DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Journal of Synchrotron Radiation (Online)
ORCiD logo [1];  [2];  [3];  [1];  [1];  [1]; ORCiD logo [4];  [4]
  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)

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1456895
Report Number(s):
BNL-205779-2018-JAAM; JSYRES; TRN: US1901254
Journal Information:
Journal of Synchrotron Radiation (Online), Vol. 25, Issue 3; ISSN 1600-5775
Publisher:
International Union of CrystallographyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

References (46)

Room-temperature ferroelectricity in strained SrTiO3 journal August 2004
Theory of x-ray absorption and linear dichroism at the Ca L 23 -edge of CaCO 3 journal May 2016
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
Impact of local strain on Ti-L 2,3 electron energy-loss near-edge structures of BaTiO 3 : a first-principles multiplet study journal April 2014
Ferroelectricity: Octahedral Rotation-Induced Ferroelectricity in Cation Ordered Perovskites (Adv. Mater. 15/2012) journal April 2012
Semiconductor Composites: Strategies for Enhancing Charge Carrier Separation to Improve Photocatalytic Activity journal December 2013
Oxide Nanoelectronics on Demand journal February 2009
Resonant inelastic scattering at the L edge of Ti in Barium Strontium Titanate by soft X-ray fluorescence spectroscopy journal August 1997
Emergent phenomena at oxide interfaces journal January 2012
Restricted Open-Shell Configuration Interaction Cluster Calculations of the L-Edge X-ray Absorption Study of TiO 2 and CaF 2 Solids journal May 2014
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface journal January 2004
Superconducting Interfaces Between Insulating Oxides journal August 2007
Switchable Ferroelectric Diode and Photovoltaic Effect in BiFeO 3 journal February 2009
Multiplet calculations of L 2,3 x-ray absorption near-edge structures for 3d transition-metal compounds journal February 2009
Final-State Projection Method in Charge-Transfer Multiplet Calculations: An Analysis of Ti L-Edge Absorption Spectra journal April 2015
Band alignment of epitaxial SrTiO3 thin films with (LaAlO3)0.3-(Sr2AlTaO6)0.7 (001) journal September 2015
L 2,3 edge photoabsorption spectra of bulk V 2 O 5 : A two components relativistic time dependent density functional theory description with finite cluster model journal December 2012
Efficient implementation of core-excitation Bethe–Salpeter equation calculations journal December 2015
Strain Tuning of Ferroelectric Thin Films journal August 2007
Probing ferroelectricity in PbZr 0.2 Ti 0.8 O 3 with polarized soft x rays journal October 2010
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
Multichannel multiple scattering calculation of L 2 , 3 -edge spectra of TiO 2 and SrTiO 3 : Importance of multiplet coupling and band structure journal March 2010
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
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
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
Ferroelectric distortion in SrTiO 3 thin films on Si ( 001 ) by x-ray absorption fine structure spectroscopy: Experiment and first-principles calculations journal April 2007
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
Structural, electronic, and magnetic properties of Sr Ru O 3 under epitaxial strain journal September 2006
Asymmetric orbital-lattice interactions in ultra-thin correlated oxide films text January 2010
Bethe-Salpeter Equation Calculations of Core Excitation Spectra text January 2010
Multiplet ligand-field theory using Wannier orbitals text January 2011
Efficient implementation of core-excitation Bethe Salpeter equation calculations text January 2016
Physics of thin-film ferroelectric oxides text January 2005
Structural, electronic and magnetic properties of SrRuO$_3$ under epitaxial strain text January 2006

Figures / Tables (6)