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Title: Experimental assignment of many-electron excitations in the photoionization of NiO

Abstract

The absorption of a photon and the emission of an electron is not a simple, two-particle process. The complicated many-electron features observed during core photoionization can therefore reveal many of the hidden secrets about the ground and excited-state electronic structures of a material. Careful analysis of the photon-energy dependence of the Ni KLL Auger deexcitation spectra at and above the Ni 1s photoionization threshold has identified the satellite structure that appears in both the photoelectron emission and the x-ray absorption spectra of NiO as Ni metal 3d e g → Ni metal 3d e g and O ligand 2p e g → Ni metal 3d e g charge-transfer excitations, respectively. These assignments clarify the conflicting theoretical predictions of the last five decades in addition to other anomalous effects in the spectroscopy of this unique material.

Authors:
 [1];  [2];  [1];  [3];  [1];  [4];  [4]
  1. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Materials Measurement Science Division and Material Measurement Lab.
  2. Synchrotron SOLEIL, Saint-Aubin (France)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Sciences Directorate
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Contributing Org.:
[Synchrotron SOLEIL, Saint-Aubin (France)]
OSTI Identifier:
1464105
Alternate Identifier(s):
OSTI ID: 1457212
Report Number(s):
[BNL-207955-2018-JAAM]
[Journal ID: ISSN 2469-9950; PRBMDO; TRN: US1902360]
Grant/Contract Number:  
[SC0012704; 20170393; 10122]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
[ Journal Volume: 97; Journal Issue: 24]; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 74 ATOMIC AND MOLECULAR PHYSICS; electronic structure; auger electron spectroscopy; photoemission spectroscopy; x-ray absorption spectroscopy; photoexcitation

Citation Formats

Woicik, J. C., Ablett, J. M., Quackenbush, N. F., Rumaiz, A. K., Weiland, C., Droubay, T. C., and Chambers, S. A. Experimental assignment of many-electron excitations in the photoionization of NiO. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.245142.
Woicik, J. C., Ablett, J. M., Quackenbush, N. F., Rumaiz, A. K., Weiland, C., Droubay, T. C., & Chambers, S. A. Experimental assignment of many-electron excitations in the photoionization of NiO. United States. doi:10.1103/PhysRevB.97.245142.
Woicik, J. C., Ablett, J. M., Quackenbush, N. F., Rumaiz, A. K., Weiland, C., Droubay, T. C., and Chambers, S. A. Tue . "Experimental assignment of many-electron excitations in the photoionization of NiO". United States. doi:10.1103/PhysRevB.97.245142. https://www.osti.gov/servlets/purl/1464105.
@article{osti_1464105,
title = {Experimental assignment of many-electron excitations in the photoionization of NiO},
author = {Woicik, J. C. and Ablett, J. M. and Quackenbush, N. F. and Rumaiz, A. K. and Weiland, C. and Droubay, T. C. and Chambers, S. A.},
abstractNote = {The absorption of a photon and the emission of an electron is not a simple, two-particle process. The complicated many-electron features observed during core photoionization can therefore reveal many of the hidden secrets about the ground and excited-state electronic structures of a material. Careful analysis of the photon-energy dependence of the Ni KLL Auger deexcitation spectra at and above the Ni 1s photoionization threshold has identified the satellite structure that appears in both the photoelectron emission and the x-ray absorption spectra of NiO as Ni metal 3d eg → Ni metal 3d eg and O ligand 2p eg → Ni metal 3d eg charge-transfer excitations, respectively. These assignments clarify the conflicting theoretical predictions of the last five decades in addition to other anomalous effects in the spectroscopy of this unique material.},
doi = {10.1103/PhysRevB.97.245142},
journal = {Physical Review B},
number = [24],
volume = [97],
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

FIG. 1. FIG. 1.: Ni 1s, 2p, and 3d (valence) photoelectron spectra of NiO. The photon energies were = 10000 eV for the Ni 1s level and = 2570 eV for the Ni 2p and 3d levels, respectively. Also shown is a fit to the data points of the Nimore » 1s spectrum. The spectra have been aligned relative to their maximum intensity.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.