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arXiv:1303.1154 · Physical Review B

Quantum spin liquids in the absence of spin-rotation symmetry: Application to herbertsmithite

Tyler Dodds, Subhro Bhattacharjee, Yong Baek Kim

Published Dec 12, 2013• 48 citations
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Abstract

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-$1/2$ excitations called spinons. For two of the previously proposed ${Z}_{2}$ 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 ${Z}_{2}$ 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.

DOI
10.1103/physrevb.88.224413

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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.
In recent work, we argued that a particular algebraic spin liquid (ASL) may be the ground state of the S=1/2S=1/2S=1/2 kagome lattice Heisenberg antiferromagnet. Furthermore, this state, which lacks a spin gap, is appealing in light of recent experiments on herbertsmithite [ZnCu3(OH)6Cl2][{\text{ZnCu}}_{3}{(\text{OH})}_{6}{\text{Cl}}_{2}][ZnCu3​(OH)6​Cl2​]. Here, we study the properties of this ASL in more detail using both the low-energy effective field theory and Gutzwiller-projected wave functions of fermionic spinons. We identify the competing orders of the ASL, which are observables having slowly decaying power-law correlations---among them we find a set of magnetic orders lying at the MMM points of the Brillouin zone, the familiar $\mathbit{q}=0$ magnetic ordered state, the ``Hastings'' valence-bond solid (VBS) state, and a pattern of vector spin-chirality ordering corresponding to one of the Dzyaloshinskii--Moriya (DM) interaction terms present in herbertsmithite. Identification of some of these orders requires an understanding of the quantum numbers of magnetic monopole operators in the ASL. We discuss the detection of the magnetic and VBS competing orders in experiments. While we primarily focus on a clean system without DM interaction, we consider the effects of small DM interaction and argue that, surprisingly, it leads to spontaneously broken time-reversal symmetry (for DM interaction that preserves XYXYXY spin rotation symmetry, there is also XYXYXY magnetic order). Our analysis of the projected wave function provides an estimate of the ``Fermi velocity'' vF{v}_{F}vF​ that characterizes all low-energy excitations of the ASL---this allows us to estimate the specific heat, which compares favorably with experiments. We also study the spin and bond correlations of the projected wave function and compare these results with those of the effective field theory. While the spin correlations in the effective field theory and wave function seem to match rather well (although not completely), the bond correlations are more puzzling. We conclude with a discussion of experiments in herbertsmithite and make several predictions.
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.
Herbertsmithite (ZnCu3_33​(OH)6_66​Cl2_22​) is one of the most extensively studied quantum spin liquid (QSL) candidates, yet the precise nature of its ground state remains unresolved. Here, we compare the results of high-resolution inelastic neutron scattering on single crystals of herbertsmithite (Znx_\mathrm{x}x​Cu4−x_\mathrm{4-x}4−x​(OD)6_66​Cl2_22​, x≃0.85x\simeq 0.85x≃0.85) with large-scale density-matrix renormalization group (DMRG) and dynamical DMRG simulations to benchmark the spin Hamiltonian and uncover fundamental properties of the ground state. The measured spin correlations determine an energy density for the Heisenberg model that closely matches simulations, an essential verification of the Hamiltonian. In parallel, DMRG simulations reveal two nearly degenerate QSL states. Both preserve translational symmetry, but one retains the lattice point-group symmetries whereas the other develops anisotropic spin correlations that break point-group symmetry. These two QSLs have distinct spin structure factors, and, remarkably, close agreement with the neutron spectra is achieved with an admixture of the two states. Our results establish a quantitative correspondence between neutron scattering and simulations, and suggest that herbertsmithite realizes a regime in which two proximate gapped QSL states coexist.
Due to strong geometric frustration and quantum fluctuation, the S=1/2S=1/2S=1/2 quantum Heisenberg antiferromagnet on the kagome\text{kagome}kagome lattice has long been considered as an ideal platform to realize a spin liquid (SL), a phase exhibiting fractionalized excitations without any symmetry breaking. A recent numerical study (Yan et al., e-print arXiv:1011.6114) of the Heisenberg S=1/2,kagomeS=1/2,\text{kagome}S=1/2,kagome lattice model (HKLM) shows, in contrast to earlier results, that the ground state is a singlet-gapped SL with signatures of Z2{\mathbb{Z}}_{2}Z2​ topological order. Motivated by this numerical discovery, we use the projective symmetry group to classify all 20 possible Schwinger fermion mean-field states of Z2{\mathbb{Z}}_{2}Z2​ SLs on the kagome\text{kagome}kagome lattice. Among them we found only one gapped Z2{\mathbb{Z}}_{2}Z2​ SL (which we call the ${\mathbb{Z}}_{2}[0,\ensuremath{\pi}]\ensuremath{\beta}$ state) in the neighborhood of the U(1) Dirac SL state. Since its parent state, i.e., the U(1) Dirac SL, was found [Ran et al., Phys. Rev. Lett. 98, 117205 (2007)] to be the lowest among many other candidate U(1) SLs, including the uniform resonating-valence-bond states, we propose this ${\mathbb{Z}}_{2}[0,\ensuremath{\pi}]\ensuremath{\beta}$ state to be the numerically discovered SL ground state of the HKLM.
We analyze the antiferromagnetic spin-1/2 XXZ model on the kagome lattice at finite external magnetic field with the help of a non-perturbative zero-temperature renormalization group (RG) technique. The exact nature of the ground and excited state properties (e.g. gapped or gapless spectrum etc) of this system are still debated. Approximate methods have typically been adopted towards understanding the low-energy spectrum. Following the work of Kumar et al (2014 Phys. Rev. B 90 174409), we use a Jordan–Wigner transformation to map the spin problem into one of spinless fermions (spinons) in the presence of a statistical gauge field, and with nearest-neighbor interactions. While the work of Kumar et al was confined mostly to the plateau at 1/3-filling (magnetization per site) in the XY regime, we analyze the role of inter-spinon interactions in shaping the phases around this plateau in the entire XXZ model. The RG phase diagram obtained contains three spin liquid phases whose position is determined as a function of the exchange anisotropy and the energy scale for fluctuations arising from spinon scattering. Two of these spins liquids are topologically ordered states of matter with gapped, degenerate states on the torus. The gap for one of these phases corresponds to the one-spinon band gap of the Azbel–Hofstadter spectrum for the XY part of the Hamiltonian, while the other arises from two-spinon interactions. The Heisenberg point of this problem is found to lie within the interaction gapped spin liquid phase, in broad agreement with a recent experimental finding. The third phase is an algebraic spin liquid with a gapless Dirac spectrum for spinon excitations, and possess properties that show departures from the Fermi liquid paradigm. The three phase boundaries correspond to critical theories, and meet at a SU (2)-symmetric multicritical point. This special critical point agrees well with the gap-closing transition point predicted by Kumar et al . We discuss the relevance of our findings to various recent experiments, as well as results obtained from other theoretical analyses.