A new spin-anisotropic harmonic honeycomb iridate

The physics of Mott insulators underlies diverse phenomena ranging from high temperature superconductivity to exotic magnetism. Although both the electron spin and the structure of the local orbitals play a key role in this physics, in most systems these are connected only indirectly --- via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) open a further dimension to this problem by introducing strong spin-orbit interactions, such that the Mott physics has a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic interactions, coupling the spin orientation to a given spatial direction of exchange and leading to strongly frustrated magnetism. The potential for new physics emerging from such interactions has driven much scientific excitement, most recently in the search for a new quantum spin liquid, first discussed by Kitaev \cite{kitaev_anyons_2006}. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb, but in a three-dimensional framework. The temperature dependence of the magnetic susceptibility exhibits a striking reordering of the magnetic anisotropy, giving evidence for highly spin-anisotropic exchange interactions. Furthermore, the basic structural units of this material suggest the possibility of a new family of structures, the `harmonic honeycomb' iridates. This compound thus provides a unique and exciting glimpse into the physics of a new class of strongly spin-orbit coupled Mott insulators.Comment: 12 pages including bibliography, 5 figure

Quantum magnets with strong spin-orbit interaction probed via neutron and x-ray scattering

This thesis presents details of x-ray and neutron scattering experiments used to probe quantum magnets with strong spin-orbit interaction. The first of these systems are the three-dimensional iridate compounds, in which the three-fold co-ordination of IrO6 octahedra has been theoretically hypothesized to stabilize anisotropic exchange between Ir4+ ions. This novel interaction between these spin-orbital entangled, Jeff=1/2 moments is described by a Hamiltonian first proposed by Kitaev, and would be the first physical realization of this Hamiltonian in a condensed matter system. This thesis details the determination of the structure of a new polytype within these compounds, the 'stripyhoneycomb' γ-Li2IrO3. Furthermore, through resonant magnetic x-ray diffraction experiments on single crystals of β-Li2IrO3 and γ-Li2IrO3, an incommensurate, non-coplanar structure with counter-rotating moments is found. The counter-rotating moment structure is a rather counter-intuitive result, as it is not stabilizied by Heisenberg exchange between magnetic sites, however, the Kitaev exchange naturally accounts for this feature. As such, these experiments reveal, for the first time, systems which exhibit dominant Kitaev interactions. The ordering wavevector of both β- and γ-Li2IrO3 polytypes are found to be identical, suggesting that the same magnetic interactions are responsible for stabilizing magnetic order in both materials, despite their different lattice topologies. Following this, the spinel FeSc2S4 is considered. Here, despite the presence of strong exchange between Fe2+,/sup>, and the fact that these ions sit in a Jahn-Teller active environment, the system does not order in the spin or orbital degrees of freedom. A 'spin-orbital singlet' has been theoretically proposed to describe the groundstate of this system, and here inelastic neutron scattering (INS) is used to probe the resulting triplon excitations. This allows determination of microscopic parameters in the single ion and exchange Hamiltonians, and moreover experiments in external magnetic field reveal the true spin-and-orbital nature of these triplon excitations. Finally, Ba3CoSb2O9, a physical realization of the canonical triangular antiferromagnet model is explored with INS and the high energy excitations from the 120 degree magnetic structure are found to display significant differences from those calculated by linear spin wave theory, suggesting the presence of quantum dynamics not captured in the 1/S linear spin wave expansion

Quantum magnets with strong spin-orbit interaction probed via neutron and x-ray scattering

This thesis presents details of x-ray and neutron scattering experiments used to probe quantum magnets with strong spin-orbit interaction. The first of these systems are the three-dimensional iridate compounds, in which the three-fold co-ordination of IrO6 octahedra has been theoretically hypothesized to stabilize anisotropic exchange between Ir4+ ions. This novel interaction between these spin-orbital entangled, Jeff=1/2 moments is described by a Hamiltonian first proposed by Kitaev, and would be the first physical realization of this Hamiltonian in a condensed matter system. This thesis details the determination of the structure of a new polytype within these compounds, the 'stripyhoneycomb' γ-Li2IrO3. Furthermore, through resonant magnetic x-ray diffraction experiments on single crystals of β-Li2IrO3 and γ-Li2IrO3, an incommensurate, non-coplanar structure with counter-rotating moments is found. The counter-rotating moment structure is a rather counter-intuitive result, as it is not stabilizied by Heisenberg exchange between magnetic sites, however, the Kitaev exchange naturally accounts for this feature. As such, these experiments reveal, for the first time, systems which exhibit dominant Kitaev interactions. The ordering wavevector of both β- and γ-Li2IrO3 polytypes are found to be identical, suggesting that the same magnetic interactions are responsible for stabilizing magnetic order in both materials, despite their different lattice topologies. Following this, the spinel FeSc2S4 is considered. Here, despite the presence of strong exchange between Fe2+,/sup&gt;, and the fact that these ions sit in a Jahn-Teller active environment, the system does not order in the spin or orbital degrees of freedom. A 'spin-orbital singlet' has been theoretically proposed to describe the groundstate of this system, and here inelastic neutron scattering (INS) is used to probe the resulting triplon excitations. This allows determination of microscopic parameters in the single ion and exchange Hamiltonians, and moreover experiments in external magnetic field reveal the true spin-and-orbital nature of these triplon excitations. Finally, Ba3CoSb2O9, a physical realization of the canonical triangular antiferromagnet model is explored with INS and the high energy excitations from the 120 degree magnetic structure are found to display significant differences from those calculated by linear spin wave theory, suggesting the presence of quantum dynamics not captured in the 1/S linear spin wave expansion.</p

Quantum magnets with strong spin-orbit interaction probed via neutron and x-ray scattering

This thesis presents details of x-ray and neutron scattering experiments used to probe quantum magnets with strong spin-orbit interaction. The first of these systems are the three-dimensional iridate compounds, in which the three-fold co-ordination of IrO6 octahedra has been theoretically hypothesized to stabilize anisotropic exchange between Ir4+ ions. This novel interaction between these spin-orbital entangled, Jeff=1/2 moments is described by a Hamiltonian first proposed by Kitaev, and would be the first physical realization of this Hamiltonian in a condensed matter system. This thesis details the determination of the structure of a new polytype within these compounds, the 'stripyhoneycomb' &gamma;-Li2IrO3. Furthermore, through resonant magnetic x-ray diffraction experiments on single crystals of &beta;-Li2IrO3 and &gamma;-Li2IrO3, an incommensurate, non-coplanar structure with counter-rotating moments is found. The counter-rotating moment structure is a rather counter-intuitive result, as it is not stabilizied by Heisenberg exchange between magnetic sites, however, the Kitaev exchange naturally accounts for this feature. As such, these experiments reveal, for the first time, systems which exhibit dominant Kitaev interactions. The ordering wavevector of both &beta;- and &gamma;-Li2IrO3 polytypes are found to be identical, suggesting that the same magnetic interactions are responsible for stabilizing magnetic order in both materials, despite their different lattice topologies. Following this, the spinel FeSc2S4 is considered. Here, despite the presence of strong exchange between Fe2+,/sup>, and the fact that these ions sit in a Jahn-Teller active environment, the system does not order in the spin or orbital degrees of freedom. A 'spin-orbital singlet' has been theoretically proposed to describe the groundstate of this system, and here inelastic neutron scattering (INS) is used to probe the resulting triplon excitations. This allows determination of microscopic parameters in the single ion and exchange Hamiltonians, and moreover experiments in external magnetic field reveal the true spin-and-orbital nature of these triplon excitations. Finally, Ba3CoSb2O9, a physical realization of the canonical triangular antiferromagnet model is explored with INS and the high energy excitations from the 120 degree magnetic structure are found to display significant differences from those calculated by linear spin wave theory, suggesting the presence of quantum dynamics not captured in the 1/S linear spin wave expansion.This thesis is not currently available in OR

Magnetic field dependence of excitations near spin-orbital quantum criticality: Data archive

The spinel FeSc2S4 has been proposed to realize a near-critical spin-orbital singlet (SOS) state, where entangled spin and orbital moments fluctuate in a global singlet state on the verge of spin and orbital order. Here we report powder inelastic neutron scattering measurements that observe the full bandwidth of magnetic excitations and we find that spin-orbital triplon excitations of an SOS state can capture well key aspects of the spectrum in both zero and applied magnetic fields up to 8.5 T. The observed shift of low-energy spectral weight to higher energies upon increasing applied field is naturally explained by the entangled spin-orbital character of the magnetic states, a behaviour that is in strong contrast to spin-only singlet ground state systems, where the spin gap decreases upon increasing applied field. The deposited package contains x-ray and neutron powder diffraction, susceptibility and inelastic neutron scattering data to characterize the crystal structure and magnetic dynamics in applied field in the spinel material FeSc2S

Magnetic field dependence of excitations near spin-orbital quantum criticality: Data archive

The spinel FeSc2S4 has been proposed to realize a near-critical spin-orbital singlet (SOS) state, where entangled spin and orbital moments fluctuate in a global singlet state on the verge of spin and orbital order. Here we report powder inelastic neutron scattering measurements that observe the full bandwidth of magnetic excitations and we find that spin-orbital triplon excitations of an SOS state can capture well key aspects of the spectrum in both zero and applied magnetic fields up to 8.5 T. The observed shift of low-energy spectral weight to higher energies upon increasing applied field is naturally explained by the entangled spin-orbital character of the magnetic states, a behaviour that is in strong contrast to spin-only singlet ground state systems, where the spin gap decreases upon increasing applied field

Realization of a three-dimensional spin-anisotropic harmonic honeycomb iridate.

Spin and orbital quantum numbers play a key role in the physics of Mott insulators, but in most systems they are connected only indirectly--via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) introduce strong spin-orbit coupling directly, such that these numbers become entwined together and the Mott physics attains a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic magnetic interactions, coupling the spin to a given spatial direction of exchange and leading to strongly frustrated magnetism. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb and exhibits striking evidence for highly spin-anisotropic exchange. The basic structural units of this material suggest that a new family of three-dimensional structures could exist, the 'harmonic honeycomb' iridates, of which the present compound is the first example