Brian T. Schrom

In silico identification software (ISIS)

MOTIVATIONnLiquid chromatography-mass spectrometry-based metabolomics has gained importance in the life sciences, yet it is not supported by software tools for high throughput identification of metabolites based on their fragmentation spectra. An algorithm (ISIS: in silico identification software) and its implementation are presented and show great promise in generating in silico spectra of lipids for the purpose of structural identification. Instead of using chemical reaction rate equations or rules-based fragmentation libraries, the algorithm uses machine learning to find accurate bond cleavage rates in a mass spectrometer employing collision-induced dissociation tandem mass spectrometry.nnnRESULTSnA preliminary test of the algorithm with 45 lipids from a subset of lipid classes shows both high sensitivity and specificity.

International challenge to predict the impact of radioxenon releases from medical isotope production on a comprehensive nuclear test ban treaty sampling station.

The International Monitoring System (IMS) is part of the verification regime for the Comprehensive Nuclear-Test-Ban-Treaty Organization (CTBTO). At entry-into-force, half of the 80 radionuclide stations will be able to measure concentrations of several radioactive xenon isotopes produced in nuclear explosions, and then the full network may be populated with xenon monitoring afterward. An understanding of natural and man-made radionuclide backgrounds can be used in accordance with the provisions of the treaty (such as event screening criteria in Annex 2 to the Protocol of the Treaty) for the effective implementation of the verification regime. Fission-based production of (99)Mo for medical purposes also generates nuisance radioxenon isotopes that are usually vented to the atmosphere. One of the ways to account for the effect emissions from medical isotope production has on radionuclide samples from the IMS is to use stack monitoring data, if they are available, and atmospheric transport modeling. Recently, individuals from seven nations participated in a challenge exercise that used atmospheric transport modeling to predict the time-history of (133)Xe concentration measurements at the IMS radionuclide station in Germany using stack monitoring data from a medical isotope production facility in Belgium. Participants received only stack monitoring data and used the atmospheric transport model and meteorological data of their choice. Some of the models predicted the highest measured concentrations quite well. A model comparison rank and ensemble analysis suggests that combining multiple models may provide more accurate predicted concentrations than any single model. None of the submissions based only on the stack monitoring data predicted the small measured concentrations very well. Modeling of sources by other nuclear facilities with smaller releases than medical isotope production facilities may be important in understanding how to discriminate those releases from releases from a nuclear explosion.

Estimates of Radioxenon Released from Southern Hemisphere Medical isotope Production Facilities Using Measured Air Concentrations and Atmospheric Transport Modeling

The International Monitoring System (IMS) of the Comprehensive-Nuclear-Test-Ban-Treaty monitors the atmosphere for radioactive xenon leaking from underground nuclear explosions. Emissions from medical isotope production represent a challenging background signal when determining whether measured radioxenon in the atmosphere is associated with a nuclear explosion prohibited by the treaty. The Australian Nuclear Science and Technology Organisation (ANSTO) operates a reactor and medical isotope production facility in Lucas Heights, Australia. This study uses two years of release data from the ANSTO medical isotope production facility and (133)Xe data from three IMS sampling locations to estimate the annual releases of (133)Xe from medical isotope production facilities in Argentina, South Africa, and Indonesia. Atmospheric dilution factors derived from a global atmospheric transport model were used in an optimization scheme to estimate annual release values by facility. The annual releases of about 6.8 × 10(14) Bq from the ANSTO medical isotope production facility are in good agreement with the sampled concentrations at these three IMS sampling locations. Annual release estimates for the facility in South Africa vary from 2.2 × 10(16) to 2.4 × 10(16) Bq, estimates for the facility in Indonesia vary from 9.2 × 10(13) to 3.7 × 10(14) Bq and estimates for the facility in Argentina range from 4.5 × 10(12) to 9.5 × 10(12) Bq.

Further developments of a robust absolute calibration method utilizing beta/gamma coincidence techniques

Performing accurate and verifiable measurements is often the most challenging goal for any radiation detector and is especially challenging for the radio-xenon detectors deployed by the International Monitoring System (IMS) of the Preparatory Commission of the Comprehensive Test Ban Treaty Organization (CTBTO). Often the accuracy of the measurement is directly tied to how well the detector is calibrated, in both energy and efficiency. Standard methods often rely on using certified sealed sources to determine the absolute efficiency. Similarly, efforts to calibrate the absolute efficiency of radioactive gas cell detectors utilize a number of methodologies which allow adequate calibration but are time consuming and prone to a host of difficulties to determine uncertainties (McIntyre et al, J Radioanal Nucl Chem 282(3):755–759, 2009; Anderson et al, Stat Probab Lett 77(88):769–773, 2007). Utilizing methods developed in the 1960s for absolute measurements of activity with beta–gamma detector systems it has become clear that it is possible to achieve higher precision results that are consistent across a range of isotopes and activities (National Council on Radiation Protection and Measurement, A handbook of radioactivity measurements procedure NCPR report, 1985). Even more compelling is the ease with which this process can be used on routine samples to determine the total activity present in the detector. Additionally, recent advances in the generation of isotopically pure radio-xenon samples of 131mXe, 133Xe, and 135Xe allow these measurement techniques to achieve much better results than have previously been possible when using mixed isotopic radio-xenon sources (Haas et al, J Radioanal Nucl Chem 282(3):677–680, 2009). This paper will discuss the beta/gamma absolute detection efficiency techniques of direct measurement of the efficiencies and the extrapolation method and compare the results using modeled and measured pure sources of 133Xe and 135Xe.

Real-time stack monitoring at the BaTek medical isotope production facility

Radioxenon emissions from fission-based radiopharmaceutical production are a major source of background concentrations affecting the radioxenon detection systems of the international monitoring system (IMS). Collection of real-time emissions data from production facilities makes it possible to screen out some medical isotope signatures from the IMS radioxenon data sets. This paper describes an effort to obtain and analyze real-time stack emissions data with the design, construction and installation of a small stack monitoring system developed by a joint CTBTO-IDC, BATAN, and Pacific Northwest National Laboratory team at the BaTek medical isotope production facility near Jakarta, Indonesia.

Multi-detection events, probability density functions, and reduced location area

Several efforts have been made in the Comprehensive Nuclear-Test-Ban Treaty (CTBT) community to assess the benefits of combining detections of radionuclides to improve the location estimates available from atmospheric transport modeling (ATM) backtrack calculations. We present a Bayesian estimation approach rather than a simple dilution field of regard approach to allow xenon detections and non-detections to be combined mathematically. This system represents one possible probabilistic approach to radionuclide event formation. Application of this method to a recent interesting radionuclide event shows a substantial reduction in the location uncertainty of that event.

Absolute Efficiency Calibration of a Beta-Gamma Detector

Identification and quantification of nuclear events such as the Fukushima reactor failure and nuclear explosions rely heavily on the accurate measurement of radioxenon releases. One radioxenon detection method depends on detecting beta-gamma coincident events paired with a stable xenon measurement to determine the concentration of a plume. Like all measurements, the beta-gamma method relies on knowing the detection efficiency for each isotope measured. Several methods are commonly used to characterize the detection efficiency for a beta-gamma detector. The first and easiest method is to use a traceable (e.g., NIST) gamma standard to determine the detection efficiency. A second method determines the detection efficiencies relative to an already characterized detector. Finally, a potentially more accurate method is to use isotopes that the system is intended to measure and the form the system is intended to measure to perform an absolute efficiency calibration; in the case of a beta-gamma detector, this relies on radioxenon gas samples. The complication of the first method is it focuses only on the gamma detectors and does not offer a solution for determining the beta efficiency. The second method listed is not similarly constrained, however it relies on another detector to have a well-known efficiency calibration. The final method using actual radioxenon samples to make an absolute efficiency determination is the most desirable, but until recently, it was not possible to produce all four isotopically pure radioxenon isotopes. The production, by University of Texas (UT), of isotopically pure radioxenon has allowed the beta-gamma detectors to be calibrated using the absolute efficiency method. The first four radioxenon isotope calibration will be discussed in this paper.

A program to generate simulated radioxenon beta–gamma data for concentration verification and validation and training exercises

PNNL developed a beta–gamma simulator (BGSim) that incorporated GEANT-modeled data sets from radioxenon decay chains, as well as functionality to use nuclear detector-acquired data sets to create new beta–gamma spectra with varying amounts of background, 133Xe, 131mXe, 133mXe, 135Xe, and 222Rn and its decay products. After BGSim was developed, additional uses began to be identified for the program output: training sets of two-dimensional spectra for data analysts at the IDC and other NDC, and spectra for exercises such as the Integrated Field Exercise 2014 held in Jordan at the Dead Sea.

Beta-gamma coincidence counting using an yttrium aluminum perovskit and bismuth germanate phoswich scintillator

Phoswich detectors (two scintillators attached to the same photomultiplier-tube) have been used in the past to measure either betas or gammas separately but were not used to measure beta-gamma coincidence signatures. These coincidence signatures are very important for the detection of many fission products and are exploited to detect four radioxenon isotopes using the automated radioxenon sampler/analyzer (ARSA). Previous PNNL work with a phoswich detector used a commercially available, thin disk of scintillating CaF/sub 2/(Eu) and a 2 thick NaI(Tl) crystal in a phoswich arrangement. Studies with this detector measured the beta-gamma coincidence signatures from /sup 133/Xe, /sup 214/Pb and /sup 214/Bi. This scintillator combination worked but was not a good match in scintillation light decay times, 940 ns for CaF/sub 2/(Eu) and 230 ns for NaI(Tl). Additionally, a 6-mm thick quartz window was placed between the NaI(Tl) and the CaF/sub 2/ to ensure a hermetic seal for the NaI(Tl) crystal . This dead layer significantly reduced the detection probability of the low energy X-rays and gammas that are part of the coincidence signatures for /sup 214/Pb, /sup 214/Bi and the radioxenons. Further research showed that Yttrium aluminum perovskit (YAP) and bismuth germanate (BGO) have very good scintillation light characteristics and no hermetic seal requirements. The 27-ns scintillation light decay time of YAP and the 300-ns decay time for BGO are a good match between fast and slow light output. The scintillation light output was measured using XIA/spl trade/ digital signal processing readout electronics, and the fast (YAP) and slow (BGO) light components allowed discrimination between the beta and gamma contributions of the radioactive decays. In this paper we discuss the experimental setup and results obtained with this new phoswich detector and the applications beyond radioxenon gas measurements. A companion paper using plastic scintillator and CsI(Na) has also shown very promising results.

Charge Prediction of Lipid Fragments in Mass Spectrometry

An artificial neural network is developed for predicting which fragment is charged and which fragment is neutral for lipid fragment pairs produced from a liquid chromatography tandem mass spectrometry simulation process. This charge predictor is integrated into software developed at PNNL for in silico spectra generation and identification of metabolites known as Met ISIS. To test the effect of including charge prediction in Met ISIS, 46 lipids are used which show a reduction in false positive identifications when the charge predictor is utilized.