Frustrated Quantum Spin Systems Research Articles

A hybrid method integrating Green’s function Monte Carlo and projected entangled pair states

Abstract This paper introduces a hybrid approach combining Green’s function Monte Carlo (GFMC) method with projected entangled pair state (PEPS) ansatz. This hybrid method regards PEPS as a trial state and a guiding wave function in GFMC. By leveraging PEPS’s proficiency in capturing quantum state entanglement and GFMC’s efficient parallel architecture, the hybrid method is well-suited for the accurate and efficient treatment of frustrated quantum spin systems. As a benchmark, we applied this approach to study the frustrated J 1–J 2 Heisenberg model on a square lattice with periodic boundary conditions (PBCs). Compared with other numerical methods, our approach integrating PEPS and GFMC shows competitive accuracy in the performance of ground-state energy. This paper provides systematic and comprehensive discussion of the approach of our previous work [Phys. Rev. B 109 235133 (2024)].

Many-body quantum sign structures as non-glassy Ising models

The non-trivial phase structure of the eigenstates of many-body quantum systems severely limits the applicability of quantum Monte Carlo, variational, and machine learning methods. Here, we study real-valued signful ground-state wave functions of frustrated quantum spin systems and, assuming that the tasks of finding wave function amplitudes and signs can be separated, show that the signs can be easily bootstrapped from the amplitudes. We map the problem of finding the sign structure to an auxiliary classical Ising model defined on a subset of the Hilbert space basis. We show that the Ising model does not exhibit significant frustrations even for highly frustrated parental quantum systems, and is solvable with a fully deterministic O(Klog K)-time combinatorial algorithm (where K is the Ising model size). Given the ground state amplitudes, we reconstruct the signs of the ground states of several frustrated quantum models, thereby revealing the hidden simplicity of many-body sign structures.

Ground-State Phase Diagram of the Kitaev–Heisenberg Model on a Three-dimensional Hyperhoneycomb Lattice

The Kitaev model, which hosts a quantum spin liquid (QSL) in the ground state, was originally defined on a two-dimensional honeycomb lattice, but can be straightforwardly extended to any tricoordinate lattices in any spatial dimensions. In particular, the three-dimensional (3D) extensions are of interest as a realization of 3D QSLs, and some materials like $\beta$-Li$_{2}$IrO$_{3}$, $\gamma$-Li$_2$IrO$_3$, and $\beta$-ZnIrO$_{3}$ were proposed for the candidates. However, the phase diagrams of the models for those candidates have not been fully elucidated, mainly due to the limitation of numerical methods for 3D frustrated quantum spin systems. Here we study the Kitaev-Heisenberg model defined on a 3D hyperhoneycomb lattice, by using the pseudofermion functional renormalization group method. We show that the ground-state phase diagram contains the QSL phases in the vicinities of the pristine ferromagnetic and antiferromagnetic Kitaev models, in addition to four magnetically ordered phases, similar to the two-dimensional honeycomb case. Our results respect the four-sublattice symmetry inherent in the model, which was violated in the previous study. Moreover, we also show how the phase diagram changes with the anisotropy in the interactions. The results provide a reference for the search of the hyperhoneycomb Kitaev materials.

Transformer Variational Wave Functions for Frustrated Quantum Spin Systems.

The transformer architecture has become the state-of-art model for natural language processing tasks and, more recently, also for computer vision tasks, thus defining the vision transformer (ViT) architecture. The key feature is the ability to describe long-range correlations among the elements of the input sequences, through the so-called self-attention mechanism. Here, we propose an adaptation of the ViT architecture with complex parameters to define a new class of variational neural-network states for quantum many-body systems, the ViT wave function. We apply this idea to the one-dimensional J_{1}-J_{2} Heisenberg model, demonstrating that a relatively simple parametrization gets excellent results for both gapped and gapless phases. In this case, excellent accuracies are obtained by a relatively shallow architecture, with a single layer of self-attention, thus largely simplifying the original architecture. Still, the optimization of a deeper structure is possible and can be used for more challenging models, most notably highly frustrated systems in two dimensions. The success of the ViT wave function relies on mixing both local and global operations, thus enabling the study of large systems with high accuracy.

Bridging the Gap between Deep Learning and Frustrated Quantum Spin System for Extreme-Scale Simulations on New Generation of Sunway Supercomputer

Efficient numerical methods are promising tools for delivering unique insights into the fascinating properties of physics, such as the highly frustrated quantum many-body systems. However, the computational complexity of obtaining the wave functions for accurately describing the quantum states increases exponentially with respect to particle number. Here we present a novel convolutional neural network (CNN) for simulating the two-dimensional highly frustrated spin-$1/2$ $J_1-J_2$ Heisenberg model, meanwhile the simulation is performed at an extreme scale system with low cost and high scalability. By ingenious employment of transfer learning and CNN's translational invariance, we successfully investigate the quantum system with the lattice size up to $24\times24$, within 30 million cores of the new generation of sunway supercomputer. The final achievement demonstrates the effectiveness of CNN-based representation of quantum-state and brings the state-of-the-art record up to a brand-new level from both aspects of remarkable accuracy and unprecedented scales.

Electric field driven flat bands: Enhanced magnetoelectric and electrocaloric effects in frustrated quantum magnets

The $J_1$-$J_2$ quantum spin sawtooth chain is a paradigmatic one-dimensional frustrated quantum spin system exhibiting unconventional ground-state and finite-temperature properties. In particular, it exhibits a flat energy band of one-magnon excitations accompanied by an enhanced magnetocaloric effect for two singular ratios of the basal interactions $J_1$ and the zigzag interactions $J_2$. In our paper, we demonstrate that one can drive the spin system into a flat-band scenario by applying an appropriate electric field, thus overcoming the restriction of fine-tuned exchange couplings $J_1$ and $J_2$ and allowing one to tune more materials towards flat-band physics, that is to show a macroscopic magnetization jump when crossing the magnetic saturation field, a residual entropy at zero temperature as well as an enhanced magnetocaloric effect. While the magnetic field acts on the spin system via the ordinary Zeeman term, the coupling of an applied electric field with the spins is given by the sophisticated Katsura-Nagaosa-Balatsky (KNB) mechanism, where the electric field effectively acts as a Dzyaloshinskii-Moriya spin-spin interaction. The resulting novel features are corresponding reciprocal effects: We find a magnetization jump driven by the electric field as well as a jump of the electric polarization driven by the magnetic field, i.e.\ the system exhibits an extraordinarily strong magnetoelectric effect. Moreover, in analogy to the enhanced magnetocaloric effect the system shows an enhanced electrocaloric effect.

Quantum Monte Carlo simulations in the trimer basis: first-order transitions and thermal critical points in frustrated trilayer magnets

The phase diagrams of highly frustrated quantum spin systems can exhibit first-order quantum phase transitions and thermal critical points even in the absence of any long-ranged magnetic order. However, all unbiased numerical techniques for investigating frustrated quantum magnets face significant challenges, and for generic quantum Monte Carlo methods the challenge is the sign problem. Here we report on a general quantum Monte Carlo approach with a loop-update scheme that operates in any basis, and we show that, with an appropriate choice of basis, it allows us to study a frustrated model of coupled spin-1/2 trimers: simulations of the trilayer Heisenberg antiferromagnet in the spin-trimer basis are sign-problem-free when the intertrimer couplings are fully frustrated. This model features a first-order quantum phase transition, from which a line of first-order transitions emerges at finite temperatures and terminates in a thermal critical point. The trimer unit cell hosts an internal degree of freedom that can be controlled to induce an extensive entropy jump at the quantum transition, which alters the shape of the first-order line. We explore the consequences for the thermal properties in the vicinity of the critical point, which include profound changes in the lines of maxima defined by the specific heat. Our findings reveal trimer quantum magnets as fundamental systems capturing in full the complex thermal physics of the strongly frustrated regime.

Stiefel Liquids: Possible Non-Lagrangian Quantum Criticality from Intertwined Orders

We propose a new type of quantum liquids, dubbed Stiefel liquids, based on $2+1$ dimensional nonlinear sigma models on target space $SO(N)/SO(4)$, supplemented with Wess-Zumino-Witten terms. We argue that the Stiefel liquids form a class of critical quantum liquids with extraordinary properties, such as large emergent symmetries, a cascade structure, and nontrivial quantum anomalies. We show that the well known deconfined quantum critical point and $U(1)$ Dirac spin liquid are unified as two special examples of Stiefel liquids, with $N=5$ and $N=6$, respectively. Furthermore, we conjecture that Stiefel liquids with $N>6$ are non-Lagrangian, in the sense that under renormalization group they flow to infrared (conformally invariant) fixed points that cannot be described by any renormalizable continuum Lagrangian. Such non-Lagrangian states are beyond the paradigm of parton gauge mean-field theory familiar in the study of exotic quantum liquids in condensed matter physics. The intrinsic absence of (conventional or parton-like) mean-field construction also means that, within the traditional approaches, it will be difficult to decide whether a non-Lagrangian state can actually emerge from a specific UV system (such as a lattice spin system). For this purpose we hypothesize that a quantum state is emergible from a lattice system if its quantum anomalies match with the constraints from the (generalized) Lieb-Schultz-Mattis theorems. Based on this hypothesis, we find that some of the non-Lagrangian Stiefel liquids can indeed be realized in frustrated quantum spin systems, for example, on triangular or Kagome lattice, through the intertwinement between non-coplanar magnetic orders and valence-bond-solid orders.

Control of superexchange interactions with DC electric fields

We discuss DC electric-field controls of superexchange interactions. We first present generic results about antiferromagnetic and ferromagnetic superexchange interactions valid in a broad class of Mott insulators, where we also estimate typical field strength to observe DC electric-field effects: $\sim 1~\mathrm{MV/cm}$ for inorganic Mott insulators such as transition-metal oxides and $\sim 0.1~\mathrm{MV/cm}$ for organic ones. Next, we apply these results to geometrically frustrated quantum spin systems. Our theory widely applies to (quasi-)two-dimensional and thin-film systems and one-dimensional quantum spin systems on various lattices such as square, honeycomb, triangular, and kagome ones. In this paper, we give our attention to those on the square lattice and on the chain. For the square lattice, we show that DC electric fields can control a ratio of the nearest-neighbor and next-nearest-neighbor exchange interactions. In some realistic cases, DC electric fields make the two next-nearest-neighbor interactions nonequivalent and eventually turns the square-lattice quantum spin system into a deformed triangular-lattice one. For the chain, DC electric fields can induce singlet-dimer and Haldane-dimer orders. We show that the DC electric-field-induced spin gap $\propto |\boldsymbol E|^{2/3}$ in the Heisenberg antiferromagnetic chain will reach $\sim 10~\%$ of the dominant superexchange interaction in the case of a spin-chain compound $\mathrm{KCuMoO_4(OH)}$ when the DC electric field of $\sim 1~\mathrm{MV/cm}$ is applied.

Frustrated quantum spins at finite temperature: Pseudo-Majorana functional renormalization group approach

The pseudofermion functional renormalization group (PFFRG) method has proven to be a powerful numerical approach to treat frustrated quantum spin systems. In its usual implementation, however, the complex fermionic representation of spin operators introduces unphysical Hilbert-space sectors which render an application at finite temperatures inaccurate. In this work we formulate a general functional renormalization group approach based on Majorana fermions to overcome these difficulties. We, particularly, implement spin operators via an $\text{SO}(3)$ symmetric Majorana representation which does not introduce any unphysical states and, hence, remains applicable to quantum spin models at finite temperatures. We apply this scheme, dubbed pseudo-Majorana functional renormalization group (PMFRG) method, to frustrated Heisenberg models on small spin clusters as well as square and triangular lattices. Computing the finite-temperature behavior of spin correlations and thermodynamic quantities such as free energy and heat capacity, we find good agreement with exact diagonalization and the high-temperature series expansion down to moderate temperatures. We observe a significantly enhanced accuracy of the PMFRG compared to the PFFRG at finite temperatures. More generally, we conclude that the development of functional renormalization group approaches with Majorana fermions considerably extends the scope of applicability of such methods.

Finite-temperature properties of the Kitaev-Heisenberg models on kagome and triangular lattices studied by improved finite-temperature Lanczos methods

Frustrated quantum spin systems such as the Heisenberg and Kitaev models on various lattices, have been known to exhibit various exotic properties not only at zero temperature but also for finite temperatures. Inspired by the remarkable development of the quantum frustrated spin systems in recent years, we investigate the finite-temperature properties of the $S=1/2$ Kitaev-Heisenberg models on kagome and triangular lattices by means of finite-temperature Lanczos methods with improved accuracy. In both lattices, multiple peaks are confirmed in the specific heat. To find the origin of the multiple peaks, we calculate the static spin structure factor. The origin of the high-temperature peak of the specific heat is attributed to a crossover from the paramagnetic state to a short-range ordered state whose static spin structure factor has zigzag or linear intensity distributions in momentum space. In the triangular Kitaev model, the "order by disorder" due to quantum fluctuation occurs. On the other hand, in the kagome Kitaev model it does not occur even with both quantum and thermal fluctuations.

Effects of staggered Dzyaloshinskii-Moriya interactions in a quasi-two-dimensional Shastry-Sutherland model

Frustrated quantum spin systems exhibit exotic physics induced by external magnetic field with anisotropic interactions. Here, we study the effect of non-uniform Dzyaloshinskii-Moriya (DM) interactions on a quasi-two-dimensional Shastry-Sutherland lattice using a matrix product states (MPS) algorithm. We first recover the magnetization plateau structure present in this geometry and then we show that both interdimer and intradimer DM interactions significantly modify the plateaux. The non-number-conserving intradimer interaction smoothens the shape of the magnetization curve, while the number-conserving interdimer interaction induces different small plateaux, which are signatures of the finite size of the system. Interestingly, the interdimer DM interaction induces chirality in the system. We thus characterize these chiral phases with particular emphasis to their robustness against intradimer DM interactions.

Topological approach to quantum liquid ground states on geometrically frustrated Heisenberg antiferromagnets

We have formulated a twist operator argument for the geometrically frustrated quantum spin systems on the kagome and triangular lattices, thereby extending the application of the Lieb–Schultz–Mattis and Oshikawa–Yamanaka–Affleck theorems to these systems. The equivalent large gauge transformation for the geometrically frustrated lattice differs from that for non-frustrated systems due to the existence of multiple sublattices in the unit cell and non-orthogonal basis vectors. Our study for the S = 1/2 kagome Heisenberg antiferromagnet at zero external magnetic field gives a criterion for the existence of a two-fold degenerate ground state with a finite excitation gap and fractionalized excitations. At finite field, we predict various plateaux at fractional magnetisation, in analogy with integer and fractional quantum Hall states of the primary sequence. These plateaux correspond to gapped quantum liquid ground states with a fixed number of singlets and spinons in the unit cell. A similar analysis for the triangular lattice predicts a single fractional magnetization plateau at 1/3. Our results are in broad agreement with numerical and experimental studies.

Thermodynamics of a gauge-frustrated Kitaev spin liquid

Two- and three-dimensional Kitaev magnets are prototypical frustrated quantum spin systems, in which the original spin degrees of freedom fractionalize into Majorana fermions and a $\mathbb{Z}_2$ gauge field -- a purely local phenomenon that reveals itself as a thermodynamic crossover at a temperature scale set by the strength of the bond-directional interactions. For conventional Kitaev magnets, the low-temperature thermodynamics reveals a second transition at which the $\mathbb{Z}_2$ gauge field orders and the system enters a spin liquid ground state. Here we discuss an explicit example that goes beyond this paradigmatic scenario -- the $\mathbb{Z}_2$ gauge field is found to be subject to geometric frustration, the thermal ordering transition is suppressed, and an extensive residual entropy arises. Deep in the quantum regime, at temperatures of the order of one per mil of the interaction strength, the degeneracy in the gauge sector is lifted by a subtle interplay between the gauge field and the Majorana fermions, resulting in the formation of a Majorana metal. We discuss the thermodynamic signatures of this physics obtained from large-scale, sign-free quantum Monte Carlo simulations.

Frustrated quantum spin systems in small triangular lattices studied with a numerical method

The study of quantum frustrated systems remains one of the most challenging subjects of quantum magnetism, as they can hold quantum spin liquids, whose characterization is quite elusive. The presence of gapped quantum spin liquids possessing long range entanglement while being locally indistinguishable often demand highly sophisticated numerical approaches for their description. Here we propose an easy computational method based on exact diagonalization with engineered boundary conditions in very small plaquettes. We apply the method to study the quantum phase diagram of diverse antiferromagnetic frustrated Heisenberg models in the triangular lattice. Our results are in qualitative agreement with previous results obtained by means of sophisticated methods like 2D-DMRG or variational quantum Monte Carlo.

Thermodynamic properties of the Shastry-Sutherland model from quantum Monte Carlo simulations

We investigate the minus-sign problem that afflicts quantum Monte Carlo (QMC) simulations of frustrated quantum spin systems, focusing on spin S=1/2, two spatial dimensions, and the extended Shastry-Sutherland model. We show that formulating the Hamiltonian in the diagonal dimer basis leads to a sign problem that becomes negligible at low temperatures for small and intermediate values of the ratio of the inter- and intradimer couplings. This is a consequence of the fact that the product state of dimer singlets is the exact ground state both of the extended Shastry-Sutherland model and of a corresponding "sign-problem-free" model, obtained by changing the signs of all positive off-diagonal matrix elements in the dimer basis. By exploiting this insight, we map the sign problem throughout the extended parameter space from the Shastry-Sutherland to the fully frustrated bilayer model and compare it with the phase diagram computed by tensor-network methods. We use QMC to compute with high accuracy the temperature dependence of the magnetic specific heat and susceptibility of the Shastry-Sutherland model for large systems up to a coupling ratio of 0.526(1) and down to zero temperature. For larger coupling ratios, our QMC results assist us in benchmarking the evolution of the thermodynamic properties by systematic comparison with exact diagonalization calculations and interpolated high-temperature series expansions.

Magnetization plateaus in the spin- 12 antiferromagnetic Heisenberg model on a kagome-strip chain

Spin-1/2 Heisenberg model on kagome lattice is a typical frustrated quantum spin system. A basic structure of kagome lattice is also present in kagome-strip lattice in one dimension, where a similar type of frustration is expected. We thus study the magnetization plateaus of the spin-1/2 Heisenberg model on a kagome-strip chain with three-independent antiferromagnetic exchange interactions by the density-matrix renormalization group method. In a certain range of exchange parameters, we find twelve kinds of magnetization plateaus, nine of which have magnetic structures breaking either translational or reflection symmetry spontaneously. The structures are classified by an array of five-site unit cells with specific bond-spin correlations. In a case with nontrivial plateau, 3/10 plateau, we find long-period magnetic structure with a period of four unit cells.

Observation of new magnetic ground state in frustrated quantum antiferromagnet spin-liquid system Cs2CuCl4

Cs2CuCl4 is known to possess a quantum spin-liquid phase with antiferromagnetic interaction below 2.8 K. We report the observation of a new metastable magnetic phase of the triangular frustrated quantum spin system Cs2CuCl4 induced by the application of hydrostatic pressure. We measured the magnetic properties of Cs2CuCl4 following the application and release of pressure after 3 days. We observed a previously unknown ordered magnetic phase with a transition temperature of 9 K. Furthermore, the recovered sample with new magnetic ground state possesses an equivalent crystal structure to the uncompressed one with antiferromagnetic quantum spinliquid phase.

Exact Ground States of Frustrated Quantum Spin Systems Consisting of Spin-Dimer Units

We study frustrated quantum spin systems consisting of dimers of spin-1/2 spins. We derive several models that have the exact ground state of the form of the direct product of dimer states. The ground states realized include the product state of dimer singlets, that of dimer triplets with zero magnetization, those of dimer-spin-nematic states, and those of a mixture of the dimer states. Pseudo spin-1/2 operators emerging in each dimer are also introduced.

Spin glass behavior in frustrated quantum spin system CuAl2O4 with a possible orbital liquid state

CuAl2O4 is a normal spinel oxide having quantum spin, S = 1/2 for Cu2+. It is a rather unique feature that the Cu2+ ions of CuAl2O4 sit at a tetrahedral position, not like the usual octahedral position for many oxides. At low temperatures, it exhibits all the thermodynamic evidence of a quantum spin glass. For example, the polycrystalline CuAl2O4 shows a cusp centered at ~2 K in the low-field dc magnetization data and a clear frequency dependence in the ac magnetic susceptibility while it displays logarithmic relaxation behavior in a time dependence of the magnetization. At the same time, there is a peak at ~2.3 K in the heat capacity, which shifts towards a higher temperature with magnetic fields. On the other hand, there is no evidence of new superlattice peaks in the high-resolution neutron powder diffraction data when cooled from 40 to 0.4 K. This implies that there is no long-ranged magnetic order down to 0.4 K, thus confirming a spin glass-like ground state for CuAl2O4. Interestingly, there is no sign of structural distortion either although Cu2+ is a Jahn–Teller active ion. Thus, we claim that an orbital liquid state is the most likely ground state in CuAl2O4. Of further interest, it also exhibits a large frustration parameter, f = |θCW/Tm| ~ 67, one of the largest values reported for spinel oxides. Our observations suggest that CuAl2O4 should be a rare example of a frustrated quantum spin glass with a good candidate for an orbital liquid state.