Valence Bond Crystal Research Articles

Emergence of chiral spin liquids via quantum melting of noncoplanar magnetic orders

Quantum spin liquids (QSLs) are long-range entangled states of quantum magnets which lie beyond the Landau paradigm of classifying phases of matter via broken symmetries. A physical route to arriving at QSLs is via frustration-induced quantum melting of ordered states such as valence bond crystals or magnetic orders. Here, we show, using extensive exact diagonalization (ED) and density-matrix renormalization group (DMRG) studies of concrete $SU(2)$ invariant spin models on honeycomb, triangular and square lattices, that chiral spin liquids (CSLs) emerge as descendants of triple-$Q$ spin crystals with tetrahedral magnetic order and a large scalar spin chirality. Such ordered-to-CSL melting transitions may yield lattice realizations of effective Chern-Simons-Higgs field theories. Our work provides a distinct unifying perspective on the emergence of CSLs, and suggests that materials with magnetic skyrmion crystal order might provide a good starting point to search for CSLs.

Translation-Invariant Parent Hamiltonians of Valence Bond Crystals.

We present a general method to construct translation-invariant and SU(2) symmetric antiferromagnetic parent Hamiltonians of valence bond crystals (VBCs). The method is based on a canonical mapping transforming S=1/2 spin operators into a bilinear form of a new set of dimer fermion operators. We construct parent Hamiltonians of the columnar and the staggered VBCs on the square lattice, for which the VBC is an eigenstate in all regimes and the exact ground state in some region of the phase diagram. We study the departure from the exact VBC regime upon tuning the anisotropy by means of the hierarchical mean field theory and exact diagonalization on finite clusters. In both Hamiltonians, the VBC phase extends over the exact regime and transits to a columnar antiferromagnet (CAFM) through a window of intermediate phases, revealing an intriguing competition of correlation lengths at the VBC-CAFM transition. The method can be readily applied to construct other VBC parent Hamiltonians in different lattices and dimensions.

Proximity effects in cold atom artificial graphene

Cold atoms in an optical lattice with brick-wall geometry have been used to mimic graphene, a two-dimensional material with characteristic Dirac excitations. Here we propose to bring such artificial graphene into the proximity of a second atomic layer with a square lattice geometry. For non-interacting fermions, we find that such bilayer system undergoes a phase transition from a graphene-like semi-metal phase, characterized by a band structure with Dirac points, to a gapped band insulator phase. In the presence of attractive interactions between fermions with pseudospin-1/2 degree of freedom, a competition between semi-metal and superfluid behavior is found at the mean-field level. Using the quantum Monte Carlo method, we also investigate the case of strong repulsive interactions. In the Mott phase, each layer exhibits a different amount of long-range magnetic order. Upon coupling both layers, a valence-bond crystal is formed at a critical coupling strength. Finally, we discuss how these bilayer systems could be realized in existing cold atom experiments.

Nonperturbative linked-cluster expansions in long-range ordered quantum systems

We introduce a generic scheme to perform non-perturbative linked cluster expansions in long-range ordered quantum phases. Clusters are considered to be surrounded by an ordered reference state leading to effective edge-fields in the exact diagonalization on clusters which break the associated symmetry of the ordered phase. Two approaches, based either on a self-consistent solution of the order parameter or on minimal sensitivity with respect to the ground-state energy per site, are formulated to find the optimal edge-field in each NLCE order. Furthermore, we investigate the scaling behavior of the NLCE data sequences towards the infinite-order limit. We apply our scheme to gapped and gapless ordered phases of XXZ Heisenberg models on various lattices and for spins 1/2 and 1 using several types of cluster expansions ranging from a full-graph decomposition, rectangular clusters, up to more symmetric square clusters. It is found that the inclusion of edge-fields allows to regularize non-perturbative linked-cluster expansions in ordered phases yielding convergent data sequences. This includes the long-range spin-ordered ground state of the spin-1/2 and spin-1 Heisenberg model on the square and triangular lattice as well as the trimerized valence bond crystal of the spin-1 Heisenberg model on the kagome lattice.

Field-Induced Quantum Phase Transitions inS= 1/2J1–J2Heisenberg Model on Square Lattice

We study the magnetic field dependence of the ground state of $S=1/2$ $J_1$-$J_2$ Heisenberg model on the square lattice by the DMRG method with the sine-square deformation. We obtain 8 different phases including plaquette valence-bond crystal with a finite spin gap, transverse N$\acute{\rm e}$el, transverse stripe, 1/2 magnetization plateau with up-up-up-down (uuud), and three new phases we named Y-like, V-like, and $\Psi$ phases around $J_2/J_1$ =0.55-0.6 depending on the magnetic field. The phase transitions to uuud and Y-like states from transverse N$\acute{\rm e}$el (at $J_2/J_1$ = 0.55) and stripe (at $J_2/J_1$ = 0.6) states are discontinuous, as in the case of spin-flop.

Quantum phase diagram of distorted J1 − J2 Heisenberg S = 1/2 antiferromagnet in honeycomb lattice: a modified spin wave study

Using the modified spin wave method, we study the Heisenberg model with first and second neighbor antiferromagnetic exchange interactions. For a symmetric S = 1/2 model, with the same couplings for all the equivalent neighbors, we find three phases in terms of the frustration parameter : (1) a commensurate collinear ordering with staggered magnetization (Néel.I state) for , (2) a magnetically gapped disordered state for , preserving all the symmetries of the Hamiltonian and lattice, which by definition is a quantum spin liquid (QSL) state and (3) a commensurate collinear ordering in which two out of the three nearest neighbor magnetizations are antiparallel and the remaining pair are parallel (Néel.II state), for . We also explore the phase diagram of a distorted model with S = 1/2. Distortion is introduced as an inequality of one nearest neighbor coupling with the other two. This yields a richer phase diagram by the appearance of a new gapped QSL, a gapless QSL and also a valence bond crystal phase in addition to the previous three phases found for the undistorted model.

Emergent quasi-one-dimensionality in a kagome magnet: A simple route to complexity

We study the ground state phase diagram of the quantum spin-$1/2$ Heisenberg model on the kagom\'{e} lattice with first- ($J_1 < 0$), second- ($J_2 < 0$), and third-neighbor interactions ($J_d > 0$) by means of analytical low-energy field theory and numerical density-matrix renormalization group (DMRG) studies. The results offer a consistent picture of the $J_d$-dominant regime in terms of three sets of spin chains weakly coupled by the ferromagnetic inter-chain interactions $J_{1,2}$. When either $J_1$ or $J_2$ is dominant, the model is found to support one of two cuboctohedral phases, cuboc1 and cuboc2. These cuboc states host non-coplanar long-ranged magnetic order and possess finite scalar spin chirality. However, in the compensated regime $J_1 \simeq J_2$, a valence bond crystal phase emerges between the two cuboc phases. We find excellent agreement between an analytical theory based on coupled spin chains and unbiased DMRG calculations, including at a very detailed level of comparison of the structure of the valence bond crystal state. To our knowledge, this is the first such comprehensive understanding of a highly frustrated two-dimensional (2d) quantum antiferromagnet. We find no evidence of either the one-dimensional (1d) gapless spin liquid or the chiral spin liquids, which were previously suggested by parton mean field theories.

Robust singlet dimers with fragile ordering in two-dimensional honeycomb lattice of Li2RuO3.

When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.

Frustrated Heisenberg antiferromagnet on the honeycomb lattice with spin quantum number s ≥ 1

The ground-state (GS) phase diagram of the frustrated spin-s J1-J2-J3 Heisenberg antiferromagnet on the honeycomb lattice is studied using the coupled cluster method implemented to high orders of approximation, for spin quantum numbers s = 1, 3/2, 2 , 5/2. The model has antiferromagnetic (AFM) nearest-neighbour, next-nearest-neighbour and next-next-nearest-neighbour exchange couplings (with strength J1 > 0, J2 > 0 and J3 > 0, respectively). We specifically study the case J3 = J2 = κJ1, in the range 0 < κ < 1 of the frustration parameter, which includes the point of maximum classical (s → ∞) frustration, viz., the classical critical point at κcl = 1/2, which separates the Neel phase for κ < κcl and the collinear striped AFM phase for κ > κcl. Results are presented for the GS energy, magnetic order parameter and plaquette valence-bond crystal (PVBC) susceptibility. For all spins s > 3/2 we find a quantum phase diagram very similar to the classical one, with a direct first-order transition between the two collinear AFM states at a value κc(s) which is slightly greater than κcl [e.g., κc(3/2) ≈ 0.53(1)] and which approaches it monotonically as s → ∞. By contrast, for the case s = 1 the transition is split into two such that the stable GS phases are one with Néel AFM order for κ < κc1 = 0.485(5) and one with striped AFM order for κ > κc2 = 0.528(5), just as in the case s = 1/2 (for which κc1 ≈ 0.47 and κc2 ≈ 0.60). For both the s = 1/2 and s = 1 models the transition at κc2 appears to be of first-order type, while that at κc1 appears to be continuous. However, whereas in the s = 1/2 case the intermediate phase appears to have PVBC order over the entire range κc1 < κ < κc2, in the s = 1 case PVBC ordering either exists only over a very small part of the region or, more likely, is absent everywhere.

Resonating-Valence-Bond Physics Is Not Always Governed by the Shortest Tunneling Loops.

It is well known that the low-energy sector of quantum spin liquids and other magnetically disordered systems is governed by short-ranged resonating-valence bonds. Here we show that the standard minimal truncation to the nearest-neighbor valence-bond basis fails completely even for systems where it should work the most, according to received wisdom. This paradigm shift is demonstrated for the quantum spin-1/2 square kagome, where strong geometric frustration, similar to the kagome, prevents magnetic ordering down to zero temperature. The shortest tunneling events bear the strongest longer-range singlet fluctuations, leading to amplitudes that donot drop exponentially with the length of the loop L, and to an unexpected loop-six valence-bond crystal, which is otherwise very high in energy at the minimal truncation level. The low-energy effective description gives in addition a clear example of correlated loop processes that depend not only on the type of the loop but also on its lattice embedding, a direct manifestation of the long-range nature of the virtual singlets.

Hexagon-singlet solid ansatz for the spin-1 kagome antiferromagnet

We perform a systematic investigation on the hexagon-singlet solid (HSS) states, which are a class of spin liquid candidates for the spin-1 kagome antiferromagnet. With the Schwinger boson representation, we show that all HSS states have exponentially decaying correlations and can be interpreted as a (special) subset of the resonating Affleck-Kennedy-Lieb-Tasaki (AKLT) loop states. We provide a compact tensor network representation of the HSS states, with which we are able to calculate physical observables efficiently. We find that the HSS states have vanishing topological entanglement entropy, suggesting the absence of intrinsic topological order. We also employ the HSS states to perform a variational study of the spin-1 kagome Heisenberg antiferromagnetic model. When we use a restricted HSS ansatz preserving lattice symmetry, the best variational energy per site is found to be ${e}_{0}=\ensuremath{-}1.3600$. In contrast, when allowing lattice symmetry breaking, we find a trimerized simplex valence-bond crystal with a lower energy, ${e}_{0}=\ensuremath{-}1.3871$.

Simplex valence-bond crystal in the spin-1 kagome Heisenberg antiferromagnet

We investigate the ground state properties of a spin-1 kagome antiferromagnetic Heisenberg model using tensor-network (TN) methods. We obtain the energy per site {$e_0=-1.41090(2)$ with $D^*=8$ multiplets retained (i.e., a bond dimension of $D=24$), and $e_0=-1.4116(4)$ from large-$D$ extrapolation,} by accurate TN calculations directly in the thermodynamic limit. The symmetry between the two kinds of triangles is spontaneously broken, with a relative energy difference of $\delta \approx$ 19\%, i.e, there is a trimerization (simplex) valence-bond order in the ground state. The spin-spin, dimer-dimer, and chirality-chirality correlation functions are found to decay exponentially with a rather short correlation length, showing that the ground state is gapped. We thus identify the ground state be a simplex valence-bond crystal (SVBC). We also discuss the spin-1 bilinear-biquadratic Heisenberg model on a kagome lattice, and determine its ground state phase diagram. Moreover, we implement non-abelian symmetries, here spin SU(2), in the TN algorithm, which improves the efficiency greatly and provides insight into the tensor structures.

Global phase diagram of competing ordered and quantum spin-liquid phases on the kagome lattice

We study the quantum phase diagram of the spin-$1/2$ Heisenberg model on the kagom\'e lattice with first-, second-, and third-neighbor interactions $J_1$, $J_2$, and $J_3$ by means of density matrix renormalization group. For small $J_2$ and $J_3$, this model sustains a time-reversal invariant quantum spin liquid phase. With increasing $J_2$ and $J_3$, we find in addition a $q=(0,0)$ N\'{e}el phase, a chiral spin liquid phase, a valence-bond crystal phase, and a complex non-coplanar magnetically ordered state with spins forming the vertices of a cuboctahedron known as a cuboc1 phase. Both the chiral spin liquid and cuboc1 phase break time reversal symmetry in the sense of spontaneous scalar spin chirality. We show that the chiralities in the chiral spin liquid and cuboc1 are distinct, and that these two states are separated by a strong first order phase transition. The transitions from the chiral spin liquid to both the $q=(0,0)$ phase and to time-reversal symmetric spin liquid, however, are consistent with continuous quantum phase transitions.

Quantum Spin Liquid in Spin 1/2J1–J2Heisenberg Model on Square Lattice: Many-Variable Variational Monte Carlo Study Combined with Quantum-Number Projections

The nature of quantum spin liquids is studied for the spin-$1/2$ antiferromagnetic Heisenberg model on a square lattice containing exchange interactions between nearest-neighbor sites, $J_1$, and those between next-nearest-neighbor sites, $J_2$. We perform variational Monte Carlo simulations together with the quantum-number-projection technique and clarify the phase diagram in the ground state together with its excitation spectra. We obtain the nonmagnetic phase in the region $0.4< J_2/J_1\le 0.6$ sandwiched by the staggered and stripe antiferromagnetic (AF) phases. Our direct calculations of the spin gap support the notion that the triplet excitation from the singlet ground state is gapless in the range of $0.4 < J_2/J_1 \le 0.5$, while the gapped valence-bond-crystal (VBC) phase is stabilized for $0.5 < J_2/J_1 \le 0.6$. The VBC order is likely to have the columnar symmetry with a spontaneous symmetry breaking of the $C_{4v}$ symmetry. The power-law behaviors of the spin-spin and dimer-dimer correlation functions in the gapless region are consistent with the emergence of the algebraic quantum-spin-liquid phase (critical phase). The exponent of the spin correlation $\langle S(0)S(r)\rangle \propto 1/r^{z+\eta}$ at a long distance $r$ appears to increase from $z+\eta\sim 1$ at $J_2/J_1\sim0.4$ toward the continuous transition to the VBC phase at $J_1/J_1\sim0.5$. Our results, however, do not fully exclude the possibility of a direct quantum transition between the staggered AF and VBC phases with a wide critical region and deconfined criticality.

Plaquette order in a dimerized frustrated spin ladder

We study the effect of spin-Peierls instability on the phase-diagram of a frustrated antiferromagnetic spin-1/2 ladder, with weak transverse and diagonal rung coupling. Our analysis focuses on a one-dimensional version of the model (i.e. a single two-leg ladder) where we consider two forms of spin-Peierls (SP) instabilities on the legs: columnar dimers (CD) and staggered dimers (SD). We particularly examine the regime of parameters (corresponding to an intermediate XXZ anisotropy) where the SP and rung coupling terms are equally relevant. In both the CD and SD cases we find that the effective field theory describing the system is a self-dual sine-Gordon model, which favors ordering and the opening of a gap to excitations. The order parameter, which reflects the interplay between the SP and rung interactions, represents a crystal of 4-spin plaquettes on which longitudinal and transverse dimers are in a superposition. Depending on the SP instability mode these plaquettes are closed or open, however both types spontaneously break reflection symmetry across the ladder. The closed plaquettes are stable, while the open plaquette-order is relatively fragile and the corresponding gap may be tuned to zero under extreme conditions. We further find that a first order transition occurs from the Plaquette order to a valence bond crystal (VBC) of dimers on the legs. It is suggestive that in a higher dimensional version of this system, this variety of distinct VBC states with comparable energies leads to the formation of domains. Effectively one-dimensional gapless spinon modes on domain boundaries can possibly account for the experimental observation of a spin-liquid behavior in a physical realization of the model.

Mott physics in the half-filled Hubbard model on a family of vortex-full square lattices

We study the half-filled Hubbard model on a one-parameter family of vortex-full square lattices ranging from the isotropic case to weakly coupled Hubbard dimers. The ground-state phase diagram consists of four phases: A semi-metal and a band insulator which are connected to the weak-coupling limit, and a magnetically ordered N\'eel phase and a valence bond crystal (VBC) which are linked to the strong-coupling Mott limit. The phase diagram is obained by quantum Monte Carlo (QMC) and continuous unitary transformations (CUTs). The CUT is performed in a two-step process: Non-perturbative graph-based CUTs are used in the Mott insulating phase to integrate out charge fluctuations. The resulting effective spin model is tackled by perturbative CUTs about the isolated dimer limit yielding the breakdown of the VBC by triplon condensation. We find three scenarios when varying the interaction for a fixed anisotropy of hopping amplitudes: i) one direct phase transition from N\'eel to semi-metal, ii) two phase transitions VBC to N\'eel and N\'eel to semi-metal, or iii) a smooth crossover from VBC to the band insultor. Our results are consistent with the absence of spin-liquid phases in the whole phase diagram.

Valence bond phases in S = 1/2 Kane–Mele–Heisenberg model

The phase diagram of the Kane–Mele–Heisenberg model in a classical limit [] contains disordered regions in the coupling space, as the result of competition between different terms in the Hamiltonian, leading to frustration in finding a unique ground state. In this work we explore the nature of these phases in the quantum limit, for a S = 1/2. Employing exact diagonalization in Sz and nearest neighbour valence bond bases, and bond and plaquette valence bond mean field theories, we show that the disordered regions are divided into ordered quantum states in the form of plaquette valence bond crystals and staggered dimerized phases.

Quantum dimer model for the spin-12kagomeZ2spin liquid

We revisit the description of the low-energy singlet sector of the spin-1/2 Heisenberg antiferromagnet on kagome in terms of an effective quantum dimer model. With the help of exact diagonalizations of appropriate finite-size clusters, we show that the embedding of a given process in its kagome environment leads to dramatic modifications of the amplitudes of the elementary loop processes, an effect not accessible to the standard approach based on the truncation of the Hamiltonian to the nearest-neighbour valence-bond basis. The resulting parameters are consistent with a Z$_2$ spin liquid rather than with a valence-bond crystal, in agreement with the last density matrix renormalization group results.

Kagome lattice Hubbard model at half filling

We investigate the Kagome lattice Hubbard model at half-filling by variational Monte-Carlo with testing the U(1)-Dirac spin liquid, uniform and valence bond crystal states. Even for the large-$U$ case the U(1) Dirac state, being the optimal state in the Heisenberg model, cannot be recovered. While the finite $U$ Hubbard model allows the introduction of vacancies in a different manner compared to the $t-J$ model, the physics appears to have many similarities. In particular a valence bond crystal is formed in the intermediate-$U$ regime. We observe an impact of the formation of this valence bond crystal on a possible Mott-transition in this model and discuss the properties of the wave-function.

Valence bond liquid phase in the honeycomb lattice materialLi2RuO3

The honeycomb lattice material Li2RuO3 undergoes a dimerization of Ru4+ cations on cooling below 270C, where the magnetic susceptibility vanishes. We use density functional theory calculations to show that this reflects the formation of a 'valence bond crystal', with a strong bond disproportionation. On warming, x-ray diffraction shows that discrete three-fold symmetry is regained on average, and the dimerization apparently disappears. In contrast, local structural measurements using high-energy x-rays, show that disordered dimers survive at the nanoscale up to at least 650C. The high temperature phase of Li2RuO3 is thus an example of a valence bond liquid, where thermal fluctuations drive resonance between different dimer coverages, a classic analogue of the resonating valence bond state often discussed in connection with high T$_c$ cuprates.