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arXiv:1309.6309 · Journal of the Physical Society of Japan

Quantum Spin-Liquid Behavior in the Spin-1/2 Random Heisenberg Antiferromagnet on the Triangular Lattice

Ken Watanabe, Hikaru Kawamura, Hiroki Nakano, Tôru Sakai

Published Feb 25, 2014• 142 citations
arXivHTMLPDF

Abstract

Experimental quest for the hypothetical "quantum spin liquid" state has recently met a few promising candidate materials including organic salts κ-(ET)2Cu2(CN)3 and EtMe3Sb[Pd(dmit)2]2, S=1/2 triangular-lattice Heisenberg antiferromagnets consisting of molecular dimers. These compounds exhibit no magnetic ordering nor the spin freezing down to very low temperature, while various physical quantities exhibit gapless behaviors. Recent dielectric measurements revealed the glassy dielectric response suggesting the random freezing of the electric polarization degrees of freedom. Inspired by this observation, we propose as a minimal model of the observed quantum spin-liquid behavior the S=1/2 antiferromagnetic Heisenberg on the triangular lattice with a quenched randomness in the exchange interaction. We study both zero- and finite-temperature properties of the model by an exact diagonalization method, to find that when the randomness exceeds a critical value the model exhibits a quantum spin-liquid ground state. This randomness-induced quantum spin-liquid state exhibits gapless behaviors including the temperature-linear specific heat. The results provide a consistent explanation of the recent experimental observations on organic salts.

DOI
10.7566/jpsj.83.034714

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Experimental quest for the hypothetical "quantum spin liquid" state has recently met a few promising candidate materials including organic salts κ-(ET)2Cu2(CN)3 and EtMe3Sb[Pd(dmit)2]2, S=1/2 triangular-lattice Heisenberg antiferromagnets consisting of molecular dimers. These compounds exhibit no magnetic ordering nor the spin freezing down to very low temperature, while various physical quantities exhibit gapless behaviors. Recent dielectric measurements revealed the glassy dielectric response suggesting the random freezing of the electric polarization degrees of freedom. Inspired by this observation, we propose as a minimal model of the observed quantum spin-liquid behavior the S=1/2 antiferromagnetic Heisenberg on the triangular lattice with a quenched randomness in the exchange interaction. We study both zero- and finite-temperature properties of the model by an exact diagonalization method, to find that when the randomness exceeds a critical value the model exhibits a quantum spin-liquid ground state. This randomness-induced quantum spin-liquid state exhibits gapless behaviors including the temperature-linear specific heat. The results provide a consistent explanation of the recent experimental observations on organic salts.
Inspired by the recent theoretical suggestion that the random-bond S=1/2S=1/2S=1/2 antiferromagnetic Heisenberg model on the triangular and the kagome lattices might exhibit a randomness-induced quantum spin liquid (QSL) behavior when the strength of the randomness exceeds a critical value, and that this ``random-singlet state'' might be relevant to the QSL behaviors experimentally observed in triangular organic salts $\ensuremath{\kappa}\text{\ensuremath{-}}{(\mathrm{ET})}_{2}{\mathrm{Cu}}_{2}{(\mathrm{CN})}_{3}\phantom{\rule{4pt}{0ex}}\mathrm{and}\phantom{\rule{4pt}{0ex}}{\mathrm{EtMe}}_{3}\mathrm{Sb}{[\mathrm{Pd}{(\mathrm{dmit})}_{2}]}_{2}$ and in kagome herbertsmithite ZnCu3(OH)6Cl2{\mathrm{ZnCu}}_{3}{(\mathrm{OH})}_{6}{\mathrm{Cl}}_{2}ZnCu3​(OH)6​Cl2​, we further investigate the nature of the static and the dynamical spin correlations of these models. We compute the static and the dynamical spin structure factors, S(q)S(\mathbf{q})S(q) and $S(\mathbf{q},\ensuremath{\omega})$, by means of an exact diagonalization method. In both triangular and kagome models, the computed $S(\mathbf{q},\ensuremath{\omega})$ in the random-singlet state depends on the wave vector q\mathbf{q}q only weakly, robustly exhibiting gapless behaviors accompanied by the broad distribution extending to higher energy $\ensuremath{\omega}$. Especially in the strongly random kagome model, $S(\mathbf{q},\ensuremath{\omega})$ hardly depends on q\mathbf{q}q, and exhibits an almost flat distribution for a wide range of $\ensuremath{\omega}$, together with a $\ensuremath{\omega}=0$ peak. These features agree semiquantitatively with the recent neutron-scattering data on a single-crystal herbertsmithite. Furthermore, the computed magnetization curve agrees almost quantitatively with the experimental one recently measured on a single-crystal herbertsmithite. These results suggest that the QSL state observed in herbertsmithite might indeed be the randomness-induced QSL state, i.e., the random-singlet state.
The effect of the quenched bond-randomness on the ordering of the S=1/2S=1/2S=1/2 antiferromagnetic Heisenberg model on the kagome lattice is investigated by means of an exact-diagonalization method. When the randomness exceeds a critical value, the ground state of the model exhibits a transition within the non-magnetic state into the randomness-relevant gapless spin-liquid state. Implications to the S=1/2 kagome-lattice antiferromagnet herbertsmithite is discussed.
We investigate the ground-state and finite-temperature properties of the bond-random s=1/2s=1/2s=1/2 Heisenberg model on a honeycomb lattice with frustrated nearest- and next-nearest-neighbor antiferromagnetic interactions, J1J_1J1​ and J2J_2J2​, by the exact diagonalization and the Hams--de Raedt methods. The ground-state phase diagram of the model is constructed in the randomness versus the frustration (J2/J1J_2/J_1J2​/J1​) plane, with the aim of clarifying the effects of randomness and frustration in stabilizing a variety of distinct phases. We find that the randomness induces the gapless quantum spin liquid (QSL)-like state, the random-singlet state, in a wide range of parameter space. The observed robustness of the random-singlet state suggests that the gapless QSL-like behaviors might be realized in a wide class of frustrated quantum magnets possessing a certain amount of randomness or inhomogeneity, without fine-tuning the interaction parameters. Possible implications to recent experiments on the honeycomb-lattice magnets Ba3_33​CuSb2_22​O9_99​ and 6HB-Ba3_33​NiSb2_22​O9_99​ exhibiting the gapless QSL-like behaviors are discussed.
Recent studies have revealed that the randomness-induced quantum spin liquid (QSL)-like state is stabilized in certain frustrated quantum magnets in two and three dimensions. In order to clarify the nature of this gapless QSL-like state, we investigate both zero- and finite-temperature properties of the random-bond one-dimensional (1D) s=12s=12s=12 Heisenberg model with the competing nearest-neighbor and next-nearest-neighbor antiferromagnetic interactions, J1J_1J1​ and J2J_2J2​, by means of the exact diagonalization, density-matrix renormalization-group and Hams--de Raedt methods. We find that, on increasing the frustration J2J_2J2​, the gapless nonmagnetic state stabilized in the unfrustrated model with J2=0J_2=0J2​=0, the {\it unfrustrated\} random-singlet (RS) state, exhibits a phase transition into different gapless nonmagnetic state, the {\it frustrated\} RS state. This frustrated RS state in 1D has properties quite similar to the randomness-induced QSL-like state recently identified in 2D and 3D frustrated magnets exhibiting the TTT-linear low-temperature (TTT) specific heat, while the unfrustrated RS state is more or less specific to the unfrustrated 1D system exhibiting the ∼1(log⁡T)3\sim 1(\log T)^3∼1(logT)3 low-TTT specific heat. Universal features and the robustness against perturbations of the frustrated RS state are emphasized.
We study the ground-state properties of the quantum spin liquid (QSL) phases of the spin-1/21/21/2 antiferromagnetic Heisenberg model on the triangular lattice with nearest- (J1)({J}_{1})(J1​), next-nearest- (J2)({J}_{2})(J2​), and third-neighbor (J3)({J}_{3})(J3​) interactions by using the density-matrix renormalization group (DMRG) method. By combining parallel DMRG with SU(2)\mathrm{SU}(2)SU(2) spin rotational symmetry, we are able to obtain accurate results on large cylinders with length up to Lx=48{L}_{x}=48Lx​=48 and circumference Ly=6−−12{L}_{y}=6--12Ly​=6−−12. Our results suggest that the QSL phase of the ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ Heisenberg model is gapped, which is characterized by the absence of a gapless mode and by short-range spin-spin and dimer-dimer correlations. In the presence of J3{J}_{3}J3​ interaction, we find that a critical QSL with a single gapless mode emerges. While both spin-spin and scalar chiral-chiral correlations are short ranged, dimer-dimer correlations are quasi long ranged and decay as a power law at long distances.