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Dipolar-octupolar (DO) pyrochlore systems Ce$_2$(Zr,Sn,Hf)$_2$O$_7$ have garnered much attention as recent investigations suggest that they may stabilize a novel quantum spin ice (QSI), a quantum spin liquid (QSL) with an emergent $U(1)$ gauge field. In particular, the experimentally estimated microscopic exchange parameters place Ce$_2$Zr$_2$O$_7$ in the $\pi$-flux QSI regime, and recent neutron scattering experiments have corroborated some key theoretical predictions. On the other hand, to make a definitive conclusion, more multifaceted experimental signatures are desirable. In this regard, recent neutron scattering investigation of the magnetic field dependence of the spin correlations in Ce$_2$Zr$_2$O$_7$ may provide valuable information. However, there have not been any comprehensive theoretical studies for comparison. In this work, we provide such information using gauge mean-field theory (GMFT), allowing for theoretical investigation beyond the perturbative regime. In particular, we construct the phase diagrams for the [110], [111], and [001] field directions. Furthermore, we demonstrate the distinctive evolution of the equal-time and dynamical spin structure factors as a function of the magnetic field for each field direction. These predictions will help future experiments confirm the true nature of the DO-QSI., Comment: 14+11 pages, 11+7 figures

A quantum spin liquid (QSL) arises from a highly entangled superposition of many degenerate classical ground states in a frustrated magnet, and is characterized by emergent gauge fields and deconfined fractionalized excitations (spinons). Because such a novel phase of matter is relevant to high-transition-temperature superconductivity and quantum computation, the microscopic understanding of QSL states is a long-sought goal in condensed matter physics. The 3D pyrochlore lattice of corner-sharing tetrahedra can host a QSL with U(1) gauge fields called quantum spin ice (QSI), which is a quantum (with effective $S=1/2$) analog of the classical (with large effective moment) spin ice. A key difference between QSI and classical spin ice is the predicted presence of the linearly dispersing collective excitations near zero energy, dubbed the "photons", arising from emergent quantum electrodynamics, in addition to the spinons at higher energies. Recently, 3D pyrochlore systems Ce2M2O7 (M = Sn, Zr, Hf) have been suggested as effective $S=1/2$ QSI candidates, but there has been no evidence of quasielastic magnetic scattering signals from photons, a key signature for a QSI. Here, we use polarized neutron scattering experiments on single crystals of Ce2Zr2O7 to conclusively demonstrate the presence of magnetic excitations near zero energy at 50 mK in addition to signatures of spinons at higher energies. By comparing the energy (E), wave vector (Q), and polarization dependence of the magnetic excitations with theoretical calculations, we conclude that Ce2Zr2O7 is the first example of a dipolar-octupolar $\pi$ flux QSI with dominant dipolar Ising interactions, therefore identifying a microscopic Hamiltonian responsible for a QSL.

Early efforts to realize exotic quantum ground states in frustrated magnets focused on frustration arising from the lattice geometry alone. Attention has shifted to bond-dependent anisotropic interactions, as well as further-neighbor interactions, on non-geometrically-frustrated lattices due to their greater versatility. The honeycomb magnet BaCo$_2$(AsO$_4$)$_2$ recently emerged as a candidate host for both bond-dependent (e.g. Kitaev) and third-neighbor ($J_3$) interactions, and has become a model experimental system due to its relatively low levels of disorder. Understanding the relative importance of different exchange interactions holds the key to achieving novel ground states, such as quantum spin liquids. Here, we use the magnetotropic susceptibility to map out the intermediate and high-field phase diagram of BaCo$_2$(AsO$_4$)$_2$ as a function of the out-of-plane magnetic field direction at $T = 1.6$ K. We show that the experimental data are qualitatively consistent with classical Monte Carlo results of the XXZ-$J_1$-$J_3$ model with small Kitaev and off-diagonal exchange couplings included. However, the calculated critical fields are systematically larger than the experimental values. Infinite-DMRG computations on the quantum model reveal that quantum corrections from a nearby ferromagnetic state are likely responsible for the suppressed critical fields. Together, our experiment and theory analyses demonstrate that, while quantum fluctuations play an important role in determining the phase diagram, most of the physics of BaCo$_2$(AsO$_4$)$_2$ can be understood in terms of the classical dynamics of long-range ordered states, leaving little room for the possibility of a quantum spin liquid., Comment: 16 pages, 12 figures

Quantum spin ice (QSI) is an emblematic three-dimensional $U(1)$ quantum spin liquid (QSL) on the pyrochlore lattice that hosts gapless photon-like modes and spinon excitations. Despite its notable status and the current rise of strong material candidates Ce$_2$(Zr, Sn, Hf)$_2$O$_7$, there are still only a few analytical approaches to model the low-energy behavior of QSI. These analytical methods are essential to gain insight into the physical interpretation of measurements. We here introduce the self-consistent exclusive boson representation (SCEBR) to model emergent spinon excitations in QSI. By treating the presence of other emergent charges in an average way, the SCEBR extends the range of validity of the exclusive boson representation previously introduced by Hao, Day, and Gingras [Hao, Day, and Gingras, Physical Review B, 90, 214430 (2014)] to numerous cases of physical relevance. We extensively benchmark the approach and provide detailed analytical expressions for the spinon dispersion, the Bogoliubov transformation that diagonalizes the system, and the dynamical spin structure factor for 0- and $\pi$-flux QSI. Finite temperature properties are further investigated to highlight essential differences between the thermodynamic behavior of the 0- and $\pi$-flux phases. We notably show that the SCEBR predicts a reduction of the spinon bandwidth with increasing temperature, consistent with previous quantum Monte-Carlo results, through suppression of spinon hopping by thermal occupation. The SCEBR thus provides a powerful analytical tool to interpret experiments on current and future candidate material that has several advantages over other widely used methods., Comment: 13+9 pages, 8 figures

Motivated by recent experiments on Ce$_2$Zr$_2$O$_7$ that reveal a dynamic, liquid-like ground state, we study the nearest neighbor XYZ Hamiltonian of dipolar-octupolar pyrochlore magnets with the pseudofermion functional renormalization group (PFFRG), which is numerically implemented by the SpinParser software. Taking the interaction between the octupolar components to be dominant and antiferromagnetic, we map out the phase diagram demarcating the quantum disordered and magnetically ordered states. We identify four distinct phases, namely the $0$-flux and $\pi$-flux quantum spin ices, and the all-in-all-out magnetic orders along the local $z$ and $x$ axes. We further use the static two-spin correlations output by the PFFRG algorithm to compute the polarized neutron scattering cross-sections, which are able to capture several qualitative features observed experimentally, in the materially relevant parameter regime that stabilizes the $\pi$-flux quantum spin ice. Our results provide support for a quantum spin liquid ground state in Ce$_2$Zr$_2$O$_7$., Comment: 10+6 pages, 6+5 figures

The triangular lattice Hubbard model at strong coupling, whose effective spin model contains both Heisenberg and ring exchange interactions, exhibits a rich phase diagram as the ratio of the hopping $t$ to onsite Coulomb repulsion $U$ is tuned. This includes a chiral spin liquid (CSL) phase. Nevertheless, this exotic phase remains challenging to realize experimentally because a given material has a fixed value of $t/U$ that can difficultly be tuned with external stimuli. One approach to address this problem is applying a DC electric field, which renormalizes the exchange interactions as electrons undergo virtual hopping processes; in addition to creating virtual doubly occupied sites, electrons must overcome electric potential energy differences. Performing a small $t/U$ expansion to fourth order, we derive the ring exchange model in the presence of an electric field and find that it not only introduces spatial anisotropy but also tends to enhance the ring exchange term compared to the dominant nearest-neighbor Heisenberg interaction. Thus, increasing the electric field serves as a way to increase the importance of the ring exchange at constant $t/U$. Through density matrix renormalization group calculations, we compute the ground state phase diagram of the ring exchange model for two different electric field directions. In both cases, we find that the electric field shifts the phase boundary of the CSL towards a smaller ratio of $t/U$. Therefore, the electric field can drive a magnetically ordered state into the CSL. This explicit demonstration opens the door to tuning other quantum spin systems into spin liquid phases via the application of an electric field., Comment: 9 + 17 pages, 10 + 13 figures

Understanding non-Fermi liquids in dimensions higher than one remains one of the most formidable challenges in modern condensed matter physics. These systems, characterized by an abundance of gapless degrees of freedom and the absence of well-defined quasiparticles, defy conventional analytical frameworks. Inspired by recent work [Delacretaz, Du, Mehta, and Son, Physical Review Research, 4, 033131 (2022)], we present a procedure for bosonizing Fermi surfaces that does not rely on the existence of sharp excitation and is thus directly applicable to non-Fermi liquids. Our method involves parameterizing the generalized fermionic distribution function through a bosonic field that describes frequency-dependent local variations of the chemical potential in momentum space. We propose an effective action that produces the collisionless quantum Boltzmann equation as its equation of motion and can be used for any dimension and Fermi surface of interest. Even at the quadratic order, this action reproduces non-trivial results obtainable only through involved analysis with alternative means. By offering an alternative method directly applicable to studying the low-energy physics of Fermi and non-Fermi liquids, our work potentially stands as an important building block in advancing the comprehension of strange metals and associated phenomena., Comment: 13+15 pages, 4 figure; the first two authors contributed equally to this work

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 Ce$_2$Sn$_2$O$_7$. 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 multiple peaks are a specific signature of the $\pi$-flux phase of QSI, providing spectroscopic evidence for fractionalization in a three-dimensional quantum spin liquid., Comment: 19 pages, 6 figures, fixes in references

Recent investigations on the dipolar-octupolar compounds Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$ suggest that they may stabilize so-called $\pi$-flux octupolar quantum spin ice ($\pi$-O-QSI), a novel three-dimensional quantum spin liquid hosting emergent photons. Confirmation of such an exotic phase would require the prediction of a distinctive signature and its subsequent experimental observation. So far, however, theoretical predictions for any such sharp smoking-gun signatures are lacking. In this Letter, we thoroughly investigate O-QSI using an extension of gauge mean-field theory. This framework produces a phase diagram consistent with previous studies and an energy-integrated neutron scattering signal with intensity-modulated rod motifs, as reported in experiments and numerical studies. We predict that the dynamical spin structure factor of $\pi$-O-QSI is characterized by a broad continuum with three distinctive peaks as a consequence of the two mostly flat spinon bands. These three peaks should be measurable by high-resolution inelastic neutron scattering. Such spectroscopic signatures would be clear evidence for the realization of $\pi$-flux quantum spin ice., Comment: 7+25 pages, 4+11 figures

Symmetry fractionalization is a ubiquitous feature of topologically ordered states that can be used to classify different symmetry-enriched topological phases and reveal some of their unique experimental signatures. Despite its vast popularity, there is currently no available framework to study symmetry fractionalization of quantum spin ice (QSI) -- a $U(1)$ quantum spin liquid (QSL) on the pyrochlore lattice supporting emergent photons -- within the most widely used theoretical framework to describe it, gauge mean-field theory (GMFT). In this work, we provide an extension of GMFT that allows for the classification of space-time symmetry fractionalization. The construction classifies all GMFT Ans\"atze that yield physical wavefunctions invariant under given symmetries and a specific low-energy gauge structure. As an application of the framework, we first show that the only two Ans\"atze with emergent $U(1)$ gauge fields that respect all space-group symmetries are the well-known 0- and $\pi$-flux states. We then showcase how the framework may describe QSLs beyond the currently known ones by classifying chiral $U(1)$ QSI. We find two new states described by $\pi/2$- and $3\pi/2$-fluxes of the emergent gauge field threading the hexagonal plaquettes of the pyrochlore lattice. We finally discuss how the different ways translation symmetries fractionalize for all these states lead to unique experimentally relevant signatures and compute their respective inelastic neutron scattering cross-section to illustrate the argument., Comment: 12+10 pages, 4+1 figures

Recently, Co-based honeycomb magnets have been proposed as promising candidate materials to host the Kitaev spin liquid state. One of the front-runners is BaCo$_2$(AsO$_4$)$_2$ (BCAO), where it was suggested that the exchange processes between Co$^{2+}$ ions via the surrounding edge-sharing oxygen octahedra could give rise to bond-dependent Kitaev interactions. In this work, we present and analyze comprehensive inelastic neutron scattering studies 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 \JKG model and the \XXZ model. We show that the existing experimental data can be consistently accounted for by the \XXZ model but not by the \JKG 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., Comment: 15 pages, 10 figures

Recent experiments on the dipolar-octupolar pyrochlore compound Ce$_2$Zr$_2$O$_7$ indicate that it may realize a three-dimensional quantum spin liquid (QSL). In particular, the analyses of available data suggest that the system is in a region of parameter space, where the so-called $\pi$-flux $U(1)$ octupolar quantum spin ice (QSI) with an emergent photon could be realized. On the other hand, because the system is far from the perturbative classical spin ice regime, it is unclear whether the quantum ground state is primarily a coherent superposition of 2-in-2-out configurations as in the canonical QSI phases. In this work, we explore other possible competing quantum spin liquid states beyond QSI using the Schwinger boson parton construction of the dipolar-octupolar pseudospin-1/2 model. After classifying all symmetric $U(1)$ and $\mathbb{Z}_2$ QSLs using the projective symmetry group (PSG), we construct a mean-field phase diagram that possesses a number of important features observed in an earlier exact diagonalization study. In the experimentally relevant frustrated region of the phase diagram, we find two closely competing gapped $\mathbb{Z}_2$ QSLs with a narrow spinon dispersion. The equal-time and dynamical spin structure factors of these states show key features similar to what was reported in neutron scattering experiments. Hence, these QSLs are closely competing ground states in addition to the $\pi$-flux $U(1)$ QSI, and they should be taken into account on equal footing for the interpretation of experiments on Ce$_2$Zr$_2$O$_7$., Comment: 11+15 pages, 7+3 figures