2016, Calder, S., Vale, J.G., Bogdanov, N.A., Liu, X., Donnerer, C., Upton, M.H., Casa, D., Said, A.H., Lumsden, M.D., Zhao, Z., Yan, J.-Q., Mandrus, D., Nishimoto, S., van den Brink, J., Hill, J.P., McMorrow, D.F., Christianson, A.D.

Much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d5 iridates (Ir4þ), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (Os5þ) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.

2018, Clancy, J.P., Gretarsson, H., Sears, J.A., Singh, Y., Desgreniers, S., Mehlawat, K., Layek, S., Rozenberg, G.K., Ding, Y., Upton, M.H., Casa, D., Chen, N., Im, J., Lee, Y., Yadav, R., Hozoi, L., Efremov, D., Van Den Brink, J., Kim, Y.-J.

Honeycomb-lattice quantum magnets with strong spin-orbit coupling are promising candidates for realizing a Kitaev quantum spin liquid. Although iridate materials such as Li2IrO3 and Na2IrO3 have been extensively investigated in this context, there is still considerable debate as to whether a localized relativistic wavefunction (J eff = 1/2) provides a suitable description for the electronic ground state of these materials. To address this question, we have studied the evolution of the structural and electronic properties of α-Li2IrO3 as a function of applied hydrostatic pressure using a combination of X-ray diffraction and X-ray spectroscopy techniques. We observe striking changes even under the application of only small hydrostatic pressure (P ≤ 0.1 GPa): A distortion of the Ir honeycomb lattice (via X-ray diffraction), a dramatic decrease in the strength of spin-orbit coupling effects (via X-ray absorption spectroscopy), and a significant increase in non-cubic crystal electric field splitting (via resonant inelastic X-ray scattering). Our data indicate that α-Li2IrO3 is best described by a J eff = 1/2 state at ambient pressure, but demonstrate that this state is extremely fragile and collapses under the influence of applied pressure.