Abstract Spin-1/2 kagome antiferromagnets are leading candidates for realizing quantum spin liquid (QSL) ground states. While QSL ground states are predicted for the pure Heisenberg model, understanding the robustness of the QSL to additional interactions that may be present in real materials is a forefront question in the field. Here we employ large-scale density-matrix renormalization group simulations to investigate the effects of next-nearest neighbor exchange couplings J 2 and Dzyaloshinskii-Moriya interactions D , which are relevant to understanding the prototypical kagome materials herbertsmithite and Zn-barlowite. By utilizing clusters as large as XC12 and extrapolating the results to the thermodynamic limit, we precisely delineate the scope of the QSL phase, which remains robust across an expanded parameter range of J 2 and D . Direct comparison of the simulated static and dynamic spin structure factors with inelastic neutron scattering reveals the parameter space of the Hamiltonians for herbertsmithite and Zn-barlowite, and, importantly, provides compelling evidence that both materials exist within the QSL phase. These results establish a powerful convergence of theory and experiment in this most elusive state of matter.
Abstract Spin-1/2 kagome antiferromagnets are leading candidates for realizing quantum spin liquid (QSL) ground states. While QSL ground states are predicted for the pure Heisenberg model, understanding the robustness of the QSL to additional interactions that may be present in real materials is a forefront question in the field. Here we employ large-scale density-matrix renormalization group simulations to investigate the effects of next-nearest neighbor exchange couplings J 2 and Dzyaloshinskii-Moriya interactions D , which are relevant to understanding the prototypical kagome materials herbertsmithite and Zn-barlowite. By utilizing clusters as large as XC12 and extrapolating the results to the thermodynamic limit, we precisely delineate the scope of the QSL phase, which remains robust across an expanded parameter range of J 2 and D . Direct comparison of the simulated static and dynamic spin structure factors with inelastic neutron scattering reveals the parameter space of the Hamiltonians for herbertsmithite and Zn-barlowite, and, importantly, provides compelling evidence that both materials exist within the QSL phase. These results establish a powerful convergence of theory and experiment in this most elusive state of matter.
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 S=1/2 kagome lattice antiferromagnet is particularly promising. Using high resolution inelastic neutron scattering measurements on Zn-barlowite (ZnxCu4−x(OD)6FBr, x≃0.80), we measure a spin excitation spectrum consistent with a QSL ground state. Continuum scattering above $\sim1meVmatchesthatofherbertsmithite(Zn_\mathrm{x}Cu_\mathrm{4-x}(OD)_6Cl_2$, x≃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) 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.
Herbertsmithite (ZnCu3(OH)6Cl2) 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 (ZnxCu4−x(OD)6Cl2, x≃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.
Unraveling the Kagome Antiferromagnetic 3J Model and Its Materials: An Integrated Approach
We investigate the ground-state and finite-temperature properties of the kagome antiferromagnetic Heisenberg model with three inequivalent couplings, dubbed the 3J model, which is designed for the candidate Dirac quantum spin liquid (QSL) material YCu3(OH)6Br2[Br1−x(OH)x] (see, e.g., Zeng et al., 2024). Employing large-scale density-matrix renormalization group (DMRG) supplemented by neural quantum states (NQS) simulations, we identify an intermediate QSL phase between two magnetically ordered phases. We also find that this QSL is separated from the kagome spin liquid ground state at the isotropic limit. To establish a direct comparison with experiments, we compute the specific heat of the model by means of advanced exponential (XTRG) and tangent-space (tanTRG) thermal tensor-network methods. In the magnetically ordered phase, the specific heat over temperature exhibits a shoulder at a temperature that is a fraction of the coupling strength Jh, which disappears in the QSL phase. These universal behaviors are consistent with the experimentally observed specific heat in 3J materials for both ordered and QSL candidate samples. Our work thus connects microscopic models with experimentally measurable signatures, exemplifying an integrated approach to understanding QSL phenomena in frustrated quantum magnets~ (see Meng et al., 2026), with 3J materials serving as a representative case and providing a foundation for future studies.
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, ${D}_{c}/J\ensuremath{\simeq}0.012(2)$, lies well below the DM strength proposed in the kagome material herbertsmithite, indicating a need to reassess the apparent spin-liquid behavior reported in this system.
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-1/2 excitations called spinons. For two of the previously proposed 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 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.