jp511931y_si_001.pdf (1.48 MB)
Probing LaMO3 Metal and Oxygen Partial Density of States Using X‑ray Emission, Absorption, and Photoelectron Spectroscopy
journal contribution
posted on 2015-01-29, 00:00 authored by Wesley T. Hong, Kelsey A. Stoerzinger, Brian Moritz, Thomas P. Devereaux, Wanli Yang, Yang Shao-HornWe examined the electronic structure
in LaMO3 perovskite
oxides (M = Cr, Mn, Fe, Co, Ni) by combining information from X-ray
emission, absorption, and photoelectron spectroscopy. Through first-principles
density functional theory simulations, we identified complementary
hybridization features present in the transition metal and oxygen
X-ray emission spectra. We then developed a method for the self-consistent
alignment of the emission data onto a common energy scale using these
features, providing a valuable supplementary technique to photoelectron
spectroscopy for studying the partial density of states in perovskites.
The combined information from X-ray emission and absorption was used
to explore trends in electronic structure characteristics under the
Zaanen–Sawatzky–Allen frameworknamely the extent
of metal–oxygen hybridization, band gap, and charge-transfer
gap. We further established a method that allows for the experimental
determination of the occupied and unoccupied band positions relative
to the oxide Fermi level, as well as on an absolute energy scale.