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

Wu, M.; Xin, Houlin L.; Wang, J. O.; Li, X. J.; Yuan, X. B.; Zeng, H.; Zheng, J. -C.; Wang, H. -Q.

doi:10.1107/S160057751800423X

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

Journal Article · 23 April 2018 · Journal of Synchrotron Radiation (Online)

DOI: https://doi.org/10.1107/S160057751800423X · OSTI ID:1456895

^[1]; Xin, Houlin L. ^[2]; Wang, J. O. ^[3]; Li, X. J. ^[1]; Yuan, X. B. ^[1]; Zeng, H. ^[1];

^[4]; Wang, H. -Q. ^[4]

Xiamen University (China). Fujian Provincial Key Laboratory of Semiconductors and Applications, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Department of Physics
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Chinese Academy of Sciences (CAS), Beijing (China). Beijing Synchrotron Radiation Facility, Institute of High Energy Physics
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)

Synchrotron-based L_2,3-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 L_2,3-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 e_g 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1456895

Report Number(s):: BNL-205779-2018-JAAM

Journal Information:: Journal of Synchrotron Radiation (Online), Journal Name: Journal of Synchrotron Radiation (Online) Journal Issue: 3 Vol. 25; ISSN 1600-5775; ISSN JSYRES

Publisher:: International Union of CrystallographyCopyright Statement

Country of Publication:: United States

Language:: English

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

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