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A nondestructive analytical method based on autoradiography and gamma spectrometry was developed to perform activity distribution analysis for particulate samples. This was applied to aerosols collected in Fukushima Japan, 40 km north of the Daiichi nuclear power plant for a 6 week period beginning shortly after the March 2011 tsunami. For an activity distribution of 990 “hot particles” from a small filter area, the hottest particle was nearly one Bq 137+134Cs but most of the activity in the filter was produced by particles having

Background radiation and radioactive sources have been measured with laser-scanned phosphor imaging plates using an image processing method that produces spectra. This enables distinction between ambient background radiation, alpha and beta radionuclides and provides a means for quantitation. The background counts span a broad spectral continuum, whereas counts resulting from alpha and beta activity are restricted to certain regions within the background continuum spectrum. The alpha-counting spectral region has a background count rate of −2 h −1 . The beta-counting region has a count rate of −2 h −1 . One region of the background spectrum is attributed to heavy ions from cosmic rays and has a count rate of −2 day −1 . With regard to imaging spectrometry, beta-particles from 3 H ( E max =0.0186 MeV) could be distinguished from higher energy beta-particles such as those from 14 C ( E max =0.157 MeV) and 40 K ( E max =1.33 MeV). Beta-particles can be distinguished from alpha-particles, and radionuclide counts can be distinguished from the background. The spectral characterization of the background, alpha-particles and beta-particles is expected to support applications in cosmic ray, heavy ion, radionuclide and electron studies.

On the morning of July 16, 1945, the first atomic bomb was exploded in New Mexico on the White Sands Proving Ground. The device was a plutonium implosion device similar to the device that destroyed Nagasaki, Japan, on August 9 of that same year. Recently, with the enactment of US public law 111-140, the “Nuclear Forensics and Attribution Act,” scientists in the government and academia have been able, in earnest, to consider what type of forensic-style information may be obtained after a nuclear detonation. To conduct a robust attribution process for an exploded device placed by a nonstate actor, forensic analysis must yield information about not only the nuclear material in the device but about other materials that went into its construction. We have performed an investigation of glassed ground debris from the first nuclear test showing correlations among multiple analytical techniques. Surprisingly, there is strong evidence, obtainable only through microanalysis, that secondary materials used in the device can be identified and positively associated with the nuclear material.

137Cesium and other contaminants have leaked from single-shell storage tanks (SSTs) into coarse-textured, relatively unweathered unconsolidated sediments. Contaminated sediments were retrieved from beneath a leaky SST to investigate the distribution of adsorbed 137Cs+ across different sediment size fractions. All fractions contained mica (biotite, muscovite, vermiculatized biotite), quartz, and plagioclase along with smectite and kaolinite in the clay-size fraction. A phosphor-plate autoradiograph method was used to identify particular sediment particles responsible for retaining 137Cs+. The Cs-bearing particles were found to be individual mica flakes or agglomerated smectite, mica, quartz, and plagioclase. Of these, only the micaceous component was capable of sorbing Cs+ strongly. Sorbed 137Cs+ could not be significantly removed from sediments by leaching with dithionite citrate buffer or KOH, but a fraction of the sorbed 137Cs+ (5-22%) was desorbable with solutions containing an excess of Rb+. The small amount of 137Cs+ that might be mobilized by migrating fluids in the future would likely sorb to nearby micaceous clasts in downgradient sediments.

We have been exploring ways to evaluate the activity of radioactive particles that have been detected by phosphor plate digital autoradiography based on photostimulated luminescence (PSL). A PSL system with 25 μm pixel digitization has been applied to particle analysis problems, both qualitatively and quantitatively. Two data evaluation methods are currently employed: (1) bulk area signal measurement, and (2) discrete event counting which may include spectral evaluation. The first method is conventional, whereas the second method requires high spatial resolution and is presented here for the first time. The counting methods can discriminate between alpha and background counts. The unshielded background signal accumulation rate was determined by the bulk area method. Using the spectral method of evaluation for α-particle events, the mean signal intensity per recorded α-particle was measured, and the detective quantum efficiency (DQE) was found to be nominally 100%. We present a comparison to gamma-spectrometry for sub-Bq 137Cs activities, and demonstrate an application for the qualitative assay of International Atomic Energy Agency swipe samples collected from uranium enrichment facilities.

Phosphor imaging plate technology has made it possible to directly image the distribution of primary beam electrons and scattered electrons in the environmental scanning electron microscope. The phosphor plate is exposed under electron scattering conditions in the microscope chamber. When processed, the electron intensity distribution is displayed as a digital image. The image is a visual representation of the electron probe and skirt and may provide the basis for a more accurate model.

Recent advances in instrumentation provide the capability to measure size, count rate, type of radiation, and the chemical composition of radioactive particles. We present a demonstration of these capabilities, using a laser-scanned phosphor imaging system and a charge injection device system for digital autoradiography, light and electron microscopy, energy dispersive X-ray spectrometry, and conventional radionuclide spectrometry. Response characteristics of the phosphor system that support these efforts are presented.

The need to locate “hot particles” during environmental radioactivity characterization benefits from autoradiography. Three detectors are compared for the evaluation of point-source alpha emitters. 238 PuO 2 particles were used to compare a detector based on a pixel array, a phosphor imaging plate system, and a track-etch detector. The pixel-array detector is based on a charge injection device (CID) having nominally 14 μm sized pixels in a 7 mm × 9 mm array. Processing at a 30 frames per second rate allows real-time display of results. Background interference is minimal even in long-duration exposures. The phosphor imaging plate system is subject to background accumulation. Track overlap makes single-event discrimination and quantification impractical, but a large exposure area and ease of use are distinct advantages. A system having a pixel size of 50 μm was used. Track-etch detectors have the largest potential exposure area and best spatial resolution, the latter being limited by the amount of material etched, resolving power of the reading system, and the number of tracks recorded per source. Readout, however, can be time-consuming, and track overlap can make quantification difficult. The best apatial resolution, 10 μm, was obtained with the track-etch detector, with a precision in location of 1 μm. The phosphor plate system was capable of detecting 0.002 Bq sources in 2 d, whereas the track-etch and semiconductor pixel array were capable of detecting 0.0002 Bq sources in 2 d. The track-etch method was the most difficult, whereas the most rapid results were obtained with the real-time display of the semiconductor pixel array.

A neutron lens has been constructed to focus cold neutrons from the exit of a58Ni neutron guide, which delivers a beam to the Prompt-Gamma Activation Analysis (PGAA) station at the NIST Cold Neutron Research Facility. The lens compresses a neutron beam of cross section 50 mm× 45 mm onto a focal spot of diameter 0.53 mm (fwhm) wich an average gain of 80 in neutron current density. PGAA measurements have been performed to demonstrate the enhanced sensitivity and detection limits for various elements and the spatial resolution in one transverse dimension. For the two test particles (a gadolinium glass bead and cadmium metal of sizes less than 0.5 mm), the gain in the γ-count rate with the lens is a factor of 60, and the detection limit is improved by a factor of 20. The system can be used for two-dimensional mapping of samples on a sub-millimeter scale to complement other analytical techniques such as neutron depth profiling (NDP).

The U-Pb and Sm-Nd dating of garnet are important tools for understanding rates of tectonometamorphic processes and have been widely applied in studies of metamorphic terranes. However, the budgets of uranium, lead, samarium, and neodymium in garnet separates from metamorphic rocks may be dominated by contributions from inclusions of monazite or zircon. A combined fission track and stepwise dissolution technique is proposed for evaluating the role of inclusions of monazite and zircon in the budgets of uranium, lead, samarium, and neodymium in garnets used for U-Pb and Sm-Nd chronology. Variations of Th/U, U/Nd, and Sm/Nd ratios between successive dissolution steps reveal the contributions of monazite and zircon inclusions. The stepwise dissolution procedure does not induce any apparent artifacts on 207Pb-206Pb and Sm-Nd ages. The technique has been applied to garnets from three metamorphic terranes. Almandine garnet samples from the high grade Pikwitonei Granulite Domain (Manitoba, Canada) and the Wind River Range (Wyoming, USA) have the majority of their uranium, samarium, neodymium, and radiogenic lead (Pb*) hosted by micrometer-scale inclusions of monazite. Fission track densities reveal that uranium is 108 times more abundant in inclusions than in garnets. Stepwise dissolution of the samples shows that neodymium and uranium are associated with the dissolution of monazite. In contrast, grossularandradite garnets from Cascade Slide (Adirondack Highlands, NY, USA) show little variation in fission track density and similar isotopic ratios between dissolution steps, indicating that the budgets of uranium, samarium, neodymium, and Pb* are not significantly influenced by inclusions. The demonstrated success of these techniques leads us to recommend similar procedures as a routine matter in U-Pb and Sm-Nd garnet geochronology of metasedimentary rocks.

A focusing neutron lens using glass polycapillary fibers has been introduced successfully into a prompt gamma activation analysis (PGAA) instrument placed at the exit of a cold neutron guide. The neutron current density gain of the lens is 80, averaged over the focused beam size of 0.53 mm diameter. PGAA measurements have been made on submillimeter particles of gadolinium and cadmium. The results indicate that elemental sensitivities of measurements are increased by ∼ 60, and that particles of sizes smaller than 0.5 mm can be discerned using the focusing lens. The measured gain in prompt gamma signals for these particles is less than anticipated, probably due to alignment difficulties. Gamma ray background associated with the lens is discussed and improvements are suggested.

This work provides examples of some of the imaging capabilities of environmental scanning electron microscopy applied to easily charged samples relevant to particle analysis. Environmental SEM (also referred to as high pressure or low vacuum SEM) can address uncoated samples that are known to be difficult to image. Most of these specimens are difficult to image by conventional SEM even when coated with a conductive layer. Another area where environmental SEM is particularly applicable is for specimens not compatible with high vacuum, such as volatile specimens. Samples from which images were obtained that otherwise may not have been possible by conventional methods included fly ash particles on an oiled plastic membrane impactor substrate, a one micrometer diameter fiber mounted on the end of a wire, uranium oxide particles embedded in oil-bearing cellulose nitrate, teflon and polycarbonate filter materials with collected air particulate matter, polystryene latex spheres on cellulosic filter paper, polystyrene latex spheres “loosely” sitting on a glass slide, and subsurface tracks in an etched nuclear track-etch detector. Surface charging problems experienced in high vacuum SEMs are virtually eliminated in the low vacuum SEM, extending imaging capabilities to samples previously difficult to use or incompatible with conventional methods. © 1993 Wiley-Liss, Inc.

When using the nuclear track technique for multi-element detection and spatial mapping, the presence of moderate to high concentrations of boron or lithium results in a large number of (n,α) reactions when using the high thermal neutron fluences required to map trace amounts of uranium. When chemically etched, tracks generated by a large number of alpha particles cannot be spatially resolved, and are manifested instead by large-scale depressions in the detector surface. High Li and B concentration samples have the most pronounced topographic development in both CR-39 and CN detectors. Samples with low concentrations of Li and B or high concentrations of Gd, Sm or Eu developed moderate depressions. These depressions can affect uranium quantitation, but simultaneously, they provide useful information about the sample. This paper is a preliminary study of observations of etched bulk depressions, variations in track revelation time, and the mapping of samples containing elements with high thermal neutron absorption cross sections such as gadolinium.

A charge injection device (CID) camera and image processing system have been used as a position sensitive detector for energetic charged particles and low energy neutrons. This video radiation detector (VRD) is simple in design but highly effective for real-time radiography and dosimetry with many advantages characteristics. The VRD currently has a dynamic range of 65,000 intensity levels for a 755 X 484 pixel matrix, an active area of 7 mm X 9 mm, a spatial mapping resolution of about 14 micrometers for single detected events (7 micrometers for radiation from a point source), and is sufficiently radiation-hard to be operated in a neutron beam for extended periods of time. Radiation images are updated at a rate of thirty frames per second. The VRD is sensitive to fission fragments, alpha particles, and slow neutrons. Using commercially available image processing hardware and software and an off-the-shelf camera, the system is inexpensive, easy to use with simple interpretation of data, and is capable of performing radiography with only minimal adaptations. Applications in our laboratory include the characterization of focused cold neutron beams, the mapping of uranium and lithium distributions in samples by the detection of neutron absorption reaction products, and the mapping of spontaneous alpha radioactivity from environmental samples. Results provide information on x-y position, counts received, and energy deposited per count, each as a function of time.© (1993) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.

Often, good results in materials analysis depend on good sample preparation. Although sample preparation can often be simple and straightforward, particles sometimes present special challenges. Sometimes just a few tricks make the only difference between the success and failure of sample preparation and analysis. Without adequate insight and care in specimen preparation, there may be loss of sample, over-expended effort and loss of time, contamination (sample or instrument), adverse morphological changes, misrepresentation of elemental composition or phase distribution, and other artifacts. This tutorial will cover a variety of topics dealing with sample preparation methods, the tools, equipment and supplies used, and artifacts primarily of concern to analytical electron beam techniques.The many combinations of numerous parameters that can affect sample treatment and analysis make it difficult to produce a simple flow-chart for sample preparation. Various factors that determine optimal preparation methods include the physical state of the received sample (e.g., bulk, powder or single particle, wet or dry, homogeneous or heterogeneous), and the known chemical properties of the received sample.