Valence Bond Solid State Research Articles

Triplon analysis of magnetic disorder and order in maple-leaf Heisenberg magnet

The nearest-neighbor spin-1/2 Heisenberg model on the maple-leaf lattice formed by hexagons (couplingJh), triangles (couplingJt), and dimers (couplingJd), is investigated in a parameter regime whereJh>0andJt,Jd<0. This investigation aims to identify regions hosting exotic valence-bond solid states. Two potential magnetically disordered ground states are identified, and their stability is assessed through plaquette-triplon mean-field analyses. The resulting quantum phase diagram reveals that at large|Jt|and|Jd|, the system adopts a magnetically disordered dimerized VBS state, while for small|Jd|, it stabilizes a Néel state. A second-order phase transition from the dimerized phase to a Néel phase is observed, which, being Landau-forbidden, suggests the potential presence of exotic phenomena such as a deconfined quantum critical point or the appearance of a quantum spin liquid. This work provides insights into the phase diagram of the nearest-neighbor spin-1/2 Heisenberg model on the maple-leaf lattice and lays the groundwork for further investigations into its intriguing physics.

Vison condensation and spinon confinement in a kagome-lattice Z2 spin liquid: A numerical study of a quantum dimer model

Quantum spin liquids are exotic many-body states featured with long-range entanglement and fractional anyon quasiparticles. Quantum phase transitions of spin liquids are particularly interesting problems related with novel phenomena of anyon condensation and anyon confinement. Here we study a quantum dimer model, which implements a transition between a Z2 spin liquid (Z2SL) and a valence bond solid (VBS) on the kagome lattice. The transition is driven by the condensation of vison excitation of the Z2 spin liquid, which impacts on other anyon excitations especially leading to the confinement of spinon excitations. By numerical exact diagonalization of the dimer model, we directly measure the vison condensation using vison string operators, and explicitly check a confining potential acting on spinon excitations in the VBS state. It is observed that topological degeneracy of the spin-liquid state is lifted concomitantly with the vison condensation. The dimer ordering pattern of the VBS state is identified by investigating dimer structure factor. Furthermore, we find an interesting state that exhibits features of spin liquid and VBS simultaneously. We discuss the origin of the mixed behaviors and possible scenarios expected in thermodynamic limit. This work complements the previous analytical studies on the dimer model [ and ] by providing numerical evidences on the vison condensation and the spinon confinement in the Z2SL-to-VBS transition. Published by the American Physical Society 2024

Structural and magnetic studies of the frustrated S = 1 kagome magnet NH4Ni2Mo2O10H3

The strong geometric frustration of the kagome antiferromagnets (KAFMs) can destabilise conventional magnetic order and lead to exotic electronic states, such as the quantum spin-liquid state observed in some S=12 KAFM materials. However, the ground state of S = 1 KAFM systems are less well understood. Spin nematic phases and valence bond solid ground states have been predicted to form but a paucity of experimental realisations restricts understanding. Here, the S = 1 KAFM NH4Ni2Mo2O10H3 is presented, which has the 3-fold symmetry of the kagome lattice but significant site depletion, with ∼64% site occupancy. Frustration and a competition between exchange interactions are evidenced through the suppression of order below the Weiss temperature |θW| and observation of ferromagnetic and antiferromagnetic characteristics in the magnetisation data. A semi spin glass ground state is predicted based on the ac-field frequency dependence of the magnetic transition and ferromagnetic signal.

Preparing valence-bond-solid states on noisy intermediate-scale quantum computers

Quantum state preparation is a key step in all digital quantum simulation algorithms. Here we propose methods to initialize on a gate-based quantum computer a general class of quantum spin wave functions, the so-called valence-bond-solid (VBS) states, that are important for two reasons. First, VBS states are the exact ground states of a class of interacting quantum spin models introduced by Affleck, Kennedy, Lieb, and Tasaki (AKLT). Second, the two-dimensional VBS states are universal resource states for measurement-based quantum computing. We find that schemes to prepare VBS states based on their tensor-network representations yield quantum circuits that are too deep to be within reach of noisy intermediate-scale quantum (NISQ) computers. We then apply the general nondeterministic method herein proposed to the preparation of the spin-1 and spin-$3/2$ VBS states, the ground states of the AKLT models defined in one dimension and in the honeycomb lattice, respectively. Shallow quantum circuits of depth independent of the lattice size are explicitly derived for both cases, making use of optimization schemes that outperform standard basis gate decomposition methods. The probabilistic nature of the proposed routine translates into an average number of repetitions to successfully prepare the VBS state that scales exponentially with the number of lattice sites $N$. However, two strategies to quadratically reduce this repetition overhead for any bipartite lattice are devised. Our approach should permit to use NISQ processors to explore the AKLT model and variants thereof, outperforming conventional numerical methods in the near future.

The asymmetric valence-bond-solid states in quantum spin chains: The difference between odd and even spins

The qualitative difference in low-energy properties of spin S quantum antiferromagnetic chains with integer S and half-odd-integer S discovered by Haldane [F. D. M. Haldane, arXiv:1612.00076 (1981); Phys. Lett. A 93, 464–468 (1983); Phys. Rev. Lett. 50, 1153–1156 (1983)] and Tasaki [Tasaki, Graduate Texts in Physics (Springer, 2020)] can be intuitively understood in terms of the valence-bond picture proposed by Affleck et al. [I. Affleck, Phys. Rev. Lett. 59, 799 (1987); Commun. Math. Phys. 115, 477–528 (1988)]. Here, we develop a similarly intuitive diagrammatic explanation of the qualitative difference between chains with odd S and even S, which is at the heart of the theory of symmetry-protected topological (SPT) phases. (There is a 24 min video in which the essence of the present work is discussed: https://youtu.be/URsf9e_PLlc.) More precisely, we define one-parameter families of states, which we call the asymmetric valence-bond solid (VBS) states, that continuously interpolate between the Affleck–Kennedy–Lieb–Tasaki (AKLT) state and the trivial zero state in quantum spin chains with S = 1 and 2. The asymmetric VBS state is obtained by systematically modifying the AKLT state. It always has exponentially decaying truncated correlation functions and is a unique gapped ground state of a short-ranged Hamiltonian. We also observe that the asymmetric VBS state possesses the time-reversal, the Z2×Z2, and the bond-centered inversion symmetries for S = 2 but not for S = 1. This is consistent with the known fact that the AKLT model belongs to the trivial SPT phase if S = 2 and to a nontrivial SPT phase if S = 1. Although such interpolating families of disordered states were already known, our construction is unified and is based on a simple physical picture. It also extends to spin chains with general integer S and provides us with an intuitive explanation of the essential difference between models with odd and even spins.

Functional renormalization group study of the two-dimensional Su-Schrieffer-Heeger-Hubbard model

We study the Hubbard model on the square lattice coupled in addition to the optical Su-Schrieffer-Heeger (SSH) phonons, using the singular-mode functional renormalization group method. At half-filling and in the absence of the Hubbard interaction $U$, we find the degenerate spin-density-wave (SDW)/charge-density-wave (CDW)/s-wave superconductivity (sSC) state at smaller electron-phonon coupling strength $\lambda$ and higher phonon frequency $\omega$, and the valence bond solid (VBS) state at larger $\lambda$ and lower $\omega$. After switching on a positive $U$, the VBS state is suppressed, while the SDW state is enhanced. At finite doping, the SSH phonon is found to favor sSC at $U=0$. With increasing positive $U$, we find d-wave superconductivity (dSC) and incommensurate SDW states. In a narrow window of moderate $U$ and $\lambda$, we also find the incommensurate VBS state. The sSC and dSC here can be naturally related to the CDW and SDW fluctuations, both of which can be triggered by the SSH phonons. In contrast, the repulsive interaction $U$ enhances SDW but suppresses CDW fluctuations. Our results at half filling are consistent with quantum Monte Carlo (QMC), and provide insights at finite doping where QMC may suffer from the minus sign problem.

Phonon renormalization effects accompanying the 6 K anomaly in the quantum spin liquid candidate κ−(BEDT-TTF)2Cu2(CN)3

Inelastic neutron scattering measurements have revealed an abrupt change in the phonon damping at the 6 K anomaly in the quantum spin liquid candidate $\ensuremath{\kappa}$-(BEDT-TTF)${}_{2}$Cu${}_{2}$(CN)${}_{3}$. This is interpreted as a phase transition to the valence bond solid state on the basis of an effective model describing the spin-charge coupling in the dimer-Mott system.

Phase diagram and magnetic excitations of J1–J3 Heisenberg model on the square lattice

We study the phase diagram and the dynamical spin structure factor of the spin-1/2 ${J}_{1}--{J}_{3}$ Heisenberg model on the square lattice using density matrix renormalization group, exact diagonalization (ED), and cluster perturbation theory (CPT). By extrapolating the order parameters and studying the level crossings of the low-lying energy and entanglement spectra, we obtain the phase diagram of this model and identify a narrow region of quantum spin liquid (QSL) phase followed by a plaquette valence-bond solid (PVBS) state in the intermediate region, whose nature has been controversial for many years. More importantly, we use CPT and ED to study the dynamical spin structure factor in the QSL and the PVBS phase. In the QSL phase, the high-energy magnon mode completely turns into some dispersive weak excitations around the $X$ and $M$ points. For the PVBS phase, the low-energy spectrum is characterized by a gapped triplet excitation, and at the high energy, we find another branch of dispersive excitation with broad continua, which is unlike the plaquette phase in the $2\ifmmode\times\else\texttimes\fi{}2$ checkerboard model. In the latter case, the second branch of excitation is nearly flat due to the weak effective interactions between the local excitations of the plaquettes. And in the ${J}_{1}--{J}_{3}$ Heisenberg model, the uniform interactions and the spontaneously translational symmetry breaking of the PVBS phase make the difference in the excitation spectra.

Supersymmetry and multicriticality in a ladder of constrained fermions

Supersymmetric lattice models of constrained fermions are known to feature exotic phenomena such as superfrustration, with an extensive degeneracy of ground states, the nature of which is however generally unknown. Here we address this issue by considering a superfrustrated model, which we deform from the supersymetric point. By numerically studying its two-parameter phase diagram, we reveal a rich phenomenology. The vicinity of the supersymmetric point features period-4 and period-5 density waves which are connected by a floating phase (incommensurate Luttinger liquid) with smoothly varying density. The supersymmetric point emerges as a multicritical point between these three phases. Inside the period-4 phase we report a valence-bond solid type ground state that persists up to the supersymmetric point. Our numerical data for transitions out of density-wave phases are consistent with the Pokrovsky-Talapov universality class. Furthermore, our analysis unveiled a period-3 phase with a boundary determined by a competition between single and two-particle instabilities accompanied by a doubling of the wavevector of the density profiles along a line in the phase diagram.

Deconfined criticality and a gapless Z2 spin liquid in the square-lattice antiferromagnet

The theory for the vanishing of N\'eel order in the spin $S=1/2$ square lattice antiferromagnet has been the focus of attention for many decades. A consensus appears to have emerged in recent numerical studies on the antiferromagnet with first and second neighbor exchange interactions (the $J_1$-$J_2$ model): a gapless spin liquid is present for a narrow window of parameters between the vanishing of the N\'eel order and the onset of a gapped valence bond solid state. We propose a deconfined critical SU(2) gauge theory for a transition into a stable $\mathbb{Z}_2$ spin liquid with massless Dirac spinon excitations; on the other side the critical point, the SU(2) spin liquid (the `$\pi$-flux' phase) is presumed to be unstable to confinement to the N\'eel phase. We identify a dangerously irrelevant coupling in the critical SU(2) gauge theory, which contributes a logarithm-squared renormalization. This critical theory is also not Lorentz invariant, and weakly breaks the SO(5) symmetry which rotates between the N\'eel and valence bond solid order parameters. We also propose a distinct deconfined critical U(1) gauge theory for a transition into the same gapless $\mathbb{Z}_2$ spin liquid; on the other side of the critical point, the U(1) spin liquid (the `staggered flux' phase) is presumed to be unstable to confinement to the valence bond solid. This critical theory has no dangerously irrelevant coupling, dynamic critical exponent $z \neq 1$, and no SO(5) symmetry. All of these phases and critical points are unified in a SU(2) gauge theory with Higgs fields and fermionic spinons which can naturally realize the observed sequence of phases with increasing $J_2/J_1$: N\'eel, gapless $\mathbb{Z}_2$ spin liquid, and valence bond solid.

An optimized cluster density matrix embedding theory

We propose an optimized cluster density matrix embedding theory (CDMET). It reduces the computational cost of CDMET with simpler bath states. And the result is as accurate as the original one. As a demonstration, we study the distant correlations of the Heisenberg J 1–J 2 model on the square lattice. We find that the intermediate phase (0.43 ≲ J 2 ≲ 0.62) is divided into two parts. One part is a near-critical region (0.43 ≲ J 2 ≲ 0.50). The other part is the plaquette valence bond solid (PVB) state (0.51 ≲ J 2 ≲ 0.62). The spin correlations decay exponentially as a function of distance in the PVB.

Gapped magnetic ground state in quantum spin liquid candidate κ-(BEDT-TTF)2Cu2(CN)3.

Geometrical frustration, quantum entanglement, and disorder may prevent long-range ordering of localized spins with strong exchange interactions, resulting in an exotic state of matter. κ-(BEDT-TTF)2Cu2(CN)3 is considered the prime candidate for this elusive quantum spin liquid state, but its ground-state properties remain puzzling. We present a multifrequency electron spin resonance (ESR) study down to millikelvin temperatures, revealing a rapid drop of the spin susceptibility at 6 kelvin. This opening of a spin gap, accompanied by structural modifications, is consistent with the formation of a valence bond solid ground state. We identify an impurity contribution to the ESR response that becomes dominant when the intrinsic spins form singlets. Probing the electrons directly manifests the pivotal role of defects for the low-energy properties of quantum spin systems without magnetic order.

Effects of Mn-substitution on the valence bond solid in Li2RuO3

$Li_{2}RuO_{3}$ with a honeycomb structure undergoes a drastic transition from a regular honeycomb lattice with the $C2/m$ space group to a valence bond solid state of the $P2_{1}/m$ space group with an extremely strong dimerization at 550 K. We synthesized $Li_{2}Ru_{1-x}Mn_{x}O_{3}$ with a full solid solution and investigated doping effects on the valence bond solid state as a function of Mn content. The valence bond solid state is found to be stable up to $x = 0.2$, based on our extensive experiments: structural studies, resistivity, and magnetic susceptibility. On the other hand, the extended x-ray absorption fine structure analyses show that the dimer local structure remains robust even above $x = 0.2$ with a minimal effect on the dimer bond length. This indicates that the locally-disordered dimer structure survives well into the Mn-rich phase even though the thermodynamically stable average structure has the $C2/m$ space group. Our results prove that the dimer formation in $Li_{2}RuO_{3}$ is predominantly a local phenomenon driven by the formation of orbitally-assisted metal-metal bonds and that these dimers are relatively robust against doping-induced disorder.

Valence-bond solids, vestigial order, and emergent SO(5) symmetry in a two-dimensional quantum magnet

We introduce a quantum spin-1/2 model with many-body correlated Heisenberg-type interactions on the 2D square lattice, designed to host a plaquette valence-bond solid (PVBS) ground state breaking $\mathbb{Z}_4$ symmetry. We carry out a detailed quantum Monte Carlo study of the quantum phase transition between the antiferromagnetic (AFM) and PVBS states. We find a first-order transition, in contrast to previously studied continuous 'deconfined' transitions between the AFM and columnar valence-bond solids. We show that the coexistence state at the AFM--PVBS transition is unexpectedly associated with SO(5) symmetry, which may indicate that the transition is connected to a deconfined critical point. We also discuss the first-order transition in the context of a recent proposal of spinons with fracton properties in the PVBS state, concluding that the fracton scenario is unlikely. Further, we discover a novel type of eight-fold degenerate VBS phase that breaks the remaining $\mathbb{Z}_2$ symmetry of the PVBS phase. The PVBS phase can then be regarded as an intermediate 'vestigial' phase, and we develop a general graph-theoretic approach to describe the two-stage discrete symmetry breaking. At finite temperature, we observe fluctuation-induced first-order transitions, which are hallmarks of vestigial phase transitions. We also mention possible connections to the SO(5) theory of high-T$_{\rm c}$ superconductivity.

Magnon Bose–Einstein condensation and superconductivity in a frustrated Kondo lattice

Motivated by recent experiments on magnetically frustrated heavy fermion metals, we theoretically study the phase diagram of the Kondo lattice model with a nonmagnetic valence bond solid ground state on a ladder. A similar physical setting may be naturally occurring in [Formula: see text], [Formula: see text], and [Formula: see text] compounds. In the insulating limit, the application of a magnetic field drives a quantum phase transition to an easy-plane antiferromagnet, which is described by a Bose-Einstein condensation of magnons. Using a combination of field theoretical techniques and density matrix renormalization group calculations we demonstrate that in one dimension this transition is stable in the presence of a metallic Fermi sea, and its universality class in the local magnetic response is unaffected by the itinerant gapless fermions. Moreover, we find that fluctuations about the valence bond solid ground state can mediate an attractive interaction that drives unconventional superconducting correlations. We discuss the extensions of our findings to higher dimensions and argue that depending on the filling of conduction electrons, the magnon Bose-Einstein condensation transition can remain stable in a metal also in dimensions two and three.

Consistent Scaling Exponents at the Deconfined Quantum-Critical Point**Supported by the National Science Foundation (USA) under Grant No. DMR-1710170 and by the Simons Foundation under a Simons Investigator Award.

We report a quantum Monte Carlo study of the phase transition between antiferromagnetic and valence-bond solid ground states in the square-lattice S = 1/2 J–Q model. The critical correlation function of the Q terms gives a scaling dimension corresponding to the value ν = 0.455 ± 0.002 of the correlation-length exponent. This value agrees with previous (less precise) results from conventional methods, e.g., finite-size scaling of the near-critical order parameters. We also study the Q-derivatives of the Binder cumulants of the order parameters for L2 lattices with L up to 448. The slope grows as L1/ν with a value of ν consistent with the scaling dimension of the Q term. There are no indications of runaway flow to a first-order phase transition. The mutually consistent estimates of ν provide compelling support for a continuous deconfined quantum-critical point.

Bose-Einstein condensation of deconfined spinons in two dimensions

The transition between the N\'{e}el antiferromagnet and the valence-bond solid state in two dimensions has become a paradigmatic example of deconfined quantum criticality, a non-Landau transition characterized by fractionalized excitations (spinons). We consider an extension of this scenario whereby the deconfined spinons are subject to a magnetic field. The primary purpose is to identify the exotic scenario of a Bose-Einstein condensate of spinons. We employ quantum Monte Carlo simulations of the \mbox{$J$-$Q$} model with a magnetic field and perform a quantum field theoretic analysis of the magnetic field and temperature dependence of thermodynamic quantities. The combined analysis provides compelling evidence for the Bose-Einstein condensation of spinons and also demonstrates an extended temperature regime in which the system is best described as a gas of spinons interacting with an emergent gauge field.

Variety of order-by-disorder phases in the asymmetric J1−J2 zigzag ladder: From the delta chain to the J1−J2 chain

We study an asymmetric $J_1$-$J_2$ zigzag ladder consisting of two different spin-$\frac{1}{2}$ antiferromagnetic (AFM; $J_2$, $\gamma J_2>0$) Heisenberg legs coupled by zigzag-shaped ferromagnetic (FM; $J_1<0$) inter-leg interaction. On the basis of density-matrix renormalization group based calculations the ground-state phase diagram is obtained as functions of $\gamma$ and $J_2/|J_1|$. It contains four kinds of frustration-induced ordered phases except a trivial FM phase. Two of the ordered phases are valence bond solid (VBS) with spin-singlet dimerization, which is a rather conventional order by disorder. Still, it is interesting to note that the VBS states possess an Affleck-Kennedy-Lieb-Tasaki-type topological hidden order. The remaining two phases are ferrimagnetic orders, each of which is distinguished by commensurate or incommensurate spin-spin correlation. It is striking that the ferrimagnetic orders are not associated with geometrical symmetry breaking; instead, the global spin-rotation symmetry is broken. In other words, the system lowers its energy via the FM inter-leg interaction by polarizing both of the AFM Heisenberg legs. This is a rare type of order by disorder. Besides, the incommensurate ferrimagnetic state appears as a consequence of the competition between a polarization and a critical Tomonaga-Luttinger-liquid behavior in the AFM Heisenberg legs.

Bilayer, Hydrogenated and Fluorinated Graphene: QED versus SU(2) QCD Theory

Motivated by recent experimental and calculational investigations of bilayer, hydrogenated and fluorinated graphene, we apply the formalisms of U(1) QED (quantum electrodynamics) and SU(2) QCD (quantum chromodynamics) theories of strongly correlated state. Unlike non-bipartite triangular lattice, on bipartite honeycomb lattice there always exists a monopole that transforms trivially under all the microscopic symmetries, destabilizing the Dirac spin liquid (DSL), so that one can continuously tune the DSL state to the state with parent SU(2) instead of U(1) gauge group. The SU(2) theory describes a spin-liquid state which is different from usual DSL and is probably unstable with respect to Neel or valence-bond solid (VBS) phases, except for the quantum critical point. This point of view means a possibility of VBS states in graphene systems.

BILAYER, HYDROGENATED AND flUORINATED GRAPHENE: QED VS SU(2) QCD THEORY

Motivated by recent experimental and calculational investigations of bilayer, hydrogenated and fluorinated graphene, we apply the formalisms of U(1) QED (quantum electrodynamics) and SU(2) QCD (quantum chromodynamics) theories of strongly correlated state. Unlike non-bipartite triangular lattice, on bipartite honeycomb lattice there always exists a monopole that transforms trivially under all the microscopic symmetries, destabilizing the Dirac spin liquid (DSL), so that one can continuously tune the DSL state to the state with parent SU(2) instead of U(1) gauge group. The SU(2) theory describes a spin-liquid state which is different from usual DSL and is probably unstable with respect to Neel or valence-bond solid (VBS) phases, except for the quantum critical point. This point of view means a possibility of VBS states in graphene systems.