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arXiv:0902.1752 · Physical Review B

Valence bond solid phases on deformed kagome lattices: Application to Rb2Cu3SnF12

Bohm‐Jung Yang, Yong Baek Kim

Published Jun 12, 2009• 19 citations
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Abstract

Motivated by a recent experiment on ${\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}$, where spin-1/2 ${\text{Cu}}^{2+}$ moments reside on the layers of kagome-like lattices, we investigate quantum ground states of the antiferromagnetic Heisenberg model on a series of deformed kagome lattices. The deformation is characterized by a weaker exchange coupling $\ensuremath{\alpha}J$ on certain lattice links appropriate for ${\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}$ with $\ensuremath{\alpha}=1$ corresponding to the ideal kagome lattice. In particular, we study possible valence bond solid phases using the perturbation theory around isolated dimer limits, dimer series expansion, and self-consistent bond operator mean-field theory. It is shown that the valence bond solid phase with a 36-site unit cell of the ideal kagome lattice is quite sensitive to a small lattice distortion as the kind discovered in ${\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}$. As a result, we find that a more likely quantum ground state in ${\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}$ is the valence bond solid phase with a 12-site unit cell, where six dimers form a pinwheel structure, leading to strong modification of the elementary triplet and singlet excitation spectra in the deformed kagome lattices.

DOI
10.1103/physrevb.79.224417

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Motivated by a recent experiment on Rb2Cu3SnF12{\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}Rb2​Cu3​SnF12​, where spin-1/2 Cu2+{\text{Cu}}^{2+}Cu2+ moments reside on the layers of kagome-like lattices, we investigate quantum ground states of the antiferromagnetic Heisenberg model on a series of deformed kagome lattices. The deformation is characterized by a weaker exchange coupling \ensuremathαJ\ensuremath{\alpha}J\ensuremathαJ on certain lattice links appropriate for Rb2Cu3SnF12{\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}Rb2​Cu3​SnF12​ with \ensuremathα=1\ensuremath{\alpha}=1\ensuremathα=1 corresponding to the ideal kagome lattice. In particular, we study possible valence bond solid phases using the perturbation theory around isolated dimer limits, dimer series expansion, and self-consistent bond operator mean-field theory. It is shown that the valence bond solid phase with a 36-site unit cell of the ideal kagome lattice is quite sensitive to a small lattice distortion as the kind discovered in Rb2Cu3SnF12{\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}Rb2​Cu3​SnF12​. As a result, we find that a more likely quantum ground state in Rb2Cu3SnF12{\text{Rb}}_{2}{\text{Cu}}_{3}{\text{SnF}}_{12}Rb2​Cu3​SnF12​ is the valence bond solid phase with a 12-site unit cell, where six dimers form a pinwheel structure, leading to strong modification of the elementary triplet and singlet excitation spectra in the deformed kagome lattices.
Motivated by experimental results for the thermodynamic properties of the Rb 2 Cu 3 SnF 12 material and the discovery of its valence-bond solid ground state, we utilize the numerical linked-cluster expansions (NLCEs) and devise an expansion tailored to solve the Heisenberg model on a pinwheel-distorted kagome lattice. Using the exchange interactions that are relevant to Rb 2 Cu 3 SnF 12 , we calculate its uniform spin susceptibility and find a very good agreement with experiment. Next, we focus on the ground state of a simplified model of the distorted kagome lattice and take advantage of a zero-temperature Lanczos-based NLCE to study the approach to the ground state of the uniform kagome lattice Heisenberg model using a tuning parameter. Together with results from exact diagonalization of finite clusters, we find evidence that a phase transition occurs before the uniform limit is reached.
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.
A proposed ground state for the kagome lattice Heisenberg model consists of a valence bond crystal (VBC) with a 36-site unit cell. We calculate the low-lying triplet and singlet excitations in the VBC phase for the infinite-lattice model and for the 36-site cluster. For the infinite lattice, the lowest triplet excitation is found to have a spin gap of approximately $0.08\ifmmode\pm\else\textpm\fi{}0.02J$ and a bandwidth of only about 0.01J0.01J0.01J. For the 36-site cluster, which consists of a single unit cell with periodic boundary conditions, there are substantial finite-size effects: the spin gap there is estimated to be approximately 0.2J0.2J0.2J, which is close to the exact diagonalization result of 0.164J0.164J0.164J. The triplet excitations attract one another and form many bound states in the spin-singlet channel. We find a large number of such bound states for the 36-site cluster, many of which appear to lie below the spin gap, which is again in agreement with the results from exact diagonalization.
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.
Motivated by the recent neutron-scattering experiment on Rb2{}_{2}2​Cu3{}_{3}3​SnF12{}_{12}12​ [Nature Phys. 6, 865 (2010)], we investigate the effect of Dzyaloshinskii-Moriya interactions in a theoretical model for the magnetic structure of this material. Considering the valence bond solid ground state, which has a 12-site unit cell, we develop the bond operator mean-field theory. It is shown that the Dzyaloshinskii-Moriya interactions significantly modify the triplon dispersions around the $\ensuremath{\Gamma}$ point and cause a shift of the spin-gap (the minimum triplon gap) position from the KKK to $\ensuremath{\Gamma}$ point in the first Brillouin zone. The spin gap is also evaluated in exact diagonalization studies on a 24-site cluster. We discuss a magnetic transition induced by the Dzyaloshinskii-Moriya interactions in the bond operator framework. Moreover, the magnetization process under external magnetic fields is studied within the exact diagonalization approach. We find that the results of both approaches are consistent with the experimental findings.
The spin-12\frac{1}{2}21​ Heisenberg model on the kagome lattice, which is closely realized in layered Mott insulators such as ZnCu3(OH)6Cl2{\mathrm{ZnCu}}_{3}{(\mathrm{OH})}_{6}{\mathrm{Cl}}_{2}ZnCu3​(OH)6​Cl2​, is one of the oldest and most enigmatic spin-12\frac{1}{2}21​ lattice models. While the numerical evidence has accumulated in favor of a quantum spin liquid, the debate is still open as to whether it is a Z2{Z}_{2}Z2​ spin liquid with very short-range correlations (some kind of resonating valence bond spin liquid), or an algebraic spin liquid with power-law correlations. To address this issue, we have pushed the program started by Rokhsar and Kivelson in their derivation of the effective quantum dimer model description of Heisenberg models to unprecedented accuracy for the spin-12\frac{1}{2}21​ kagome, by including all the most important virtual singlet contributions on top of the orthogonalization of the nearest-neighbor valence bond singlet basis. Quite remarkably, the resulting picture is a competition between a Z2{Z}_{2}Z2​ spin liquid and a diamond valence bond crystal with a 12-site unit cell, as in the density-matrix renormalization group simulations of Yan et al. Furthermore, we found that, on cylinders of finite diameter ddd, there is a transition between the Z2{Z}_{2}Z2​ spin liquid at small ddd and the diamond valence bond crystal at large ddd, the prediction of the present microscopic description for the two-dimensional lattice. These results show that, if the ground state of the spin-12\frac{1}{2}21​ kagome antiferromagnet can be described by nearest-neighbor singlet dimers, it is a diamond valence bond crystal, and, a contrario, that, if the system is a quantum spin liquid, it has to involve long-range singlets, consistent with the algebraic spin liquid scenario.