A spin-orbital-entangled quantum liquid on a honeycomb lattice.

The honeycomb lattice is one of the simplest lattice structures. Electrons and spins on this simple lattice, however, often form exotic phases with non-trivial excitations. Massless Dirac fermions can emerge out of itinerant electrons, as demonstrated experimentally in graphene, and a topological quantum spin liquid with exotic quasiparticles can be realized in spin-1/2 magnets, as proposed theoretically in the Kitaev model. The quantum spin liquid is a long-sought exotic state of matter, in which interacting spins remain quantum-disordered without spontaneous symmetry breaking. The Kitaev model describes one example of a quantum spin liquid, and can be solved exactly by introducing two types of Majorana fermion. Realizing a Kitaev model in the laboratory, however, remains a challenge in materials science. Mott insulators with a honeycomb lattice of spin-orbital-entangled pseudospin-1/2 moments have been proposed, including the 5d-electron systems α-Na2IrO3 (ref. 5) and α-Li2IrO3 (ref. 6) and the 4d-electron system α-RuCl3 (ref. 7). However, these candidates were found to magnetically order rather than form a liquid at sufficiently low temperatures, owing to non-Kitaev interactions. Here we report a quantum-liquid state of pseudospin-1/2 moments in the 5d-electron honeycomb compound H3LiIr2O6. This iridate does not display magnetic ordering down to 0.05 kelvin, despite an interaction energy of about 100 kelvin. We observe signatures of low-energy fermionic excitations that originate from a small number of spin defects in the nuclear-magnetic-resonance relaxation and the specific heat. We therefore conclude that H3LiIr2O6 is a quantum spin liquid. This result opens the door to finding exotic quasiparticles in a strongly spin-orbit-coupled 5d-electron transition-metal oxide.

Large spin-wave energy gap in the bilayer iridate Sr3Ir2O7: evidence for enhanced dipolar interactions near the mott metal-insulator transition.

Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ≈92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ≈70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudodipolar interactions that are strongly enhanced near the metal-insulator transition boundary. This suggests that novel magnetism, such as that inspired by the Kitaev model built on the pseudodipolar interactions, may emerge in small charge-gap iridates.

Dimensionality driven spin-flop transition in layered iridates.

Using resonant x-ray diffraction, we observe an easy c-axis collinear antiferromagnetic structure for the bilayer Sr3Ir2O7, a significant contrast to the single layer Sr2IrO4 with in-plane canted moments. Based on a microscopic model Hamiltonian, we show that the observed spin-flop transition as a function of number of IrO2 layers is due to strong competition among intra- and interlayer bond-directional pseudodipolar interactions of the spin-orbit entangled J(eff)=1/2 moments. With this we unravel the origin of anisotropic exchange interactions in a Mott insulator in the strong spin-orbit coupling regime, which holds the key to the various types of unconventional magnetism proposed in 5d transition metal oxides.

Mott insulators in the strong spin-orbit coupling limit: from Heisenberg to a quantum compass and Kitaev models.

We study the magnetic interactions in Mott-Hubbard systems with partially filled t_{2g} levels and with strong spin-orbit coupling. The latter entangles the spin and orbital spaces, and leads to a rich variety of the low energy Hamiltonians that extrapolate from the Heisenberg to a quantum compass model depending on the lattice geometry. This gives way to "engineer" in such Mott insulators an exactly solvable spin model by Kitaev relevant for quantum computation. We, finally, explain "weak" ferromagnetism, with an anomalously large ferromagnetic moment, in Sr2IrO4.

Spin, orbital, and charge order at the interface between correlated oxides.

The collective behavior of correlated electrons in the VO2 interface layer of the LaVO(3)/SrTiO(3) heterostructure is studied within a quarter-filled t(2g)-orbital Hubbard model on a square lattice. We argue that the ground state is ferromagnetic, driven by the double-exchange mechanism, and is orbitally and charge ordered due to a confined geometry and electron correlations. The orbital and charge density waves open gaps on the entire Fermi surfaces of all orbitals. The theory explains the observed insulating behavior of the p-type interface between LaVO3 and SrTiO3.

Classical dimers and dimerized superstructure in an orbitally degenerate honeycomb antiferromagnet.

We discuss the ground state of the spin-orbital model for spin-one ions with partially filled t_{2g} levels on a honeycomb lattice. We find that the orbital degrees of freedom induce a spontaneous dimerization of spins and drive them into nonmagnetic manifold spanned by hard-core dimer (spin-singlet) coverings of the lattice. The cooperative "dimer Jahn-Teller" effect is introduced through a magnetoelastic coupling and is shown to lift the orientational degeneracy of dimers leading to a peculiar valence bond crystal pattern. The present theory provides a theoretical explanation of nonmagnetic dimerized superstructure experimentally seen in Li2RuO3 compound at low temperatures.

Valence-bond crystal in a pyrochlore antiferromagnet with orbital degeneracy.

We discuss the ground state of a pyrochlore lattice of threefold orbitally degenerate S=1/2 magnetic ions. We derive an effective spin-orbital Hamiltonian and show that the orbital degrees of freedom can modulate the spin exchange, removing the infinite spin-degeneracy characteristic of pyrochlore structures. The resulting state is a collection of spin-singlet dimers, with a residual degeneracy due to their relative orientation. This latter is lifted by a magnetoelastic interaction, induced in the spin-singlet phase space, that forces a tetragonal distortion. Such a theory provides an explanation for the helical spin-singlet pattern observed in the B spinel MgTi2O4.