Advanced EXAFS analysis techniques applied to the L-edges of the lanthanide oxides

Smerigan, Adam; Hoffman, Adam S.; Ostervold, Lars; Hong, Jiyun; Perez-Aguillar, Jorge; Caine, Ash C.; Greenlee, Lauren; Bare, Simon R.

doi:10.1107/s1600576724010240

Title: Advanced EXAFS analysis techniques applied to the L-edges of the lanthanide oxides

Journal Article · 21 November 2024 · Journal of Applied Crystallography (Online)

DOI: https://doi.org/10.1107/s1600576724010240 · OSTI ID:2476855

Smerigan, Adam ^[1]; Hoffman, Adam S. ^[2]; Ostervold, Lars ^[1]; Hong, Jiyun ^[2]; Perez-Aguillar, Jorge ^[2]; Caine, Ash C. ^[3]; Greenlee, Lauren ^[1]; Bare, Simon R. ^[2]

Pennsylvania State Univ., University Park, PA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Washington Univ., St. Louis, MO (United States)

The unique properties of the lanthanide (Ln) elements make them critical components of modern technologies, such as lasers, anti-corrosive films and catalysts. Thus, there is significant interest in establishing structure–property relationships for Ln-containing materials to advance these technologies. Extended X-ray absorption fine structure (EXAFS) is an excellent technique for this task considering its ability to determine the average local structure around the Ln atoms for both crystalline and amorphous materials. However, the limited availability of EXAFS reference spectra of the Ln oxides and challenges in the EXAFS analysis have hindered the application of this technique to these elements. The challenges include the limited k-range available for the analysis due to the superposition of L-edges on the EXAFS, multielectron excitations (MEEs) creating erroneous peaks in the EXAFS and the presence of inequivalent absorption sites. Herein, we removed MEEs to model the local atomic environment more accurately for light Ln oxides. Further, we investigated the use of cubic and non-cubic lattice expansion to minimize the fitting parameters needed and connect the fitting parameters to physically meaningful crystal parameters. The cubic expansion reduced the number of fitting parameters but resulted in a statistically worse fit. The non-cubic expansion resulted in a similar quality fit and showed non-isotropic expansion in the crystal lattice of Nd₂O₃. In total, the EXAFS spectra and the fits for the entire set of Ln oxides (excluding promethium) are included. The knowledge developed here can assist in the structural determination of a wide variety of Ln compounds and can further studies on their structure–property relationships.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2476855

Journal Information:: Journal of Applied Crystallography (Online), Journal Name: Journal of Applied Crystallography (Online) Journal Issue: 6 Vol. 57; ISSN 1600-5767

Publisher:: International Union of CrystallographyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
EXAFS
cubic crystal expansion
extended X-ray absorption fine structure
lanthanide oxides
multielectron excitation
non-cubic crystal expansion
rare earth elements

Title: Advanced EXAFS analysis techniques applied to the L-edges of the lanthanide oxides

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