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Title: Investigation of the multiplet features of SrTiO3 in X-ray absorption spectra based on configuration interaction calculations

Abstract

Synchrotron-based L2,3-edge absorption spectra show strong sensitivities to the local electronic structure and chemical environment. However, detailed physical information cannot be extracted easily without computational aids. Here in this study using the experimental Ti L2,3-edges absorption spectrum of SrTiO3as a fingerprint and considering full multiplet effects, calculations yield different energy parameters characterizing local ground state properties. The peak splitting and intensity ratios of the L3 and L2 set of peaks are carefully analyzed quantitatively, giving rise to a small hybridization energy around 1.2 eV, and the different hybridization energy values reported in the literature are further addressed. Finally, absorption spectra with different linearly polarized photons under various tetragonal crystal fields are investigated, revealing a non-linear orbital–lattice interaction, and a theoretical guidance for material engineering of SrTiO3-based thin films and heterostructures is offered. Finally, detailed analysis of spectrum shifts with different tetragonal crystal fields suggests that the eg crystal field splitting is a necessary parameter for a thorough analysis of the spectra, even though it is not relevant for the ground state properties.

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [1];  [1]; ORCiD logo [4];  [4]
+ Show Author Affiliations
  1. Xiamen University (China). Fujian Provincial Key Laboratory of Semiconductors and Applications, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Department of Physics
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Chinese Academy of Sciences (CAS), Beijing (China). Beijing Synchrotron Radiation Facility, Institute of High Energy Physics
  4. Xiamen University (China). Fujian Provincial Key Laboratory of Semiconductors and Applications, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Department of Physics; Xiamen University Malaysia, Selangor (Malaysia)
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:
1456895
Report Number(s):
BNL-205779-2018-JAAM
Journal ID: ISSN 1600-5775; JSYRES; TRN: US1901254
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Synchrotron Radiation (Online)
Additional Journal Information:
Journal Name: Journal of Synchrotron Radiation (Online); Journal Volume: 25; Journal Issue: 3; Journal ID: ISSN 1600-5775
Publisher:
International Union of Crystallography
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; X ray absorbance spectra; soft X‐ray absorption; configuration interaction cluster calculation; 3 d transition metal oxide; crystal field effect

Citation Formats

Wu, M., Xin, Houlin L., Wang, J. O., Li, X. J., Yuan, X. B., Zeng, H., Zheng, J. -C., and Wang, H. -Q. Investigation of the multiplet features of SrTiO3 in X-ray absorption spectra based on configuration interaction calculations. United States: N. p., 2018. Web. doi:10.1107/S160057751800423X.
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Wu, M., Xin, Houlin L., Wang, J. O., Li, X. J., Yuan, X. B., Zeng, H., Zheng, J. -C., & Wang, H. -Q. Investigation of the multiplet features of SrTiO3 in X-ray absorption spectra based on configuration interaction calculations. United States. https://doi.org/10.1107/S160057751800423X
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Wu, M., Xin, Houlin L., Wang, J. O., Li, X. J., Yuan, X. B., Zeng, H., Zheng, J. -C., and Wang, H. -Q. Tue . "Investigation of the multiplet features of SrTiO3 in X-ray absorption spectra based on configuration interaction calculations". United States. https://doi.org/10.1107/S160057751800423X. https://www.osti.gov/servlets/purl/1456895.
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@article{osti_1456895,
title = {Investigation of the multiplet features of SrTiO3 in X-ray absorption spectra based on configuration interaction calculations},
author = {Wu, M. and Xin, Houlin L. and Wang, J. O. and Li, X. J. and Yuan, X. B. and Zeng, H. and Zheng, J. -C. and Wang, H. -Q.},
abstractNote = {Synchrotron-based L2,3-edge absorption spectra show strong sensitivities to the local electronic structure and chemical environment. However, detailed physical information cannot be extracted easily without computational aids. Here in this study using the experimental Ti L2,3-edges absorption spectrum of SrTiO3as a fingerprint and considering full multiplet effects, calculations yield different energy parameters characterizing local ground state properties. The peak splitting and intensity ratios of the L3 and L2 set of peaks are carefully analyzed quantitatively, giving rise to a small hybridization energy around 1.2 eV, and the different hybridization energy values reported in the literature are further addressed. Finally, absorption spectra with different linearly polarized photons under various tetragonal crystal fields are investigated, revealing a non-linear orbital–lattice interaction, and a theoretical guidance for material engineering of SrTiO3-based thin films and heterostructures is offered. Finally, detailed analysis of spectrum shifts with different tetragonal crystal fields suggests that the eg crystal field splitting is a necessary parameter for a thorough analysis of the spectra, even though it is not relevant for the ground state properties.},
doi = {10.1107/S160057751800423X},
journal = {Journal of Synchrotron Radiation (Online)},
number = 3,
volume = 25,
place = {United States},
year = {2018},
month = {4}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1107/S160057751800423X
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Figures / Tables:

Figure 1 Figure 1: Comparison between the experimental x-ray absorption spectrum for a STO single crystal (miscut angle <0.05, purchased from Crystec) and the calculated spectrum of STO (bottom line).
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Probing ferroelectricity in PbZr 0.2 Ti 0.8 O 3 with polarized soft x rays
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Electronic structure of early 3 d -transition-metal oxides by analysis of the 2 p core-level photoemission spectra
journal, January 1996

Time-dependent density functional theory applied to x-ray absorption spectroscopy
journal, April 2012

Asymmetric Orbital-Lattice Interactions in Ultrathin Correlated Oxide Films
journal, September 2011

Physics of thin-film ferroelectric oxides
journal, October 2005

L 2 , 3 x-ray-absorption edges of d 0 compounds: K + , Ca 2 + , Sc 3 + , and Ti 4 + in O h (octahedral) symmetry
journal, January 1990

Multiplet ligand-field theory using Wannier orbitals
journal, April 2012

Satellite structure in photoelectron and Auger spectra of copper dihalides
journal, May 1981

Comparison of x-ray absorption with x-ray photoemission of nickel dihalides and NiO
journal, March 1986

Understanding the L 2 , 3 x-ray absorption spectra of early 3 d transition elements
journal, November 2010

Split-Off State Formation in the Final State of Photoemission in Ti Compounds
journal, August 1994

  • Okada, Kozo; Uozumi, Takayuki; Kotani, Akio
  • Journal of the Physical Society of Japan, Vol. 63, Issue 8
  • DOI: 10.1143/JPSJ.63.3176

A non-empirical calculation of 2p core-electron excitation in compounds with 3d transition metal ions using ligand-field and density functional theory (LFDFT)
journal, January 2017

  • Ramanantoanina, Harry; Daul, Claude
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 31
  • DOI: 10.1039/C7CP03140H

Structural effects on the spin-state transition in epitaxially strained LaCoO 3 films
journal, February 2009

Simplified LCAO Method for the Periodic Potential Problem
journal, June 1954

Resonant 3 d , 3 p and 3 s Photoemission in Transition Metal Oxides Predicted at 2 p Threshold
journal, July 1994

  • Tanaka, Arata; Jo, Takeo
  • Journal of the Physical Society of Japan, Vol. 63, Issue 7
  • DOI: 10.1143/JPSJ.63.2788

Spectroscopic mapping of local structural distortions in ferroelectric PbTiO 3 /SrTiO 3 superlattices at the unit-cell scale
journal, December 2011

Bethe-Salpeter equation calculations of core excitation spectra
journal, March 2011

Strain and composition dependence of orbital polarization in nickel oxide superlattices
journal, September 2013

Investigation of the multiplet structures and crystal field effects of a TiO 6 3 d 1 cluster based on configuration interaction calculations
journal, March 2017

  • Wu, Meng; Zheng, Jin-Cheng; Wang, Hui-Qiong
  • Journal of Applied Crystallography, Vol. 50, Issue 2
  • DOI: 10.1107/S160057671700334X

Structural, electronic, and magnetic properties of Sr Ru O 3 under epitaxial strain
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Multiplet ligand-field theory using Wannier orbitals
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Efficient implementation of core-excitation Bethe Salpeter equation calculations
text, January 2016

Physics of thin-film ferroelectric oxides
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