Resonant inelastic x-ray scattering in layered trimer iridate Ba4Ir3 O10 : the density functional approach

TL;DR

This study uses density functional theory to analyze the electronic structure and RIXS spectra of layered iridate Ba4Ir3O10, revealing the interplay of dimerization and Mott insulating behavior.

Contribution

It provides a detailed theoretical investigation of the electronic and RIXS spectra of Ba4Ir3O10, highlighting the combined effects of dimerization and strong correlations in its insulating state.

Findings

Bonding-antibonding splitting stabilizes antibonding states.

Energy gap arises from both dimerization and Mott physics.

Calculated RIXS spectra agree with experimental data.

Abstract

We have investigated the electronic structure of Ba4Ir3O10 within the density-functional theory (DFT) using the generalized gradient approximation while considering strong Coulomb correlations (GGA+U) in the framework of the fully relativistic spin-polarized Dirac linear muffin-tin orbital band-structure method. Ba4Ir3O10 has a quasi-2D structure composed of buckled sheets, which constitute corner-connected Ir3O12 trimers containing three distorted face-sharing IrO6 octahedra. The Ir atoms are distributed over two symmetrically inequivalent sites: the center of the trimer (Ir1) and its two tips (Ir2). The Ir1 - Ir2 distance within the trimer is quite small and equals to 2.58 A at low temperature. As a result, the clear formation of bonding and antibonding states at the Ir1 site occurs. The large bonding-antibonding splitting stabilizes the dyz-orbital-dominant antibonding state of t2g holes and produces a wide energy gap at the Fermi level. However, the energy gap opens up only with taking into account strong Coulomb correlations at the Ir2 site. Therefore, we have quite a unique situation when the insulating state is driven by both the dimerization at the Ir1 site and Mott insulating behavior at the Ir2 one. We have investigated resonant inelastic x-ray scattering (RIXS) spectra at the Ir L3 edge. The calculated results are in good agreement with experimental data. The RIXS spectrum possesses several sharp features below 2.1 eV corresponding to transitions within the Ir t2g levels. The excitation located from 2.1 to 4.6 eV is due to t2g to eg and O2p to t2g transitions. The wide structure situated at 6.2-12 eV appears due to charge transfer and O2p to eg transitions. We have also presented comprehensive theoretical calculations of the RIXS spectrum at the oxygen K edge.