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Further improvement in the precision of 233U measurements by accelerator mass spectrometry at the Lawrence Livermore National Laboratory.

Description: In response to sponsor interest in October 2005 we proposed two methods for enhancing the precision of {sup 233}U accelerator mass spectrometry (AMS) capabilities at the Lawrence Livermore National Laboratory (LLNL). In a previous report we evaluated the first method and demonstrated that by increasing sample loading by a factor of four coupled with performing four replicates of each sample, we could achieve measurement precision of {approx}1%. Recent modifications to our system have enabled us to test the second proposed method. By changing our setup to normalize {sup 233}U ions counted in a gas ionization chamber to {sup 238}U measured as a current in an off-axis Faraday cup we were able to attain 1% precision without the need for replicate analysis. This method could be further refined to achieve 0.5% precision in samples of interest.
Date: February 4, 2008
Creator: Tumey, S. J.; Brown, T. A.; Hamilton, T. F. & Buchholz, B. A.
Partner: UNT Libraries Government Documents Department

Use of {sup 59}Ni, {sup 99}Tc, and {sup 236}U to monitor the release of radionuclides from objects containing spent nuclear fuel dumped in the Kara Sea

Description: Between 1965 and 1981, five objects - six naval reactor pressure vessels (RPVs) from four former Soviet Union submarines and a special containers from the icebreaker Lenin, each of which contained damaged spent nuclear fuel (SNF) - were dumped in a variety of containments, using a number of sealing methods, at four sites in the Kara Sea. All objects were dumped at sites that varied in depth from 12 to 300 m. This paper examines the use of the long-lived radionuclides {sup 59}Ni, {sup 99}Tc, and {sup 236}U encased within these objects to monitor the breakdown of the containments due to corrosion. Included are discussions of the radionuclide inventory and their release rate model, the estimated radionuclide mass in a typical seawater sample, and the potential for radionuclide measurement via Accelerator Mass Spectrometry (AMS).
Date: April 1, 1998
Creator: Mount, M.E.; Layton, D.W.; Lynn, N.M. & Hamilton, T.F.
Partner: UNT Libraries Government Documents Department

137Cs(90Sr) and Pu isotopes in the Pacific Ocean sources & trends

Description: The main source of artificial radioactivity in the world`s oceans can be attributed to worldwide fallout from atmospheric nuclear weapons testing. Measurements of selected artificial radionuclides in the Pacific Ocean were first conducted in the 1960`s where it was observed that fallout radioactivity had penetrated the deep ocean. Extensive studies carried out during the 1973-74 GEOSECS provided the first comprehensive data on the lateral and vertical distributions of {sup 9O}Sr, {sup 137}Cs and Pu isotopes in the Pacific on a basin wide scale. Estimates of radionuclide inventories in excess of amounts predicted to be delivered by global fallout alone were attributed to close-in fallout and tropospheric inputs from early U.S. tests conducted on Bikini and Enewetak Atolls in the Equatorial Pacific. In general, levels of fallout radionuclides (including {sup 9O}Sr, {sup 137}Cs and Pu isotopes) in the surface waters of the Pacific Ocean have decreased considerably over the past 4 decades and are now much more homogeneously distributed. Resuspension and the subsequent deposition of fallout radionuclides from previously deposited debris on land has become an important source term for the surface ocean. This can be clearly seen in measurements of fallout radionuclides in mineral aerosols over the Korean Peninsula (Yellow dust events). Radionuclides may also be transported from land to sea in river runoff-these transport mechanisms are more important in the Pacific Ocean where large quantities of river water and suspended sands/fluvial sediments reach the coastal zone. Another unique source of artificial radionuclides in the Pacific Ocean is derived from the slow resolubilization and transport of radionuclides deposited in contaminated lagoon and slope sediments near U.S. and French test sites. Although there is a small but significant flux of artificial radionuclides depositing on the sea floor, > 80% of the total 239, {sup 240}Pu inventory and > 95% of the ...
Date: November 1, 1996
Creator: Hamilton, T.F., Millies-Lacrox, J.C. & Hong, G.H.
Partner: UNT Libraries Government Documents Department

Spatial variations of particle scavenging rates within the central and northern Adriatic Sea: use of U--Th disequilibria

Description: Dissolved and particlulate Thorium-234 ({sup 234}Th) were measured in near surface waters from the Central and Northern Adriatic Sea in order to gain an insight into the intensity and variability of active scavenging and particle removal processes. Dissolved {sup 234}Th to Uranium-238 ({sup 238}U) activity ratios vary from 0.21 to 0.75 and clearly imply that {sup 234}Th is being actively scavenged from sea water on a timescale of <3 months. The scavenging rate of dissolved {sup 234}Th with respect to scavenging onto particles appears to correlate with primary productivity measurements. Scavenging and rapid removal of particulate {sup 234}Th from the water column is best explained by a mechanism of zooplankton grazing and fecal pellet production. At one sight in the Jabuka Pit, particulate {sup 234}Th residence times below the pycnocline are long (30-40 days) suggesting that particles are being more readily recycled at these depths. By comparison, in a seawater profile collected near the Po outflow region, {sup 234}Th is depleted with respect to {sup 238}U through the entire water column. We conclude from this assessment that particles in waters near the Po River outflow will be more efficiently transported to bottom sediments compared with those in deeper waters over the Jabuka Pit.
Date: April 1, 1998
Creator: Hamilton, T. F.
Partner: UNT Libraries Government Documents Department

{sup 210}Pb dating of sediments from the central and northern Adriatic Sea: deposition and preservation of sedimentary organic carbon

Description: Lead-210 ({sup 21O}Pb) and organic C depth distribution profiles in sediments from the northern and central Adriatic Sea were measured as part of the EEC funded project on Eutrophic Limits of the Northern Adriatic (ELNA). {sup 210}Pb derived mass-accumulation rates decrease southward from between 0.15 and 0.2 g cm{sup -2}y{sup -1} close to the Po River outflow (> 24 m, water depth) to less than 0.04 g cm{sup -2}y{sup -1} in the Jabuka Pit (246 m, water depth) in the central Adriatic Sea. The mass- accumulation rates obtained in the Jabuka Pit correspond to mean sedimentation rates of about 0.03 cm y{sup -1} (ref. porosity = 0.5) and fall between 5 to 20 times lower than rates found for north Adriatic shelf cores. Estimated sedimentation rates are considered as upper limits because of the possible effects of bioturbation and physical disturbance on the {sup 21O}Pb sedimentary record but are consistent with data from previous work. Rates of sediment accumulation and carbon burial appear to be strongly influenced by the transport of fluvial materials from land and transport of fine-grained particles. First-order estimates of organic C burial rates into surface sediment ranged from 1 to 0.028 mMol cm{sup -2}y{sup -1} between the Po delta and the Jabuka Pit regions, respectively. We estimate that a maximum of 50% of organic C preserved in surface sediment may be derived from biological production in the overlying water column.
Date: April 1, 1998
Creator: Hamilton, T. F., LLNL
Partner: UNT Libraries Government Documents Department

Effect of carbonate soil on transport and dose estimates from long-lived radionuclides at U. S. Pacific Test Site

Description: The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137} Cs), Strontium-90 ({sup 90} Sr), Plutonium-239+ 240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentration ratios (CR) (kBq kg{sup {minus}1} dry weight plant/kBq kg {sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil. The uptake of {sup 137}Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. {sup 137}Cs is bound to the organic fraction of the soil, whereas {sup 90}Sr, {sup 239+240}Pu and {sup 241}Am are primarily bound to soil particles. Assessment of plant uptake for {sup 137}Cs and {sup 90}Sr into locally grown food crops was a major contributing ...
Date: September 1, 1998
Creator: Conrado, C.L.; Hamilton, T.F.; Robison, W.L. & Stoker, A.C.
Partner: UNT Libraries Government Documents Department

Marshall Island radioassay quality assurance program an overview

Description: The Lawrence Livermore National Laboratory has developed an extensive quality assurance program to provide high quality data and assessments in support of the Marshall Islands Dose Assessment and Radioecology Program. Our quality assurance objectives begin with the premise of providing integrated and cost-effective program support (to meet wide-ranging programmatic needs, scientific peer review, litigation defense, and build public confidence) and continue through from design and implementation of large-scale field programs, sampling and sample preparation, radiometric and chemical analyses, documentation of quality assurance/quality control practices, exposure assessments, and dose/risk assessments until publication. The basic structure of our radioassay quality assurance/quality control program can be divided into four essential elements; (1) sample and data integrity control; (2) instrument validation and calibration; (3) method performance testing, validation, development and documentation; and (4) periodic peer review and on-site assessments. While our quality assurance objectives are tailored towards a single research program and the evaluation of major exposure pathways/critical radionuclides pertinent to the Marshall Islands, we have attempted to develop quality assurance practices that are consistent with proposed criteria designed for laboratory accre
Date: September 1, 1998
Creator: Conrado, C.L.; Hamilton, T.F.; Kehl, S.R.; Robison, W.L. & Stoker, A.C.
Partner: UNT Libraries Government Documents Department

Resettlement of Bikini Atoll U.S. Nuclear Test Site

Description: The US conducted a nuclear testing program at Bikini and Enewetak Atolls in the Marshall Islands from 1946 through 1958. Several atolls, including Bikini, were contaminated as a result of the nuclear detonations. Since 1974 the authors have conducted an extensive research and monitoring program to determine the radiological conditions at the atolls, identify the critical radionuclides and pathways, estimate the radiological dose to current or resettling populations, and develop remedial measures to reduce the dose to atoll populations. This paper describes exposure pathways and radionuclides; composition of atoll soils; radionuclide transport and dose estimates; remedial measures; and reduction in dose from a combined option.
Date: September 9, 1999
Creator: Robinson, W.L.; Conrado, C.L.; Stuart, M.L.; Stoker, A.C. & Hamilton, T.F.
Partner: UNT Libraries Government Documents Department

Second interlaboratory comparison study for the analysis of 239Pu in synthetic urine at the microBq (-100 aCi) level by mass spectrometry

Description: As a follow up to the initial 1998 intercomparison study, a second study was initiated in 2001 as part of the ongoing evaluation of the capabilities of various ultra-sensitive methods to analyze {sup 239}Pu in urine samples. The initial study was sponsored by the Department of Energy, Office of International Health Programs to evaluate and validate new technologies that may supersede the existing fission tract analysis (FTA) method for the analysis of {sup 239}Pu in urine at the {micro}Bq/l level. The ultra-sensitive techniques evaluated in the second study included accelerator mass spectrometry (AMS) by LLNL, thermal ionization mass spectrometry (TIMS) by LANL and FTA by the University of Utah. Only the results for the mass spectrometric methods will be presented. For the second study, the testing levels were approximately 4, 9, 29 and 56 {micro}Bq of {sup 239}Pu per liter of synthetic urine. Each test sample also contained {sup 240}Pu at a {sup 240}Pu/{sup 239}Pu atom ratio of {approx}0.15 and natural uranium at a concentration of 50 {micro}Bq/ml. From the results of the two studies, it can be inferred that the best performance at the {micro}Bq level is more laboratory specific than method specific. The second study demonstrated that LANL-TIMS and LLNL-AMS had essentially the same quantification level for both isotopes. Study results for bias and precision and acceptable performance compared to ANSI N13.30 and ANSI N42.22 have been compiled.
Date: January 28, 2005
Creator: McCurdy, D.; Lin, Z.; Inn, K. W.; Bell, R., III; Wagner, S.; Efurd, D. W. et al.
Partner: UNT Libraries Government Documents Department