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Electrons at the border of localization generate exotic states of matter across all classes of strongly correlated electron materials and many other quantum materials with emergent functionality. Heavy electron metals are a model example, in which magnetic interactions arise from the opposing limits of localized and itinerant electrons. This remarkable duality is intimately related to the emergence of a plethora of novel quantum matter states such as unconventional superconductivity, electronic-nematic states, hidden order and most recently topological states of matter such as topological Kondo insulators and Kondo semimetals and putative chiral superconductors. The outstanding challenge is that the archetypal Kondo lattice model that captures the underlying electronic dichotomy is notoriously difficult to solve for real materials. Here we show, using the prototypical strongly-correlated antiferromagnet CeIn3, that a multi-orbital periodic Anderson model embedded with input from ab initio bandstructure calculations can be reduced to a simple Kondo-Heisenberg model, which captures the magnetic interactions quantitatively. We validate this tractable Hamiltonian via high-resolution neutron spectroscopy that reproduces accurately the magnetic soft modes in CeIn3, which are believed to mediate unconventional superconductivity. Our study paves the way for a quantitative understanding of metallic quantum states such as unconventional superconductivity.
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Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr3Ir2O7. By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high symmetry points and which decays upon heating concurrent with a decrease in the material's resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr3Ir2O7 indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulator phase.
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Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth-based magnets because of the large effective spin anisotropy induced by the combination of strong spin-orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO3 provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga-Luttinger liquid behavior and spinon confinement-deconfinement transitions in different regions of magnetic field-temperature phase diagram.
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The original version of this Article omitted the following from the Acknowledgements: 'J. Ma's primary affiliation is Shanghai Jiao Tong University.' This has been corrected in both the PDF and HTML versions of the Article.
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Magnetization plateaus in quantum magnets-where bosonic quasiparticles crystallize into emergent spin superlattices-are spectacular yet simple examples of collective quantum phenomena escaping classical description. While magnetization plateaus have been observed in a number of spin-1/2 antiferromagnets, the description of their magnetic excitations remains an open theoretical and experimental challenge. Here, we investigate the dynamical properties of the triangular-lattice spin-1/2 antiferromagnet Ba3CoSb2O9 in its one-third magnetization plateau phase using a combination of nonlinear spin-wave theory and neutron scattering measurements. The agreement between our theoretical treatment and the experimental data demonstrates that magnons behave semiclassically in the plateau in spite of the purely quantum origin of the underlying magnetic structure. This allows for a quantitative determination of Ba3CoSb2O9 exchange parameters. We discuss the implication of our results to the deviations from semiclassical behavior observed in zero-field spin dynamics of the same material and conclude they must have an intrinsic origin.
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An exact mapping between quantum spins and boson gases provides fresh approaches to the creation of quantum condensates and crystals. Here we report on magnetization measurements on the dimerized quantum magnet SrCu2(BO3)2 at cryogenic temperatures and through a quantum-phase transition that demonstrate the emergence of fractionally filled bosonic crystals in mesoscopic patterns, specified by a sequence of magnetization plateaus. We apply tens of Teslas of magnetic field to tune the density of bosons and gigapascals of hydrostatic pressure to regulate the underlying interactions. Simulations help parse the balance between energy and geometry in the emergent spin superlattices. The magnetic crystallites are the end result of a progression from a direct product of singlet states in each short dimer at zero field to preferred filling fractions of spin-triplet bosons in each dimer at large magnetic field, enriching the known possibilities for collective states in both quantum spin and atomic systems.
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We present single-crystal neutron scattering measurements of the spin-1/2 equilateral triangular-lattice antiferromagnet Ba_{3}CoSb_{2}O_{9}. Besides confirming that the Co^{2+} magnetic moments lie in the ab plane for zero magnetic field and then determining all the exchange parameters of the minimal quasi-2D spin Hamiltonian, we provide conclusive experimental evidence of magnon decay through observation of intrinsic line broadening. Through detailed comparisons with the linear and nonlinear spin-wave theories, we also point out that the large-S approximation, which is conventionally employed to predict magnon decay in noncollinear magnets, is inadequate to explain our experimental observation. Thus, our results call for a new theoretical framework for describing excitation spectra in low-dimensional frustrated magnets under strong quantum effects.
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We have used high-resolution neutron spectroscopy experiments to determine the complete spin wave spectrum of the heavy-fermion antiferromagnet CeRhIn5. The spin wave dispersion can be quantitatively reproduced with a simple frustrated J1-J2 model that also naturally explains the magnetic spin-spiral ground state of CeRhIn5 and yields a dominant in-plane nearest-neighbor magnetic exchange constant J0=0.74(3) meV. Our results pave the way to a quantitative understanding of the rich low-temperature phase diagram of the prominent CeTIn5 (T=Co, Rh, Ir) class of heavy-fermion materials.
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Insulating magnets can display novel signatures of quantum fluctuations as similar to the case of metallic magnets. However, their weak spin-lattice coupling has made such observations challenging. Here we find that antiferromagnetic (AF) quantum fluctuations manifest in the dielectric properties of multiferroic Ba2CoGe2O7, where a ferroelectric polarization develops concomitant to an AF ordering. Upon application of a magnetic field (H), dielectric constant shows a characteristic power-law dependence near absolute zero temperature and close to the critical field Hc=37.1 T due to enhanced AF quantum fluctuations. When H>Hc, the dielectric constant shows the temperature-dependent anomalies that reflect a crossover from a field-tuned quantum critical to a gapped spin-polarized state. We uncover theoretically that a linear relation between AF susceptibility and dielectric constant stems from the generic magnetoelectric coupling and directly explains the experimental findings, opening a new pathway for studying quantum criticality in condensed matter.
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We study vanadium spinels AV2O4 (A = Cd,Mg) in pulsed magnetic fields up to 65 T. A jump in magnetization at µ0H≈40 T is observed in the single-crystal MgV2O4, indicating a field induced quantum phase transition between two distinct magnetic orders. In the multiferroic CdV2O4, the field induced transition is accompanied by a suppression of the electric polarization. By modeling the magnetic properties in the presence of strong spin-orbit coupling characteristic of vanadium spinels, we show that both features of the field induced transition can be successfully explained by including the effects of the local trigonal crystal field.
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Spin chains are among the simplest physical systems in which electron-electron interactions induce novel states of matter. Here we propose to combine atomic scale engineering and spectroscopic capabilities of state of the art scanning tunnel microscopy to probe the fractionalized edge states of individual atomic scale S=1 spin chains. These edge states arise from the topological order of the ground state in the Haldane phase. We also show that the Haldane gap and the spin-spin correlation length can be measured with the same technique.
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The mechanisms producing strong coupling between electric and magnetic order in multiferroics are not always well understood, since their microscopic origins can be quite different. Hence, gaining a deeper understanding of magnetoelectric coupling in these materials is the key to their rational design. Here, we use ultrafast optical spectroscopy to show that the influence of magnetic ordering on quantum charge fluctuations via the double-exchange mechanism can govern the interplay between electric polarization and magnetism in the charge-ordered multiferroic LuFe2O4.
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We study the strongly anisotropic quasi-one-dimensional S = 1 quantum magnet NiCl2·4SC(NH2)2 using elastic and inelastic neutron scattering. We demonstrate that a magnetic field splits the excited doublet state and drives the lower doublet state to zero energy at a critical field Hc1. For Hc1 < H < Hc2, where Hc2 indicates the transition to a fully magnetized state, three-dimensional magnetic order is established with the AF moment perpendicular to the magnetic field. We mapped the temperature/magnetic field phase diagram, and we find that the total ordered magnetic moment reaches m(tot) = 2.1 µB at the field µ(0)H = 6 T and is thus close to the saturation value of the fully ordered moment. We study the magnetic spin dynamics in the fully magnetized state for H > Hc2, and we demonstrate the presence of an AF interaction between Ni(2+) on the two interpenetrating sublattices. In the antiferromagnetically ordered phase, the spin-waves that develop from the lower-energy doublet are split into two modes. This is most likely the result of the presence of the AF interaction between the interpenetrating lattices.
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Gapless electronic systems containing topologically nontrivial Fermi points are sources of various topological insulators. Whereas, most of these special band-crossing points are built in the electronic structure of the noninteracting lattice models, we show that a quadratic Fermi point characterized by a nonzero winding number emerges with a collinear triple-Q spin-density-wave state that arises from a perfectly nested but topologically trivial Fermi surface. We obtain a universal low-energy Hamiltonian for the quadratic Fermi point and show that such collinear orderings are unstable against the onset of scalar spin chirality that opens a gap and induces a spontaneous quantum Hall insulator as the temperature tends to zero.
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Motivated by recent experiments on vanadium spinels, AV2O4, that show an increasing degree of electronic delocalization for smaller cation sizes, we study the evolution of orbital ordering (OO) between the strong and intermediate-coupling regimes of a multiorbital Hubbard Hamiltonian. The underlying magnetic ordering of the Mott insulating state leads to a rapid suppression of OO due to enhanced charge fluctuations along ferromagnetic bonds. Orbital double occupancy is rather low at the transition point indicating that the system is in the crossover region between strong and intermediate-coupling regimes when the orbital degrees of freedom become disordered.
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We study a frustrated quantum Ising model relevant for Ca3Co2O6 that consists of a triangular lattice of weakly coupled ferromagnetic chains. According to our quantum Monte Carlo simulations, the chains become ferromagnetic and form a three-sublattice "up-up-down" structure for T≤T(CI). In contrast, long-wavelength spin-density-wave microphases are stabilized along the chains for T(CI)
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We present magnetization and magnetostriction studies of LaCoO3 in magnetic fields approaching 100 T. In contrast with expectations from single-ion models, the data reveal two distinct first-order transitions and well-defined magnetization plateaus. The magnetization at the higher plateau is only about half the saturation value expected for spin-1 Co3+ ions. These findings strongly suggest collective behavior induced by interactions between different electronic configurations of Co3+ ions. We propose a model that predicts crystalline spin textures and a cascade of four magnetic phase transitions at high fields, of which the first two account for the experimental data.
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We demonstrate multiferroic behavior in trimerized Mott insulators through the interplay between spins and electric dipole moments resulting from electronic charge fluctuations in frustrated units. The model consists of stacked triangular layers of trimers with small intertrimer exchange interactions J' and J''. Ferroelectric states coexist with ferro- or antiferromagnetic orderings depending on the value of the magnetic field H and the sign of the interlayer exchange J''. The electric polarization undergoes abrupt changes as a function of H.
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We derive the exact ground space of a family of spin-1/2 Heisenberg chains with uniaxial exchange anisotropy (XXZ) and interactions between nearest and next-nearest-neighbor spins. The Hamiltonian family, H(eff)(Q), is parametrized by a single variable Q. By using a generalized Jordan-Wigner transformation that maps spins into anyons, we show that the exact ground states of H(eff)(Q) correspond to a condensation of anyons with a statistical phase φ=-4Q. We also provide matrix-product state representations of some ground states that allow for the efficient computation of spin-spin correlation functions.
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We develop a theory of the coexistence of superconductivity (SC) and antiferromagnetism (AFM) in CeCoIn(5). We show that in Pauli-limited nodal superconductors the nesting of the quasiparticle pockets induced by Zeeman pair breaking leads to incommensurate AFM with the magnetic moment normal to the field. We compute the phase diagram and find a first order transition to the normal state at low temperatures, the absence of normal state AFM, and the coexistence of SC and AFM at high fields, in agreement with experiments. We also predict the existence of a new double-Q magnetic phase.