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arXiv:1806.11081

Revealing quantum spin liquid in the herbertsmithite $\rm ZnCu_{3}(OH)_6Cl_{2}$

Vasily R. Shaginyan, M. Ya. Amusia, J. W. Clark, G. S. Japaridze, ALFRED Z. MSEZANE, V. A. Stephanovich, Y. S. Leevik, Elena V. Kirichenko

Published Jun 28, 2018• 1 citation
arXivHTMLPDF

Abstract

Based on experimental data and our theoretical analysis, we provide a strategy for unambiguous establishing of gapless quantum spin liquid state (QSL) in herbertsmithite and other materials. To clarify the nature of QSL, we recommend measurements of heat transport, low-energy inelastic neutron scattering and optical conductivity under the application of external magnetic field at low temperatures. We also suggest that artificially introduced inhomogeneity into $\rm ZnCu_{3}(OH)_6Cl_2$ can stabilize QSL, and serves as a test elucidating the contribution coming from impurities. We predict the results of these measurements in the case of gapless QSL.

DOI
10.48550/arxiv.1806.11081

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Revealing quantum spin liquid in the herbertsmithite ZnCu3(OH)6Cl2\rm ZnCu_{3}(OH)_6Cl_{2}ZnCu3​(OH)6​Cl2​
Based on experimental data and our theoretical analysis, we provide a strategy for unambiguous establishing of gapless quantum spin liquid state (QSL) in herbertsmithite and other materials. To clarify the nature of QSL, we recommend measurements of heat transport, low-energy inelastic neutron scattering and optical conductivity under the application of external magnetic field at low temperatures. We also suggest that artificially introduced inhomogeneity into ZnCu3(OH)6Cl2\rm ZnCu_{3}(OH)_6Cl_2ZnCu3​(OH)6​Cl2​ can stabilize QSL, and serves as a test elucidating the contribution coming from impurities. We predict the results of these measurements in the case of gapless QSL.
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.
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.
An exotic quantum spin liquid (QSL) is formed with such hypothetic particles as fermionic spinons carrying spin 1/2 and no charge. Here we calculate its thermodynamic and relaxation properties. Our calculations unveil the fundamental properties of QSL, forming a strongly correlated Fermi system located at a fermion condensation quantum phase transition. These are in good agreement with experimental data and allow us to detect the behavior of QSL as that observed in heavy-fermion metals. We predict that the thermal resistivity of QSL under the application of magnetic fields at fixed temperature demonstrates a very specific behavior. The key features of our findings are the presence of spin-charge separation and QSL formed with itinerant heavy spinons in herbertsmithite.
Coexisting localized and itinerant gapless excitations in a quantum spin liquid candidate 1T-TaS2_22​
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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.