Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition
Abstract
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.
- Authors:
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[4];
[5];
[2];
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- 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)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1726212
- Report Number(s):
- LA-UR-20-24149
Journal ID: ISSN 1944-8244
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 31; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; epitaxial stabilization; uranium oxides; thin films; optical properties
Citation Formats
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, and Chen, Aiping. Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition. United States: N. p., 2020.
Web. doi:10.1021/acsami.0c08635.
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. Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition. United States. https://doi.org/10.1021/acsami.0c08635
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, and Chen, Aiping. Wed .
"Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition". United States. https://doi.org/10.1021/acsami.0c08635. https://www.osti.gov/servlets/purl/1726212.
@article{osti_1726212,
title = {Structural and Optical Properties of Phase-Pure UO2, α-U3O8, and α-UO3 Epitaxial Thin Films Grown by Pulsed Laser Deposition},
author = {Enriquez, Erik and Wang, Gaoxue and Sharma, Yogesh and Sarpkaya, Ibrahim and Wang, Qiang and Chen, Di and Winner, Nicholas and Guo, Xiaofeng and Dunwoody, John and White, Joshua and Nelson, Andrew and Xu, Hongwu and Dowden, Paul and Batista, Enrique and Htoon, Han and Yang, Ping and Jia, Quanxi and Chen, Aiping},
abstractNote = {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.},
doi = {10.1021/acsami.0c08635},
journal = {ACS Applied Materials and Interfaces},
number = 31,
volume = 12,
place = {United States},
year = {Wed Jul 15 00:00:00 EDT 2020},
month = {Wed Jul 15 00:00:00 EDT 2020}
}
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