Irradiation-Driven Restructuring of UO2 Thin Films: Amorphization and Crystallization

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

doi:10.1021/acsami.1c08682

Irradiation-Driven Restructuring of UO₂ Thin Films: Amorphization and Crystallization

Journal Article · Fri Jul 16 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c08682· OSTI ID:1820113

Majumdar, Ashabari ^[1]; ^[2]; Dede, Stefania ^[3]; Roach, Jordan M. ^[2]; Robertson, Daniel ^[2]; ^[2]; Aprahamian, Ani ^[4]

Univ. of Notre Dame, IN (United States); University of Notre Dame
Univ. of Notre Dame, IN (United States)
Univ. of Notre Dame, IN (United States); Texas A & M Univ., College Station, TX (United States)
Univ. of Notre Dame, IN (United States); A. Alikhanyan National Science Lab. of Armenia, Yerevan (Armenia)

Combustion synthesis in uranyl nitrate–acetylacetone–2-methoxyethanol solutions was used to deposit thin UO₂ films on aluminum substrates to investigate the irradiation-induced restructuring processes. Thermal analysis revealed that the combustion reactions in these solutions are initiated at ~160 °C. The heat released during the process and the subsequent brief annealing at 400 °C allow the deposition of polycrystalline films with 5–10 nm UO₂ grains. The use of multiple deposition cycles enables tuning of the film thicknesses in the 35–260 nm range. Irradiation with Ar²⁺ ions (1.7 MeV energy and a fluence of up to 1 × 10¹⁷ ions/cm²) is utilized to generate a uniform distribution of atomic displacements within the films. X-ray fluorescence (XRF) and alpha-particle emission spectroscopy showed that the films were stable under irradiation and did not undergo sputtering degradation. X-ray photoelectron spectroscopy (XPS) showed that the stoichiometry and uranium ionic concentrations remain stable during irradiation. The high-resolution electron microscopy imaging and electron diffraction analysis demonstrated that at the early stages of irradiation (below 1 × 10¹⁶ ion/cm²) UO₂ films show complete amorphization and beam-induced densification (sintering), resulting in a pore-free disordered film. Prolonged irradiation (5 × 10¹⁶ ion/cm²) is shown to trigger a crystallization process at the surface of the films that moves toward the UO₂/Al interface, converting the entire amorphous material into a highly crystalline film. This work reports on an entirely different radiation-induced restructuring of the nanoscale UO₂ compared to the coarse-grained counterpart. The preparation of thin UO₂ films deposited on Al substrates fills an area of national need within the stockpile stewardship program of the National Nuclear Security Administration and fundamental research with actinides. Here, the method reported in this work produces pure, robust, and uniform thin-film actinide targets for nuclear science measurements

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Research Organization:: Univ. of Notre Dame, IN (United States)

Sponsoring Organization:: U.S. Army Research Office; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003888

OSTI ID:: 1820113

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 29 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Irradiation-Driven Restructuring of UO2 Thin Films: Amorphization and Crystallization

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