Dichotomous dynamics of magnetic monopole fluids.

A recent advance in the study of emergent magnetic monopoles was the discovery that monopole motion is restricted to dynamical fractal trajectories [J. N. Hallén et al., Science 378, 1218 (2022)], thus explaining the characteristics of magnetic monopole noise spectra [R. Dusad et al., Nature 571, 234 (2019); A. M. Samarakoon et al., Proc. Natl. Acad. Sci. U.S.A. 119, e2117453119 (2022)]. Here, we apply this novel theory to explore the dynamics of field-driven monopole currents, finding them composed of two quite distinct transport processes: initially swift fractal rearrangements of local monopole configurations followed by conventional monopole diffusion. This theory also predicts a characteristic frequency dependence of the dissipative loss angle for AC field-driven currents. To explore these novel perspectives on monopole transport, we introduce simultaneous monopole current control and measurement techniques using SQUID-based monopole current sensors. For the canonical material Dy2Ti2O7, we measure [Formula: see text], the time dependence of magnetic flux threading the sample when a net monopole current [Formula: see text] is generated by applying an external magnetic field [Formula: see text] These experiments find a sharp dichotomy of monopole currents, separated by their distinct relaxation time constants before and after t ~[Formula: see text] from monopole current initiation. Application of sinusoidal magnetic fields [Formula: see text] generates oscillating monopole currents whose loss angle [Formula: see text] exhibits a characteristic transition at frequency [Formula: see text] over the same temperature range. Finally, the magnetic noise power is also dichotomic, diminishing sharply after t ~[Formula: see text]. This complex phenomenology represents an unprecedented form of dynamical heterogeneity generated by the interplay of fractionalization and local spin configurational symmetry.

Competing gauge fields and entropically driven spin liquid to spin liquid transition in non-Kramers pyrochlores.

Gauge theories are powerful theoretical physics tools that allow complex phenomena to be reduced to simple principles and are used in both high-energy and condensed matter physics. In the latter context, gauge theories are becoming increasingly popular for capturing the intricate spin correlations in spin liquids, exotic states of matter in which the dynamics of quantum spins never ceases, even at absolute zero temperature. We consider a spin system on a three-dimensional pyrochlore lattice where emergent gauge fields not only describe the spin liquid behavior at zero temperature but crucially determine the system's temperature evolution, with distinct gauge fields giving rise to different spin liquid phases in separate temperature regimes. Focusing first on classical spins, in an intermediate temperature regime, the system shows an unusual coexistence of emergent vector and tensor gauge fields where the former is known from classical spin ice systems while the latter has been associated with fractonic quasiparticles, a peculiar type of excitation with restricted mobility. Upon cooling, the system transitions into a low-temperature phase where an entropic selection mechanism depopulates the degrees of freedom associated with the tensor gauge field, rendering the system spin-ice-like. We further provide numerical evidence that in the corresponding quantum model, a spin liquid with coexisting vector and tensor gauge fields has a finite window of stability in the parameter space of spin interactions down to zero temperature. Finally, we discuss the relevance of our findings for non-Kramers magnetic pyrochlore materials.

Deconstructing magnetization noise: Degeneracies, phases, and mobile fractionalized excitations in tetris artificial spin ice.

Direct detection of spontaneous spin fluctuations, or "magnetization noise," is emerging as a powerful means of revealing and studying magnetic excitations in both natural and artificial frustrated magnets. Depending on the lattice and nature of the frustration, these excitations can often be described as fractionalized quasiparticles possessing an effective magnetic charge. Here, by combining ultrasensitive optical detection of thermodynamic magnetization noise with Monte Carlo simulations, we reveal emergent regimes of magnetic excitations in artificial "tetris ice." A marked increase of the intrinsic noise at certain applied magnetic fields heralds the spontaneous proliferation of fractionalized excitations, which can diffuse independently, without cost in energy, along specific quasi-1D spin chains in the tetris ice lattice.

Geometrical frustration versus Kitaev interactions in BaCo2(AsO4)2.

Recently, Co-based honeycomb magnets have been proposed as promising candidate materials to host the Kitaev spin liquid (KSL) state. One of the front-runners is BaCo2(AsO4)2 (BCAO), where it was suggested that the exchange processes between Co2+ ions via the surrounding edge-sharing oxygen octahedra could give rise to bond-dependent Kitaev interactions. In this work, we present and analyze a comprehensive inelastic neutron scattering (INS) study of BCAO with fields in the honeycomb plane. Combining the constraints from the magnon excitations in the high-field polarized state and the inelastic spin structure factor measured in zero magnetic field, we examine two leading theoretical models: the Kitaev-type [Formula: see text] model and the XXZ[Formula: see text]model. We show that the existing experimental data can be consistently accounted for by the XXZ[Formula: see text]model but not by the [Formula: see text] model, and we discuss the implications of these results for the realization of a spin liquid phase in BCAO and more generally for the realization of the Kitaev model in cobaltates.

Signatures of a magnetic superstructure phase induced by ultrahigh magnetic fields in a breathing pyrochlore antiferromagnet.

The mutual coupling of spin and lattice degrees of freedom is ubiquitous in magnetic materials and potentially creates exotic magnetic states in response to the external magnetic field. Particularly, geometrically frustrated magnets serve as a fertile playground for realizing magnetic superstructure phases. Here, we observe an unconventional two-step magnetostructural transition prior to a half-magnetization plateau in a breathing pyrochlore chromium spinel by means of state-of-the-art magnetization and magnetostriction measurements in ultrahigh magnetic fields available up to 600 T. Considering a microscopic magnetoelastic theory, the intermediate-field phase can be assigned to a magnetic superstructure with a three-dimensional periodic array of 3-up-1-down and canted 2-up-2-down spin molecules. We attribute the emergence of the magnetic superstructure to a unique combination of the strong spin-lattice coupling and large breathing anisotropy.

Theory of Moiré Magnetism in Twisted Bilayer α-RuCl3.

Motivated by the recent developments in moiré superlattices of van der Waals magnets and the desire to control the magnetic interactions of α-RuCl3, here we present a comprehensive theory of the long-range ordered magnetic phases of twisted bilayer α-RuCl3. Using a combination of first-principles calculations and atomistic simulations, we show that the stacking-dependent interlayer exchange gives rise to an array of magnetic phases that can be realized by controlling the twist angle. In particular, we discover a complex hexagonal domain structure in which multiple zigzag orders coexist. This multidomain order minimizes the interlayer energy while enduring the energy cost due to domain wall formation. Further, we show that quantum fluctuations can be enhanced across the phase transitions. Our results indicate that magnetic frustration due to stacking-dependent interlayer exchange in moiré superlattices can be exploited to tune quantum fluctuations and the magnetic ground state of α-RuCl3.

From caged compounds with isolated U atoms to frustrated magnets with 2- or 3-atom clusters: a review of Al-rich uranium aluminides with transition metals.

Crystal structures and physical properties of four families of Al-rich ternary uranium compounds with transition metals (TE) are reviewed, namely UTE2Al20, UTE2Al10, U6TE4Al43, and U3TE4Al12. The compounds can be described as consisting of 1 (isolated), 2 (dumbbells) or 3 (triangles) uranium atom clusters, surrounded (1-2-20, 1-2-10 and 6-4-43) or not (3-4-12) by large cages, which strongly influence their magnetic and related properties. Indeed, the ground states of the described systems evolve from Curie-like paramagnetism in the case of the phases with well-isolated, single U-atoms, to complex magnetic order or possible frustrated magnetism in the case of the systems with uranium triangles forming a breathing kagome lattice. We argue that the four families of uranium aluminides described in this review provide a unique opportunity to study magnetic interactions between U magnetic moments while gradually increasing the number of their nearest magnetic neighbors, and may also be helpful in understanding the fundamental origin of magnetic freezing phenomena.

Pseudo-fermion functional renormalization group for spin models.

For decades, frustrated quantum magnets have been a seed for scientific progress and innovation in condensed matter. As much as the numerical tools for low-dimensional quantum magnetism have thrived and improved in recent years due to breakthroughs inspired by quantum information and quantum computation, higher-dimensional quantum magnetism can be considered as the final frontier, where strong quantum entanglement, multiple ordering channels, and manifold ways of paramagnetism culminate. At the same time, efforts in crystal synthesis have induced a significant increase in the number of tangible frustrated magnets which are generically three-dimensional in nature, creating an urgent need for quantitative theoretical modeling. We review the pseudo-fermion (PF) and pseudo-Majorana (PM) functional renormalization group (FRG) and their specific ability to address higher-dimensional frustrated quantum magnetism. First developed more than a decade ago, the PFFRG interprets a Heisenberg model Hamiltonian in terms of Abrikosov pseudofermions, which is then treated in a diagrammatic resummation scheme formulated as a renormalization group flow ofm-particle pseudofermion vertices. The article reviews the state of the art of PFFRG and PMFRG and discusses their application to exemplary domains of frustrated magnetism, but most importantly, it makes the algorithmic and implementation details of these methods accessible to everyone. By thus lowering the entry barrier to their application, we hope that this review will contribute towards establishing PFFRG and PMFRG as the numerical methods for addressing frustrated quantum magnetism in higher spatial dimensions.

Mn2Ga2S5 and Mn2Al2Se5 van der Waals Chalcogenides: A Source of Atomically Thin Nanomaterials.

Layered chalcogenides containing 3d transition metals are promising for the development of two-dimensional nanomaterials with interesting magnetic properties. Both mechanical and solution-based exfoliation of atomically thin layers is possible due to the low-energy van der Waals bonds. In this paper, we present the synthesis and crystal structures of the Mn2Ga2S5 and Mn2Al2Se5 layered chalcogenides. For Mn2Ga2S5, we report magnetic properties, as well as the exfoliation of nanofilms and nanoscrolls. The synthesis of both polycrystalline phases and single crystals is described, and their chemical stability in air is studied. Crystal structures are probed via powder X-ray diffraction and high-resolution transmission electron microscopy. The new compound Mn2Al2Se5 is isomorphous with Mn2Ga2S5 crystallizing in the Mg2Al2Se5 structure type. The crystal structure is built by the ABCBCA sequence of hexagonal close-packing layers of chalcogen atoms, where Mn2+ and Al3+/Ga3+ species preferentially occupy octahedral and tetrahedral voids, respectively. Mn2Ga2S5 exhibits an antiferromagnetic-like transition at 13 K accompanied by the ferromagnetic hysteresis of magnetization. Significant frustration of the magnetic system may yield spin-glass behavior at low temperatures. The exfoliation of Mn2Ga2S5 layers was performed in a non-polar solvent. Nanolayers and nanoscrolls were observed using high-resolution transmission electron microscopy. Fragments of micron-sized crystallites with a thickness of 70-100 nanometers were deposited on a glass surface, as evidenced by atomic force microscopy.

Simulations of frustrated Ising Hamiltonians using quantum approximate optimization.

Novel magnetic materials are important for future technological advances. Theoretical and numerical calculations of ground-state properties are essential in understanding these materials, however, computational complexity limits conventional methods for studying these states. Here we investigate an alternative approach to preparing materials ground states using the quantum approximate optimization algorithm (QAOA) on near-term quantum computers. We study classical Ising spin models on unit cells of square, Shastry-Sutherland and triangular lattices, with varying field amplitudes and couplings in the material Hamiltonian. We find relationships between the theoretical QAOA success probability and the structure of the ground state, indicating that only a modest number of measurements ([Formula: see text]) are needed to find the ground state of our nine-spin Hamiltonians, even for parameters leading to frustrated magnetism. We further demonstrate the approach in calculations on a trapped-ion quantum computer and succeed in recovering each ground state of the Shastry-Sutherland unit cell with probabilities close to ideal theoretical values. The results demonstrate the viability of QAOA for materials ground state preparation in the frustrated Ising limit, giving important first steps towards larger sizes and more complex Hamiltonians where quantum computational advantage may prove essential in developing a systematic understanding of novel materials. This article is part of the theme issue 'Quantum annealing and computation: challenges and perspectives'.

Multiphase magnetism in Yb2Ti2O7.

We use neutron scattering to show that ferromagnetism and antiferromagnetism coexist in the low T state of the pyrochlore quantum magnet [Formula: see text] While magnetic Bragg peaks evidence long-range static ferromagnetic order, inelastic scattering shows that short-range correlated antiferromagnetism is also present. Small-angle neutron scattering provides direct evidence for mesoscale magnetic structure that we associate with metastable antiferromagnetism. Classical Monte Carlo simulations based on exchange interactions inferred from [Formula: see text]-oriented high-field spin wave measurements confirm that antiferromagnetism is metastable within the otherwise ferromagnetic ground state. The apparent lack of coherent spin wave excitations and strong sensitivity to quenched disorder characterizing [Formula: see text] is a consequence of this multiphase magnetism.

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.

Block-spiral magnetism: An exotic type of frustrated order.

Competing interactions in quantum materials induce exotic states of matter such as frustrated magnets, an extensive field of research from both the theoretical and experimental perspectives. Here, we show that competing energy scales present in the low-dimensional orbital-selective Mott phase (OSMP) induce an exotic magnetic order, never reported before. Earlier neutron-scattering experiments on iron-based 123 ladder materials, where OSMP is relevant, already confirmed our previous theoretical prediction of block magnetism (magnetic order of the form [Formula: see text]). Now we argue that another phase can be stabilized in multiorbital Hubbard models, the block-spiral state. In this state, the magnetic islands form a spiral propagating through the chain but with the blocks maintaining their identity, namely rigidly rotating. The block-spiral state is stabilized without any apparent frustration, the common avenue to generate spiral arrangements in multiferroics. By examining the behavior of the electronic degrees of freedom, parity-breaking quasiparticles are revealed. Finally, a simple phenomenological model that accurately captures the macroscopic spin spiral arrangement is also introduced, and fingerprints for the neutron-scattering experimental detection are provided.

Modal Frustration and Periodicity Breaking in Artificial Spin Ice.

Here, an artificial spin ice lattice is introduced that exhibits unique Ising and non-Ising behavior under specific field switching protocols because of the inclusion of coupled nanomagnets into the unit cell. In the Ising regime, a magnetic switching mechanism that generates a uni- or bimodal distribution of states dependent on the alignment of the field is demonstrated with respect to the lattice unit cell. In addition, a method for generating a plethora of randomly distributed energy states across the lattice, consisting of Ising and Landau states, is investigated through magnetic force microscopy and micromagnetic modeling. It is demonstrated that the dispersed energy distribution across the lattice is a result of the intrinsic design and can be finely tuned through control of the incident angle of a critical field. The present manuscript explores a complex frustrated environment beyond the 16-vertex Ising model for the development of novel logic-based technologies.

Emergence of nontrivial magnetic excitations in a spin-liquid state of kagomé volborthite.

When quantum fluctuations destroy underlying long-range ordered states, novel quantum states emerge. Spin-liquid (SL) states of frustrated quantum antiferromagnets, in which highly correlated spins fluctuate down to very low temperatures, are prominent examples of such quantum states. SL states often exhibit exotic physical properties, but the precise nature of the elementary excitations behind such phenomena remains entirely elusive. Here, we use thermal Hall measurements that can capture the unexplored property of the elementary excitations in SL states, and report the observation of anomalous excitations that may unveil the unique features of the SL state. Our principal finding is a negative thermal Hall conductivity [Formula: see text] which the charge-neutral spin excitations in a gapless SL state of the 2D kagomé insulator volborthite Cu3V2O7(OH)2[Formula: see text]2H2O exhibit, in much the same way in which charged electrons show the conventional electric Hall effect. We find that [Formula: see text] is absent in the high-temperature paramagnetic state and develops upon entering the SL state in accordance with the growth of the short-range spin correlations, demonstrating that [Formula: see text] is a key signature of the elementary excitation formed in the SL state. These results suggest the emergence of nontrivial elementary excitations in the gapless SL state which feel the presence of fictitious magnetic flux, whose effective Lorentz force is found to be less than 1/100 of the force experienced by free electrons.

Tunable nonequilibrium dynamics of field quenches in spin ice.

We present nonequilibrium physics in spin ice as a unique setting that combines kinematic constraints, emergent topological defects, and magnetic long-range Coulomb interactions. In spin ice, magnetic frustration leads to highly degenerate yet locally constrained ground states. Together, they form a highly unusual magnetic state--a "Coulomb phase"--whose excitations are point-like defects--magnetic monopoles--in the absence of which effectively no dynamics is possible. Hence, when they are sparse at low temperature, dynamics becomes very sluggish. When quenching the system from a monopole-rich to a monopole-poor state, a wealth of dynamical phenomena occur, the exposition of which is the subject of this article. Most notably, we find reaction diffusion behavior, slow dynamics owing to kinematic constraints, as well as a regime corresponding to the deposition of interacting dimers on a honeycomb lattice. We also identify potential avenues for detecting the magnetic monopoles in a regime of slow-moving monopoles. The interest in this model system is further enhanced by its large degree of tunability and the ease of probing it in experiment: With varying magnetic fields at different temperatures, geometric properties--including even the effective dimensionality of the system--can be varied. By monitoring magnetization, spin correlations or zero-field NMR, the dynamical properties of the system can be extracted in considerable detail. This establishes spin ice as a laboratory of choice for the study of tunable, slow dynamics.

Magnetic Properties of Restacked 2D Spin 1/2 honeycomb RuCl3 Nanosheets.

Spin 1/2 honeycomb materials have gained substantial interest due to their exotic magnetism and possible application in quantum computing. However, in all current materials out-of-plane interactions are interfering with the in-plane order, hence a true 2D magnetic honeycomb system is still in demand. Here, we report the exfoliation of the magnetic semiconductor α-RuCl3 into the first halide monolayers and the magnetic characterization of the spin 1/2 honeycomb arrangement of turbostratically stacked RuCl3 monolayers. The exfoliation is based on a reductive lithiation/hydration approach, which gives rise to a loss of cooperative magnetism due to the disruption of the spin 1/2 state by electron injection into the layers. The restacked, macroscopic pellets of RuCl3 layers lack symmetry along the stacking direction. After an oxidative treatment, cooperative magnetism similar to the bulk is restored. The oxidized pellets of restacked single layers feature a magnetic transition at TN = 7 K if the field is aligned parallel to the ab-plane, while the magnetic properties differ from bulk α-RuCl3 if the field is aligned perpendicular to the ab-plane. The deliberate introduction of turbostratic disorder to manipulate the magnetic properties of RuCl3 is of interest for research in frustrated magnetism and complex magnetic order as predicted by the Kitaev-Heisenberg model.

Response functions for electric field induced two-dimensional nonlinear spectroscopy in a Kitaev magnet.

We study the dynamical response functions relevant for electric field induced two-dimensional (2D) coherent nonlinear optical spectroscopy in a Kitaev magnet at finite temperature. We show that these response functions are susceptible to both types of fractional quasiparticles of this quantum spin-liquid, i.e. fermions and flux visons. Focusing on the second order response, we find a strong antidiagonal feature in the 2D frequency plane, related to the galvanoelectric effect of the fractional fermions. Perpendicular to the antidiagonal, the width of this feature is set by quasiparticle relaxation rates beyond the bare Kitaev magnet, thereby providing access to single-particle characteristics within a multi-particle continuum. While the 2D spectrum of the response is set by the fermionic quasiparticles and displays Fermi blocking versus temperature, the emergent bond randomness which arises due to thermally populated visons strongly modifies the fermionic spectrum. Therefore also the presence of gauge excitations is manifest in the 2D nonlinear response as the temperature is increased beyond the flux proliferation crossover.

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.

Entropy driven incommensurate structures in the frustrated kagome staircase Co3V2O8.

Co3V2O8features spin-3/2 moments arrayed on a kagome staircase lattice. A spin density wave with a continuously evolving propagation vector ofk⃗=(0,δ,0), showing both incommensurate states and multiple commensurate lock-ins, is observed at temperatures above the ferromagnetic ground state. Previous work has suggested that this changing propagation vector could be driven by changes in exchange interactions due to Co atom displacements. We present a straightforward model showing that a Hamiltonian with competing (but temperature independent) interactions can semi-quantitatively reproduce this behavior using a mean field approximation. The simulated spin density wave magnetic structures feature buckled kagome planes that are either ferromagnetically or antiferromagnetically ordered. Propagation vectors that differ fromδ=1/2will have multiple different ways of arranging these ferromagnetic layers that have very similar energies. This classical stacking entropy appears to be crucial in stabilizing the temperature-dependent propagation vector.