Abstract
Phase purity, morphology, and defect structures on plutonium oxide surfaces likely influence reactivity of plutonium, and high quality PuO2 crystalline substrates are needed to probe the effects of these properties on a model plutonium oxide surface. Indeed, different thin film thicknesses are required for conducting the range of state-of-the-art measurements available for studying these surfaces. In this Article, modification of a polymer-assisted deposition method is employed to grow various film thicknesses of PuO2 on yttria stabilized zirconia (YSZ) substrates, and measurements are carried out to characterize these films. Phase purity and epitaxial qualities of the films are assessed using thin film X-ray diffraction analysis, and the first Grazing Incidence Extended X-ray Absorption Fine Structure measurements carried out on a PuO2 thin film are reported, providing information about the short-range order of the lattice structure. Elemental purity is measured via X-ray photoelectron spectroscopy. Thicknesses and densities of the films are evaluated using neutron reflectivity, revealing that phase-pure PuO2 thin films of high epitaxial quality are formed. Micro-Raman spectroscopy suggests development of structural agglomerates of PuO2 on the surfaces, likely resulting from defects in the lattice match between the PuO2 film and the YSZ substrate.
| Original language | English |
|---|---|
| Article number | 121696 |
| Journal | Surface Science |
| Volume | 701 |
| DOIs | |
| State | Published - Nov 2020 |
| Externally published | Yes |
Funding
This work was supported by the U.S. Department of Homeland Security, Domestic Nuclear Detection Office [competitively awarded contract/IAA HSHQDC-15-X-B0003]; Independent Research and Development program from the National Science Foundation (J. Majewski). The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security or the Government. The content is solely the responsibility of the authors and does not necessarily represent the official view of the National Science Foundation. All X-ray absorption data were collected at the Stanford Synchrotron Radiation Lightsource. Use of the Stanford Synchrotron Radiation Lightsource, SSRL, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02–76SF00515. Los Alamos National Laboratory is managed by Triad National Security, LLC, for the National Nuclear Security Administration for the U.S. Department of Energy (Contract DE-SOL-801206). LA-UR-19–24139. This work was supported by the U.S. Department of Homeland Security , Domestic Nuclear Detection Office [competitively awarded contract/IAA HSHQDC-15-X-B0003]; Independent Research and Development program from the National Science Foundation (J. Majewski). The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security or the Government. The content is solely the responsibility of the authors and does not necessarily represent the official view of the National Science Foundation. All X-ray absorption data were collected at the Stanford Synchrotron Radiation Lightsource. Use of the Stanford Synchrotron Radiation Lightsource, SSRL, is supported by the U.S. Department of Energy , Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02–76SF00515. Los Alamos National Laboratory is managed by Triad National Security, LLC, for the National Nuclear Security Administration for the U.S. Department of Energy (Contract DE-SOL-801206 ). LA-UR-19–24139.
Keywords
- Grazing incidence X-ray absorption spectroscopy
- X-ray photoelectron spectroscopy
- microscopy
- neutron reflectivity
- plutonium oxide thin film
- thin film X-ray diffraction analysis