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arXiv:1909.00583

Effect of quenched disorder on a quantum spin liquid state of triangular-lattice antiferromagnet 1T-TaS$_2$

H. Murayama, Yuki Sato, Tomoya Taniguchi, Ryosuke Kurihara, Xiangzhuo Xing, Wantong Huang, S. Kasahara, Y. Kasahara, Itamar Kimchi, Makoto Yoshida, Yoshihiro Iwasa, Yuta Mizukami, T. Shibauchi, M. Kończykowski, Yuji Matsuda

Published Sep 2, 2019• 8 citations
arXivHTMLPDF

Abstract

A quantum spin liquid (QSL) is an exotic state of matter characterized by quantum entanglement and the absence of any broken symmetry. A long-standing open problem, which is a key for fundamental understanding the mysterious QSL states, is how the quantum fluctuations respond to randomness due to quenched disorder. Transition metal dichalcogenide 1T-TaS$_2$ is a candidate material that hosts a QSL ground state with spin-1/2 on the two-dimensional perfect triangular lattice. Here, we performed systematic studies of low-temperature heat capacity and thermal conductivity on pure, Se-substituted and electron irradiated crystals of 1T-TaS$_2$. In pure 1T-TaS$_2$, the linear temperature term of the heat capacity $γT$ and the finite residual linear term of the thermal conductivity in the zero-temperature limit $κ_{0}/T\equivκ/T(T\rightarrow0)$ are clearly resolved, consistent with the presence of gapless spinons with a Fermi surface. Moreover, while the strong magnetic field slightly enhances $κ_0/T$, it strongly suppresses $γ$. These unusual contrasting responses to magnetic field imply the coexistence of two types of gapless excitations with itinerant and localized characters. Introduction of additional weak random exchange disorder in 1T-Ta(S$_{1-x}$Se$_x$)$_2$ leads to vanishing of $κ_0/T$, indicating that the itinerant gapless excitations are sensitive to the disorder. On the other hand, in both pure and Se-substituted systems, the magnetic contribution of the heat capacity obeys a universal scaling relation, which is consistent with a theory that assumes the presence of localized orphan spins forming random singlets. Electron irradiation in pure 1T-TaS$_2$ largely enhances $γ$ and changes the scaling function dramatically, suggesting a possible new state of spin liquid.

DOI
10.48550/arxiv.1909.00583

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Effect of quenched disorder on a quantum spin liquid state of triangular-lattice antiferromagnet 1T-TaS2_22​
A quantum spin liquid (QSL) is an exotic state of matter characterized by quantum entanglement and the absence of any broken symmetry. A long-standing open problem, which is a key for fundamental understanding the mysterious QSL states, is how the quantum fluctuations respond to randomness due to quenched disorder. Transition metal dichalcogenide 1T-TaS2_22​ is a candidate material that hosts a QSL ground state with spin-1/2 on the two-dimensional perfect triangular lattice. Here, we performed systematic studies of low-temperature heat capacity and thermal conductivity on pure, Se-substituted and electron irradiated crystals of 1T-TaS2_22​. In pure 1T-TaS2_22​, the linear temperature term of the heat capacity γTγTγT and the finite residual linear term of the thermal conductivity in the zero-temperature limit κ0/T≡κ/T(T→0)κ_{0}/T\equivκ/T(T\rightarrow0)κ0​/T≡κ/T(T→0) are clearly resolved, consistent with the presence of gapless spinons with a Fermi surface. Moreover, while the strong magnetic field slightly enhances κ0/Tκ_0/Tκ0​/T, it strongly suppresses γγγ. These unusual contrasting responses to magnetic field imply the coexistence of two types of gapless excitations with itinerant and localized characters. Introduction of additional weak random exchange disorder in 1T-Ta(S1−x_{1-x}1−x​Sex_xx​)2_22​ leads to vanishing of κ0/Tκ_0/Tκ0​/T, indicating that the itinerant gapless excitations are sensitive to the disorder. On the other hand, in both pure and Se-substituted systems, the magnetic contribution of the heat capacity obeys a universal scaling relation, which is consistent with a theory that assumes the presence of localized orphan spins forming random singlets. Electron irradiation in pure 1T-TaS2_22​ largely enhances γγγ and changes the scaling function dramatically, suggesting a possible new state of spin liquid.
This paper reports the effect of randomness on a quantum spin liquid state of 1T-TaS2{}_{2}2​ with a two-dimensional perfect triangular lattice. Systematic measurements of heat capacity and thermal conductivity in pure, Se-substituted, and electron-irradiated crystals reveal the microscopic coexistence of localized orphan spins that form random valence bonds and itinerant spinons that appear to form a Fermi surface.
Coexisting localized and itinerant gapless excitations in a quantum spin liquid candidate 1T-TaS2_22​
To reveal the nature of elementary excitations in a quantum spin liquid (QSL), we measured low temperature thermal conductivity and specific heat of 1T-TaS2_22​, a QSL candidate material with frustrated triangular lattice of spin-1/2. The nonzero temperature linear specific heat coefficient γγγ and the finite residual linear term of the thermal conductivity in the zero temperature limit κ0/T=κ/T(T→0)κ_0/T=κ/T(T\rightarrow 0)κ0​/T=κ/T(T→0) are clearly resolved. This demonstrates the presence of highly mobile gapless excitations, which is consistent with fractionalized spinon excitations that form a Fermi surface. Remarkably, an external magnetic field strongly suppresses γγγ, whereas it enhances κ0/Tκ_0/Tκ0​/T. This unusual contrasting behavior in the field dependence of specific heat and thermal conductivity can be accounted for by the presence of two types of gapless excitations with itinerant and localized characters, as recently predicted theoretically (I. Kimchi et al., arXiv:1803.00013 (2018)). This unique feature of 1T-TaS2_22​ provides new insights into the influence of quenched disorder on the QSL.
Mott insulators with localized magnetic moments will exhibit a quantum spin liquid state when the quantum fluctuations are strong enough to suppress the ordering of the spins. Such an entangled state will give rise to collective excitations, in which spin and charge information are carried separately. Our angle-resolved photoemission spectroscopy measurements on single-layer 1T-TaS_{2} show a flat band around the zone center and a gap opening of about 200 meV in the low temperature, indicating 2D Mott insulating nature in the system. This flat band is dispersionless in momentum space but shows anomalously broad width around the zone center and the spectral weight decays rapidly as momentum increases. The observation is described as a spectral continuum from electron fractionalization, corroborated by a low energy effective model. The intensity of the flat band is reduced by surface doping with magnetic adatoms and the gap is closing, a result from the interaction between spin impurities coupled with spinons and the chargons, which gives rise to a charge redistribution. Doping with nonmagnetic impurities behaves differently as the chemical potential shift dominates. These findings provide insight into the quantum spin liquid states of strongly correlated electrons on 2D triangular lattices.
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.
Frustrated magnetism provides a rich platform for realizing exotic quantum phases in condensed matter systems. Among these, quantum spin liquids (QSLs) are a particularly intriguing class of states that exhibit no magnetic ordering and preserve all symmetries down to zero temperature. Just as conventional magnets can be thought of as spin crystals,QSLs represent their liquid analogs. This thesis explores two broad types of QSLs in two-dimensional magnets, with a focus on their dynamic properties and the nature of transitions from conventional magnetic states into QSL phases. QSLs are topological phases that host fractionalized excitations known as spinons. In these states, mobile spinons are coupled to an emergent gauge field, forming a highly entangled phase of matter. The first part of this thesis focuses on Dirac spin liquids (DSLs), a class of QSLs where spinons exhibit a gapless Dirac dispersion. To study the dynamicsof these spin liquids beyond leading-order mean-field theory, we develop a novel large-N fermionic limit of gapless spinons. In this limit, all gauge excitations are suppressed, and the leading-order corrections instead arise from order parameter fluctuations, which may condense and drive transitions into symmetry-broken phases from the parent DSL. Incorporating random phase approximation (RPA) corrections to the spin susceptibility, we find that sharp, spin-wave–like modes are recovered in the excitation spectrum. This methodology successfully captures characteristic features of the dynamics near phase transitions and in weakly symmetry-broken phases proximate to a DSL. We apply this approach to microscopic models, including the J1-J2 XXZ model on the triangular lattice and the J1-J3 XXZ model on the honeycomb lattice. These models closely represent a wide range of frustrated materials, such as triangular and honeycomb cobaltates and triangular ytterbium compounds. Our theoretical predictions show excellent agreement with experimentally measured inelastic neutron scattering spectra from these materials. Gapless spinons can also sometimes become gapped through chiral symmetry breaking, leading to the formation of a chiral spin liquid (CSL). The CSL is an archetypal bosonic realization of a fractional quantum Hall (FQH) state at half-filling, and has been proposed as a time-reversal–breaking ground state in a variety of frustrated spin models. The second part of this thesis addresses the intriguing possibility of realizing a CSL through the "melting" of a chiral spin crystal—a conventional magnet with non-coplanar ordering. Such a transition offers a physically appealing analogue to the melting of a Wigner crystal into a fermionic FQH liquid. Focusing on the kagome lattice, where chiral interactions are knownto stabilize a CSL ground state, we study the effects of additional long-range Heisenberg interactions and demonstrate a phase transition into a non-coplanar octahedral magnetic order. To describe the universal class of transition between a CSL and a non-coplanar anti-ferromagnetic order, we then develop a novel Chern-Simons–matter field theory framework, constrained by symmetry principles and symmetry fractionalization patterns. This thesis thus provides new insights into the dynamical signatures and phase transitions of quantum spin liquids, offering a bridge between theoretical models and experimental observations in frustrated magnetic systems.
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 ≤