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Cannon, Bret D.

Publications and source records attributed to Cannon, Bret D..

16 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Fixed-Angle Reflectance from Uranium Compounds and U-Bearing Minerals: Experimental Challenges to Determine the Optical Constants n and k

Fixed-angle reflectance spectroscopy using a commercial Fourier transform infrared (FTIR) spectrometer was employed to derive the optical constants n and k of several uranium compounds. This technique relies upon measurement of the quantitative reflectance R(?) spectra from a polished surface across a broad spectral range (in this case, the mid- and far-IR covering ca. 7500 to 50 cm-1) followed by application of the Kramers-Kronig transformation (KKT). Near-normal fixed-angle measurements as used in this technique require continuous reflectance spectra to as low a wavenumber value as possible. Here, we discuss some of the many challenges in measuring the far-IR and very far-IR (terahertz) spectra using an interferometric instrument, particularly those stemming from small sample sizes, typically just millimeters on a face for crystalline samples, as well as limitations due to optical components and diffraction. We apply this method to single-crystal UO2 and its mineralogical form uraninite, as well as other U-bearing minerals such as autunite [Ca(UO2)2(PO4)2·8-12H2O] and the dehydrated form of autunite, meta-autunite. In addition to the specular reflectance spectra, x-ray diffractometry was used as a confirmatory technique to analyze the surface composition of the species. Deriving the infrared optical constants for such U-bearing species (as well as other solids) will enable nondestructive detection under a variety of environmental and compositional conditions.

Uranium Minerals, infrared spectroscopy, optical c↗
DOE OSTI2018

LASER-BASED MEASUREMENT TOOLS FOR FUTURE ENRICHMENT PLANT SAFEGUARDS

The International Atomic Energy Agency (IAEA) has a long history of testing and using laser-based technologies for a variety of safeguards applications. Notable laser-based on-site applications include: 3-dimensional laser range (3DLR) instruments, used for facility design information and verification (DIV); laser measurements to verify unique labels and detect signs of tampering; and laser spectroscopy, for non-contact process monitoring. The IAEA is also evaluating analytical laboratory instruments, such as laser-ablation inductively-coupled plasma mass spectrometry (LA-ICP-MS) for interrogating individual particles to determine uranium isotopic ratios in collected environment samples. Recent laser technology advancements will likely continue to fuel future IAEA adoption of new and novel laser-based safeguards tools. The Pacific Northwest National Laboratory (PNNL) is currently developing one such tool, called laser ablation, absorption ratio spectrometry (LAARS), for quantitative measurements of uranium material. LAARS uses three tunable diode lasers to simultaneously measure atomic 235U and 238U absorption in an ablation plume created by a fourth pulsed laser. Commercial availability of compact pulsed ablation lasers and the extreme wavelength accuracy and stability of PNNL’s tunable diode laser architecture play a pivotal role in achieving high fidelity LAARS assay measurements. The LAARS method is ultimately targeted for either on-site or laboratory-based 235U relative abundance measurements of destructive assay (DA) samples in support of uranium enrichment plant safeguards. DA samples are currently collected on-site, and then shipped to an analytical laboratory for mass spectrometric assay, because the measurement uncertainty requirements for this application are quite challenging. This paper will present the key elements of the LAARS laser system design, recent assay results on collected uranium hexafluoride (UF6) DA samples, and future operational configurations that may provide immediate on-site DA inspection results or rapid laboratory DA sample screening to prioritize further analysis by mass spectrometry.

IAEA, Safeguards, Uranium Enrichment Plants↗
DOE OSTI2018

Laser Ablation, Absorbance Ratio Spectrometry (LAARS) Assay Performance Study (FY2018 Annual Report)

The International Atomic Energy Agency (IAEA) has a long history of testing and using laser-based technologies for a variety of safeguards applications. Notable laser-based on-site applications include: 3-dimensional laser range (3DLR) instruments, used for facility design information and verification (DIV); laser measurements to verify unique labels and detect signs of tampering; and laser spectroscopy, for non-contact process monitoring. The IAEA is also evaluating analytical laboratory instruments, such as laser-ablation inductively-coupled plasma mass spectrometry (LA-ICP-MS) for interrogating individual particles to determine uranium isotopic ratios in collected environment samples. Recent laser technology advancements will continue to fuel future IAEA adoption of new and novel laser-based safeguards tools. Pacific Northwest National Laboratory (PNNL) is developing one such tool, called the Laser Ablation, Absorbance Ratio Spectrometry (LAARS) technology, which is designed to provide high-fidelity 235 U/ 238 U isotope ratio measurements to support either on-site enrichment plant or off-site laboratory destructive assay (DA). Analyzing uranium hexafluoride (UF 6 ) DA samples on-site by LAARS could provide early indication of discrepancies with operator declarations during physical inventory verifications, so that such discrepancies could be addressed immediately, rather than after off-site analysis is completed. The IAEA is also seeking on-site DA options, because sample shipping time can be long and evolving restrictions on radioactive/corrosive material shipments may increasingly limit the IAEA’s ability to easily transport UF 6 samples. Routine on-site LAARS analysis could provide timely assay results and reduce the DA sample shipment inventory to just those needed for more definitive determination. A laboratory-based LAARS instrument could also provide rapid, cost-effective prescreening of selected DA samples shipped to the IAEA’s Nuclear Materials Laboratory in Seibersdorf, Austria. PNNL has also developed a complementary UF 6 sampling technology and method, called the Single-Use Destructive Assay (SUDA) sampler to easily collect DA samples that are ideal for on-site analysis by LAARS. Combining the LAARS and SUDA sampler technologies could provide a powerful new on-site DA option for the IAEA.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2018

Optical and Chemical Characterization of Uranium Dioxide (UO 2 ) and Uraninite Mineral: Calculation of the Fundamental Optical Constants

Quantitative infrared single-angle reflectance spectroscopic measurements using a calibrated Fourier transform infrared spectrometer were performed on synthetic uranium dioxide (UO2), high-purity crystalline uraninite, and massive uraninite mineral. The massive uraninite mineral was found to contain not only UO2 but also large amounts of calcite and silicates. From the experimentally measured reflectance spectra across two spectral domains (the far- and mid-infrared) the fundamental optical constants n and k were calculated using the Kramers-Kronig transformation for each species. We discuss both the derived n and k results for these species as well as the careful sample preparation needed in order to mount, polish, and measure such samples through a wide spectral range using modern instrumentation and data processing techniques. Our results for the optical constants n and k of synthetic UO2 differ significantly from previously published literature values. This is attributed to both improved spectroscopic resolution but also to a better understanding of potential surface oxidation effects on the measured reflectance values, and hence the calculated optical constants.

DeVetter, Brent M.↗
DOE OSTI2017

Gamma irradiation of Fabry–Perot interband cascade lasers

Two Fabry-Perot interband cascade lasers (ICLs) were exposed to Cobalt-60 gamma rays for a dosage of 500 krad(Si) each, which is higher than is typically encountered in space applications. The ICLs do not show any significant changes in threshold current or slope efficiency, suggesting the suitability of ICLs for use in radiation environments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Shock wave mediated plume chemistry for molecular formation in laser ablation plasmas

Laser ablation is used in a variety of applications albeit formation mechanisms of molecules and nanoclusters are not well understood. We investigated the formation mechanisms of AlO molecules during complex interactions between an Al laser plume expanding into ambient air at atmospheric pressure levels. To produce the plasma a high-purity Al target was ablated using 1064 nm, 6 ns laser pulses. Our results show that the plasma chemistry leading to the formation of AlO is mediated by shock waves. During the early times of plasma expansion, the generated shock waves at the plume edges act as a barrier for the combustion process and the molecular formation is prevalent after the shockwave collapse. The temporally and spatially resolved contour mapping of Al and AlO highlight the formation routes and persistence of species in the plasma and its relation to plume hydrodynamics.

2D fast imaging↗
DOE OSTI2015

Three Dimensional Speckle Imaging Employing a Frequency-Locked Tunable Diode Laser

We describe a high accuracy frequency stepping method for a tunable diode laser to improve a three dimensional (3D) imaging approach based upon interferometric speckle imaging. The approach, modeled after Takeda, exploits tuning an illumination laser in frequency as speckle interferograms of the object (specklegrams) are acquired at each frequency in a Michelson interferometer. The resulting 3D hypercube of specklegrams encode spatial information in the x-y plane of each image with laser tuning arrayed along its z-axis. We present laboratory data of before and after results showing enhanced 3D imaging resulting from precise laser frequency control.

hree dimensional imaging↗
DOE OSTI2015

Annual Report for the QCL Calibration Project

Under the Quantum Cascade Laser (QCL) Calibrations project, Pacific Northwest National Laboratory (PNNL) is collaborating with Utah State University and Space Dynamics Laboratory to design, build, and test a QCL calibration source system suitable for insertion into remote sensing platforms. In FY14, the second year of this project, PNNL completed the radiation testing of QCLs using radiation levels that are typical for a space environment. These tests involved both 64-MeV protons, and 1.17-MeV and 1.33-MeV gamma rays. No changes were observed above the measurement uncertainty indicating that QCLs are viable sources for space-based missions. High-level testing was also carried out with gamma rays to determine if QCLs are sensitive to high doses of gamma radiation. After an accumulated dose of 1.5 Mrad(Si), the QCLs continue to demonstrate high performance although a small increase in threshold current, 0.11 ± 0.14% and 0.51 ± 0.15% for M1244D and M664M, respectively, was observed. At this stage, it is unclear if this small increase is from the radiation exposure, because generally it is within the observed experimental uncertainty, which is most likely because of mechanical changes through repeated mounting cycles. There was also some accidental damage to the laser chips and their front facets from the extensive but necessary handling of the devices during these tests. Regardless, the QCLs are robust and should not be susceptible to degradation for most missions.

36 MATERIALS SCIENCE↗
DOE OSTI2014

A Laser-Based Method for On-Site Analysis of UF6 at Enrichment Plants

The International Atomic Energy Agency’s (IAEA’s) long-term research and development plan calls for more cost-effective and efficient safeguard methods to detect and deter misuse of gaseous centrifuge enrichment plants (GCEPs). The IAEA’s current safeguards approaches at GCEPs are based on a combination of routine and random inspections that include environmental sampling and destructive assay (DA) sample collection from UF6 in-process material and selected cylinders. Samples are then shipped offsite for subsequent laboratory analysis. In this paper, a new DA sample collection and onsite analysis approach that could help to meet challenges in transportation and chain of custody for UF6 DA samples is introduced. This approach uses a handheld sampler concept and a Laser Ablation, Laser Absorbance Spectrometry (LAARS) analysis instrument, both currently under development at the Pacific Northwest National Laboratory. A LAARS analysis instrument could be temporarily or permanently deployed in the IAEA control room of the facility, in the IAEA data acquisition cabinet, for example. The handheld PNNL DA sampler design collects and stabilizes a much smaller DA sample mass compared to current sampling methods. The significantly lower uranium mass reduces the sample radioactivity and the stabilization approach diminishes the risk of uranium and hydrogen fluoride release. These attributes enable safe sample handling needed during onsite LAARS assay and may help ease shipping challenges for samples to be processed at the IAEA’s offsite laboratory. The LAARS and DA sampler implementation concepts will be described and preliminary technical viability results presented.

LAARS↗
DOE OSTI2014

Adsorptive Films in Support of In-field UF6 Destructive Assay Sample Collection and Analysis

International Atom Energy Agency (IAEA) safeguard verification measures in gaseous centrifuge enrichment plants (GCEPs) rely on environmental sampling, non-destructive assay (NDA), and destructive assay (DA) sampling and analysis to determine uranium enrichment. UF6 bias defect measurements are made by DA sampling and analysis to assure that enrichment is consistent with declarations. DA samples are collected from a limited number of cylinders for high precision, offsite mass spectrometer analysis. Samples are typically drawn from a sampling tap into a UF6 sample bottle, then packaged, sealed, and shipped under IAEA chain of custody to an offsite analytical laboratory. Future DA safeguard measures may require improvements in efficiency and effectiveness as GCEP capacities increase and UF6 shipping regulations become increasingly more restrictive. The Pacific Northwest National Laboratory (PNNL) DA sampler concept and Laser Ablation Absorption Ratio Spectrometry (LAARS) assay method are under development to potentially provide DA safeguard tools that increase inspection effectiveness and reduce sample shipping constraints. The PNNL DA sampler concept uses a handheld sampler to collect DA samples for either onsite LAARS assay or offsite laboratory analysis. The DA sampler design will use a small sampling planchet that is coated with an adsorptive film to collect controlled quantities of UF6 gas directly from a cylinder or process sampling tap. Development efforts are currently underway at PNNL to enhance LAARS assay performance to allow high-precision onsite bias defect measurements. In this paper, we report on the experimental investigation to develop adsorptive films for the PNNL DA sampler concept. These films are intended to efficiently capture UF6 and then stabilize the collected DA sample prior to onsite LAARS or offsite laboratory analysis. Several porous material composite films were investigated, including a film designed to maximize the chemical adsorption and binding of gaseous UF6 onto the sampling planchet.

destructive assay↗
DOE OSTI2014

Qualification of quantum cascade lasers for space environments

Laser-based instruments are enabling a new generation of scientific instruments for space environments such as those used in the exploration of Mars. The lasers must be robust and able to withstand the harsh environment of space, including radiation exposure. Quantum cascade lasers (QCLs), which are semiconductor lasers that emit in the infrared spectral region, offer the potential for the development of novel laser-based instruments for space applications. The performance of QCLs after radiation exposure, however, has not been reported. We report on work to quantify the performance of QCLs after exposure to two different radiation sources, 64 MeV protons and Cobalt-60 gamma rays, at radiation levels likely to be encountered during a typical space flight mission. No significant degradation in threshold current or slope efficiency is observed for any of the seven Fabry-Perot QCLs that are tested.

gamma radiation↗
DOE OSTI2014

Three Dimensional Imaging with Multiple Wavelength Speckle Interferometry

We present the design, modeling, construction, and results of a three-dimensional imager based upon multiple-wavelength speckle interferometry. A surface under test is illuminated with tunable laser light in a Michelson interferometer configuration while a speckled image is acquired at each laser frequency step. The resulting hypercube is Fourier transformed in the frequency dimension and the beat frequencies that result map the relative offsets of surface features. Synthetic wavelengths resulting from the laser tuning can probe features ranging from 18 microns to hundreds of millimeters. Three dimensional images will be presented along with modeling results.

speckle interferometry↗
DOE OSTI2014

Real-Time Trace Gas Sensing of Fluorocarbons using a Swept-wavelength External Cavity Quantum Cascade Laser

We present results demonstrating real-time sensing of four different fluorocarbons at low-ppb concentrations using an external cavity quantum cascade laser (ECQCL) operating in a swept-wavelength configuration. The ECQCL was repeatedly swept over its full tuning range at a 20 Hz rate with a scan rate of 3535 cm-1/s, and a detailed characterization of the ECQCL scan stability and repeatability is presented. The sensor was deployed on a mobile automotive platform to provide spatially resolved detection of fluorocarbons in outdoor experiments. Noise-equivalent detection limits of 800-1000 parts-per-trillion (ppt) are demonstrated for 1 s integration times.

infrared spectroscopy↗