic Heisenberg (HAF) model on the Kagome lattice may be a good starting point to understand the quantum spin-liquid (QSL) behaviour discovered in Herbertsmithite. We investigate possible QSL phases in the presence of experimentally relevant spin-rotation symmetry-breaking perturbations such as Dzyaloshinskii-Moriya and Ising interactions, as well as second-neighbour antiferromagnetic Heisenberg interactions. We use the projective symmetry group analysis within the slave-fermion framework of QSL phases and systematically classi…
Spinon mediation of witness spin dynamics in herbertsmithite
University of Oxford（牛津大学）；University College Cork（科克大学学院）；Cardiff University（卡迪夫大学）；University of Bristol（布里斯托大学）；Max Planck Institute for Solid State Research（马克斯·普朗克固体的研究所）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Argonne National Laboratory（阿贡国家实验室）；Cornell University（康奈尔大学）
We present a theory for site dilution in the Valence Bond Crystal Phase of the Kagome Lattice Heisenberg Model. The presence of an empty site leads to strong singlet bond across the impurity. It also creates a free spin, which delocalizes inside the unit cell. Finite concentration of quenched impurities leads to a Valence Bond Glass phase. This phase has short-range Valence Bond order, no spin-gap, large spin susceptibilities, linear specific heat due to two-level systems, as well as singlet and triplet excitations that decompose into kink-antikink pairs delocalized over a few lattice constant…
Arguably the most favorable situation for spins to enter the long-sought quantum spin liquid (QSL) state is when they sit on a kagome lattice. No consensus has been reached in theory regarding the true ground state of this promising platform. The experimental efforts, relying mostly on one archetypal material ZnCu$_3$(OH)$_6$Cl$_2$, have also led to diverse possibilities. Apart from subtle interactions in the Hamiltonian, there is the additional degree of complexity associated with disorder in the real material ZnCu$_3$(OH)$_6$Cl$_2$ that haunts most experimental probes. Here we resort to heat…
In frustrated magnets the Dzyaloshinsky-Moriya interaction arising from spin-orbit coupling can induce a magnetic long-range order. Here, we report a theoretical prediction of thermal Hall effect in frustrated kagomé magnets such as KCr$_3$(OH)$_6$(SO4)$_2$ and KFe$_3$(OH)$_{6}$(SO$_{4}$)$_2$. The thermal Hall effects in these materials are induced by scalar spin chirality as opposed to DMI in previous studies. The scalar spin chirality originates from magnetic-field-induced chiral spin configuration due to non-coplanar spin textures, but in general it can be spontaneously developed as a macro…
Motivated by spin-wave continuum (SWC) observed in recent neutron scattering experiments in Herbertsmithite, we use Gutzwiller-projected wave functions to study dynamic spin structure factor $S(\mathbf{q},ω)$ of spin liquid states on the kagome lattice. Spin-1 excited states in spin liquids are represented by Gutzwiller-projected two-spinon excited wave functions. We investigate three different spin liquid candidates, spinon Fermi-surface spin liquid (FSL), Dirac spin liquid (DSL) and random-flux spin liquid (RSL). FSL and RSL have low energy peaks in $S(\mathbf{q},ω)$ at $K$ points in the ext…
We present thermodynamic studies of a new spin-1/2 antiferromagnet containing undistorted kagome lattices---barlowite Cu$_{4}$(OH)$_{6}$FBr. Magnetic susceptibility gives $θ_{CW}$ = $-$136 K, while long-range order does not happen until $T_{N}$ = 15 K with a weak ferromagnetic moment $μ$ $<$ 0.1$μ_{B}$/Cu. A 60 T magnetic field induces a moment less than 0.5$μ_{B}$/Cu at $T$ = 0.6 K. Specific-heat measurements have observed multiple phase transitions at $T \ll$ $\mid$$θ_{CW}$$\mid$. The magnetic entropy of these transitions is merely 18% of $k_{B}$ln2 per Cu spin. These observations suggest th…
The effect of the quenched bond-randomness on the ordering of the $S=1/2$ antiferromagnetic Heisenberg model on the kagome lattice is investigated by means of an exact-diagonalization method. When the randomness exceeds a critical value, the ground state of the model exhibits a transition within the non-magnetic state into the randomness-relevant gapless spin-liquid state. Implications to the S=1/2 kagome-lattice antiferromagnet herbertsmithite is discussed.
Herbertsmithite, ZnCu$_3$(OH)$_6$Cl$_2$, is a two dimensional kagomé lattice realization of a spin liquid, with evidence for fractionalized excitations and a gapped ground state. Such a quantum spin liquid has been proposed to underlie high temperature superconductivity and is predicted to produce a wealth of new states, including a Dirac metal at $1/3$rd electron doping. Here we report the topochemical synthesis of electron-doped ZnLi$_x$Cu$_3$(OH)$_6$Cl$_2$ from $x$ = 0 to $x$ = 1.8 ($3/5$th per Cu$^{2+}$). Contrary to expectations, no metallicity or superconductivity is induced. Instead, we…
Barlowite $Cu_4(OH)_6FBr$ is a newly found mineral containing $Cu^{2+}$ kagome planes. Despite similarities in many aspects to Herbertsmithite $Cu_3Zn(OH)_6Cl_2$, the well-known quantum spin liquid (QSL) candidate, intrinsic Barlowite turns out not to be a QSL, possibly due to the presence of $Cu^{2+}$ ions in between kagome planes that induce interkagome magnetic interaction [PRL, 113, 227203 (2014)]. Using first-principles calculation, we systematically study the feasibility of selective substitution of the interkagome Cu ions with isovalent nonmagnetic ions. Unlike previous speculation of u…
We address the problem of a lightly doped spin-liquid through a large-scale density-matrix renormalization group (DMRG) study of the $t$-$J$ model on a Kagome lattice with a small but non-zero concentration, $δ$, of doped holes. It is now widely accepted that the undoped ($δ=0$) spin 1/2 Heisenberg antiferromagnet has a spin-liquid groundstate. Theoretical arguments have been presented that light doping of such a spin-liquid could give rise to a high temperature superconductor or an exotic topological Fermi liquid metal (FL$^\ast$). Instead, we infer that the doped holes form an insulating cha…
The spin-1/2 kagomé Heisenberg antiferromagnet is generally accepted as one of the most promising two-dimensional models to realize a quantum spin liquid state. Previous experimental efforts were almost exclusively on only one archetypal material, the herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$, which unfortunately suffers from the notorious orphan spins problem caused by magnetic disorders. Here we turn to YCu$_3$(OH)$_{6.5}$Br$_{2.5}$, recently recognized as another host of a globally undistorted kagomé Cu$^{2+}$ lattice free from the orphan spins, thus a more feasible system for studying the int…
Spin liquids are exotic phases of quantum matter challenging Landau's paradigm of symmetry-breaking phase transitions. Despite strong exchange interactions, spins do not order or freeze down to zero temperature. While well-established for 1D quantum antiferromagnets, in higher dimension where quantum fluctuations are less acute, realizing and understanding such states represent major issues, both theoretical and experimental. In this respect the simplest nearest-neighbor Heisenberg antiferromagnet Hamiltonian on the highly frustrated kagome lattice has proven to be a fascinating and inspiring …
We followed the Shastry--Shraiman formulation of Raman scattering in Hubbard systems and considered the Raman intensity profile in the spin-1/2 "perfect" kagome lattice herbertsmithite ZnCu_3(OH)_6Cl_2, assuming the ground state is well-described by the U(1) Dirac spin-liquid state. In the derivation of the Raman T-matrix, we found that the spin chirality term appears in the A_{2g} channel in the kagome lattice at the t^4/(ω_i-U)^3 order, but (contrary to the claims by Shastry and Shraiman) vanishes in the square lattice to that order. In the ensuing calculations on the spin-1/2 kagome lattice…
We report measurements of the specific heat and magnetization of single crystal samples of the spin-1/2 kagome compound ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$ (herbertsmithite), a promising quantum spin-liquid candidate, in high magnetic fields and at low temperatures. The magnetization was measured up to $μ_{0}H$ = 55 T at $T$ = 0.4 K, showing a saturation of the weakly interacting impurity moments in fields above $\sim10$ T. The specific heat was measured down to $T < 0.4$ K in magnetic fields up to 18 T, revealing $T$-linear and $T$-squared contributions. The $T$-linear contribution is surprisingly l…
The spin-$\frac{1}{2}$ kagome antiferromagnet is considered an ideal host for a quantum spin liquid ground state. We find that when the bonds of the kagome lattice are modulated with a periodic pattern, new quantum ground states emerge. Newly synthesized crystalline barlowite (Cu$_4$(OH)$_6$FBr) and Zn-substituted barlowite demonstrate the delicate interplay between singlet states and spin order on the spin-$\frac{1}{2}$ kagome lattice. Comprehensive structural measurements demonstrate that our new variant of barlowite maintains hexagonal symmetry at low temperatures with an arrangement of dis…
We study dynamical spin structure factor (DSSF) of S = 1/2 Heisenberg model on the kagome lattice (KAFM) by means of density-matrix renormalization group. By comparison with the well-defined magnetic ordered state and chiral spin liquid sitting nearby in the phase diagram, the KAFM with the nearest-neighbor interaction shows distinct dynamical response behaviors. First of all, the DSSF displays important spectral intensity predominantly at low frequency region around Q = M point in momentum space, and shows a broad spectral distribution at high frequency region for momenta along the boundary o…
We present a successful synthesis method of the series Ga$_{x}$Cu$_{4-x}$(OD)$_{6}$Cl$_{2}$ with substitutions up to $x=0.8$. The compound remains a frustrated kagome system with an insulating ground state similar to herbertsmithite for these substitutions, as the additional charge of Ga$^{3+}$ is most likely bound to additional OH$^{-}$ and Cl$^{-}$. Besides infrared measurements, we present magnetic and specific-heat data down to 2 K for selected samples with $0\leq x\leq0.8$. With increasing $x$ the long-range magnetic order is suppressed, similar to what was observed in the series Zn$_{x}$…
