Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition

Enriquez, Erik; Wang, Gaoxue; Sharma, Yogesh; Sarpkaya, Ibrahim; Wang, Qiang; Chen, Di; Winner, Nicholas; Guo, Xiaofeng; Dunwoody, John; White, Joshua; Nelson, Andrew; Xu, Hongwu; Dowden, Paul; Batista, Enrique; Htoon, Han; Yang, Ping; Jia, Quanxi; Chen, Aiping

doi:10.1021/acsami.0c08635

Structural and Optical Properties of Phase-Pure UO₂, α-U₃O₈, and α-UO₃ Epitaxial Thin Films Grown by Pulsed Laser Deposition

Journal Article · Wed Jul 15 00:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c08635· OSTI ID:1726212

Enriquez, Erik ^[1]; ^[2]; ^[1]; ^[1]; Wang, Qiang ^[3]; ^[4]; Winner, Nicholas ^[1]; ^[5]; Dunwoody, John ^[2]; ^[2]; ^[2]; ^[2]; Dowden, Paul ^[1]; ^[2]; ^[1]; ^[2]; ^[6]; ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
West Virginia Univ., Morgantown, WV (United States)
Univ. of Houston, TX (United States)
Washington State Univ., Pullman, WA (United States)
Univ. at Buffalo, NY (United States)

Fundamental understanding of the electronic, chemical, and structural properties of uranium oxides requires the synthesis of high-crystalline-quality epitaxial films of different polymorphs of one material or different phases with various oxygen valence states. Here we report the growth of single-phase epitaxial UO₂, α-U₃O₈, and α-UO₃ thin films using pulsed laser deposition. Both oxygen partial pressure and substrate temperature play critical roles in determining the crystal structure of the uranium oxide films. X-ray diffraction and Raman spectroscopy demonstrate that the films are single phase with excellent crystallinity and epitaxially grown on a variety of substrates. Chemical valance states and optical properties of epitaxial uranium oxide films are studied by X-ray photoelectron spectroscopy and UV–vis spectroscopy, which further confirm the high-quality stoichiometric phase-pure uranium oxide thin films. Epitaxial UO2 films show a direct band gap of 2.61 eV, while epitaxial α-UO₂, α-U₃O₈ and α-UO₃ films exhibit indirect band gaps of 1.89 and 2.26 eV, respectively. The ability to grow high-quality epitaxy actinide oxide thin films and to access their different phases and polymorphous will have significant benefits to the future applications in nuclear science and technology.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1726212

Report Number(s):: LA-UR--20-24149

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 31 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
epitaxial stabilization
optical properties
thin films
uranium oxides

Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition

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Structural and Optical Properties of Phase-Pure UO₂, α-U₃O₈, and α-UO₃ Epitaxial Thin Films Grown by Pulsed Laser Deposition