Abstract
Raman spectroscopy is an emerging technique for rapid and nondestructive analysis of nuclear materials for forensic and nonproliferation applications as it is a powerful tool for distinguishing multiple chemical forms of materials with similar stoichiometries. Recent developments in spectroscopic software have enabled rapid data collection with high-speed Raman spectroscopic mapping capabilities. However, some uranium-rich materials are susceptible to degradation in humid air and/or laser-induced phase transformations. To mitigate environmental or measurement-related sample degradation of potential samples of interest, we have taken a systematic approach to define optimized data collection parameters for high-throughput measurements of uranyl fluoride (UO2F2), which is an important intermediate material in the nuclear fuel cycle. First, we systematically describe the influence of optical magnification (5× to 100×), laser power, and exposure time on obtained signal for identical particles of UO2F2 and find that at low laser power and exposure times, comparable signal is obtained regardless of optical magnification. Second, we ensure sample integrity during data collection, and third, collect spectroscopic maps that employ optimized parameters to reduce the time required to obtain spatially resolved spectroscopic information. Reductions of 90% and 99% in measurement times are discussed as they relate to differences in resolving spectroscopic features of particles in identical mapping areas. During this work, we found that additional data processing options were needed and thus developed a customized Python script for importing, processing, analyzing, and visualizing Raman spectroscopic map data.
| Original language | English |
|---|---|
| Pages (from-to) | 815-824 |
| Number of pages | 10 |
| Journal | Applied Spectroscopy |
| Volume | 78 |
| Issue number | 8 |
| DOIs | |
| State | Published - Aug 2024 |
Funding
The authors thank J. J. Quinn, Dusty Summers, and Keith Gilbert for their support. This paper was improved by helpful comments and revisions from Luke Sadergaski, Michael Lance, and an anonymous reviewer. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this paper or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). The authors disclosed receipt of the following financial support for the research, authorship, and/or publication of this article: This research was funded by the Laboratory Directed Research and Development Program at Oak Ridge National Laboratory.
Keywords
- Raman spectroscopic mapping
- UOF
- high-speed mapping
- nuclear materials analysis
- uranyl fluoride