Site-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates
Rebecca W. Smaha, Idris Boukahil, Charles J. Titus, Jack Mingde Jiang, John P. Sheckelton, Wei He, Jiajia Wen, John Vinson, Suyin Grass Wang, Yu-Sheng Chen, Sim… 展开作者
Rebecca W. Smaha, Idris Boukahil, Charles J. Titus, Jack Mingde Jiang, John P. Sheckelton, Wei He, Jiajia Wen, John Vinson, Suyin Grass Wang, Yu-Sheng Chen, Simon J. Teat, Thomas P. Devereaux, C. Das Pemmaraju, Young S. Lee
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 and long-range structures of the two leading kagome QSL candidates, Zn-substituted barlowite Cu$_3$Zn$_{x}$Cu$_{1-x}$(OH)$_6$FBr and herbertsmithite Cu$_3$Zn(OH)$_6$Cl$_2$. On all length scales probed, there is no evidence that Zn substitutes onto the kagome layers, thereby preserving the QSL physics of the kagome lattice. Our calculations show that antisite disorder is not energetically favorable and is even less favorable in Zn-barlowite compared to herbertsmithite. Site-specific X-ray diffraction measurements of Zn-barlowite reveal that Cu$^{2+}$ and Zn$^{2+}$ selectively occupy distinct interlayer sites, in contrast to herbertsmithite. Using the first measured Zn L-edge inelastic X-ray absorption spectra combined with calculations, we discover a systematic correlation between the loss of inversion symmetry from pseudo-octahedral (herbertsmithite) to trigonal prismatic coordination (Zn-barlowite) with the emergence of a new peak. Overall, our measurements suggest that Zn-barlowite has structural advantages over herbertsmithite that make its magnetic properties closer to an ideal QSL candidate: its kagome layers are highly resistant to nonmagnetic defects while the interlayers can accommodate a higher amount of Zn substitution.
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…
We investigate the low temperature magnetic properties of a $S=\frac{5}{2}$ Heisenberg kagomé antiferromagnet, the layered monodiphosphate Li$_9$Fe$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$, using magnetization measurements and $^{31}$P nuclear magnetic resonance. An antiferromagnetic-type order sets in at $T_{\rm N}=1.3$ K and a characteristic magnetization plateau is observed at 1/3 of the saturation magnetization below $T^* \sim 5$ K. A moderate $^{31}$P NMR line broadening reveals the development of anisotropic short-range correlations within the plateau phase concomitantly with a gapless spin-latti…
A three-dimensional system of interacting spins typically develops static long-range order when it is cooled. If the spins are quantum (S = 1/2), however, novel quantum paramagnetic states may appear. The most highly sought state among them is the resonating valence bond (RVB) state in which every pair of neighboring quantum spins form entangled spin singlets (valence bonds) and the singlets are quantum mechanically resonating amongst all the possible highly degenerate pairing states. Here we provide experimental evidence for such quantum paramagnetic states existing in frustrated antiferromag…
Quantum spin-1/2 kagome Heisenberg antiferromagnet is the representative frustrated system possibly hosting a spin liquid. Clarifying the nature of this elusive topological phase is a key challenge in condensed matter, however, even identifying it still remains unsettled. Here, we apply a magnetic field and discover a series of spin gapped phases appearing at five different fractions of magnetization by means of grand canonical density matrix renormalization group, an unbiased state-of-art numerical technique. The magnetic field dopes magnons and first gives rise to a possible Z3 spin liquid p…
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…
By using the density matrix renormalization group, we study the spin-liquid phases of spin-$1/2$ XXZ kagome antiferromagnets. We find that the emergence of spin liquid phase does not depend on the anisotropy of the XXZ interaction. In particular, the two extreme limits---Ising (strong $S^z$ interaction) and XY (zero $S^z$ interaction)---host the same spin-liquid phases as the isotropic Heisenberg model. Both the time-reversal-invariant spin liquid and the chiral spin liquid with spontaneous time-reversal symmetry breaking are obtained. We show they evolve continuously into each other by tuning…
The theoretical description of non-Fermi liquids is among the most challenging questions in strongly correlated quantum matter. While there are many experimental candidates for such phases, few examples can be studied using controlled theoretical approaches. Here we introduce a novel conceptual perspective to analytically describe the non-Fermi liquid physics of gapless spin liquids arising in a family of two- and three-dimensional Kagome models. We first discuss a symmetry-protection mechanism that is responsible for the stability of the gapless phase. We then re-cast the two-dimensional Kago…
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 investigate the nature of quantum spin liquid (QSL) phase of the spin-$1/2$ nearest-neighbor XXZ antiferromagnet on the kagome lattice. Recent numerical calculations suggest that such a kagome spin liquid is insensitive to the XXZ anisotropy and is adjacent to a chiral spin liquid phase. Reformulating the problem in terms of a $U(1)$ lattice gauge theory with dynamical bosonic spinons, we propose that the kagome spin liquid can be understood as a deconfined critical phase extended by the $U(1)$ gauge fluctuation from a deconfined critical point between a symmetry-protected topological phase…
We investigate the stability and the nature of the chiral spin liquids which were recently uncovered in extended Heisenberg models on the kagome lattice. Using a Gutzwiller projected wave function approach -- i.e. a parton construction -- we obtain large overlaps with ground states of these extended Heisenberg models. We further suggest that the appearance of the chiral spin liquid in the time-reversal invariant case is linked to a classical transition line between two magnetically ordered phases.
In a recent paper [arXiv:1601.02165], Tao Li claimed that a gapped $\mathbb{Z}_2$ spin liquid, obtained using projected Gutzwiller fermionic wave functions, can be stabilized in the Heisenberg model on the kagome lattice. We perform very accurate variational calculations and confirm with unprecedented accuracy the fact, that the $\mathbb{Z}_{2}$ spin liquid is a local energy minimum that goes away with system size, thus reaffirming the scenario of a gapless $U(1)$ Dirac spin liquid ground state.
A preponderance of evidence suggests that the ground state of the nearest-neighbor $S = 1/2$ antiferromagnetic Heisenberg model on the kagome lattice is a gapless spin liquid. Many candidate materials for the realization of this model possess in addition a Dzyaloshinskii-Moriya (DM) interaction. We study this system by tensor-network methods and deduce that a weak but finite DM interaction is required to destabilize the gapless spin-liquid state. The critical magnitude, $D_c/J \simeq 0.012(2)$, lies well below the DM strength proposed in the kagome material herbertsmithite, indicating a need t…
In quantum spin liquid states, the fractionalized spinon excitations can carry fractional crystal symmetry quantum numbers, and this symmetry fractionalization distinguishes different topologically ordered spin liquid states. In this work we propose a simple way to detect signatures of such crystal symmetry fractionalizations from the crystal symmetry representations of the ground state wave function. We demonstrate our method on projected $\mathbb Z_2$ spin liquid wave functions on the kagome lattice, and show that it can be used to classify generic wave functions. Particularly our method can…
We present the results of first-principle calculations using the Vienna Ab-initio Simulation Package (VASP) for a new class of organometallics labeled TM3C6O6 (TM =Sc, Ti, V, Cr, Fe, Co, Ni and Cu) in the form of planar, two-dimensional, periodic free-standing layers. These materials, which can be produced by on-surface coordination on metallic surfaces, have a kagome lattice of TM ions. Calculating the structural properties, we show that all considered materials have local magnetic moments in the ground state, but four of them (with Fe, Co, Ni and Cu) show spin-crossover behavior by changing …
Dynamical magnetic correlations in the geometrically frustrated Nd$\_3$Ga$\_5$SiO$\_{14}$ compound were probed by inelastic neutron scattering on a single crystal. A scattering signal with a ring shape distribution in reciprocal space and unprecedented dispersive features was discovered. Comparison with calculated static magnetic scattering from models of correlated spins suggests that the observed phase is a spin liquid inherent to an antiferromagnetic kagomé-like lattice of anisotropic Nd moments.
Highly frustrated spin systems such as the kagome lattice (KL) are a treasure trove of new quantum states with large entanglements. We thus study the spin-$\frac{1}{2}$ Heisenberg model on a kagome-strip chain (KSC), which is one-dimensional KL, using the density-matrix renormalization group (DMRG) method. Calculating central charge and entanglement spectrum for the KSC, we find a novel gapless spin liquid state with doubly degenerate entanglement spectra in a 1/5 magnetization plateau. We also obtain a gapless low-lying continuum in the dynamic spin structure calculated by dynamical DMRG meth…
We study an exactly solvable quantum spin model of Kitaev type on the kagome lattice. We find a rich phase diagram which includes a topological (gapped) chiral spin liquid with gapless chiral edge states, and a gapless chiral spin liquid phase with a spin Fermi surface. The ground state of the current model contains an odd number of electrons per unit cell which qualitatively distinguishes it from previously studied exactly solvable models with a spin Fermi surface. Moreover, we show that the spin Fermi surface is stable against weak perturbations.
We construct a lattice model of topological order (kagome quantum spin liquids) and solve it with unbiased quantum Monte Carlo simulations. A three-stage anyon condensation with two transitions from a $\mathbb Z_2\boxtimes\mathbb Z_2$ topological order to a $\mathbb Z_2$ topological order and eventually to a trivial symmetric phase is revealed. These results provide concrete examples of phase transitions between topological orders in quantum magnets. The designed quantum spin liquid model and its numerical solution offer a playground for further investigations on vestigial anyon condensation.
General conditions in which disordered, spin liquid, and valence-bond ordered phases occur in quantum Ising antiferromagnets are studied using the prototype Kagome lattice spin models. A range of quantum dynamical processes in the Ising model, with and without total Ising spin conserved, are analytically shown to yield all three characteristic quantum paramagnetic phases in the Kagome system. Special emphasis is given to the XXZ model that can be sensibly compared to the Kagome lattice Heisenberg antiferromagnet. It is explicitly demonstrated that the total-spin-conserving dynamics can yield a…
We report synthesis of polycrystalline samples of the recently discovered spin liquid material Ca$_{10}$Cr$_7$O$_{28}$ and present measurements of the ambient and high pressure magnetic susceptibility $χ$ versus temperature $T$, magnetization $M$ versus magnetic field $H$ at various $T$, and heat capacity $C$ versus $T$ at various $H$. The ambient pressure magnetic measurements indicate the presence of both ferromagnetic and antiferromagnetic exchange interactions with dominant ferromagnetic interactions and with the largest magnetic energy scale $\sim 10$~K\@. The $χ(T)$ measurements under ex…
Motivated by recent experiments on the vanadium oxyfluoride material DQVOF, we examine possible spin liquid phases on a breathing kagome lattice of S=1/2 spins. By performing a projective symmetry group analysis, we determine the possible phases for both fermionic and bosonic $\mathbb{Z}_2$ spin liquids on this lattice, and establish the correspondence between the two. The nature of the ground state of the Heisenberg model on the isotropic kagome lattice is a hotly debated topic, with both $\mathbb{Z}_2$ and U(1) spin liquids argued to be plausible ground states. Using variational Monte Carlo …
We construct a phenomenological Z_2 lattice gauge theory to describe the spin-liquid state of the S=1/2 kagome Heisenberg antiferromagnet in the sector with zero total spin. The model is a natural generalization of the Misguich-Serban-Pasquier Hamiltonian with added interactions that are strongly constrained by lattice symmetries. We are able to reproduce qualitatively many of the characteristic features observed in recent numerical studies. We also make connections to the previous works along similar lines.
We report the thermodynamic and muon spin relaxation ($μ$SR) evidences for a possible gapless spin liquid in Tm$_{3}$Sb$_{3}$Zn$_{2}$O$_{14}$, with the rare-earth ions Tm$^{3+}$ forming a two-dimensional kagomé lattice. We extract the magnetic specific heat of Tm$_{3}$Sb$_{3}$Zn$_{2}$O$_{14}$ by subtracting the phonon contribution of the non-magnetic isostructural material La$_{3}$Sb$_{3}$Zn$_{2}$O$_{14}$. We obtain a clear linear-$T$ temperature dependence of magnetic specific heat at low temperatures, with the heat-capacity coefficient $γ$ = 26.6(1) mJ mol-Tm$^{-1}$ K$^{-2}$ in the zero temp…
We propose in this work an effective field theory description of the chiral spin liquid state in Heisenberg spin system on kagomé lattice.To this end, we derive the low-energy effective theory of kagomé (isotropic) Heisenberg antiferromagnet around its ordered ground states found numerically and show that quantum fluctuations induced by further neighbor spin exchanges are equally strong as those from first neighbor.We use a chiral order parameter theory to argue for the occurrence of finite temperature chiral symmetry breaking transition into chiral ordered state in kagomé antiferromagnet with…
We introduce quantum dimer models on lattices made of corner-sharing triangles. These lattices includes the kagome lattice and can be defined in arbitrary geometry. They realize fully disordered and gapped dimer-liquid phase with topological degeneracy and deconfined fractional excitations, as well as solid phases. Using geometrical properties of the lattice, several results are obtained exactly, including the full spectrum of a dimer-liquid. These models offer a very natural - and maybe the simplest possible - framework to illustrate general concepts such as fractionalization, topological ord…
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…
Using a perturbative renormalization group approach, we show that the extended ($J_1$-$J_2$-$J_d$) Heisenberg model on the kagome lattice with a staggered chiral interaction ($J_χ$) can exhibit a gapless chiral quantum spin liquid phase. Within a coupled-chains construction, this phase can be understood as a chiral sliding Luttinger liquid with algebraic decay of spin correlations along the chain directions. We calculate the low-energy properties of this gapless chiral spin liquid using the effective field theory and show that they are compatible with the predictions from parton mean-field the…
We obtain a classical spin liquid (CSL) phase by applying a magnetic field in $J_1$-$J_2$-$J_3$ Ising model on a kagome lattice. As we proved in the previous study [Phys. Rev. Lett. {\bf 119}, 077207 (2017)], this model realizes one species of CSL, the hexamer CSL, at zero magnetic field, which consists of macroscopically degenerate spin configurations with mixed total magnetization, $M$. The magnetic field selects its subset, which can be mapped to a trimer covering of the dual lattice, and forms a magnetization plateau of $M=1/9$. In addition to this CSL, we find two other magnetization plat…
Motivated by recent numerical and experimental studies of the spin-1/2 Heisenberg antiferromagnet on kagome, we formulate a many-body model for fermionic spinons introduced by us earlier [Phys. Rev. Lett. 103, 187203 (2009)]. The spinons interact with an emergent U(1) gauge field and experience strong short-range attraction in the S=0 channel. The ground state of the model is generically a $Z_2$ liquid. We calculate the edge of the two-spinon continuum and compare the theory to the slave-fermion approach to the Heisenberg model.
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 density-matrix renormalization group (DMRG) study of the S=1/2 Heisenberg antiferromagnet on the kagome lattice to identify the conjectured spin liquid ground state. Exploiting SU(2) spin symmetry, which allows us to keep up to 16,000 DMRG states, we consider cylinders with circumferences up to 17 lattice spacings and find a spin liquid ground state with an estimated per site energy of -0.4386(5), a spin gap of 0.13(1), very short-range decay in spin, dimer and chiral correlation functions and finite topological entanglement gamma consistent with gamma=ld 2, ruling out gapless, ch…
The breaking of chiral and time-reversal symmetries provides a pathway to exotic quantum phenomena and topological phases. In particular, the breaking of chiral (mirror) symmetry in quantum materials has been shown to have important technological applications. Recent work has extensively explored the resulting emergence of chiral charge orders and chiral spin liquids on the kagomé lattice. Such chiral spin liquids are closely tied to bosonic fractional quantum Hall states and host anyonic quasiparticles; however, their connection to nearby magnetically ordered states has remained a mystery. He…
The vanadium oxyfluoride [NH4]2[C7H14N][V7O6F18] (DQVOF) is a geometrically frustrated magnetic bilayer material. The structure consists of S=1/2 kagome planes of V4+ d1 ions with S=1 V3+ d2 ions located between the kagome layers. Muon spin relaxation measurements demonstrate the absence of spin freezing down to 40 mK despite an energy scale of 60 K for antiferromagnetic exchange interactions. From magnetization and heat capacity measurements we conclude that the S=1 spins of the interplane V3+ ions are weakly coupled to the kagome layers, such that DQVOF can be viewed as an experimental model…
We report muSR experiments on Mg{x}Cu{4-x}(OH)6Cl2 with x \sim 1, a new material isostructural to Herbertsmithite exhibiting regular kagome planes of spin 1/2 (Cu^{2+}), and therefore a candidate for a spin liquid ground state. We evidence the absence of any magnetic ordering down to 20 mK (\sim J/10^4). We investigate in detail the spin dynamics on well characterized samples in zero and applied longitudinal fields and propose a low T defect based interpretation to explain the unconventional dynamics observed in the quantum spin liquid phase.
Quantum spin liquids (QSLs) define an exotic class of quantum ground states where spins are disordered down to zero temperature. We propose routes to QSLs in kagome optical lattices using applied flux. An optical flux lattice can be applied to induce a uniform flux and chiral three-spin interactions that drive the formation of a gapped chiral spin liquid. A different approach based on recent experiments using laser-assisted tunneling and lattice tilt implements a staggered flux pattern which can drive a gapless spin liquid with symmetry protected nodal lines. Our proposals, therefore, establis…
There is growing evidence from both experiment and numerical studies that low half-odd integer quantum spins on a kagome lattice with predominant antiferromagnetic near neighbor interactions do not order magnetically or break lattice symmetries even at temperatures much lower than the exchange interaction strength. Moreover, there appear to be a plethora of low energy excitations, predominantly singlets but also spin carrying, which suggest that the putative underlying quantum spin liquid is a gapless ``critical spin liquid'' rather than a gapped spin liquid with topological order. Here, we de…
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 revisit the description of the low-energy singlet sector of the spin-1/2 Heisenberg antiferromagnet on kagome in terms of an effective quantum dimer model. With the help of exact diagonalizations of appropriate finite-size clusters, we show that the embedding of a given process in its kagome environment leads to dramatic modifications of the amplitudes of the elementary loop processes, an effect not accessible to the standard approach based on the truncation of the Hamiltonian to the nearest-neighbour valence-bond basis. The resulting parameters are consistent with a Z$_2$ spin liquid rathe…
Recent years have seen the discovery of a chiral spin liquid state - a bosonic analogue of a fractional Quantum Hall state first put forward by Kalmeyer and Laughlin in 1987 - in several deformations of the Heisenberg model on the Kagome lattice. Here, we apply state-of-the-art numerical techniques to one such model, where breaking of the time-reversal symmetry drives the system into the chiral phase. Our methods allow us to obtain explicit matrix-product state representations of the low-lying excitations of the chiral spin liquid state, including the topologically non-trivial semionic excitat…
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…
Recent numerical studies have provided strong evidence for a gapped $Z_2$ quantum spin liquid in the kagome lattice spin-1/2 Heisenberg model. A special feature of spin liquids is that symmetries can be fractionalized, and different patterns of symmetry fractionalization imply distinct phases. The symmetry fractionalization pattern for the kagome spin liquid remains to be determined. A popular approach to studying spin liquids is to decompose the physical spin into partons obeying either bose (Schwinger bosons) or fermi (Abrikosov fermions) statstics, which are then treated within the mean-fie…
We investigate the extended Heisenberg model on the Kagome lattice by using Gutzwiller projected fermionic states and the variational Monte Carlo technique. In particular, when both second- and third-neighbor super-exchanges are considered, we find that a gapped spin liquid described by non-trivial magnetic fluxes and long-range chiral-chiral correlations is energetically favored compared to the gapless U(1) Dirac state. Furthermore, the topological Chern number, obtained by integrating the Berry curvature, and the degeneracy of the ground state, by constructing linearly independent states, le…
The Dirac spin liquid ground state of the spin 1/2 Heisenberg kagome antiferromagnet has potential instabilities[1-4]. This has been suggested as the reason why it is not strongly supported in large-scale numerical calculations[5]. However, previous attempts to observe these instabilities have failed. We report on the discovery of a projected BCS state with lower energy than the projected Dirac spin liquid state which provides new insight into the stability of the ground state of the kagome antiferromagnet. The new state has three remarkable features. First, it breaks both spatial symmetry in …
We study $S=1$ spin liquid states on the kagome lattice constructed by Gutzwiller-projected $p_x+ip_y$ superconductors. We show that the obtained spin liquids are either non-Abelian or Abelian topological phases, depending on the topology of the fermionic mean-field state. By calculating the modular matrices $S$ and $T$, we confirm that projected topological superconductors are non-Abelian chiral spin liquid (NACSL). The chiral central charge and the spin Hall conductance we obtained agree very well with the $SO(3)_1$ (or, equivalently, $SU(2)_2$) field theory predictions. We propose a local H…
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…
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.
We study the system size dependence of the singlet-triplet excitation gap in the $S=1/2$ kagome-lattice Heisenberg antiferromagnet by numerical diagonalization. We successfully obtain a new result of a cluster of 42 sites. The two sequences of gaps of systems with even-number sites and that with odd-number sites are separately analyzed. Careful examination clarifies that there is no contradiction when we consider the system to be gapless.
We study the nearest neighbor $XXZ$ Heisenberg quantum antiferromagnet on the kagome lattice. Here we consider the effects of several perturbations: a) a chirality term, b) a Dzyaloshinski-Moriya term, and c) a ring-exchange type term on the bowties of the kagome lattice, and inquire if they can suppport chiral spin liquids as ground states. The method used to study these Hamiltonians is a flux attachment transformation that maps the spins on the lattice to fermions coupled to a Chern-Simons gauge field on the kagome lattice. This transformation requires us to consistently define a Chern-Simon…
Recent experiments indicate that Na$_4$Ir$_3$O$_8$, a material in which s=1/2 iridium local moments form a three dimensional network of corner-sharing triangles, may have a quantum spin liquid ground state with gapless spin excitations. Using a combination of exact diagonalization, symmetry analysis of fermionic mean field ground states and Gutzwiller projected variational wavefunction studies, we propose a quantum spin liquid with spinon Fermi surfaces as a favorable candidate for the ground state of the Heisenberg model on the hyper-kagome lattice of Na$_4$Ir$_3$O$_8$. We present a renormali…
Motivated by recent experiments on Nd-langasite, we consider the effect of strong easy axis single-ion anisotropy $D$ on $S > 3/2$ spins interacting with antiferromagnetic exchange $J$ on the Kagome lattice. When $T \ll DS^2$, the collinear low energy states selected by the anisotropy map on to configurations of the classical Kagome lattice Ising antiferromagnet. However, the low temperature limit is quite different from the cooperative Ising paramagnet that obtains classically for $T \ll JS^2$. We find that sub-leading ${\mathcal O}(J^3S/D^2)$ multi-spin interactions arising from the transver…
We study a class of disordered continuous classical spin systems including the kagome Heisenberg magnet. While each term in its local Hamiltonian can be independently minimised, we find {\it discrete} degenerate ground states whose number grows exponentially with system size. These states do not exhibit zero-energy `excitations' characteristic of highly frustrated magnets but instead are local minima of the energy landscape, albeit with an anomalously soft excitation spectrum. This represents a spin liquid version of the phenomenon of jamming familiar from granular media and structural glasses…
The anyonic excitations of a spin-liquid can feature fractional quantum numbers under space-group symmetries. Detecting these fractional quantum numbers, which are analogs of the fractional charge of Laughlin quasiparticles, may prove easier than the direct observation of anyonic braiding and statistics. Motivated by the recent numerical discovery of spin-liquid phases in the kagome Heisenberg antiferromagnet, we theoretically predict the pattern of space group symmetry fractionalization in the kagome lattice chiral spin liquid. We provide a method to detect these fractional quantum numbers in…
We provide strong numerical evidence, using improved variational wave functions, for a ground state with vanishing spin gap in the spin-$1/2$ quantum Heisenberg model on the kagome lattice. Starting from the algebraic $U(1)$ Dirac spin liquid state proposed by Y. Ran $et al.$ [Phys. Rev. Lett. $98$, $117205$ ($2007$)] and iteratively applying a few Lanczos steps, we compute the lowest $S=2$ excitation constructed by exciting spinons close to the Dirac nodes. Our results are compatible with a vanishing spin gap in the thermodynamic limit and in consonance with a power-law decay of long distance…
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…
Magnetic susceptibility, NMR, muSR, and inelastic neutron scattering measurements show that kapellasite, Cu3Zn(OH)6Cl2, a geometrically frustrated spin-1/2 kagome antiferromagnet polymorphous with the herbertsmithite mineral, is a gapless spin liquid with frustrated interactions showing unusual dynamic short-range correlations of non-coplanar cuboc2 type which persist down to 20 mK. The Hamiltonian is determined from a fit of a high-temperature series expansion to thermodynamical data. The experimental data are compared to theoretical calculations using the Schwinger-boson approach.
We calculate dynamical spin structure factors for gapped chiral spin liquid states in the spin-1/2 Heisenberg antiferromagnet on the kagome lattice using Schwinger-boson mean-field theory. In contrast to static (equal-time) structure factors, the dynamical structure factor shows clear signatures of time-reversal symmetry breaking for chiral spin liquid states. In particular, momentum inversion $\bm{k} \to -\bm{k}$ symmetry as well as the six-fold rotation symmetry around the $Γ$-point are lost. We highlight other interesting features, such as a relatively flat onset of the two-spinon continuum…
The kagome Heisenberg antiferromagnet is a leading candidate in the search for a spin system with a quantum spin-liquid ground state. The nature of its ground state remains a matter of great debate. We conducted 17-O single crystal NMR measurements of the S=1/2 kagome lattice in herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$, which is known to exhibit a spinon continuum in the spin excitation spectrum. We demonstrate that the intrinsic local spin susceptibility $χ_{kagome}$ deduced from the 17-O NMR frequency shift asymptotes to zero below temperature T ~ 0.03 J, where J ~ 200 K is the Cu-Cu super-exc…
We find an exact spin liquid state without time reversal symmetry on the kagome lattice with odd number of electrons per unit cell and explicit wave functions for all eigenstates. We also obtain that all spin-spin correlations are zero except trivial cases. We then show that there are anyonic excitations in our model. Finally, we demonstrate the existence of ground state degeneracy and gapless edge states indicating nontrivial topological order in our model. We also label all eiginstates on torus by local and global string operators.
