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The search for quantum spin liquids—topological magnets with fractionalized excitations—has been a central theme in condensed matter and materials physics. Despite numerous theoretical proposals, connecting experiment with detailed theory exhibiting a robust quantum spin liquid has remained a central challenge. Here, focusing on the strongly spin-orbit coupled effectiveS = 1/2 pyrochlore magnet Ce₂Zr₂O₇, we analyze recent thermodynamic and neutron-scattering experiments, to identify a microscopic effective Hamiltonian through a combination of finite temperature Lanczos, Monte Carlo, and analytical spin dynamics calculations. Its parameter values suggest the existence of an exotic phase, aπ-flux U(1) quantum spin liquid. Intriguingly, the octupolar nature of the moments makes them less prone to be affected by magnetic disorder, while also hiding some otherwise characteristic signatures from neutrons, making this spin liquid arguably more stable than its more conventional counterparts.

 

New phases of matter emerge at the edge of magnetic instabilities, which can occur in materials with moments that are localized, itinerant or intermediate between these extremes. In local moment systems, such as heavy fermions, the magnetism can be tuned towards a zero-temperature transition at a quantum critical point (QCP) via pressure, chemical doping, and, rarely, magnetic field. By contrast, in itinerant moment systems, QCPs are more rare, and they are induced by pressure or doping; there are no known examples of field induced transitions. This means that no universal behaviour has been established across the whole itinerant-to-local moment range—a substantial gap in our knowledge of quantum criticality. Here we report an itinerant antiferromagnet, Ti₃Cu₄, that can be tuned to a QCP by a small magnetic field. We see signatures of quantum criticality and the associated non-Fermi liquid behaviour in thermodynamic and transport measurements, while band structure calculations point to an orbital-selective, spin density wave ground state, a consequence of the square net structural motif in Ti₃Cu₄. Ti₃Cu₄thus provides a platform for the comparison and generalisation of quantum critical behaviour across the whole spectrum of magnetism.

 

Abstract Magnetic order in most materials occurs when magnetic ions with finite moments arrange in a particular pattern below the ordering temperature. Intriguingly, if the crystal electric field (CEF) effect results in a spin-singlet ground state, a magnetic order can still occur due to the exchange interactions between neighboring ions admixing the excited CEF levels. The magnetic excitations in such a state are spin excitons generally dispersionless in reciprocal space. Here we use neutron scattering to study stoichiometric Ni 2 Mo 3 O 8 , where Ni 2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has magnetic order. Furthermore, CEF spin excitons from the tetrahedral sites form a dispersive diffusive pattern around the Brillouin zone boundary, likely due to spin entanglement and geometric frustrations. 

The hallmark of highly frustrated systems is the presence of many states close in energy to the ground state. Fluctuations between these states can preclude the emergence of any form of order and lead to the appearance of spin liquids. Even on the classical level, spin liquids are not all alike: they may have algebraic or exponential correlation decay, and various forms of long wavelength description, including vector or tensor gauge theories. Here, we introduce a classification scheme, allowing us to fit the diversity of classical spin liquids (CSLs) into a general framework as well as predict and construct new kinds. CSLs with either algebraic or exponential correlation-decay can be classified via the properties of the bottom flat band(s) in their soft-spin Hamiltonians. The classification of the former is based on the algebraic structures of gapless points in the spectra, which relate directly to the emergent generalized Gauss's laws that control the low temperature physics. The second category of CSLs, meanwhile, are classified by the fragile topology of the gapped bottom band(s). Utilizing the classification scheme we construct new models realizing exotic CSLs, including one with anisotropic generalized Gauss's laws and charges with subdimensional mobility, one with a network of pinch-line singularities in its correlation functions, and a series of fragile topological CSLs connected by zero-temperature transitions. 

Electronic spins can form long-range entangled phases of condensed matter named quantum spin liquids. Their existence is conceptualized in models of two- or three-dimensional frustrated magnets that evade symmetry-breaking order down to zero temperature. Quantum spin ice (QSI) is a theoretically well-established example described by an emergent quantum electrodynamics, with excitations behaving like photon and matter quasiparticles. The latter are fractionally charged and equivalent to the `spinons' emerging from coherent phases of singlets in one dimension, where clear experimental proofs of fractionalization exist. However, in frustrated magnets it remains difficult to establish consensual evidence for quantum spin liquid ground states and their fractional excitations. Here, we use backscattering neutron spectroscopy to achieve extremely high resolution of the time-dependent magnetic response of the candidate QSI material Ce2Sn2O7. We find a gapped spectrum featuring a threshold and peaks that match theories for pair production and propagation of fractional matter excitations (spinons) strongly coupled to a background gauge field. The observed peaks provide evidence for a QSI through spectroscopic signatures of space-time symmetry fractionalization, while the threshold behavior corroborates the regime of strong light-matter interaction predicted for the emergent universe in a QSI. 

We investigate the correlated state of Ce2Hf2O7 using neutron scattering, finding signatures of correlations of both dipolar and octupolar character. A dipolar inelastic signal is also observed, as expected for spinons in a quantum spin ice (QSI). Fits of thermodynamic data using exact diagonalization methods indicate that the largest interaction is an octupolar exchange, with a strength roughly twice as large as other terms. This hierarchy of exchange interactions - far from a perturbative regime but still in the octupolar QSI phase - rationalises observations in neutron scattering, which illustrate the multipolar nature of degrees of freedom in Ce3+ pyrochlores. 

Classical spin liquids (CSL) lack long-range magnetic order and are characterized by an extensive ground state degeneracy. We propose a classification scheme of CSLs based on the structure of the flat bands of their Hamiltonians. Depending on absence or presence of the gap from the flat band, the CSL are classified as algebraic or fragile topological, respectively. Each category is further classified: the algebraic case by the nature of the emergent Gauss's law at the gap-closing point(s), and the fragile topological case by the homotopy of the eigenvector winding around the Brillouin zone. Previously identified instances of CSLs fit snugly into our scheme, which finds a landscape where algebraic CSLs are located at transitions between fragile topological ones. It also allows us to present a new, simple family of models illustrating that landscape, which hosts both fragile topological and algebraic CSLs, as well as transitions between them 

We study the nature of the debated thermal Hall effect in the candidate Kitaev material α-RuCl3. Without assuming the existence of a gapped spin liquid, we show that a realistic minimal spin model in the canted zigzag phase suffices, at the level of linear spin-wave theory, to qualitatively explain the observed temperature and magnetic field dependence of the non-quantized thermal Hall conductivity κ_xy, with its origin lying in the Berry curvature of the magnon bands. The magnitude of the effect is however too small compared to the measurement by Czajka et al. [Nat. Mater. 22, 36-41 (2023)], even after scanning a broad range of model parameters so as to maximize κ_xy/T. Recent experiments suggest that phonons play an important role, which we show couple to the spins, endowing phonons with chirality. The resulting intrinsic contribution, from both magnons and phonons, is however still insufficient to explain the observed magnitude of the Hall signal. After careful analysis of the extrinsic phonon mechanisms, we use the recent experimental data on thermal transport in α-RuCl3 by Lefrançois et al. [Phys. Rev. X 12, 021025 (2022)] to determine the phenomenological ratio of the extrinsic and intrinsic contributions η≡κ_E/κ_I. We find η=1.2±0.5, which when combined with our computed intrinsic value, explains quantitavely both the magnitude and detailed temperature dependence of the experimental thermal Hall effect in α-RuCl3.