Irradiation-induced amorphization of UO2 films prepared by spraying-assisted combustion synthesis

Stefania Dede; Khachatur V. Manukyan; Jordan M. Roach; Ashabari Majumdar; Peter C. Burns; Ani Aprahamian

doi:10.1016/j.apsusc.2022.154437

Irradiation-induced amorphization of UO₂ films prepared by spraying-assisted combustion synthesis

Stefania Dede
, Khachatur V. Manukyan
, Jordan M. Roach
, Ashabari Majumdar
, Peter C. Burns
, Ani Aprahamian

Research output: Contribution to journal › Article › peer-review

6 Scopus citations

Abstract

Spraying-assisted combustion synthesis with uranyl nitrate − acetylacetone − 2-methoxyethanol solutions was used to prepare UO₂ films on an aluminum alloy substrate. The tuning of the spraying parameters and annealing temperatures allowed the preparation of UO₂ films with thicknesses varying from 10–300 nm and 5–10 nm UO₂ grain size. High-resolution electron microscopy and X-ray photoelectron spectroscopy showed that increasing the annealing temperature promotes Mg diffusion from the substrate into the films. The incorporation of Mg reduced the overall crystallinity of the films. The irradiation with Ar²⁺ ions (1.7 MeV energy and a fluence of 2 × 10¹⁶ ions/cm²) did not degrade the quality of the films. However, the Mg content significantly influenced the irradiation-induced restructuring of the UO₂ films. Irradiated films with low or no Mg content exhibit high crystallinity, and the UO₂/Al interfacial layer becomes highly porous. Films with higher Mg content are mostly amorphized after irradiation. The origin of irradiation-induced amorphization was related to the formation of Mg_yU_1-yO_2±x solid solutions. Chemically complex, pore-free, and amorphous Mg-Al-O film/substrate interfacial layers enable continuous Mg diffusion during irradiation. Furthermore, the gradual increase in Mg amounts triggers irradiation-induced precipitation of a crystalline MgO-rich phase within the amorphous films.

Original language	English
Article number	154437
Journal	Applied Surface Science
Volume	603
DOIs	https://doi.org/10.1016/j.apsusc.2022.154437
State	Published - Nov 30 2022
Externally published	Yes

Funding

The work was performed with financial support in part from the U.S. Department of Energy's (DOE) National Nuclear Security Administration (NNSA, Grant # DE-NA0003888 ), U.S. National Science Foundation (NSF, PHY-2011890 ), and JINA-CEE NSF Physics Frontiers Centers (Award #1430152). A.A. acknowledges support from the Fulbright U.S. Scholar grant. K.M. also acknowledges funding from the U.S. Army Research Office Grant # W911NF2110045 under the Materials Synthesis & Processing Program, with Dr. Michael P. Bakas as the program manager. The authors also acknowledge Notre Dame Center for Environmental Science & Technology (CEST), Materials Characterization Facility (MCF), and Integrated Imaging Facility (NDIIF) for instrumental usage. The work was performed with financial support in part from the U.S. Department of Energy's (DOE) National Nuclear Security Administration (NNSA, Grant # DE-NA0003888), U.S. National Science Foundation (NSF, PHY-2011890), and JINA-CEE NSF Physics Frontiers Centers (Award #1430152). A.A. acknowledges support from the Fulbright U.S. Scholar grant. K.M. also acknowledges funding from the U.S. Army Research Office Grant # W911NF2110045 under the Materials Synthesis & Processing Program, with Dr. Michael P. Bakas as the program manager. The authors also acknowledge Notre Dame Center for Environmental Science & Technology (CEST), Materials Characterization Facility (MCF), and Integrated Imaging Facility (NDIIF) for instrumental usage.

Keywords

Amorphization
Ion irradiation
Solution combustion synthesis
UO thin films

Access to Document

10.1016/j.apsusc.2022.154437

Cite this

@article{e8aa341483534fe5a9d40c9731c717e5,

title = "Irradiation-induced amorphization of UO2 films prepared by spraying-assisted combustion synthesis",

abstract = "Spraying-assisted combustion synthesis with uranyl nitrate − acetylacetone − 2-methoxyethanol solutions was used to prepare UO2 films on an aluminum alloy substrate. The tuning of the spraying parameters and annealing temperatures allowed the preparation of UO2 films with thicknesses varying from 10–300 nm and 5–10 nm UO2 grain size. High-resolution electron microscopy and X-ray photoelectron spectroscopy showed that increasing the annealing temperature promotes Mg diffusion from the substrate into the films. The incorporation of Mg reduced the overall crystallinity of the films. The irradiation with Ar2+ ions (1.7 MeV energy and a fluence of 2 × 1016 ions/cm2) did not degrade the quality of the films. However, the Mg content significantly influenced the irradiation-induced restructuring of the UO2 films. Irradiated films with low or no Mg content exhibit high crystallinity, and the UO2/Al interfacial layer becomes highly porous. Films with higher Mg content are mostly amorphized after irradiation. The origin of irradiation-induced amorphization was related to the formation of MgyU1-yO2±x solid solutions. Chemically complex, pore-free, and amorphous Mg-Al-O film/substrate interfacial layers enable continuous Mg diffusion during irradiation. Furthermore, the gradual increase in Mg amounts triggers irradiation-induced precipitation of a crystalline MgO-rich phase within the amorphous films.",

keywords = "Amorphization, Ion irradiation, Solution combustion synthesis, UO thin films",

author = "Stefania Dede and Manukyan, \{Khachatur V.\} and Roach, \{Jordan M.\} and Ashabari Majumdar and Burns, \{Peter C.\} and Ani Aprahamian",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2022",

month = nov,

day = "30",

doi = "10.1016/j.apsusc.2022.154437",

language = "English",

volume = "603",

journal = "Applied Surface Science",

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T1 - Irradiation-induced amorphization of UO2 films prepared by spraying-assisted combustion synthesis

AU - Dede, Stefania

AU - Manukyan, Khachatur V.

AU - Roach, Jordan M.

AU - Majumdar, Ashabari

AU - Burns, Peter C.

AU - Aprahamian, Ani

PY - 2022/11/30

Y1 - 2022/11/30

N2 - Spraying-assisted combustion synthesis with uranyl nitrate − acetylacetone − 2-methoxyethanol solutions was used to prepare UO2 films on an aluminum alloy substrate. The tuning of the spraying parameters and annealing temperatures allowed the preparation of UO2 films with thicknesses varying from 10–300 nm and 5–10 nm UO2 grain size. High-resolution electron microscopy and X-ray photoelectron spectroscopy showed that increasing the annealing temperature promotes Mg diffusion from the substrate into the films. The incorporation of Mg reduced the overall crystallinity of the films. The irradiation with Ar2+ ions (1.7 MeV energy and a fluence of 2 × 1016 ions/cm2) did not degrade the quality of the films. However, the Mg content significantly influenced the irradiation-induced restructuring of the UO2 films. Irradiated films with low or no Mg content exhibit high crystallinity, and the UO2/Al interfacial layer becomes highly porous. Films with higher Mg content are mostly amorphized after irradiation. The origin of irradiation-induced amorphization was related to the formation of MgyU1-yO2±x solid solutions. Chemically complex, pore-free, and amorphous Mg-Al-O film/substrate interfacial layers enable continuous Mg diffusion during irradiation. Furthermore, the gradual increase in Mg amounts triggers irradiation-induced precipitation of a crystalline MgO-rich phase within the amorphous films.

AB - Spraying-assisted combustion synthesis with uranyl nitrate − acetylacetone − 2-methoxyethanol solutions was used to prepare UO2 films on an aluminum alloy substrate. The tuning of the spraying parameters and annealing temperatures allowed the preparation of UO2 films with thicknesses varying from 10–300 nm and 5–10 nm UO2 grain size. High-resolution electron microscopy and X-ray photoelectron spectroscopy showed that increasing the annealing temperature promotes Mg diffusion from the substrate into the films. The incorporation of Mg reduced the overall crystallinity of the films. The irradiation with Ar2+ ions (1.7 MeV energy and a fluence of 2 × 1016 ions/cm2) did not degrade the quality of the films. However, the Mg content significantly influenced the irradiation-induced restructuring of the UO2 films. Irradiated films with low or no Mg content exhibit high crystallinity, and the UO2/Al interfacial layer becomes highly porous. Films with higher Mg content are mostly amorphized after irradiation. The origin of irradiation-induced amorphization was related to the formation of MgyU1-yO2±x solid solutions. Chemically complex, pore-free, and amorphous Mg-Al-O film/substrate interfacial layers enable continuous Mg diffusion during irradiation. Furthermore, the gradual increase in Mg amounts triggers irradiation-induced precipitation of a crystalline MgO-rich phase within the amorphous films.

KW - Amorphization

KW - Ion irradiation

KW - Solution combustion synthesis

KW - UO thin films

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