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arXiv:1710.06860 · Physical Review X

Valence Bonds in Random Quantum Magnets: Theory and Application to YbMgGaO 4

Itamar Kimchi, Adam Nahum, T. Senthil

Published Jul 27, 2018• 227 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevx.8.031028

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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.

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We explore the effects of non-magnetic impurities (vacancy disorder) on the quantum paramagnetic phases stabilized by SU($N$) designer Hamiltonians on bipartite lattices. Using the results of our quantum Monte Carlo simulations, we demonstrate that isolated vacancies seed emergent spin $S=1/2$ moments in their vicinity when the low-temperature state has valence bond solid order. Indeed, our quantum Monte Carlo results for the low-temperature susceptibility in such regimes shows clear evidence of the vacancy-induced Curie tails associated with these emergent moments, and our zero-temperature projector Monte Carlo results on the ground-state wavefunction in the valence bond basis provide additional evidence in support of this picture. Further, for such designer Hamiltonians on the Lieb lattice with two additional sites on each bond of a square lattice, we identify a low-temperature spin liquid-like regime with no sign of spin or valence bond order. This liquid-like regime serves as a test bed for validating a recently-developed argument concerning the effects of vacancy disorder in such low temperature regimes. Consistent with this argument, we find that isolated vacancies do not seed emergent local moments in such spin liquids. Instead, in the presence of vacancy disorder, emergent local moments are associated with the presence of monomers in maximum-density dimer packings of the corresponding diluted lattice.

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

H. Murayama, Yuki Sato, Tomoya Taniguchi +12 more

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.

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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.
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.
We study the effect of a small density n_{v} of quenched nonmagnetic impurities, i.e., vacancy disorder, in gapped short-range resonating valence bond (RVB) spin liquid states and valence bond solid (VBS) states of quantum magnets. We argue that a large class of short-range RVB liquids are stable to vacancy disorder at small n_{v} on the kagome lattice, while the corresponding states on triangular, square, and honeycomb lattices are unstable to vacancy disorder at any nonzero n_{v} due to the presence of emergent vacancy-induced local moments. In contrast, VBS states are argued to be generically unstable (independent of lattice geometry) to vacancy disorder at any nonzero n_{v} due to such a local-moment instability. Our arguments rely in part on an analysis of the statistical mechanics of maximally packed dimer covers of the diluted lattice, and are fully supported by our computational results on O(N) symmetric designer Hamiltonians. These arguments also imply that short-range RVB spin liquid states are generically unstable to bond dilution on all these lattices.
The quantum nature of electrons emerges in various exotic ways when they are put together with quantum many-body interactions. In Mott insulating systems with strong electron correlation, frustration and strong quantum fluctuations promote localized electron spins to form nontrivial quantum paramagnetic phases such as quantum spin liquid and valence bond solid preventing the development of conventional magnetic orders. In this thesis, we study such exotic quantum phases in various different frustrated quantum magnets. First, encouraged by the spin liquid phenomenology observed in Ba3XSb2O9 (X=Cu, Ni), we investigate Z2 spin liquids on a three dimensional triangular lattice by employing the Schwinger boson mean-field theory with projective symmetry group analysis. It is found that a nematic spin liquid is energetically favorable on this lattice structure rather than symmetric spin liquids. Next, we study various valence bond solid phases that can appear in kagome lattice antiferromagnets by generalizing the recently proposed phenomenological Z2 gauge theory for the topological Z2 spin liquid state found in the nearest-neighbor kagome lattice Heisenberg model. This work provides a bridge between the topological spin liquid and valence bond solid phases previously proposed for kagome lattice antiferromagnets via vison condensation in the gauge theory. Then, we consider optical conductivity in Mott insulators as an experimental probe to detect quantum paramagnetic phases like valence bond solid. Applying this idea to deformed kagome lattice antiferromagnet Rb2Cu3SnF12 with a 12-site valence bond solid state, we estimate the size of optical conductivity in this quantum magnet. After this, another quantum paramagnet BiCu2PO6 is carefully investigated to clarify its puzzling ground state nature and quasiparticle excitations. Utilizing recent high resolution neutron scattering data, we construct a microscopic spin model and also an effective theory for the low energy spin excitations in the compound. We find significant influences of magnetic anisotropies on the ground state and quasiparticle dynamics. Lastly, we investigate emergent quantum phases in the thin film geometries of the pyrochlore iridates, where a number of exotic quantum ground states are proposed to occur in bulk materials as a result of the interplay between electron correlation and strong spin-orbit coupling. The fate of these bulk phases, as well as the novel quantum states that may arise only in a thin film setting, are studied via a theoretical model that allows layer-dependent magnetic structures.
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 ≤
Vacancy-induced local moments in quantum paramagnetic phases: An SU(NNN) designer Hamiltonian study
We explore the effects of non-magnetic impurities (vacancy disorder) on the quantum paramagnetic phases stabilized by SU(NNN) designer Hamiltonians on bipartite lattices. Using the results of our quantum Monte Carlo simulations, we demonstrate that isolated vacancies seed emergent spin S=1/2S=1/2S=1/2 moments in their vicinity when the low-temperature state has valence bond solid order. Indeed, our quantum Monte Carlo results for the low-temperature susceptibility in such regimes shows clear evidence of the vacancy-induced Curie tails associated with these emergent moments, and our zero-temperature projector Monte Carlo results on the ground-state wavefunction in the valence bond basis provide additional evidence in support of this picture. Further, for such designer Hamiltonians on the Lieb lattice with two additional sites on each bond of a square lattice, we identify a low-temperature spin liquid-like regime with no sign of spin or valence bond order. This liquid-like regime serves as a test bed for validating a recently-developed argument concerning the effects of vacancy disorder in such low temperature regimes. Consistent with this argument, we find that isolated vacancies do not seed emergent local moments in such spin liquids. Instead, in the presence of vacancy disorder, emergent local moments are associated with the presence of monomers in maximum-density dimer packings of the corresponding diluted lattice.
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.