Leah M. Arrigo

Integrated separation scheme for measuring a suite of fission and activation products from a fresh mixed fission and activation product sample

Mixed fission and activation materials resulting from various nuclear processes and events contain a wide range of isotopes for analysis spanning almost the entire periodic table. This work describes the production of a complex synthetic sample containing fission products, activation products, and irradiated soil, and determines the percent chemical recovery of select isotopes through the integrated chemical separation scheme. Based on the results of this experiment, a complex synthetic sample can be prepared with low atom/fission ratios and isotopes of interest accurately and precisely measured following an integrated chemical separation method.

Using Atmospheric Dispersion Theory to Inform the Design of a Short-lived Radioactive Particle Release Experiment.

AbstractAtmospheric dispersion theory can be used to predict ground deposition of particulates downwind of a radionuclide release. This paper uses standard formulations found in Gaussian plume models to inform the design of an experimental release of short-lived radioactive particles into the atmosphere. Specifically, a source depletion algorithm is used to determine the optimum particle size and release height that maximizes the near-field deposition while minimizing both the required source activity and the fraction of activity lost to long-distance transport. The purpose of the release is to provide a realistic deposition pattern that might be observed downwind of a small-scale vent from an underground nuclear explosion. The deposition field will be used, in part, to study several techniques of gamma radiation survey and spectrometry that could be used by an On-Site Inspection team investigating such an event.

PRex: An Experiment to Investigate Detection of Near-field Particulate Deposition from a Simulated Underground Nuclear Weapons Test Vent.

AbstractA radioactive particulate release experiment to produce a near-field ground deposition representative of small-scale venting from an underground nuclear test was conducted to gather data in support of treaty capability development activities. For this experiment, a CO2‐driven “air cannon” was used to inject 140La, a radioisotope of lanthanum with 1.7‐d half-life and strong gamma-ray emissions, into the lowest levels of the atmosphere at ambient temperatures. Witness plates and air samplers were laid out in an irregular grid covering the area where the plume was anticipated to deposit based on climatological wind records. This experiment was performed at the Nevada National Security Site, where existing infrastructure, radiological procedures, and support personnel facilitated planning and execution of the work. A vehicle-mounted NaI(Tl) spectrometer and a polyvinyl toluene-based backpack instrument were used to survey the deposited plume. Hand-held instruments, including NaI(Tl) and lanthanum bromide scintillators and high purity germanium spectrometers, were used to take in situ measurements. Additionally, three soil sampling techniques were investigated and compared. The relative sensitivity and utility of sampling and survey methods are discussed in the context of on-site inspection.

Analysis of 161Tb by radiochemical separation and liquid scintillation counting

The determination of 161Tb activity is problematic due to its very low fission yield, short half-life, and the complication of its gamma spectrum. At AWE, radiochemically purified 161Tb solution was measured on a PerkinElmer 1220 QuantulusTM Liquid Scintillation Spectrometer. Since there was no 161Tb certified standard solution available commercially, the counting efficiency was determined by the CIEMAT/NIST Efficiency Tracing method. The method was validated during a recent inter-laboratory comparison exercise involving the analysis of a uranium sample irradiated with thermal neutrons. The measured 161Tb result was in excellent agreement with the result using gamma spectrometry and the result obtained by Pacific Northwest National Laboratory.

Particle Release Experiment (PRex) Final Report

...................................................................................................................................................... iii Executive Summary .................................................................................................................................... v Acknowledgments ..................................................................................................................................... vii Acronyms and Abbreviations ................................................................................................................... ix 1.0 Introduction ............................................................................................................................ 1 1.1 Background .............................................................................................................................. 1 1.2 Objective .................................................................................................................................. 2 1.3 Scope of Document .................................................................................................................. 2 2.0 Experimental Considerations ................................................................................................ 3 2.1 Overview of PRex .................................................................................................................... 3 2.2 Constraints ............................................................................................................................... 3 2.3 Assumptions ............................................................................................................................. 4 2.4 Pre-Execution Release Parameters ........................................................................................... 4 3.0 PRex Experiment Preparation .............................................................................................. 6 3.1 Experiment Plan ....................................................................................................................... 6 3.2 Site Selection............................................................................................................................ 6 3.3 Background Measurements, September and October 2012 ..................................................... 7 3.4 Source Production .................................................................................................................... 9 3.4.1 Preparation of La2O3 Powder .................................................................................................................. 9 3.4.2 Irradiation at Washington State University ........................................................................................... 12 3.4.3 Source Transport ................................................................................................................................... 14 3.5 Release Mechanism ................................................................................................................ 19 3.6 Meteorology Planning and Modeling ..................................................................................... 22 3.7 NNSS Experiment Site Preparation ....................................................................................... 22 3.7.1 Posting Contamination and High Contamination Areas ....................................................................... 22 3.7.2 Prepositioned Sampling ........................................................................................................................ 22 4.0 PRex Experiment Execution ............................................................................................... 28 4.1 Time and Location ................................................................................................................. 28 4.2 Meteorological Conditions during Release ............................................................................ 28 4.3 Sampling Network ................................................................................................................. 32 4.3.1 Collection of Witness Plates ................................................................................................................. 32 4.3.2 Soil Sampling ....................................................................................................................................... 33 4.3.3 Air Sampling ......................................................................................................................................... 36 4.4 Radiation Survey .................................................................................................................... 36 4.4.1 Vehicle Survey...................................................................................................................................... 37 4.4.2 Handheld/Man-portable ........................................................................................................................ 38 4.4.3 Aerial Survey ........................................................................................................................................ 39 4.5 Field Laboratory ..................................................................................................................... 40

FY 2009 Progress: Process Monitoring Technology Demonstration at PNNL

Pacific Northwest National Laboratory (PNNL) is developing and demonstrating three technologies designed to assist in the monitoring of reprocessing facilities in near-real time. These technologies include 1) a multi-isotope process monitor (MIP), 2) a spectroscopy-based monitor that uses UV-Vis-NIR (ultraviolet-visible-near infrared) and Raman spectrometers, and 3) an electrochemically modulated separations approach (EMS). The MIP monitor uses gamma spectroscopy and pattern recognition software to identify off-normal conditions in process streams. The UV-Vis-NIR and Raman spectroscopic monitoring continuously measures chemical compositions of the process streams including actinide metal ions (uranium, plutonium, neptunium), selected fission products, and major cold flow sheet chemicals. The EMS approach provides an on-line means for separating and concentrating elements of interest out of complex matrices prior to detection via nondestructive assay by gamma spectroscopy or destructive analysis with mass spectrometry. A general overview of the technologies and ongoing demonstration results are described in this report.