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arXiv:1804.03333 · Proceedings of the National Academy of Sciences

Identifying spinon excitations from dynamic structure factor of spin-1/2 Heisenberg antiferromagnet on the Kagome lattice

Wei Kang Zhu, Shou-Shu Gong, D. N. Sheng

Published Mar 4, 2019• 41 citations
arXivHTMLPDF

Abstract

A spin-[Formula: see text] lattice Heisenberg Kagome antiferromagnet (KAFM) is a prototypical frustrated quantum magnet, which exhibits exotic quantum spin liquids that evade long-range magnetic order due to the interplay between quantum fluctuation and geometric frustration. So far, the main focus has remained on the ground-state properties; however, the theoretical consensus regarding the magnetic excitations is limited. Here, we study the dynamic spin structure factor (DSSF) of the KAFM by means of the density matrix renormalization group. By comparison with the well-defined magnetically ordered state and the chiral spin liquid sitting nearby in the phase diagram, the KAFM with nearest neighbor interactions shows distinct dynamical responses. The DSSF displays important spectral intensity predominantly in the low-frequency region around the [Formula: see text] point in momentum space and shows a broad spectral distribution in the high-frequency region for momenta along the boundary of the extended Brillouin zone. The excitation continuum identified from momentum- and energy-resolved DSSF signals emergent spinons carrying fractional quantum numbers. These results capture the main observations in the inelastic neutron scattering measurements of herbertsmithite and indicate the spin liquid nature of the ground state. By tracking the DSSF across quantum-phase transition between the chiral spin liquid and the magnetically ordered phase, we identify the condensation of two-spinon bound state driving the quantum-phase transition.

DOI
10.1073/pnas.1807840116

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Understanding the nature of the excitation spectrum in quantum spin liquids is of fundamental importance, in particular for the experimental detection of candidate materials.However, current theoretical and numerical techniques have limited capabilities, especially in obtaining the dynamical structure factor, which gives a crucial characterization of the ultimate nature of the quantum state and may be directly assessed by inelastic neutron scattering.In this work, we investigate the low-energy properties of the S ¼ 1=2 Heisenberg model on the triangular lattice, including both nearest-neighbor J 1 and next-nearestneighbor J 2 superexchanges, by a dynamical variational Monte Carlo approach that allows accurate results on spin models.For J 2 ¼ 0, our calculations are compatible with the existence of a well-defined magnon in the whole Brillouin zone, with gapless excitations at K points (i.e., at the corners of the Brillouin zone).The strong renormalization of the magnon branch (also including rotonlike minima around the M points, i.e., midpoints of the border zone) is described by our Gutzwiller-projected state, where Abrikosov fermions are subject to a nontrivial magnetic π flux threading half of the triangular plaquettes.When increasing the frustrating ratio J 2 =J 1 , we detect a progressive softening of the magnon branch at M, which eventually becomes gapless within the spin-liquid phase.This feature is captured by the band structure of the unprojected wave function (with two Dirac points for each spin component).In addition, we observe an intense signal at low energies around the K points, which cannot be understood within the unprojected picture and emerges only when the Gutzwiller projection is considered, suggesting the relevance of gauge fields for the low-energy physics of spin liquids.

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A spin-[Formula: see text] lattice Heisenberg Kagome antiferromagnet (KAFM) is a prototypical frustrated quantum magnet, which exhibits exotic quantum spin liquids that evade long-range magnetic order due to the interplay between quantum fluctuation and geometric frustration. So far, the main focus has remained on the ground-state properties; however, the theoretical consensus regarding the magnetic excitations is limited. Here, we study the dynamic spin structure factor (DSSF) of the KAFM by means of the density matrix renormalization group. By comparison with the well-defined magnetically ordered state and the chiral spin liquid sitting nearby in the phase diagram, the KAFM with nearest neighbor interactions shows distinct dynamical responses. The DSSF displays important spectral intensity predominantly in the low-frequency region around the [Formula: see text] point in momentum space and shows a broad spectral distribution in the high-frequency region for momenta along the boundary of the extended Brillouin zone. The excitation continuum identified from momentum- and energy-resolved DSSF signals emergent spinons carrying fractional quantum numbers. These results capture the main observations in the inelastic neutron scattering measurements of herbertsmithite and indicate the spin liquid nature of the ground state. By tracking the DSSF across quantum-phase transition between the chiral spin liquid and the magnetically ordered phase, we identify the condensation of two-spinon bound state driving the quantum-phase transition.
Quantum spin liquids exhibit fractionalized spin excitations as a consequence of strong quantum many-body effects. The kagome antiferromagnetic Heisenberg model is a promising candidate for a quantum spin-liquid ground state; however, the nature of its excitation spectrum remains controversial, particularly regarding the presence of a spin gap and the gauge structure coupled to fractional quasiparticles. To address these issues, parton approaches have been extensively employed, where spin operators are represented in terms of fermionic or bosonic quasiparticles within the Abrikosov fermion and Schwinger boson frameworks. Thus far, these approaches have been pursued independently, and it has remained unclear how the results obtained from these frameworks compare, particularly with respect to the spin dynamics and gauge structure of the kagome antiferromagnet. Here, we investigate the dynamical spin structure factor of the antiferromagnetic Heisenberg model with a Dzyaloshinskii-Moriya interaction on the kagome lattice, relevant to herbertsmithite, by employing both approaches. We find that the dynamical spin structure factor obtained from the Abrikosov fermion mean-field theory exhibits dome-shaped features, and that its continuum structure significantly depends on the gauge structure of the spin-liquid ansatz. On the other hand, the Schwinger boson mean-field theory yields a concave-down structure in the low-energy region, distinct from that obtained using the Abrikosov fermion approach. Moreover, incorporating many-body effects beyond the mean-field approximation substantially reduces the low-energy gap and enhances the low-energy spectral weight, consistent with experimental observations. Our results suggest the importance of many-body effects in the Schwinger boson theory for capturing the low-energy spin dynamics of kagome antiferromagnets.
It has been suggested that the nearest-neighbor antiferromagnetic Heisenberg model on the Kagome lattice may be a good starting point for understanding the spin-liquid behavior discovered in herbertsmithite. In this work, we investigate possible quantum spin liquid phases in the presence of spin-rotation symmetry-breaking perturbations such as Dzyaloshinskii-Moriya and Ising interactions, as well as second-neighbor antiferromagnetic Heisenberg interactions. Experiments suggest that such perturbations are likely to be present in herbertsmithite. We use the projective symmetry group analysis within the framework of the slave-fermion construction of quantum spin liquid phases and systematically classify possible spin liquid phases in the presence of perturbations mentioned above. The dynamical spin-structure factor for relevant spin liquid phases is computed and the effect of those perturbations are studied. Our calculations reveal dispersive features in the spin structure factor embedded in a generally diffuse background due to the existence of fractionalized spin-1/21/21/2 excitations called spinons. For two of the previously proposed Z2{Z}_{2}Z2​ states, the dispersive features are almost absent, and diffuse scattering dominates over a large energy window throughout the Brillouin zone. This resembles the structure factor observed in recent inelastic neutron-scattering experiments on singlet crystals of herbertsmithite. Furthermore, one of the Z2{Z}_{2}Z2​ states with the spin structure factor with mostly diffuse scattering is gapped, and it may be adiabatically connected to the gapped spin liquid state observed in recent density-matrix renormalization group calculations for the nearest-neighbor antiferromagnetic Heisenberg model. The perturbations mentioned above are found to enhance the diffuse nature of the spin structure factor and reduce the momentum dependencies of the spin gap. We also calculate the electron spin resonance (ESR) absorption spectra that further characterize the role of spin-rotation symmetry-breaking perturbations in these states. We suggest that the measurement of ESR spectra can shed more light into the nature of the ground state in herbertsmithite.
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(q,ω)S(\mathbf{q},ω)S(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(q,ω)S(\mathbf{q},ω)S(q,ω) at KKK points in the extended magnetic Brillouin zone, in contrast to experiments where low energy peaks are found at MMM points. There is no obviuos contradiction between DSL and neutron scattering measurements. Besides a fractionalized spin (i.e. spin-1/2), spinons in DSL carry a fractionalized crystal momentum which is potentially detectable in SWC in the neutron scattering measurements.
Quantum spin liquids (QSLs) host exotic fractionalized magnetic and gauge-field excitations whose microscopic origins and experimental verification remain frustratingly elusive. In the absence of static magnetic order, the spin excitation spectrum constitutes the crucial probe of QSL behavior, but its theoretical computation is a serious challenge. Here we employ state-of-the-art tensor-network methods to obtain the full dynamical spectral function of the J1J_1J1​-J2J_2J2​ kagome Heisenberg model and benchmark our results by tracking their evolution across the magnetically ordered and QSL phases. Reducing ∣J2∣/J1|J_2|/J_1∣J2​∣/J1​ causes increasingly strong spin-wave renormalization, flattening these modes then merging them into a continuum characteristic of deconfined spinons at all finite energies in the QSL. The low-energy continuum and the occurrence of gap closure at multiple high-symmetry points identify this gapless QSL as the U(1) Dirac spin liquid. These results establish a unified understanding of spin excitations in highly frustrated quantum magnets and provide clear spectral fingerprints for experimental detection in candidate kagome QSL materials.
Understanding the nature of the excitation spectrum in quantum spin liquids is of fundamental importance, in particular for the experimental detection of candidate materials.However, current theoretical and numerical techniques have limited capabilities, especially in obtaining the dynamical structure factor, which gives a crucial characterization of the ultimate nature of the quantum state and may be directly assessed by inelastic neutron scattering.In this work, we investigate the low-energy properties of the S ¼ 1=2 Heisenberg model on the triangular lattice, including both nearest-neighbor J 1 and next-nearestneighbor J 2 superexchanges, by a dynamical variational Monte Carlo approach that allows accurate results on spin models.For J 2 ¼ 0, our calculations are compatible with the existence of a well-defined magnon in the whole Brillouin zone, with gapless excitations at K points (i.e., at the corners of the Brillouin zone).The strong renormalization of the magnon branch (also including rotonlike minima around the M points, i.e., midpoints of the border zone) is described by our Gutzwiller-projected state, where Abrikosov fermions are subject to a nontrivial magnetic π flux threading half of the triangular plaquettes.When increasing the frustrating ratio J 2 =J 1 , we detect a progressive softening of the magnon branch at M, which eventually becomes gapless within the spin-liquid phase.This feature is captured by the band structure of the unprojected wave function (with two Dirac points for each spin component).In addition, we observe an intense signal at low energies around the K points, which cannot be understood within the unprojected picture and emerges only when the Gutzwiller projection is considered, suggesting the relevance of gauge fields for the low-energy physics of spin liquids.
A quantum spin liquid (QSL) is an exotic quantum state of matter characterized by fluctuating spins which may exhibit long-range entanglement. Among the possible host candidates for a QSL ground state, the SSS=1/2 kagome lattice antiferromagnet is particularly promising. Using high resolution inelastic neutron scattering measurements on Zn-barlowite (Znx_\mathrm{x}x​Cu4−x_\mathrm{4-x}4−x​(OD)6_\mathrm{6}6​FBr, x≃0.80x\simeq 0.80x≃0.80), we measure a spin excitation spectrum consistent with a QSL ground state. Continuum scattering above $\sim1meVmatchesthatofherbertsmithite(Zn1 meV matches that of herbertsmithite (Zn1meVmatchesthatofherbertsmithite(Zn_\mathrm{x}CuCuCu_\mathrm{4-x}(OD)(OD)(OD)_6ClClCl_2$, x≃0.85x\simeq 0.85x≃0.85), another prominent kagome QSL material, indicating universal spinon excitations. A detailed analysis of the spin-spin correlations, compared with density matrix renormalization group calculations, further indicate a QSL ground state for the physically relevant Hamiltonian parameters. The measured spectra in Zn-barlowite are consistent with gapped behavior with a gap size Δ=1.1(2)Δ= 1.1(2)Δ=1.1(2) meV. Comparison with a simple pair correlation model allows us to clearly distinguish intrinsic kagome correlations from impurity-induced correlations. Our results clarify the behavior that is universal within this important family of QSL candidate materials.