We report the determination of the Dzyaloshinsky-Moriya interaction, the dominant magnetic anisotropy term in the \kagome spin-1/2 compound {\herbert}. Based on the analysis of the high-temperature electron spin resonance (ESR) spectra, we find its main component $|D_z|=15(1)$ K to be perpendicular to the \kagome planes. Through the temperature dependent ESR line-width we observe a building up of nearest-neighbor spin-spin correlations below $\sim$150 K.
The recent NMR experiments on ZnCu3(OH)6Cl2 motivate our study of the effect of non- magnetic defects on the antiferromagnetic spin-1/2 kagome lattice. We use exact diagonalization methods to study the effect of two such defects on finite size systems. Our results, obtained without adjustable parameters, are in good quantitative agreement with recent Oxygen 17 NMR data. They provide support for the experimental interpretation of the presence of defects within the kagome layers due to Zn/Cu substitutions. Our results also show that disorder effects become relevant at lower temperatures, raising…
Motivated by the recent experiments on the new spin half Kagome compound ZnCu3(OH)6Cl2, we study a phenomenological model of a frustrated quantum magnet. The model has a spin liquid groundstate and is constructed so as to mimic the macroscopically large quasi-degeneracies expected in the low-lying energy structure of a Kagome system. We use numerical studies of finite size systems to investigate the static as well as the dynamical response at finite temperatures. The results obtained using our simple model are compatible with a large number of recent experiments including neutron scattering da…
We report thermodynamic measurements of the S=1/2 kagome lattice antiferromagnet ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$, a promising candidate system with a spin-liquid ground state. Using single crystal samples, the magnetic susceptibility both perpendicular and parallel to the kagome plane has been measured. A small, temperature-dependent anisotropy has been observed, where $χ_{z}/ χ_{p} > 1$ at high temperatures and $χ_{z}/ χ_{p} < 1$ at low temperatures. Fits of the high-temperature data to a Curie-Weiss model also reveal an anisotropy. By comparing with theoretical calculations, the presence of a s…
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…
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.
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.
ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$ ($S=1/2$) is a promising new candidate for an ideal Kagomé Heisenberg antiferromagnet, because there is no magnetic phase transition down to $\sim$50 mK. We investigated its local magnetic and lattice environments with NMR techniques. We demonstrate that the intrinsic local spin susceptibility {\it decreases} toward T=0, but that slow freezing of the lattice near $\sim$50 K, presumably associated with OH bonds, contributes to a large increase of local spin susceptibility and its distribution. Spin dynamics near T=0 obey a power-law behavior in high magnetic fields.
We characterize the ground state and excitation spectrum of the $S=1/2$, nominally pure and perfect kagomé system ZnCu$_{3}$(OH)$_{6}$Cl$_{2}$ using the following measurements: magnetization, muon spin rotation frequency shift $K$, transverse relaxation time $T_{2}^{\ast}$, and zero field relaxation, and Cl nuclear spin-lattice relaxation $T_{1}$. We found no sign of singlet formation, no long range order or spin freezing, and no sign of spin-Peierls transition even at temperatures as low as 60 mK. The density of states has $E^{1/4}$ energy dependence with a negligible gap to excitation.
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.
We report through 17O NMR, an unambiguous local determination of the intrinsic kagome lattice spin susceptibility as well as that created around non-magnetic defects issued from natural Zn/ Cu exchange in the S=1/2 (Cu2+) herbertsmithite ZnCu3(OH)6Cl2 compound. The issue of a singlet-triplet gap is addressed. The magnetic response around a defect is found to markedly differ from that observed in non-frustrated antiferromagnetic materials. Finally, we discuss our relaxation measurements in the light of Cu and Cl NMR data [cond-mat 070314] and suggest a flat q-dependence of the excitations.
Motivated by recent nuclear magnetic resonance experiments on ZnCu$_3$(OH)$_6$Cl$_2$, we present an exact-diagonalization study of the combined effects of non-magnetic impurities and Dzyaloshinskii-Moriya (DM) interactions in the $s = 1/2$ kagome antiferromagnet. The local response to an applied field and correlation-matrix data reveal that the dimer freezing which occurs around each impurity for $D = 0$ persists at least up to $D/J\simeq 0.06$, where $J$ and $D$ denote respectively the exchange and DM interaction energies. The phase transition to the ($Q = 0$) semiclassical, 120$^\circ$ state…
Experimental evidence for a plethora of low energy spin excitations in the spin-1/2 kagome antiferromagnet ZnCu3(OH)6Cl2 may be understandable in terms of an extended Fermi surface of spinons coupled to a U(1) gauge field. We carry out variational calculations to examine the possibility that such a state may be energetically viable. A Gutzwiller-projected wavefunction reproduces the dimerization of a kagome strip found previously by DMRG. Application to the full kagome lattice shows that the inclusion of a small ferromagnetic next-nearest-neighbor interaction favors a ground state with a spino…
Due to the particular geometry of the kagomé lattice, it is shown that antisymmetric Dzyaloshinsky-Moriya interactions are allowed and induce magnetic ordering. The symmetry of the obtained low temperature magnetic phases are studied through mean field approximation and classical Monté Carlo simulations. A phase diagram relating the geometry of the interaction and the ordering temperature has been derived. The order of magnitude of the anisotropies due to Dzyaloshinsky-Moriya interactions are more important than in non-frustrated magnets, which enhances its appearance in real systems. Applicat…
We use $^{79}$Br nuclear quadrupole resonance (NQR) to demonstrate that ultra slow lattice dynamics set in below the temperature scale set by the Cu-Cu super-exchange interaction $J$~($\simeq160$~K) in the kagome lattice Heisenberg antiferromagnet Zn-barlowite. The lattice completely freezes below 50~K, and $^{79}$Br NQR lineshapes become twice broader due to increased lattice distortions. Moreover, the frozen lattice exhibits an oscillatory component in the transverse spin echo decay, a typical signature of pairing of nuclear spins by indirect nuclear spin-spin interaction. This indicates tha…
We have performed thermodynamic and neutron scattering measurements on the S=1/2 kagome lattice antiferromagnet Zn Cu_3 (OH)_6 Cl_2. The susceptibility indicates a Curie-Weiss temperature of ~ -300 K; however, no magnetic order is observed down to 50 mK. Inelastic neutron scattering reveals a spectrum of low energy spin excitations with no observable gap down to 0.1 meV. The specific heat at low-T follows a power law with exponent less than or equal to 1. These results suggest that an unusual spin-liquid state with essentially gapless excitations is realized in this kagome lattice system.
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 report an electron spin resonance investigation of the geometrically frustrated spin-1/2 kagome antiferromagnet vesignieite, BaCu$_3$V$_2$O$_8$(OH)$_2$. Analysis of the line widths and line shifts indicates the dominance of in-plane Dzyaloshinsky-Moriya anisotropy that is proposed to suppress strongly quantum spin fluctuations and thus to promote long-range ordering rather than a spin-liquid state. We also evidence an enhanced spin-phonon contribution that might originate from a lattice instability and discuss the origin of a low-temperature mismatch between intrinsic and bulk susceptibilit…
We consider the polarization function P^{exp}_Z(t) measured by the muon-spin relaxation (muSR) technique for the SrCr8Ga4O19 and ZnCu3(OH)6Cl2 spin-liquid systems. We show the functional form of P^{exp}_Z(t) to imply that, in the temperature range of order 0.1 K, the spectral-weight function F(ω) of the magnetic correlations scales with 1/|ω|^{1 -x} (0 < x < 1) in the energy range of one microelectronvolt, i.e. \hbar ω~ 1 μeV. We derive the parameters involved in F(ω) from fits to available experimental data. Inelastic neutron scattering data probing F(ω) in the millielectronvolt energy range …
We study the consequences of in-plane (D_p) and out-of-plane (D_z) Dzyaloshinsky-Moriya (DM) interactions on the thermodynamic properties of spin-1/2} Heisenberg model on the kagome lattice using numerical linked cluster expansions and exact diagonalization, and contrast them with those of other perturbations such as exchange anisotropy and dilution. We find that different combinations of the DM anisotropies lead to a wide variety of thermodynamic behavior, which are quite distinct from those of most other perturbations. We argue that the sudden upturn seen experimentally in the susceptibility…
We report single-crystal 2-D NMR investigation of the nearly ideal spin S=1/2 kagome lattice ZnCu3(OD)6Cl2. We successfully identify 2-D NMR signals originating from the nearest-neighbors of Cu2+ defects occupying Zn sites. From the 2-D Knight shift measurements, we demonstrate that weakly interacting Cu2+ spins at these defects cause the large Curie-Weiss enhancement toward T=0 commonly observed in the bulk susceptibility data. We estimate the intrinsic spin susceptibility of the kagome planes by subtracting defect contributions, and explore several scenarios.
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…
We compute the magnetic susceptibility and specific heat of the spin-1/2 Heisenberg model on the kagome lattice with high-temperature expansions and exact diagonalizations. We compare the results with the experimental data on ZnCu3(OH)6Cl2 obtained by Helton et al. [Phys. Rev. Lett. 98, 107204 (2007)]. Down to k_BT/J~0.2, our calculations reproduce accurately the experimental susceptibility, with an exchange interaction J~190K and a contribution of 3.7% of weakly interacting impurity spins. The comparison between our calculations of the specific heat and the experiments indicate that the low-t…
In order to clarify why the experimental magnetization curve of the spherical kagome cluster in {W72V30} at 0.5 K shows no sign of staircase behavior up to 50 T, we study the effects of Dzyaloshinsky-Moriya (DM) interactions and tilts of the g tensors, both of which lead to the breaking of the total-S z conservation, by using the exact diagonalization method. It is found that the D vector component parallel to the radiation direction of the polyhedron cancels out the staircase in a low magnetic field region efficiently. The tilts of the g tensors are inherent to systems defined on the poly- he…
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…
We analyze the experimental data for the magnetic susceptibility of the material ZnCu3(OH)6Cl2 in terms of the Kagome Lattice Heisenberg model (KLHM), discussing possible role of impurity spins, dilution, exchange anisotropy, and both out-of-plane and in-plane Dzyaloshinsky-Moriya (DM) anisotropies, with explicit theoretical calculations using the Numerical Linked Cluster (NLC) method and exact diagonalization (ED). The high-temperature experimental data are well described by the pure Heisenberg model with J=170 K. We show that the sudden upturn in the susceptibility around T=75 K is due to DM…
We investigate the antiferromagnetic canting instability of the spin-1/2 kagome ferromagnet, as realized in the layered cuprates Cu$_3$Bi(SeO$_3)_2$O$_2$X (X=Br, Cl, and I). While the local canting can be explained in terms of competing exchange interactions, the direction of the ferrimagnetic order parameter fluctuates strongly even at short distances on account of frustration which gives rise to an infinite ground state degeneracy at the classical level. In analogy with the kagome antiferromagnet, the accidental degeneracy is fully lifted only by non-linear 1/S corrections, rendering the sel…
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 ($\mat…
We find that the best RVB state of the spin-$\frac{1}{2}$ Kagome antiferromagnetic Heisenberg model(spin-$\frac{1}{2}$ KAFH) is described by a $Z_{2}$ gapped mean field ansatz, which hosts a mean field spinon dispersion very different from that of the widely studied $U(1)$ Dirac spin liquid state. However, we find that the physical spin fluctuation spectrum calculated from the Gutzwiller projected RPA(GRPA) theory above such an RVB state is actually gapless and is almost identical to that above the $U(1)$ Dirac spin liquid state. We find that such a peculiar behavior can be attributed to the u…
Quantum spin liquid (QSL) is a novel state of matter with exotic excitations and was theoretically predicted to be realized most possibly in an S=1/2 kagome antiferromagnet. Experimentally searching for the candidate materials is a big challenge in condensed matter physics and only two such candidates were reported so far. Here we report the successful synthesis of a new spin-1/2 kagome antiferromagnet ZnCu3(OH)6SO4. No magnetic ordering is observed down to 50 mK, despite a moderately high Weiss temperature of θW ~ -79 K. It strongly suggests that the material is a new QSL candidate. Most inte…
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.
A single crystal S=3/2 perfect kagome lattice antiferromagnet $\mathrm{KCr_3(OH)_6(SO_4)_2}$ (Cr-jarosite) has been studied by X-band and high-frequency electron spin resonance (ESR). The g-values perpendicular to the kagome plane (c-axis) and in the plane are determined to be $g_c=1.9704 \pm 0.0002$ and $g_ξ=1.9720 \pm 0.0003$, respectively, by high-frequency ESR observed at 265 K. Antiferromagnetic resonances (AFMR) with the antiferromagnetic gap of 120 GHz are observed at 1.9 K, which is below $T_N$=4.5 K. The analysis of AFMR modes by the conventional molecular field theory shows $d_p=0.27…
The kagome Heisenberg antiferromagnet formed by frustrated spins arranged in a lattice of corner-sharing triangles is a prime candidate for hosting a quantum spin liquid (QSL) ground state consisting of entangled spin singlets. But the existence of various competing states makes a convincing theoretical prediction of the QSL ground state difficult, calling for experimental clues from model materials. The kagome lattice materials Zn-barlowite ZnCu$_{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 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…
Motivated by recent experiments on ZnCu$_3$(OH)$_6$Cl$_2$, we study the inhomogeneous Knight shifts (local susceptibilities) of spin 1/2 Kagome antiferromagnet in the presence of nonmagnetic impurities. Using high temperature series expansion, we calculate the local susceptibility and its histogram down to about T=0.4J. At low temperatures, we explore a Dirac spin liquid proposal and calculate the local susceptibility in the mean field and beyond mean field using Gutzwiller projection, finding the overall picture to be consistent with the NMR experiments.
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.
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…
We argue that the S=1/2 kagome antiferromagnet undergoes a quantum phase transition when the Dzyaloshinskii-Moriya coupling is increased. For $D<D_c$ the system is in a moment-free phase and for $D>D_c$ the system develops antiferromagnetic long-range order. The quantum critical point is found to be $D_c \simeq 0.1J$ using exact diagonalizations and finite-size scaling. This suggests that the kagome compound ZnCu$_3(OH)$_6$Cl$_3$ may be in a quantum critical region controlled by this fixed point.
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…
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.
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…
Neutron scattering measurements have been performed on deuterated powder samples of claringbullite and Zn-doped claringbullite (Zn$_x$Cu$_{4-x}$(OD)$_{6}$FCl). At low temperatures, claringbullite Cu$_4$(OD)$_{6}$FCl forms a distorted pyrochlore lattice with long-range magnetic order and spin-wave-like magnetic excitations. Partial Zn doping leads to the nominal ZnCu$_3$(OD)$_{6}$FCl compound, a geometrically frustrated spin-1/2 kagome antiferromagnet that shows no transition to magnetic order down to 1.5 K. The magnetic excitations form a gapless continuum, a signature of fractional excitation…
Impurities, which are inherently present in any real material, may play an important role in the magnetism of frustrated spin systems with spin-liquid ground states. We address the impurity issue in quantum kagome antiferromagnets by investigating ZnCu$_3$(OH)$_6$SO$_4$ (Zn-brochantite) by means of muon spin spectroscopy. We show that muons couple to the impurity magnetism, originating from Cu-Zn intersite disorder, and that the impurities are highly correlated with the kagome spins, allowing us to probe the intrinsic kagome physics via a Kondo-like effect. The low-temperature plateau in local…
The emergent behavior of spin liquids that are born out of geometrical frustration makes them an intriguing state of matter. We show that in the quantum kagome antiferromagnet ZnCu$_3$(OH)$_6$SO$_4$ several different correlated, yet fluctuating states exist. By combining complementary local-probe techniques with neutron scattering, we discover a crossover from a critical regime into a gapless spin-liquid phase with decreasing temperature. An additional unconventional instability of the latter phase leads to a second, distinct spin-liquid state that is stabilized at the lowest temperatures. We …
We perform a Gutzwiller projected wavefunction study for the spin-1/2 Heisenberg model on the Kagome lattice to compare energies of several spin-liquid states. The result indicates that a U(1)-Dirac spin-liquid state has the lowest energy. Furthermore, even without variational parameters, the energy turns out to be very close to that found by exact diagonalization. We show that such a U(1)-Dirac state represents a quantum phase whose low energy physics is governed by four flavors of two-component Dirac fermions coupled to a U(1) gauge field. These results are discussed in the context of recent…
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…
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…
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…
We present the hydrothermal synthesis, as well as structural and chemical analysis of single crystals on the compounds EuCu$_{3}$(OH)$_{6}$Cl$_{3}$, Zn$_{x}$Cu$_{4-x}$(OH)$_{6}$(NO$_{3}$)$_{2}$ and haydeeite, MgCu$_{3}$(OH)$_{6}$Cl$_{2}$ all arising from the atacamite family. Magnetic and specific-heat measurements down to 1.8 K are carried out for these systems. EuCu$_{3}$(OH)$_{6}$Cl$_{3}$ has a frustrated antiferromagnetic Cu$^{2+}$ ground state with order at 15 K, a strong anisotropy and increased magnetization from Van Vleck paramagnetic Eu$^{3+}$ contributions. ZnCu$_{3}$(OH)$_{6}$(NO$_{…
In frustrated magnets the Dzyaloshinsky-Moriya interaction arising from spin-orbit coupling can induce a magnetic long-range order. Here, we report a theoretical prediction of thermal Hall effect in frustrated kagomé magnets such as KCr$_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…
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 report the study of high quality samples of the frustrated S = 1/2 kagome antiferromagnet vesignieite, Cu3Ba(VO5H)2. Neutron powder diffraction measurements evidence the high quality of the kagome lattice and show no sign of a transition to long-range order. A kink in the susceptibility below T = 9 K is matched to a reduction in paramagnetic-like correlations in the diffraction data and a slowing of the spin dynamics observed by MuSR. Our results point to an exotic quantum state below 9 K with coexistance of both dynamical and small frozen moments \sim 0.1 \muB. We propose that Dzyaloshinsk…
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 …
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…
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…
The kagomé lattice exhibits peculiar magnetic properties due to its strongly frustated cristallographic structure, based on corner sharing triangles. For nearest neighbour antiferromagnetic Heisenberg interactions there is no Neel ordering at zero temperature both for quantum and classical s pins. We show that, due to the peculiar structure, antisymmetric Dzyaloshinsky-Moriya interactions (${\bf D} . ({\bf S}_i \times {\bf S}_j)$) are present in this latt ice. In order to derive microscopically this interaction we consider a set of localized d-electronic states. For classical spins systems, we…
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 …
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…
