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Register a new userSpin-orbit effects in pentavalent Iridates: Models and materials
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Spin-orbit effects in heavy 5$d$ transition metal oxides, in particular, iridates, have received enormous current interest due to the prediction as well as the realization of a plethora of exotic and unconventional magnetic properties. While a bulk of these works are based on tetravalent iridates ($d^5$), where the counter-intuitive insulating state of the rather extended 5$d$ orbitals are explained by invoking strong spin-orbit coupling, the recent quest in iridate research has shifted to the other valencies of Ir, of which pentavalent iridates constitute a notable representative. In contrast to the tetravalent iridates, spin-orbit entangled electrons in $d^4$ systems are expected to be confined to the $J = 0$ singlet state without any resultant moment or magnetic response. However, it has been recently predicted that, magnetism in $d^4$ systems may occur via magnetic condensation of excitations across spin-orbit-coupled states. In reality, the magnetism in Ir$^{5+}$ systems are often quite debatable both from theoretical as well as experimental point of view. Here we provide a comprehensive overview of the spin-orbit coupled $d^4$ model systems and its implications in the studied pentavalent iridates. In particular, we review here the current experimental and theoretical understanding of the double perovskite ($A_2B$YIrO$_6$, $A =$ Sr, Ba, $B =$Y, Sc, Gd), 6H-perovskite (Ba$_3M$Ir$_2$O$_9$, $M =$ Zn, Mg, Sr, Ca), post-perovskite (NaIrO$_3$), and Hexagonal (Sr$_3$MIrO$_6$) iridates, along with a number of open questions that require future investigation.
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Motivated by RIXS experiments on a wide range of complex heavy oxides, including rhenates, osmates, and iridates, we discuss the theory of RIXS for site-localized $t_{2g}$ orbital systems with strong spin-orbit coupling. For such systems, we present exact diagonalization results for the spectrum at different electron fillings, showing that it accesses single-particle and multi-particle excitations. This leads to a simple picture for the energies and intensities of the RIXS spectra in Mott insulators such as double perovskites which feature highly localized electrons, and yields estimates of the spin-orbit coupling and Hunds coupling in correlated $5d$ oxides. We present new higher resolution RIXS data at the Re-L$_3$ edge in Ba$_2$YReO$_6$ which finds a previously unresolved peak splitting, providing further confirmation of our theoretical predictions. Using ab initio electronic structure calculations on Ba$_2$${cal M}$ReO$_6$ (with ${cal M}$=Re, Os, Ir) we show that while the atomic limit yields a reasonable effective Hamiltonian description of the experimental observations, effects such as $t_{2g}$-$e_g$ interactions and hybridization with oxygen are important. Our ab initio estimate for the strength of the intersite exchange coupling shows that, compared to the osmates, the exchange is one or two orders of magnitude weaker in the rhenates and iridates, which may partly explain the suppression of long-range magnetic order in the latter compounds. As a way to interpolate between the site-localized picture and our electronic structure band calculations, we discuss the spin-orbital levels of the ${cal M}$O$_6$ cluster. This suggests a possible role for non-dispersive intra-cluster excitons in Ba$_2$YIrO$_6$ which may lead to a weak breakdown of the atomic $J_{rm eff}=0$ picture and to small magnetic moments.
In the search for topological phases in correlated electron systems, iridium-based pyrochlores A2Ir2O7 -- materials with 5d transition-metal ions -- provide fertile grounds. Several novel topological states have been predicted but the actual realization of such states is believed to critically depend on the strength of local potentials arising from distortions of IrO6-cages. We test this hypothesis by measuring with resonant x-ray scattering the electronic level splittings in the A= Y, Eu systems, which we show to agree very well with ab initio electronic structure calculations. We find, however, that not distortions of IrO6-octahedra are the primary source for quenching the spin-orbit interaction, but strong long-range lattice anisotropies, which inevitably break the local cubic symmetry and will thereby be decisive in determining the systems topological ground state.
Novel phases of two dimensional electron systems resulting from new surface or interface modified electronic structures have generated significant interest in material science. We utilize photoemission spectroscopy to show that the near-surface electronic structure of a bulk insulating iridate Sr$_3$Ir$_2$O$_7$ lying near metal-Mott insulator transition exhibit weak metallicity signified by finite electronic spectral weight at the Fermi level. The surface electrons exhibit a unique spin structure resulting from an interplay of spin-orbit, Coulomb interaction and surface quantum magnetism, distinct from a topological insulator state. Our results suggest the experimental realization of a novel quasi two dimensional interacting electron surface ground state, opening the door for exotic quantum entanglement and transport phenomena in iridate-based oxide devices.
Spin-orbit coupling in magnetic systems lacking inversion symmetry can give rise to non trivial spin textures. Magnetic thin films and heterostructures are potential candidates for the formation of skyrmions and other non-collinear spin configurations as inversion symmetry is inherently lost at their surfaces and interfaces. However, manganites, in spite of their extraordinarily rich magnetic phase diagram, have not yet been considered of interest within this context as their spin-orbit coupling is assumed to be negligible. We demonstrate here, by means of angular dependent X-ray linear dichroism experiments and theoretical calculations, the existence of a noncollinear antiferromagnetic ordering at the surface of ferromagnetic La$_{2/3}$Sr$_{1/3}$MnO$_3$ thin films whose properties can only be explained by an unexpectedly large enhancement of the spin-orbit interaction. Our results reveal that spin-orbit coupling, usually assumed to be very small on manganites, can be significantly enhanced at surfaces and interfaces adding a new twist to the possible magnetic orders that can arise in electronically reconstructed systems.
We study spin-orbit coupling in metallic carbon nanotubes (CNTs) within the many-body Tomonaga-Luttinger liquid (TLL) framework. For a well defined sub-class of metallic CNTs, that contains both achiral zig-zag as well as a sub-set of chiral tubes, an effective low energy field theory description is derived. We aim to describe system at finite dopings, but close to the charge neutrality point (commensurability). A new regime is identified where spin-orbit coupling leads to an inverted hierarchy of mini-gaps of bosonic modes. We then add a proximity coupling to a superconducting (SC) substrate and show that the only order parameter that is supported within the novel, spin-orbit induced phase is a topologically trivial s-SC.
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