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arXiv:1006.5370 · Physical Review B

Impurity-doped kagome antiferromagnet: A quantum dimer model approach

Didier Poilblanc, Arnaud Ralko

Published Nov 19, 2010• 27 citations
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Abstract

The doping of quantum Heisenberg antiferromagnets on the kagome lattice by nonmagnetic impurities is investigated within the framework of a generalized quantum dimer model (QDM) describing (a) the valence-bond crystal (VBC), (b) the dimer liquid, and (c) the critical region on equal footing. Following the approach by Ralko et al. [Phys. Rev. Lett. 101, 117204 (2008)] for the square and triangular lattices, we introduce the (minimal) extension of the QDM on the kagome lattice to account for spontaneous creation of mobile $S=1/2$ spinons at finite magnetic field. Modulations of the dimer density (at zero or finite magnetic field) and of the local field-induced magnetization in the vicinity of impurities are computed using Lanczos exact diagonalization techniques on small clusters (48 and 75 sites). The VBC is clearly revealed from its pinning by impurities, while, in the dimer liquid, crystallization around impurities involves only two neighboring dimers. We also find that a next-nearest-neighbor ferromagnetic coupling favors VBC order. Unexpectedly, a small-size spinon-impurity bound state appears in some region of the dimer-liquid phase. In contrast, in the VBC phase the spinon delocalizes within a large region around the impurity, revealing the weakness of the VBC confining potential. Lastly, we observe that an impurity concentration as small as 4% enhances dimerization substantially. These results are confronted to the valence-bond glass scenario [R. R. P. Singh, Phys. Rev. Lett. 104, 177203 (2010)] and implications to the interpretation of the nuclear magnetic resonance spectra of the Herbertsmithite compound are outlined.

DOI
10.1103/physrevb.82.174424

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The doping of quantum Heisenberg antiferromagnets on the kagome lattice by nonmagnetic impurities is investigated within the framework of a generalized quantum dimer model (QDM) describing (a) the valence-bond crystal (VBC), (b) the dimer liquid, and (c) the critical region on equal footing. Following the approach by Ralko et al. [Phys. Rev. Lett. 101, 117204 (2008)] for the square and triangular lattices, we introduce the (minimal) extension of the QDM on the kagome lattice to account for spontaneous creation of mobile S=1/2S=1/2S=1/2 spinons at finite magnetic field. Modulations of the dimer density (at zero or finite magnetic field) and of the local field-induced magnetization in the vicinity of impurities are computed using Lanczos exact diagonalization techniques on small clusters (48 and 75 sites). The VBC is clearly revealed from its pinning by impurities, while, in the dimer liquid, crystallization around impurities involves only two neighboring dimers. We also find that a next-nearest-neighbor ferromagnetic coupling favors VBC order. Unexpectedly, a small-size spinon-impurity bound state appears in some region of the dimer-liquid phase. In contrast, in the VBC phase the spinon delocalizes within a large region around the impurity, revealing the weakness of the VBC confining potential. Lastly, we observe that an impurity concentration as small as 4% enhances dimerization substantially. These results are confronted to the valence-bond glass scenario [R. R. P. Singh, Phys. Rev. Lett. 104, 177203 (2010)] and implications to the interpretation of the nuclear magnetic resonance spectra of the Herbertsmithite compound are outlined.
In this paper, we do a complete classification of valence-bond crystals (VBCs) on the kagomé lattice based on general arguments of symmetry only and thus identify many new VBCs for different unit cell sizes. For the spin-1/2 Heisenberg antiferromagnet, we study the relative energetics of competing gapless spin liquids (SLs) and VBC phases within the class of Gutzwiller-projected fermionic wave functions using variational Monte Carlo techniques, hence implementing exactly the constraint of one fermion per site. By using a state-of-the-art optimization method, we conclusively show that the U(1) Dirac SL is remarkably stable towards dimerizing into all 6-, 12- and 36-site unit cell VBCs. This stability is also preserved on addition of a next-nearest-neighbor super-exchange coupling of both antiferromagnetic and ferromagnetic (FM) type. However, we find that a 36-site unit cell VBC is stabilized on addition of a very small next-nearest-neighbor FM super-exchange coupling, i.e. | J 2 | ≈ 0.045, and this VBC is the same in terms of space-group symmetry as that obtained in an effective quantum dimer model study. It breaks reflection symmetry, has a nontrivial flux pattern and is a strong dimerization of the uniform RVB SL.
The low-energy singlet dynamics of the quantum Heisenberg antiferromagnet on the kagome lattice is described by a quantitative quantum dimer model. Using advanced numerical tools, the latter is shown to exhibit valence-bond crystal (VBC) order with a large 36-site unit cell and hidden degeneracy between even odd parities. Evidences are given that this ground state lies in the vicinity of a Z2{\mathbb{Z}}_{2}Z2​ dimer-liquid region separated by a quantum critical point (QCP). Implications regarding numerical analysis and experiments are discussed.
The highly frustrated spin-12\frac{1}{2}21​ quantum Heisenberg model with both nearest (J1{J}_{1}J1​) and next-nearest (J2{J}_{2}J2​) neighbor exchange interactions is revisited by using an extended variational space of projected wave functions that are optimized with state-of-the-art methods. Competition between modulated valence-bond crystals (VBCs) proposed in the literature and the Dirac spin liquid (DSL) is investigated. We find that the addition of a small ferromagnetic next-nearest-neighbor exchange coupling ∣J2∣>0.09J1|{J}_{2}|>0.09{J}_{1}∣J2​∣>0.09J1​ leads to stabilization of a 36-site unit cell VBC, although the DSL remains a local minimum of the variational parameter landscape. This implies that the VBC is not trivially connected to the DSL; instead it possesses a nontrivial flux pattern and large dimerization.
The singlet dynamics, which plays a major role in the physics of the spin-1/2 quantum Heisenberg antiferromagnet (QHAF) on the kagome lattice, can be approximately described by projecting onto the nearest-neighbor valence bond (NNVB) singlet subspace. We revisit here the effective quantum dimer model, which originates from the latter NNVB-projected Heisenberg model via a nonperturbative Rokhsar-Kivelson-like scheme. By using Lanczos exact diagonalization on a 108-site cluster supplemented by a careful symmetry analysis, it is shown that a previously found 36-site valence bond crystal (VBC) in fact competes with a new type of 12-site ``resonating-columnar'' VBC. Interestingly, these two VBCs ``emerge'' in different topological sectors. The exceptionally large degeneracy of the ground-state multiplets (144 on our 108-site cluster) and the proximity of a Z2{\mathbb{Z}}_{2}Z2​ dimer liquid have implications for the interpretation of numerical results on the QHAF, which are outlined. The possibility of a chiral VBC (i.e., spontaneously breaking time-reversal symmetry) is also discussed.
We revisit the description of the low-energy singlet sector of the spin-12\frac{1}{2}21​ 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-neighbor valence-bond basis. The resulting parameters are consistent with a Z2{Z}_{2}Z2​ spin liquid rather than with a valence-bond crystal, in agreement with the last density matrix renormalization group results.
Using series expansions around the dimer limit, we find that the ground state of the spin-1/2 Heisenberg antiferromagnet on the kagome lattice appears to be a valence bond crystal (VBC) with a 36 site unit cell, and ground-state energy per site $E=\ensuremath{-}0.433\ifmmode\pm\else\textpm\fi{}0.001\phantom{\rule{0.3em}{0ex}}\mathrm{J}$. It consists of a honeycomb lattice of ``perfect hexagons.'' The energy difference between the ground state and other ordered states with the maximum number of perfect hexagons, such as a stripe-ordered state, is of order 0.001J0.001\phantom{\rule{0.3em}{0ex}}\mathrm{J}0.001J. The expansion is also done for the 36 site system with periodic boundary conditions; its energy per site is $0.005\ifmmode\pm\else\textpm\fi{}0.001\phantom{\rule{0.3em}{0ex}}\mathrm{J}$ lower than the infinite system, consistent with exact diagonalization results. Every unit cell of the VBC has two singlet states whose degeneracy is not lifted to sixth order in the expansion. We estimate this energy difference to be less than 0.001J0.001\phantom{\rule{0.3em}{0ex}}\mathrm{J}0.001J. The dimerization order parameter is found to be robust. Two leading orders of perturbation theory give lowest triplet excitations to be dispersionless and confined to the perfect hexagons.