Electronic reconstruction and charge transfer in strained Sr$_2$CoIrO$_6$ double perovskite

Abstract

The electronic, magnetic and optical properties of the double perovskite Sr$_2$CoIrO$_6$ (SCIO) under biaxial strain are explored in the framework of density functional theory (DFT) including a Hubbard $U$ term and spin-orbit coupling (SOC) in combination with absorption spectroscopy measurements on epitaxial thin films. While the end member SrIrO$_3$ is a semimetal with a quenched spin and orbital moment and bulk SrCoO$_3$ is a ferromagnetic (FM) metal with spin and orbital moment of 2.50 and 0.13 $μ_{B}$, respectively, the double perovskite SCIO emerges as an antiferromagnetic Mott insulator with antiparallel alignment of Co, Ir planes along the [110]-direction. Co exhibits a spin and enhanced orbital moment of $\sim 2.35-2.45$ and $0.31-$0.45 $μ_{B}$, respectively. Most remarkably, Ir acquires a significant spin and orbital moment of 1.21-1.25 and 0.13 $μ_{B}$, respectively. Analysis of the orbital occupation indicates an electronic reconstruction due to a substantial charge transfer from minority to majority spin states in Ir and from Ir to Co, signaling an Ir$^{4+δ}$, Co$^{4-δ}$ configuration. Biaxial strain, varied from -1.02% ($a_{\rm NdGaO_3}$) through 0% ($a_{\rm SrTiO_3}$) to 1.53% ($a_{\rm GdScO_3}$), influences in partcular the orbital polarization of the $t_{2g}$ states and leads to a nonmonotonic change of the band gap between 163 and 235 meV. The absorption coefficient reveals a two plateau fearure due to transitions from the valence to the lower lying narrow $t_{2g}$ and the higher lying broader $e_{g}$ bands. Inclusion of many body effects, in particular, excitonic effects by solving the Bethe-Salpeter equation (BSE), increases the band gap by $\sim0.2$ and improves the agreement with the measured spectrum concerning the position of the second peak at $\sim 2.6$ eV.