Uranium hexafluoride (UF6) is a commonly used material feedstock for uranium enrichment processes. When introduced to water in the atmosphere, it reacts rapidly to form uranyl fluoride (UO2F2). Here, we investigate the UF6 hydrolysis reaction by cryogenically trapping reaction intermediates and characterizing the trapped species by Fourier transform infrared (FTIR) spectroscopy. The reactant species are sequentially layered onto a diamond substrate held at 10K by a closed-cycle liquid helium cryostat. At this temperature, the hydrolysis reaction is not spontaneous and can be catalyzed by the introduction of heat. Upon heating, the reaction moves through several intermediate compounds before proceeding to the final UO2F2 product. Several previously unobserved bands appear while the reaction progresses. These bands may help to elucidate the mechanism behind UF6 hydrolysis.
The Savannah River National Laboratory (SRNL) has been developing advanced spectroscopic tools for the characterization of plutonium-bearing compounds with the intent to develop material and process signatures for nuclear forensics. Plutonium in a production, refining, or finishing facility will exist in many forms including oxide precursors (PuF4, PuF3, Pu oxalate, etc.), oxide, and metal. The ability to identify plutonium in each of these chemical forms and determine their processing history is crucial for the development of spectroscopic signatures. This presentation will focus on our work to develop and apply spectroscopic tools at SRNL using doubled-walled cells (DWC) to characterize the thermal decomposition of oxalates, calcination chemistry, alpha-decay-induced chemistry, age dating since last calcination, and other signatures related to plutonium processing.
The Savannah River National Laboratory (SRNL) collected thermal imagery and ground truth data at two commercial
power plant cooling lakes to investigate the applicability of laboratory empirical correlations between surface heat flux
and wind speed, and statistics derived from thermal imagery. SRNL demonstrated in a previous paper [1] that a linear
relationship exists between the standard deviation of image temperature and surface heat flux. In this paper, SRNL will
show that the skewness of the temperature distribution derived from cooling lake thermal images correlates with
instantaneous wind speed measured at the same location. SRNL collected thermal imagery, surface meteorology and
water temperatures from helicopters and boats at the Comanche Peak and H. B. Robinson nuclear power plant cooling
lakes. SRNL found that decreasing skewness correlated with increasing wind speed, as was the case for the laboratory
experiments. Simple linear and orthogonal regression models both explained about 50% of the variance in the skewness
- wind speed plots. A nonlinear (logistic) regression model produced a better fit to the data, apparently because the
thermal convection and resulting skewness are related to wind speed in a highly nonlinear way in nearly calm and in
windy conditions.
Semi-conducting CdZnTe (or CZT) crystals can be used in a variety of detector-type applications. CZT
shows great promise for use as a gamma radiation spectrometer. However, its performance is adversely
affected by point defects, structural and compositional heterogeneities within the crystals, such as twinning,
pipes, grain boundaries (polycrystallinity), secondary phases and in some cases, damage caused by external
forces. One example is damage that occurs during characterization of the surface by a laser during Raman
spectroscopy. Even minimal laser power can cause Te enriched areas on the surface to appear. The Raman
spectra resulting from measurements at moderate intensity laser power show large increases in peak intensity
that is attributed to Te. Atomic Force Microscopy (AFM) was used to characterize the extent of damage to the
CZT crystal surface following exposure to the Raman laser. AFM data reveal localized surface damage in the
areas exposed to the Raman laser beam. The degree of surface damage to the crystal is dependent on the laser
power, with the most observable damage occurring at high laser power. Moreover, intensity increases in the Te
peaks of the Raman spectra are observed even at low laser power with little to no visible damage observed by
AFM. AFM results also suggest that exposure to the same amount of laser power yields different amounts of
surface damage depending on whether the exposed surface is the Te terminating face or the Cd terminating face
of CZT.
Laboratory experiments show a linear relationship between the total heat flux from a water surface to air and the
standard deviation of the surface temperature field, σ, derived from thermal images of the water surface over a range of
heat fluxes from 400 to 1800 Wm-2. Thermal imagery and surface data were collected at two power plant cooling lakes
to determine if the laboratory relationship between heat flux and σ exists in large heated bodies of water. The heat fluxes
computed from the cooling lake data range from 200 to 1400 Wm-2. The linear relationship between σ and Q is evident
in the cooling lake data, but it is necessary to apply band pass filtering to the thermal imagery to remove camera artifacts
and non-convective thermal gradients. The correlation between σ and Q is improved if a correction to the measured σ is
made that accounts for wind speed effects on the thermal convection. Based on more than a thousand cooling lake
images, the correlation coefficients between σ and Q ranged from about 0.8 to 0.9.
Power plant-heated lakes are characterized by a temperature gradient in the thermal plume originating at the discharge of
the power plant and terminating at the water intake. The maximum water temperature discharged by the power plant into
the lake depends on the power generated at the facility and environmental regulations on the temperature of the lake.
Besides the observed thermal plume, cloud-like thermal cells (convection cell elements) are also observed on the water
surface. The size, shape and temperature of the convection cell elements depends on several parameters such as the lake water temperature, wind speed, surfactants and the depth of the thermocline. The Savannah River National Laboratory (SRNL) and Clemson University are collaborating to determine the applicability of laboratory empirical correlations between surface heat flux and thermal convection intensity. Laboratory experiments at Clemson University have demonstrated a simple relationship between the surface heat flux and the standard deviation of temperature fluctuations. Similar results were observed in the aerial thermal imagery SRNL collected at different locations along the thermal plume and at different elevations. SRNL will present evidence that the results at Clemson University are applicable to cooling lakes.
KEYWORDS: Bidirectional reflectance transmission function, Reflection, Reflectivity, Process modeling, Sensors, Black bodies, Infrared imaging, Solid modeling, Digital imaging, 3D modeling
Determining the temperature of an internal surface within cavernous targets, such as the interior wall of a mechanical draft cooling tower, from remotely sensed imagery is important for many surveillance applications that provide input to process models. The surface leaving radiance from an observed target is a combination of the self-emitted radiance and the reflected background radiance. The self-emitted radiance component is a function of the temperature-dependent blackbody radiation and the view-dependent directional emissivity. The reflected background radiance component depends on the bidirectional reflectance distribution function (BRDF) of the surface, the incident radiance from surrounding sources, and the BRDF for each of these background sources. Inside a cavity, the background radiance emanating from any of the multiple internal surfaces will be a combination of the self-emitted and reflected energy from the other internal surfaces as well as the downwelling sky radiance. This scenario provides for a complex radiometric inversion problem in order to arrive at the absolute temperature of any of these internal surfaces. The cavernous target has often been assumed to be a blackbody, but in field experiments it has been determined that this assumption does not always provide an accurate surface temperature. The Digital Imaging and Remote Sensing Image Generation (DIRSIG) modeling tool is being used to represent a cavity target. The model demonstrates the dependence of the radiance reaching the sensor on the emissivity of the internal surfaces and the multiple internal interactions between all the surfaces that make up the overall target. The cavity model is extended to a detailed model of a mechanical draft cooling tower. The predictions of derived temperature from this model are compared to those derived from actual infrared imagery collected with a helicopter-based broadband infrared imaging system collected over an operating tower located at the Savannah River National Laboratory site.
This report describes laboratory development and process plant applications of Raman spectroscopy for detection of hydrogen isotopes in the Tritium Facilities at the Savannah River Site (SRS), a U.S. Department of Energy complex. Raman spectroscopy provides a lower-cost, in situ alternative to mass spectrometry techniques currently employed at SRS. Using conventional Raman and fiber optics, we have measured, in the production facility glove boxes, process mixtures of protium and deuterium at various compositions and total pressures ranging from 1000 - 4000 torr, with detection limits ranging from 1-2% for as low as 3-second integration times. We are currently investigating fabrication techniques for SERS surfaces in order to measure trace (0.01-0.1%) amounts of one isotope in the presence of the other. These efforts have concentrated on surfaces containing palladium, which promotes hydrogen dissociation and forms metal hydride bonds, essentially providing a chemical enhancement mechanism.
The Savannah River Technology Center (SRTC) conducted four vicarious reflectance calibrations at Ivanpah Playa, California since July 2000 in support of the MTI satellite. The potential of the playa as a thermal calibration site was also investigated in the campaigns with a mobile Fourier transform infrared spectrometer. The multi-year study shows time and spatial variability in the spectral emissivity. The ground truth temperature and emissivity correlate quite well with the data from the MTI satellite imagery. The research paper will show the time-dependent emissivities measured during our ground truth campaigns and the corresponding satellite imagery.
The Savannah River Technology Center (SRTC) conducted four reflectance vicarious calibrations at Ivanpah Playa, California since July 2000 in support of the MTI satellite. The multi-year study shows temporal, spatial and spectral variability at the playa. The temporal variability in the wavelength dependent reflectance and emissivity across the playa suggests a dependency witt precipitation during the winter and early spring seasons. Satellite imagery acquired on September and November 2000, May 2001 and March 2002 in conjunction with ground truth during the September, May and March campaigns and water precipitation records were used to demonstrate the correlation observed at the playa.
The Multispectral Thermal Imager (MTI) is a research and development satellite sponsored by the Department of Energy (DOE) for accurate water surace temperature retrieval. MTI uses five thermal spectral bands to retrieve ground temperatures. The application of MTI for land-based temperature and emissivity retrieval has been limited. Savannah River Technology Center conducted several ground truth campaigns at Ivanpah Playa to measure reflectance, temperature and emissivity. The results of MTI temperature and emissivity retrievals and material identification will be discussed in context with the ground truth data.
The Savannah River Technology Center (SRTC) is conducting measurements in the visible, near-infrared and infrared spectral regions of selected ground targets in support to the Department of Energy Multispectral Thermal Imager (MTI) satellite. Radiometers have been used to retrieve surface temperature from water and land targets. Surface temperature measurements of land targets are often complicated by the wavelength dependent emissivity. Conical cavities have been employed on land targets to increase the surface effective emissivity and therefore the apparent surface temperature. Surface effective emissivity values near unity offer the opportunity for absolute surface temperature retrieval. The efficacy of conical cavities for absolute surface temperature retrievals was studied with a calibrated Fourier transform infrared spectrometer (FTIR). The research paper presents the results of surface temperature retrievals of targets with low emissivity values with the aid of conical cavities.
Temperatures of the water surface of a cold, mid-latitude lake and the tropical Pacific Ocean were determined from MTI images and from in situ concurrent measurements. In situ measurements were obtained at the time of the MTI image with a floating, anchored platform, which measured the surface and bulk water temperatures and relevant meteorological variables, and also from a boat moving across the target area. Atmospheric profiles were obtained from concurrent radiosonde soundings. Radiances at the satellite were calculated with the Modtran radiative transfer model. The MTI infrared radiances were within 1% of the calculated values at the Pacific Ocean site but were 1-2% different over the mid-latitude lake.
The Savannah River Technology Center (SRTC) is currently calibrating the Multispectral Thermal Imager (MTI) satellite sponsored by the Department of Energy. The MTI is a research and development project with 15 wavebands in the 0.45-11.50 micrometers spectral range. The reflective bands of the MTI satellite are calibrated in desert playas such as Ivanpah Playa in the Nevada/California border. The five MTI thermal bands are calibrated with targets of know emissivity and temperature such as power plant heated lakes. In order to accomplish a full calibration at the desert playas, a Fourier transform infrared spectrometer was used to measure soil surface radiance and temperature during the satellite overpass. The results obtained with the mobile FTIR during the ground truth campaign at Ivanpah Playa will be presented.
Natural bodies of water have several advantages as IR calibration targets in remote sensing. Among these are availability, homogeneity, and accurate knowledge of emissivity. A portable, low-cost, floating apparatus is described for calibration of remote IR sensors to within 0.15 C. The apparatus measures the surface and bulk water temperature as well as the wind speed, direction, temperature, and relative humidity. The apparatus collects data automatically and can be deployed for up to 24 hours. The sources of uncertainty, including the effects of skin temperature and waves are discussed. Data from several field campaigns to calibrate IR bands of DOE's Multi-Spectral Thermal Imager are described along with estimates of error.
KEYWORDS: Temperature metrology, Skin, Astatine, Solar radiation models, Data modeling, 3D modeling, Thermography, Atmospheric modeling, Radiometry, Wind energy
The Savannah River Technology Center (SRTC) measured water skin temperatures at four of the Multi-spectral Thermal Imager (MTI) core sites. The depression of the skin temperature relative to the bulk water temperature ((Delta) T) a few centimeters below the surface is a complex function of the weather conditions, turbulent mixing in the water and the bulk water temperature. Observed skin temperature depressions range from near zero to more than 1.0 degree(s)C. Skin temperature depressions tend to be larger when the bulk water temperature is high, but large depressions were also observed in cool bodies of water in calm conditions at night. We compared (Delta) T predictions from three models (SRTC, Schlussel and Wick) against measured (Delta) T's from 15 data sets taken at the MTI core sites. The SRTC and Wick models performed somewhat better than the Schlussel model, with RMSE and average absolute errors of about 0.2 degree(s)C, relative to 0.4 degree(s)C for the Schlussel model. The average observed (Delta) T for all 15 databases was -0.7 degree(s)C.
The Savannah River Technology Center (SRTC) selected 13 sites across the continental US and one site in the western Pacific to serve as the primary or core site for collection of ground truth data for validation of MTI science algorithms. Imagery and ground truth data from several of these sites are presented in this paper. These sites are the Comanche Peak, Pilgrim and Turkey Point power plants, Ivanpah playas, Crater Lake, Stennis Space Center and the Tropical Western Pacific ARM site on the island of Nauru. Ground truth data includes water temperatures (bulk and skin), radiometric data, meteorological data and plant operating data. The organizations that manage these sites assist SRTC with its ground truth data collections and also give the MTI project a variety of ground truth measurements that they make for their own purposes. Collectively, the ground truth data from the 14 core sites constitute a comprehensive database for science algorithm validation.
The Savannah River Technology Center (SRTC) is currently calibrating the Multispectral Thermal Imager (MTI) satellite sponsored by the Department of Energy. The MTI imager is a research and development project with 15 wavebands in the visible, near-infrared, short-wave infrared, mid-wave infrared and long-wave infrared spectral regions. A plethora of targets with known temperatures such as power plant heated lakes, volcano lava vents, desert playas and aluminized Mylar tarps are being used in the validation of the five thermal bands of the MTI satellite. SRTC efforts in the production of cold targets with aluminized Mylar tarps will be described. Visible and thermal imagery and wavelength dependent radiance measurements of the calibration targets will be presented.
Remote sensing temperature measurements of water bodies is complicated by the temperature differences between the true surface or `skin' water and the bulk water below. Weather conditions control the reduction of the skin temperature relative to the bulk water temperature. Typical skin temperature depressions range from a few tenths of a degree Celsius to more than one degree. In this research project, the Savannah River Technology Center used aerial thermography and surface-based meteorological and water temperature measurements to study a power plant cooling lake in South Carolina. Skin and bulk water temperatures were measured simultaneously for imagery calibration and to product a database for modeling of skin temperature depressions as a function of weather and bulk water temperatures. This paper will present imagery that illustrates how the skin temperature depression was affected by different conditions in several locations on the lake and will present skin temperature modeling results.
Sandia National Laboratories (SNL), Los Alamos National Laboratory (LANL) and the Savannah River Technology Center (SRTC) have developed a diverse group of algorithms for processing and analyzing the data that will be collected by the Multispectral Thermal Imager (MTI) after launch late in 1999. Each of these algorithms must be verified by comparison to independent surface and atmospheric measurements. SRTC has selected 13 sites in the continental U.S. for ground truth data collections. These sites include a high altitude cold water target (Crater Lake), cooling lakes and towers in the warm, humid southeastern U.S., Department of Energy (DOE) climate research sites, the NASA Stennis satellite Validation and Verification (V&V) target array, waste sites at the Savannah River Site, mining sites in the Four Corners area and dry lake beds in Nevada. SRTC has established mutually beneficial relationships with the organizations that manage these sites to make use of their operating and research data and to install additional instrumentation needed for MTI algorithm V&V.
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