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Title: Charge-transfer satellites and chemical bonding in photoemission and x-ray absorption of SrTi O 3 and rutile Ti O 2 : Experiment and first-principles theory with general application to spectroscopic analysis

Abstract

First-principles, real-time-cumulant, and Bethe-Salpeter-equation calculations fully capture the detailed satellite structure that occurs in response to the sudden creation of the core hole in both photoemission and x-ray absorption spectra of the transition-metal compounds SrTi O 3 and rutile Ti O 2 . Analysis of the excited-state, real-space charge-density fluctuations betrays the physical nature of these many electron excitations that are shown to reflect the materials’ solid-state electronic structure and chemical bonding. This first-principles development of the cumulant-based core hole spectral function is generally applicable to other systems and should become a standard tool for all similar spectroscopic analysis going beyond the quasiparticle physics of the photoelectric effect.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1];  [3]; ORCiD logo [3]
  1. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  3. Univ. of Washington, Seattle, WA (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1635472
Report Number(s):
BNL-216083-2020-JAAM
Journal ID: ISSN 2469-9950; PRBMDO
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 101; Journal Issue: 24; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Electronic structure; Ab initio calculations; Density functional calculations; First-principles calculations; X-ray absorption spectroscopy

Citation Formats

Woicik, J. C., Weiland, C., Jaye, C., Fischer, D. A., Rumaiz, A. K., Shirley, E. L., Kas, J. J., and Rehr, J. J.. Charge-transfer satellites and chemical bonding in photoemission and x-ray absorption of SrTiO3 and rutile TiO2: Experiment and first-principles theory with general application to spectroscopic analysis. United States: N. p., 2020. Web. https://doi.org/10.1103/PhysRevB.101.245119.
Woicik, J. C., Weiland, C., Jaye, C., Fischer, D. A., Rumaiz, A. K., Shirley, E. L., Kas, J. J., & Rehr, J. J.. Charge-transfer satellites and chemical bonding in photoemission and x-ray absorption of SrTiO3 and rutile TiO2: Experiment and first-principles theory with general application to spectroscopic analysis. United States. https://doi.org/10.1103/PhysRevB.101.245119
Woicik, J. C., Weiland, C., Jaye, C., Fischer, D. A., Rumaiz, A. K., Shirley, E. L., Kas, J. J., and Rehr, J. J.. Wed . "Charge-transfer satellites and chemical bonding in photoemission and x-ray absorption of SrTiO3 and rutile TiO2: Experiment and first-principles theory with general application to spectroscopic analysis". United States. https://doi.org/10.1103/PhysRevB.101.245119. https://www.osti.gov/servlets/purl/1635472.
@article{osti_1635472,
title = {Charge-transfer satellites and chemical bonding in photoemission and x-ray absorption of SrTiO3 and rutile TiO2: Experiment and first-principles theory with general application to spectroscopic analysis},
author = {Woicik, J. C. and Weiland, C. and Jaye, C. and Fischer, D. A. and Rumaiz, A. K. and Shirley, E. L. and Kas, J. J. and Rehr, J. J.},
abstractNote = {First-principles, real-time-cumulant, and Bethe-Salpeter-equation calculations fully capture the detailed satellite structure that occurs in response to the sudden creation of the core hole in both photoemission and x-ray absorption spectra of the transition-metal compounds SrTiO3 and rutile TiO2. Analysis of the excited-state, real-space charge-density fluctuations betrays the physical nature of these many electron excitations that are shown to reflect the materials’ solid-state electronic structure and chemical bonding. This first-principles development of the cumulant-based core hole spectral function is generally applicable to other systems and should become a standard tool for all similar spectroscopic analysis going beyond the quasiparticle physics of the photoelectric effect.},
doi = {10.1103/PhysRevB.101.245119},
journal = {Physical Review B},
number = 24,
volume = 101,
place = {United States},
year = {2020},
month = {6}
}

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