First-Principles Design of the Spinel Iridate Ir_{2}O_{4} for High-Temperature Quantum Spin Ice.

Insulating magnetic rare-earth pyrochlores related to spin ice host emergent bosonic monopolar spinons, which obey a magnetic analogue of quantum electrodynamics and may open a route to spinonics. However, the energy scales of the interactions among rare-earth moments are so low (∼ 1 K) that the possible quantum coherence can be achieved at a sub-Kelvin scale. Here, we design high-temperature quantum spin ice materials from first principles. It is shown that the A-site deintercalated spinel iridate Ir_{2}O_{4}, which has been experimentally grown as epitaxial thin films, is a promising candidate for quantum spin ice with a spin-ice-rule interaction of a few tens of meV. Controlling electronic structures of Ir_{2}O_{4} through substrates, it is possible to tune magnetic interactions so that a magnetic Coulomb liquid persists at high temperatures.

Quantum Spin Ice under a [111] Magnetic Field: From Pyrochlore to Kagome.

Quantum spin ice, modeled for magnetic rare-earth pyrochlores, has attracted great interest for hosting a U(1) quantum spin liquid, which involves spin-ice monopoles as gapped deconfined spinons, as well as gapless excitations analogous to photons. However, the global phase diagram under a [111] magnetic field remains open. Here we uncover by means of unbiased quantum Monte Carlo simulations that a supersolid of monopoles, showing both a superfluidity and a partial ionization, intervenes the kagome spin ice and a fully ionized monopole insulator, in contrast to classical spin ice where a direct discontinuous phase transition takes place. We also show that on cooling, kagome spin ice evolves towards a valence-bond solid similar to what appears in the associated kagome lattice model [S. V. Isakov et al., Phys. Rev. Lett. 97, 147202 (2006)PRLTAO0031-900710.1103/PhysRevLett.97.147202]. Possible relevance to experiments is discussed.

Numerical Evidence of Quantum Melting of Spin Ice: Quantum-to-Classical Crossover.

Unbiased quantum Monte Carlo simulations are performed on the nearest-neighbor spin-1/2 pyrochlore XXZ model with an antiferromagnetic longitudinal and the weak ferromagnetic transverse exchange couplings, J and J_{⊥}. The specific heat exhibits a broad peak at T_{CSI}~0.2J associated with a crossover to a classical Coulomb liquid regime showing a suppressed spin-ice monopole density, a broadened pinch-point singularity, and the Pauling entropy for |J_{⊥}|≪J, as in classical spin ice. On further cooling, the entropy restarts decaying for J_{⊥}>J_{⊥c}∼-0.104J, producing another broad specific heat peak for a crossover to a bosonic quantum Coulomb liquid, where the spin correlation contains both photon and quantum spin-ice monopole contributions. With negatively increasing J_{⊥} across J_{⊥c}, a first-order thermal phase transition occurs from the quantum Coulomb liquid to an XY ferromagnet. Relevance to magnetic rare-earth pyrochlore oxides is discussed.

Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb2Ti2O7.

In a class of frustrated magnets known as spin ice, magnetic monopoles emerge as classical defects and interact via the magnetic Coulomb law. With quantum-mechanical interactions, these magnetic charges are carried by fractionalized bosonic quasi-particles, spinons, which can undergo Bose-Einstein condensation through a first-order transition via the Higgs mechanism. Here, we report evidence of a Higgs transition from a magnetic Coulomb liquid to a ferromagnet in single-crystal Yb(2)Ti(2)O(7). Polarized neutron scattering experiments show that the diffuse [111]-rod scattering and pinch-point features, which develop on cooling are suddenly suppressed below T(C)~0.21 K, where magnetic Bragg peaks and a full depolarization of the neutron spins are observed with thermal hysteresis, indicating a first-order ferromagnetic transition. Our results are explained on the basis of a quantum spin-ice model, whose high-temperature phase is effectively described as a magnetic Coulomb liquid, whereas the ground state shows a nearly collinear ferromagnetism with gapped spin excitations.

Quantum melting of spin ice: emergent cooperative quadrupole and chirality.

Quantum melting of spin ice is proposed for pyrochlore-lattice magnets Pr2TM2O7 (TM=Ir, Zr, and Sn). The quantum superexchange Hamiltonian having a nontrivial magnetic anisotropy is derived on the basis of atomic non-Kramers magnetic doublets. The ground states exhibit a cooperative ferroquadrupole and pseudospin chirality, forming a magnetic analog of smectic liquid crystals. Our theory accounts for dynamic spin-ice behaviors experimentally observed in Pr2TM2O7.

Chain of Majorana states from superconducting Dirac fermions at a magnetic domain wall.

We study theoretically a strongly type-II s-wave superconducting state of two-dimensional Dirac fermions in proximity to a ferromagnet having in-plane magnetization. It is shown that a magnetic domain wall can host a chain of equally spaced vortices in the superconducting order parameter, each of which binds a Majorana-fermion state. The overlap integral of neighboring Majorana states is sensitive to the position of the chemical potential of the Dirac fermions. Thermal transport and scanning tunneling microscopy experiments to probe the Majorana fermions are discussed.

Chiral order and electromagnetic dynamics in one-dimensional multiferroic cuprates.

We show by unbiased numerical calculations that the ferromagnetic nearest-neighbor exchange interaction stabilizes a vector spin chiral order against the quantum fluctuation in a frustrated spin-1/2 chain relevant to multiferroic cuprates, LiCu2O2 and LiCuVO4. Our realistic semiclassical analyses for LiCu2O2 resolve controversies on the helical magnetic structure and unveil the pseudo-Nambu-Goldstone modes as the origin of experimentally observed electromagnons.

Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole order.

Spin liquids are magnetically frustrated systems, in which spins are prevented from ordering or freezing, owing to quantum or thermal fluctuations among degenerate states induced by the frustration. Chiral spin liquids are a hypothetical class of spin liquids in which the time-reversal symmetry is macroscopically broken in the absence of an applied magnetic field or any magnetic dipole long-range order. Even though such chiral spin-liquid states were proposed more than two decades ago, an experimental realization and observation of such states has remained a challenge. One of the characteristic order parameters in such systems is a macroscopic average of the scalar spin chirality, a solid angle subtended by three nearby spins. In previous experimental reports, however, the spin chirality was only parasitic to the non-coplanar spin structure associated with a magnetic dipole long-range order or induced by the applied magnetic field, and thus the chiral spin-liquid state has never been found. Here, we report empirical evidence that the time-reversal symmetry can be broken spontaneously on a macroscopic scale in the absence of magnetic dipole long-range order. In particular, we employ the anomalous Hall effect to directly probe the broken time-reversal symmetry for the metallic frustrated magnet Pr(2)Ir(2)O(7). An onset of the Hall effect is observed at zero field in the absence of uniform magnetization, within the experimental accuracy, suggesting an emergence of a chiral spin liquid. The origin of this spontaneous Hall effect is ascribed to chiral spin textures, which are inferred from the magnetic measurements indicating the spin ice-rule formation.

Nematic and chiral order for planar spins on a triangular lattice.

We propose a variant of the antiferromagnetic XY model which includes a biquadratic (J2) as well as the quadratic (J1) interaction on the triangular lattice. The phase diagram for large J2/J1 exhibits a phase with coexisting quasi-long-range nematic, and long-ranged vector spin chirality orders in the absence of magnetic order, which qualifies our model as the first instance of a classical spin model that exhibits a vector chiral spin liquid phase. The interplay of nematic and spin chirality orders is discussed. A variety of critical properties are derived by means of Monte Carlo simulation.

Quantum theory of multiferroic helimagnets: collinear and helical phases.

We study the quantum fluctuation in the cycloidal helical magnet in terms of the Schwinger boson approach. In sharp contrast to the classical fluctuation, the quantum fluctuation is collinear in nature which gives rise to the collinear spin density wave state slightly above the helical cycloidal state as the temperature is lowered. Physical properties such as the reduced elliptic ratio of the spiral, the neutron scattering and infrared absorption spectra are discussed from this viewpoint with the possible relevance to the quasi-one dimensional LiCu2O2 and LiCuVO4.

Chiral spin pairing in helical magnets.

A concept of chiral spin pairing is introduced to describe a vector-chiral liquid-crystal order in frustrated spin systems. It is found that the chiral spin pairing is induced by the coupling to phonons through the Dzyaloshinskii-Moriya interaction and the four-spin exchange interaction of the Coulomb origin under the edge-sharing network of magnetic and ligand ions. This produces two successive second-order phase transitions upon cooling: an O(2) chiral spin nematic, i.e., spin cholesteric, order appears with an either parity, and then the O(2) symmetry is broken to yield a helical magnetic order. Possible candidate materials are also discussed as new multiferroic systems.

Intrinsic versus extrinsic anomalous Hall effect in ferromagnets.

A unified theory of the anomalous Hall effect (AHE) is presented for multiband ferromagnetic metals with dilute impurities. In the clean limit, the AHE is mostly due to extrinsic skew scattering. When the Fermi level is located around anticrossing of band dispersions split by spin-orbit interaction, the intrinsic AHE to be calculated ab initio is resonantly enhanced by its nonperturbative nature, revealing the extrinsic-to-intrinsic crossover which occurs when the relaxation rate is comparable to the spin-orbit coupling.

Disorder-enhanced dielectric response of nanoscale and mesoscopic insulators.

Enhancement of the dielectric response of insulators by disorder is theoretically proposed, where the quantum interference of electronic waves through the nanoscale or mesoscopic system and its change due to external perturbations control the polarization. In the disordered case with all the states being localized, the resonant tunneling, which is topologically protected, plays a crucial role, and enhances the dielectric response by a factor 30-40 compared with the pure case. The realization of this idea with accessible materials or structures is also discussed.

Topological nature of polarization and charge pumping in ferroelectrics.

Electric polarization in insulators is represented by the transferred charge through a shift of the Bloch wave functions induced by an adiabatic change of external parameters Q-->. It is found that this covalent/quantum contribution is determined nonlocally by the topological structure in the Q--> space. The condition for the charge pumping for a cyclic change of Q--> is also obtained. Applications of this picture to various organic ferroelectrics and BaTiO3 are discussed.

Two-dimensional charge order in layered 2-1-4 perovskite oxides.

Monte Carlo simulations are performed on the three-dimensional (3D) Ising model with the 2-1-4 layered perovskite structure as a minimal model for checkerboard charge ordering phenomena in layered perovskite oxides. Because of the interlayer frustration, only 2D long-range order emerges with a finite correlation length along the c axis. Critical exponents of the transition change continuously as a function of the interlayer coupling constant. The interlayer long-range Coulomb interaction decays exponentially and is negligible even between the second-neighbor layers. Instead, monoclinic distortion of a tetragonal unit cell lifts the macroscopic degeneracy to induce a 3D charge ordering. The dimensionality of the charge order in La0.5Sr1.5MnO4 is discussed from this viewpoint.

Spin chirality fluctuations and anomalous Hall effect in itinerant ferromagnets.

The anomalous Hall effect due to the spin chirality order and fluctuation is studied theoretically in a Kondo lattice model without the relativistic spin-orbit interaction. Even without the correlations of the localized spins, sigma(xy) can emerge depending on the lattice structure and the spin anisotropy. We reveal the condition for this chirality-fluctuation driven mechanism for sigma(xy). Our semiquantitative estimates for a pyrochlore oxide Nd2Mo2O7 give a finite sigma(xy) approximately equal 10 Omega(-1) cm(-1) together with a high resistivity rho(xx) approximately equal 10(-4)-10(-3) Omega cm, in agreement with experiments.