Probing LaMO3 Metal and Oxygen Partial Density of States Using X-ray Emission, Absorption, and Photoelectron Spectroscopy

Hong, Wesley T.; Stoerzinger, Kelsey A.; Moritz, Brian; Devereaux, Thomas P.; Yang, Wanli; Shao-Horn, Yang

doi:10.1021/jp511931y

Title: Probing LaMO₃ Metal and Oxygen Partial Density of States Using X-ray Emission, Absorption, and Photoelectron Spectroscopy

Journal Article · Wed Jan 21 00:00:00 EST 2015 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/jp511931y· OSTI ID:1374901

Hong, Wesley T.; Stoerzinger, Kelsey A.; Moritz, Brian ^[1]; Devereaux, Thomas P. ^[2]; Yang, Wanli ^[3]; Shao-Horn, Yang

Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States, Department of Physics and Astrophysics, University of North Dakota, Grand Forks, North Dakota 58202, United States
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States
Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

We 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 framework—namely 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.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; SC0002633; AC02-05CH11231

OSTI ID:: 1374901

Alternate ID(s):: OSTI ID: 1557990

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Vol. 119 Journal Issue: 4; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 52 works

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