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arXiv:1907.06176 · Journal of Physics Condensed Matter

Nature of the randomness-induced quantum spin liquids in two dimensions

Hikaru Kawamura, Kazuki Uematsu

Published Aug 30, 2019• 65 citations
arXivHTMLPDF

Abstract

Abstract The nature of the randomness-induced quantum spin liquid state, the random-singlet state, is investigated in two dimensions (2D) by means of the exact-diagonalization and the Hams-de Raedt methods for several frustrated lattices, e.g. the triangular, the kagome and the J 1 - J 2 square lattices. Properties of the ground state, the low-energy excitations and the finite-temperature thermodynamic quantities are investigated. The ground state and the low-lying excited states consist of nearly isolated singlet-dimers, clusters of resonating singlet-dimers, and orphan spins. Low-energy excitations are either singlet-to-triplet excitations, diffusion of orphan spins accompanied by the recombination of nearby singlet-dimers, creation or destruction of resonating singlet-dimers clusters. The latter two excitations give enhanced dynamical ‘liquid-like’ features to the 2D random-singlet state. Comparison is made with the random-singlet state in a 1D chain without frustration, the similarity and the difference between in 1D and in 2D being highlighted. Frustration in a wide sense, not only the geometrical one but also including the one arising from the competition between distinct types of interactions, play an essential role in stabilizing this frustrated random singlet state. Recent experimental situations on both organic and inorganic materials are reviewed and discussed.

DOI
10.1088/1361-648x/ab400c

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Abstract The nature of the randomness-induced quantum spin liquid state, the random-singlet state, is investigated in two dimensions (2D) by means of the exact-diagonalization and the Hams-de Raedt methods for several frustrated lattices, e.g. the triangular, the kagome and the J 1 - J 2 square lattices. Properties of the ground state, the low-energy excitations and the finite-temperature thermodynamic quantities are investigated. The ground state and the low-lying excited states consist of nearly isolated singlet-dimers, clusters of resonating singlet-dimers, and orphan spins. Low-energy excitations are either singlet-to-triplet excitations, diffusion of orphan spins accompanied by the recombination of nearby singlet-dimers, creation or destruction of resonating singlet-dimers clusters. The latter two excitations give enhanced dynamical ‘liquid-like’ features to the 2D random-singlet state. Comparison is made with the random-singlet state in a 1D chain without frustration, the similarity and the difference between in 1D and in 2D being highlighted. Frustration in a wide sense, not only the geometrical one but also including the one arising from the competition between distinct types of interactions, play an essential role in stabilizing this frustrated random singlet state. Recent experimental situations on both organic and inorganic materials are reviewed and 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 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.
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.
We study the effects of bond randomness in the spin-1/21/21/2 ${J}_{1}\ensuremath{-}{J}_{2}$ triangular Heisenberg model using exact diagonalization and density-matrix renormalization group. With increasing bond randomness, we identify a randomness-induced spin-liquid-like phase without any magnetic order, dimer order, spin-glass order, or valence-bond-glass order. The finite-size scaling of gaps suggests the gapless nature of both spin triplet and singlet excitations, which is further supported by the broad continuum of the dynamical spin structure factor. By studying the bipartite entanglement spectrum of the system on cylinder geometry, we identify the features of the low-lying entanglement spectrum in the spin-liquid-like phase, which may distinguish this randomness-induced spin-liquid-like phase and the intrinsic spin-liquid phase in the clean ${J}_{1}\ensuremath{-}{J}_{2}$ triangular Heisenberg model. We further discuss the nature of this spin-liquid-like phase and the indication of our results for understanding spin-liquid-like materials with triangular-lattice structure.
We analyze the effect of quenched disorder on spin-1/2 quantum magnets in which magnetic frustration promotes the formation of local singlets. Our results include a theory for 2D valence-bond solids subject to weak bond randomness, as well as extensions to stronger disorder regimes where we make connections with quantum spin liquids. We find, on various lattices, that the destruction of a valence-bond solid phase by weak quenched disorder leads inevitably to the nucleation of topological defects carrying spin-1/2 moments. This renormalizes the lattice into a strongly random spin network with interesting low-energy excitations. Similarly, when short-ranged valence bonds would be pinned by stronger disorder, we find that this putative glass is unstable to defects that carry spin-1/2 magnetic moments, and whose residual interactions decide the ultimate low-energy fate. Motivated by these results we conjecture Lieb-Schultz-Mattis-like restrictions on ground states for disordered magnets with spin 1/2 per statistical unit cell. These conjectures are supported by an argument for 1D spin chains. We apply insights from this study to the phenomenology of YbMgGaO_{4}, a recently discovered triangular lattice spin-1/2 insulator which was proposed to be a quantum spin liquid. We instead explore a description based on the present theory. Experimental signatures, including unusual specific heat, thermal conductivity, and dynamical structure factor, and their behavior in a magnetic field, are predicted from the theory, and compare favorably with existing measurements on YbMgGaO_{4} and related materials.
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.