Emergent excitation at the magnetic metal-insulator transition in the pyrochlore osmate Cd2Os2O7

Abstract

The rich physics manifested by 5d oxides falls outside the Mott-Hubbard paradigm used to successfully explain the electronic and magnetic properties of 3d oxides. Much consideration has been given to the extent to which strong spin-orbit coupling (SOC), in the limit of increased bandwidth and reduced electron correlation, drives the formation of novel electronic states, as manifested through the existence of metal-insulator transitions (MITs). SOC is believed to play a dominant role in 5d5 systems such as iridates (Ir4+), undergoing MITs which may or may not be intimately connected to magnetic order, with pyrochlore and perovksite systems being examples of the former and latter, respectively. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (e.g Os5+) systems are expected to have an orbital singlet and consequently a reduced effect of SOC in the groundstate. The pyrochlore osmate Cd2Os2O7 nonetheless exhibits a MIT intimately entwined with magnetic order with phenomena similar to pyrochlore iridates. Here we report the first resonant inelastic X-ray scattering (RIXS) measurements on an osmium compound, allowing us to determine the salient electronic and magnetic energy scales controlling the MIT in Cd2Os2O7, which we benchmark against detailed quantum chemistry calculations. In particular, we reveal the emergence at the MIT of a magnetic excitation corresponding to a superposition of multiple spin-flip processes from an Ising-like all-in/all-out magnetic groundstate. We discuss our results with respect to the role of SOC in magnetically mediated MITs in 5d systems