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arXiv:1701.02255 · Journal of the Physical Society of Japan

Randomness-Induced Quantum Spin Liquid Behavior in the s = 1/2 Random J1–J2 Heisenberg Antiferromagnet on the Honeycomb Lattice

Kazuki Uematsu, Hikaru Kawamura

Published Mar 7, 2017• 49 citations
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Abstract

We investigate the ground-state and finite-temperature properties of the bond-random $s=1/2$ Heisenberg model on a honeycomb lattice with frustrated nearest- and next-nearest-neighbor antiferromagnetic interactions, $J_1$ and $J_2$, 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 ($J_2/J_1$) 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 Ba$_3$CuSb$_2$O$_9$ and 6HB-Ba$_3$NiSb$_2$O$_9$ exhibiting the gapless QSL-like behaviors are discussed.

DOI
10.7566/jpsj.86.044704

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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.
In frustrated magnets, the experimental realization of a quantum disordered ground state (QDGS), especially quantum spin liquid (QSL) ground state, is a central topic in condensed matter physics.Several promising candidates were reported, and a number of QSL-like behavior, such as excitation continuum, Tlinear specific heat, and so on, were observed.However, whether the QSL-like behavior is owing to the synergy between spin frustration and quantum fluctuation or bond randomness effects has not been clarified yet.Several theoretical studies have demonstrated that the synergy effect between the magnetic frustration and the bond randomness suppresses magnetic ordering and induces a QSL-like state.This QSL-like state was proposed to be a random-singlet (RS) state, where not only nearest-neighbor spins but also distant spins form singlet pairs with random coupling energy.Since thermodynamic properties of RS and QSL are predicted to be similar to each other, it is important to elucidate the microscopic nature of randomness-induced QDGSs.However, its experimental verifications are still insufficient due to a lack of model materials.In this work, I synthesized polycrystalline samples of SrLaCuSbO 6 (SLCSO) and SrLaCuNbO 6 (SLCNO) by a solid-state reaction.Magnetic Cu 2+ ions with S = 1/2 Heisenberg spins form a square lattice with nearest-neighbor (J 1 ) and next-nearest-neighbor (J 2 ) exchange interaction.Thus, SLCSO and SLCNO were magnetically described as quasi-two-dimensional S = 1/2 J 1 -J 2 square lattice Heisenberg antiferromagnet (SLHAF).The temperature dependence of the magnetic susceptibilities of both compounds shows a broad maximum characteristic of an S = 1/2 SLHAF.However, both compounds undergo magnetic phase transitions at T N = 13.6 and 15.7 K for SLCSO and SLCNO, respectively, due to weak inter-layer interactions.Neutron powder diffraction measurements reveal contrasting spin structures in both compounds.The spin structures of SLCSO and SLCNO below T N are Néel antiferromagnetic and collinear antiferromagnetic, respectively.This result demonstrates that the nearest-neighbor interaction is dominant in SLCSO, whereas the next-nearest-neighbor interaction is dominant in SLCNO.The magnitude of the ordered moment was evaluated at 3.5 K to be m = 0.39(3) µ B for SLCSO and 0.37(1) µ B for SLCNO, which are significantly reduced from 1µ B expected in the classical spin case.The shrink of the ordered magnetic moment was caused by not only magnetic frustration effects but also bond randomness effects arising from the site disorder of Sr 2+ and La 3+ ions.Next, I synthesized the mixed system SrLaCuSb 1-x Nb x O 6 with 0.1 ≤ x ≤
We study the zero-temperature quantum phase diagram of a spin-1 Heisenberg antiferromagnet on the honeycomb lattice with both nearest-neighbor exchange coupling J1>0{J}_{1}>0J1​>0 and frustrating next-nearest-neighbor coupling ${J}_{2}\ensuremath{\equiv}\ensuremath{\kappa}{J}_{1}>0$, using the coupled cluster method implemented to high orders of approximation, and based on model states with different forms of classical magnetic order. For each we calculate directly in the bulk thermodynamic limit both ground-state low-energy parameters (including the energy per spin, magnetic order parameter, spin stiffness coefficient, and zero-field uniform transverse magnetic susceptibility) and their generalized susceptibilities to various forms of valence-bond crystalline (VBC) order, as well as the energy gap to the lowest-lying spin-triplet excitation. In the range $0<\ensuremath{\kappa}<1$ we find evidence for four distinct phases. Two of these are quasiclassical phases with antiferromagnetic long-range order, one with two-sublattice N\'eel order for $\ensuremath{\kappa}<{\ensuremath{\kappa}}_{{c}_{1}}=0.250(5)$, and another with four-sublattice N\'eel-II order for $\ensuremath{\kappa}>{\ensuremath{\kappa}}_{{c}_{2}}=0.340(5)$. Two different paramagnetic phases are found to exist in the intermediate region. Over the range ${\ensuremath{\kappa}}_{{c}_{1}}<\ensuremath{\kappa}<{\ensuremath{\kappa}}_{c}^{i}=0.305(5)$ we find a gapless phase with no discernible magnetic order, which is a strong candidate for being a quantum spin liquid, while over the range ${\ensuremath{\kappa}}_{c}^{i}<\ensuremath{\kappa}<{\ensuremath{\kappa}}_{{c}_{2}}$ we find a gapped phase, which is most likely a lattice nematic with staggered dimer VBC order that breaks the lattice rotational symmetry.
Large symmetry groups in quantum many-body systems could strongly enhance quantum fluctuations and thereby stabilize exotic quantum phases. Frustrated interactions were long known to have similar effects. Here we intertwine the large SU(N\mathrm{SU}(NSU(N) symmetry and the frustration in a ${J}_{1}\text{\ensuremath{-}}{J}_{2}\phantom{\rule{0.16em}{0ex}}\mathrm{SU}(N$) Heisenberg model on a honeycomb lattice, where J1{J}_{1}J1​ is the nearest-neighbor coupling and J2{J}_{2}J2​ is the next-nearest-neighbor coupling. With a large-NNN analysis, we obtain a rich phase diagram by varying both NNN and the ratio J2/J1{J}_{2}/{J}_{1}J2​/J1​. The ground states include Dirac spin liquid, chiral spin liquid, valence cluster solids, flux ordered state, and stripe states. The physical properties of each phase are discussed.
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.