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At least 37 records · Page 2

Developing Surrogate Far-Field Nuclear Fallout and its Rapid Decontamination from Aircraft Surfaces

Naval aircraft and vehicles deployed in response to the tsunami of 2011 and subsequent nuclear meltdown at the Fukushima Daiichi nuclear power station were exposed to and contaminated with radioactive materials released to the atmosphere. In response, the Navy and Argonne National Laboratory are testing various decontamination methods to clean aircraft surfaces exposed to far-field nuclear fallout. Far-field fallout, which can travel hundreds of miles, includes dissolved radionuclides and fine particulate matter. To simulate contamination with such materials, dissolved cesium-137 ( 137 Cs) and radiolabeled particles were deposited on coupons (1 x 1 in. sections) of tire, acrylic, and painted metal surfaces. These coupons were subjected to six different decontamination methods, including ones involving four strippable products, a soap solution, and tap water. Removals of dissolved 137 Cs were generally high: over 90% of the deposited radionuclide was removed after three decontaminations. To simulate exposure to inert, radioactive fallout or other inert, airborne particulate, silica (SiO 2 ) particles were used as surrogate fine particulate matter. The silica particles were radio-labeled by first depositing europium-152 ( 152 Eu) or americium-241 ( 241 Am) on the particle surface as sesquioxides (Eu 2 O 3 or Am 2 O 3 ), then coating it with sodium silicate. Scanning electron microscopy confirmed that particle size was not altered by the treatment, while leaching studies into numerous solutions and decontamination agents confirmed that minimal amounts of the radiolabel dissolved into solution. Three different methods to apply the radioactive particles to the silica were evaluated. Pressing the coupons into a dish containing the particles resulted in particle clumping on the surface, while applying the particles within water also resulted in heterogeneous surface coverage. Suspending the particles in ethanol and then applying them to the surface supplied homogeneous surface coverage that provided acute and precise removal percentages. Finally, particle-surface interactions seemingly play an important role in radiological decontamination as the removal percentages were lower than those of soluble 137 Cs for aqueous decontamination methods. These decreased removal percentages indicate that more complex methods such as strippable decontamination agents are required to remove particulate far-field fallout from aircraft and similar vehicle surfaces.

36 MATERIALS SCIENCE↗

Improved Platform for the Benchtop Study of Complex Radiological Environments that Affect Fallout Formation: DHS Feasbility Study (Final Report)

Fallout analysis is a crucial field of study as it provides insight into the structural interactions that occur between radiological components and their surroundings following a nuclear event. Due to the complexity of actual fallout samples, setups like the plasma flow reactor (PFR) at LLNL have been developed to synthesize fallout in a controlled environment. While the PFR allows for control of parameters such as initial temperature, cooling rate, and concentration of radiological species, controlling the concentration of water has remained a challenge as samples are introduced into the setup via aqueous solution. To that end, our goal with this project was to develop methodologies to (1) monitor and (2) control the presence of water in the PFR. We found that a commercially available FTIR and MCT detector was sufficient to monitor the presence of both condensed and vapor-phase water, while a desolvating nebulizer could be used to control the amount of water injected into the system. In total, the results of this feasibility study have expanded the ability of the flow reactor to investigate key sensitivities that influence fallout formation.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Mars - Experimental study of albedo changes caused by dust fallout

A laboratory apparatus was used to simulate the uniform fallout and deposition of particles 1 to 5 microns in diameter in an experimental study on how the spectral and photometric properties of representative Martian areas are affected by fallout of atmospheric dust (smaller than or equalling 60 microns) suspended during dust storms. In this study, measurements are made in the changes in reflectance at optical and near-infrared wavelengths (0.4 to 1.2 micron) caused by deposition of varying amounts of a Mars-analog dust on bright and dark substrates before and after deposition of 6 x 10 to the -5th to 1.5 x 10 to the -3rd g/sq cm of simulated fallout. It is believed that only small amounts of dust particles (approximately 3 x 10 to the -4th g/sq cm) are needed to make significant albedo changes in dark areas of Mars, and that this would rule out uniform dust deposition on the surface of the planet. Data also indicate that other high albedo features like bright crater-related wind streaks may not be areas of significant sediment deposits. Laboratory simulations have permitted estimates of how much the reflectance of an area on Mars would change given a certain amount of dust fallout (g/sq cm) or reflectance data. These simulations may also be useful in tracking the transport and deposition of the dust.

Wells, E. N.↗

Optoelectronic Particle-Fallout Sensor

Portable optoelectronic system monitors fallout of small particles (dust and fibers) onto surface at given location during extended time. Data on accumulated fallout downloaded from system to computer for display and analysis. Typical display is plot of signal proportional to amount of accumulated fallout as function of time and read to determine when contamination occurs. In many cases, possible to establish correlations between accumulations of particles and activities in vicinity. Also capable of signaling alarm in event contamination by fallout exceeds specified level. System made very inexpensively and used to monitor accumulation of dust and fibers associated with motion of air in variety of environments. Phenomena monitored indirectly by use of system might include circulation of air in buildings, and human and animal activity. Also serves as auxiliary intrusion monitor (though probably not real-time alarm) in sealed room because motion of intruder inevitably stirs up some dust.

Ihlefeld, Curtis↗

Study of Fallout Metrics for Contamination Analysis

A challenge present in assessing contamination accumulation on many missions is predicting fallout during ground processing given the multiple and various orientations possible for surfaces such as optics and instruments. The best practice assumption has been to quantify particle build up on vertical surfaces as approximately 1/10 that of horizontal surfaces. This fractional relation is important when considering contamination allocations necessary to meet cleanliness requirements since spacecraft can be in many orientations during integration and testing. There is insufficient data to provide confidence in the 1/10 approximation, yet its use can have a significant effect on mission end of life contamination level predictions, leading to expenditures of precious resources to meet mission requirements. A study was conducted to compare and analyze the fallout in horizontal and vertical orientations. Silicon wafers were deployed in four different facilities. Data sets from a long term deployment of wafers were analyzed from a cleanroom facility housing integration of the James Webb Space Telescope (JWST) as well as from a shorter term deployment of wafers in three cleanroom facilities at Goddard Space Flight Center with lower activity. There are many variables influencing the relationship between fallout on vertical and horizontal wafers, including wafer position with respect to air flow, air changes in the facility, duration of exposure, and activity workload. The goal of this continuing study is to develop a tool to inform particulate accumulation predictions for future projects.

Contamination↗

Direct Alpha Spectrometry of Nuclear Fallout

Advanced instruments and methods are under development to allow direct alpha spectrometry of nuclear fallout debris near the point of collection, to support nuclear forensics (NF). New approaches are needed to support NF in order to accelerate the process for data generation and reduce the overall timeline for decision making. Fallout debris at short time periods following detonation can be difficult to work with for alpha spectrometry, due to the presence of intense beta radiation originating from significant quantities of high-activity fission products. Intense beta radiation can challenge traditional silicon-based high-resolution alpha spectrometers. Addressing this, single-crystal (sc) chemical vapor deposition (CVD) produced diamond semiconductors have been studied for use for alpha spectrometry for assaying nuclear fallout debris. Tests have been performed using scCVD sensors to assay a variety of actinide-bearing samples. Sample preparation, when done, has been limited to pulverization using a mechanical ball mill. To reduce measurement times, multi-chip arrays of scCVD diamond semiconductor have been developed in form factors suitable for field deployment in support of NF objectives. These arrays have been tested using high-beta-activity sol gel surrogate nuclear explosive debris (SNED) containing varying concentrations of uranium and plutonium. Results from the use of scCVD detectors with sol gel SNED will be presented.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Fallout melt debris and aerodynamically-shaped glasses in beach sands of Hiroshima Bay, Japan

An intricate association of millimeter-sized, aerodynamically-shaped debris, including glass spherules, glass filaments, and composite-fused melt particles was recovered from beach sands on the shores of the Motoujina Peninsula in Hiroshima Bay, Japan. Based on optical microscopy, this debris comprises six morphological groups ranging from clear glasses to rubber-like constituents. Scanning electron microscopy and synchrotron X-ray microdiffraction revealed dominant aluminum, silicon and calcium (Al-Si-Ca) elemental composition with some iron, mainly in glass, associated with precipitates of mullite and anorthite microcrystals, hematite dendrites and iron-chromium globules, indicative of original temperature conditions >1800 °C. Aerodynamically-shaped fallout debris, including glass spherules described in this study, are generally produced by single high-energy catastrophic events, such as an extraterrestrial body impacting Earth or a nuclear explosion. Our work interprets the large volumes of fallout debris generated under extreme temperature conditions as products of the Hiroshima August 6th, 1945 atomic bomb aerial detonation. The chemical composition of the melt debris provides clues to their origin, particularly with regard to city building materials. This study is the first published record and description of fallout resulting from the destruction of an urban environment by atomic bombing.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Plasma Flow Reactor Investigation into Nucleation of Uranium Oxide on Silica Substrates to Better Understand Fallout Formation

Understanding particulate formation in nuclear debris is critical for predicting fallout transport after a nuclear event. Improved characterization of fallout formation and transport could lead to better guidance for emergency response in a post-detonation scenario. By analyzing how U-oxides nucleate onto different forms of SiO 2 (crystalline and amorphous), we can gain insight into how entrained environmental materials may incorporate into fallout. In this experiment a Plasma Flow Reactor (PFR), was used to replicate the high temperature and extreme flow conditions in a nuclear fireball. Uranyl nitrate was injected into the plasma, and PFR-generated Uranium oxides were allowed to condense onto amorphous (nanoparticles of varying sizes) or crystalline (quartz) SiO 2 substrates. SiO 2 substrates were characterized before and after U-oxide deposition using Scanning Electron Microscopy (SEM) based techniques (i.e. EDS) in order to characterize how U-oxides may nucleate onto these substrates. After a collection time of 4 minutes at an RF coil distance of 25cm, both the amorphous SiO 2 nanoparticles and the crystalline structures demonstrated dendritic nucleation of U-oxide species as identified by SEM/EDS.

54 ENVIRONMENTAL SCIENCES↗

Web-Enabled Optoelectronic Particle-Fallout Monitor

A Web-enabled optoelectronic particle- fallout monitor has been developed as a prototype of future such instruments that (l) would be installed in multiple locations for which assurance of cleanliness is required and (2) could be interrogated and controlled in nearly real time by multiple remote users. Like prior particle-fallout monitors, this instrument provides a measure of particles that accumulate on a surface as an indication of the quantity of airborne particulate contaminants. The design of this instrument reflects requirements to: Reduce the cost and complexity of its optoelectronic sensory subsystem relative to those of prior optoelectronic particle fallout monitors while maintaining or improving capabilities; Use existing network and office computers for distributed display and control; Derive electric power for the instrument from a computer network, a wall outlet, or a battery; Provide for Web-based retrieval and analysis of measurement data and of a file containing such ancillary data as a log of command attempts at remote units; and Use the User Datagram Protocol (UDP) for maximum performance and minimal network overhead.

Lineberger, Lewis P.↗

THE DEVELOPMENT OF RADIOACTIVE GLASS SURROGATES FOR FALLOUT DEBRIS

The production of glass that emulates fallout is desired for the nuclear forensics community for training and measurement exercises. The composition of nuclear fallout is complex varying isotopic compositions . As the gaseous cloud traverses from hotter to cooler regions of the atmosphere, the processes of condensation and nucleation entrain environmental materials, vaporized nuclear materials and fission products. The elemental and isotopic composition of the fission products is altered due to chemical fractionation (i.e. the fission product composition that would be expected from fission of the original nuclear material is altered by differences in condensation rates of the elements); the fallout may be enriched or depleted in volatile or refractory fission products. This work describes preliminary results to synthesize, irradiate and fractionate the fission product content of irradiated particulate glass using a thermal distillation two hours after irradiation. The glass was synthesized using a solution-based polymerization of tetraethyl orthosilicate. Uranium was incorporated into the glass particulate at trace concentrations during polymerization. The particulate was subjected to a short thermal neutron irradiation then heated to 1273 K approximately 2 hours after the end of irradiation. Fission products of 133, 134, 135I, 132, 134Te, 135Xe, 138Cs and 91, 92Sr were observed to be distilled from the particulate. The results of these preliminary studies are discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Distribution of neptunium and plutonium in New Mexico lichen samples ( Usnea arizonica ) contaminated by atmospheric fallout

In this study, the concentrations of 237 Np, 239 Pu and 240 Pu were determined in lichen samples ( Usnea arizonica ) that were collected from ten locations in New Mexico between 2011 and 2013 using isotope dilution inductively-coupled plasma mass spectrometry (ID-ICP-MS). The observed isotopic ratios for 237 Np/ 239 Pu and 240 Pu/ 239 Pu indicate trace contamination from global and regional fallout (e.g. Trinity test and atmospheric testing at the Nevada Test Site). The fact that actinide contamination is detected in recent lichen collections suggests continuous re-suspension of fallout radionuclides even 50 years after ratification of the Limited Test Ban Treaty.

54 ENVIRONMENTAL SCIENCES↗

Iron-rich microstructure records of high temperature multi-component silicate melt behavior in nuclear fallout

Above-ground nuclear explosions that interact with the surface of the earth entrain materials from the surrounding environment, influencing the resulting physical and chemical evolution of the fireball, which can affect the final chemical phase and mobility of hazardous radionuclides that are dispersed in the environment as fallout particles. The interaction of iron with a nuclear explosion is of specific interest due to the potential for iron to act as a redox buffer and because of the likelihood of significant masses of metals to be present in urban environments. We investigated fallout from a historic surface interacting nuclear explosion conducted on a steel tower and report the discovery of widespread and diverse iron-rich micro-structures preserved within the samples, including crystalline dendrites and micron-scale iron-rich spheres with liquid immiscibility textures. We assert these micro-structures reflect local redox conditions and cooling rates and can inform interpretation of high temperature events, enabling new insights into fireball condensation physics and chemistry when metals from the local environment (i.e. structural steel) are vaporized or entrained. Finally, these observations also significantly expand the availability of silicate immiscibility datasets applicable to rapidly quenched systems such as meteorite impact melt glass.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Thermodynamics of Liquid Immiscibility in Iron-Silicate Melt Systems: A Study of Nuclear Fallout Glass

In a ground-interacting nuclear explosion, elements derived from environmental and anthropogenic material, such as iron, silicon, and aluminum, can be incorporated into the fireball. When significant amounts of metals are entrained, the resulting melt may display immiscible textures. The composition of these textures is a record of the temperature of formation and cooling rates (or thermodynamic stability) of the melts and can provide unique constraints on the early cooling conditions of these events. Here, a thermodynamic approach using calculated phase diagrams, the CALPHAD method, is used to predict temperature and composition ranges where stable liquid immiscibility might result in the textures observed in nuclear fallout glass. Sensitivity of the immiscibility to the presence of relative Al, Ca, and Mg content is also explored and compared to fallout samples, and partition coefficients are introduced to understand the preferred distribution of components into each liquid phase.

36 MATERIALS SCIENCE↗

Characterization, Chemistry, and Particle Size Distribution of Fallout Particles Isolated from Filter Samples

Nuclear particulate fallout is the radioactive byproduct of a nuclear event formed by the mixture of proximate environmental materials with vaporized bomb debris. The debris can be transported into the atmosphere during cloud rise, raining out locally and globally constituting a radiation hazard. Questions remain on how entrainment of environmental material in the fireball affects fallout formation processes and radionuclide incorporation during cooling.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A preliminary study of the particulate fallout from the space shuttle (STS-1)

Prediction of acid fallout and the dry deposition of Al2O2 was the objective of this investigation. Sampling was done at the Kennedy Space Center in Florida. The models available were not appropriate and the data available was negligible. Thus, a bimodal particle distribution was assumed normalized to the few existing data points and used as a foundation for a crude zeroth order approximation for the acid fallout. In addition, a settling spectrum for the Al2O3 particles was devised as a table look-up since the graphs in the literature at first pass could not be fitted with reasonable analytic functions. Consulting services were rendered to researchers. Special emphasis was placed on improving current techniques and adding LIDAR (Light Radar). Suggestions for future studies are made.

Hudson, G. M.↗

A non-optical real-time particle fallout monitor

The paper describes a size-selective fallout monitor that can be employed to assess the degradation of sensitive optical surfaces as well as facilitate the analysis of particle types. The device combines a vertical elutriator and a quartz crystal microbalance, and only particles greater than a specific size can pass through an upward laminar flow generated in the device. The larger particles cause a frequency shift in the crystal oscillator, thereby permitting the measurement of the fallout associated with the contamination of optical instruments.

Chuan, Raymond L.↗

Fallout Cloud Regimes

The U.S. Department of Defense (DOD), Department of Energy (DOE), and other organizations maintain operational nuclear explosion and atmospheric dispersion models to provide critical guidance on the expected effects of an accidental or deliberate explosion of a nuclear weapon (in this paper simply referred to as “device”). To be effective, these models must represent, as accurately as possible, the complex interactions of the blast, fire, and residual radiological hazards with the environment and population. One hundred atmospheric nuclear tests that form the basis for many models were conducted at the Nevada Test Site (NTS) (now referred to as the Nevada Nuclear Security Site, NNSS) in a dry desert environment. Other environments should be studied, but have less data available and are beyond the scope of the work presented in this paper. The debris clouds produced by the NTS tests, frequently called “mushroom clouds,” are familiar, with common structural elements such as a buoyant cap connected to a skirt of raised dust at the desert surface by a thin, dirt-filled stem. The film scanning project at LLNL has investigated historical film records of nuclear weapons tests. Here, we summarize findings showing that the mushroom cloud behavior for historic U.S. tests conducted in Nevada, has similar characteristics based on the distance of the device from the ground surface or Height of Burst (HOB), scaled by the energy release, or yield, of the device. This scaled height is referred to as the scaled-height-of-burst (SHOB). The findings discussed below show that mushroom clouds look and behave similarly when detonated at the same SHOB. The amount of residual radiation that is produced by a nuclear detonation is proportional to the yield. But, the amount of that residual radiation that actually becomes local fallout is strongly dependent on the SHOB and the type of surface over which the detonation occurs. In order to develop a more comprehensive model that predicts the fraction of the residual radiation that becomes local fallout, it is convenient to define a series of regimes based on SHOB values in which all detonations that occur within a given regime can be modeled using the same algorithms. The purpose of this paper is to provide a framework for defining different regimes, and, in a qualitative way, a basic understanding of the fundamental characteristics of each of these regimes.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Silicate coating to prevent leaching from radiolabeled surrogate far-field fallout in aqueous environments

Recent characterization of radioactive particles indicate that a large percentage of the radioactivity observed during the Fukushima Daiichi nuclear meltdown was insoluble 137 Cs bound within silica microparticles. Therefore, much of the decontamination research performed prior to the Fukushima incident that used either soluble radionuclides deposited onto wet surfaces or large (~100 μm) particles characteristic of nuclear weapons fallout do not accurately represent the characteristics of potential contamination. Thus, the common practice of extrapolating radioactive decontamination methods generically to all radioactive release events is, at best, suspect. In response, a method to produce chemically-inert, radiolabeled silica particles was developed. Binding 152 Eu within a sodium silicate coating required proper temperature control and ethanol was beneficial as a volatile dispersant to limit residues. In the end, a step-wise method, which first deposited 152 Eu or 241 Am as a nitrate salt, decomposed the salt to a sesquioxide, and finally coated the surface with sodium silicate led to dispersed particles of the desired 2 or 0.5 μm diameters. Dynamic light scattering and scanning election microscopy confirmed the particle size was unchanged. Leaching studies into several common decontaminants were performed to ensure particle inertness. In this paper, our approach allows for substitution of other radionuclides making it a robust, simple, and novel method to produce inert particle surrogates for a release event that allows direct comparison of decontamination techniques and contaminant fate studies, greatly aiding the development of response and recovery plans.

61 RADIATION PROTECTION AND DOSIMETRY↗