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Detection of 99Tc by accelerator mass spectrometry: preliminary investigations

Description: Accelerator mass spectrometry is an established technique for the detection of long-lived radionuclides at environmental levels. At LLNL, planned facility upgrades and advances in detection techniques are allowing us to explore the applicability of AMS to isotopes not previously pursued. One such isotope is technetium-99. We have performed a number of preliminary tests to examine the technical feasibility of AMS for the detection of {sup 99}Tc. The questions addressed were negative ion production in the cesium sputter source, transport efficiency for the ions through the spectrometer, and detection efficiency for {sup 99}Tc ions after the spectrometer. Based on the positive results of these tests, we have begun to develop a measurement protocol. Technetium is co-precipitated with rhodium, added as a carrier, which provides a sample form appropriate for sputtering and an isotope for AMS normalization. The {sup 99}Tc is determined from the measured {sup 99}Tc/{sup 103}Rh ratio. To reduce interference from the isobar {sup 99}Ru, an oxidation/distillation method was employed to lower ruthenium in the rhodium stock solution. Characteristic projectile L x-rays are used for ion detection to allow further subtraction of {sup 99}Ru. Results for a series of standards demonstrated linearity and reproducibility. A sensitivity of {approx}500 fg {sup 99}Tc was obtained in this preliminary work, and indications are that a sensitivity in the low femtogram range should be achievable.
Date: April 1, 1997
Creator: McAninch, J. E., LLNL
Partner: UNT Libraries Government Documents Department

Technetium-99 and strontium-90: Abundance determination at ultratrace sensitivity by AMS as signatures of undeclared nuclear reprocessing activity

Description: The purpose of this White Paper is to examine the use of the ultratrace technique Accelerator Mass Spectrometry (AMS) to lower detection limits for {sup 99}Tc and {sup 90}Sr, and to examine the utility of these isotopes as signatures of a convert reprocessing facility. The International Atomic Energy Agency (IAEA) has committed to improving the effectiveness of the IAEA Safeguards System. This is in some degree a result of the discovery in 1991 of an undeclared Iraqi EMIS program. Recommendations from the March 1993 Consultants Group Meeting have resulted in several studies and follow on field trials to identify environmental signatures from covert nuclear fuel reprocessing activity. In particular, the April, 1993 reports of the Standing Advisory Group on Safeguards Implementation (SAGSI) identified the long-lived radioisotopes Technetium-99 and strontium-90 as two reliable signatures of fuel reprocessing activity. This report also suggested pathways in the chemical processing of irradiated fuel where these elements would be volatilized and potentially released in amounts detectable with ultratrace sensitivity techniques. Based on measured {sup 99}Tc background levels compiled from a variety of sources, it is estimated that AMS can provide 10% measurements of environmental levels of {sup 99}Tc in a few minutes using modestly sized samples: a few grams for soils, plants, or animal tissues; one to several liters for rain or seawater samples; and tens to hundreds of cubic meters for air sampling. Small sample sizes and high sample throughput result in significant increases in feasibility, cost effectiveness, and quality of data for a regional monitoring program. Similar results are expected for {sup 90}Sr.
Date: March 1, 1995
Creator: McAninch, J.E. & Proctor, I.D.
Partner: UNT Libraries Government Documents Department

Proof-of-concept development of PXAMS (projectile x-ray accelerator mass spectrometry)

Description: Prior to the current work, accelerator mass spectrometry (AMS) was limited to a set of {approximately}8--10 isotopes. This limitation is caused primarily by the inability to discriminate against stable atomic isobars. An analysis scheme that combines the isotopic sensitivity of AMS with similar isobar selectivity would open a large new class of isotope applications. This project was undertaken to explore the use of characteristic x rays as a method for the detection and identification of ions,and to allow the post-spectrometer rejection of isobaric interferences for isotopes previously inaccessible to AMS. During the second half of FY94 (with Advanced Concepts funding from the Office of Non-Proliferation and National Security), we examined the feasability of this technique, which we are referring to as PXAMS (Projectile X ray AMS), to the detection of several isotopes at Lawrence Livermore National Laboratory (LLNL). In our first exploratory work, we measured the x ray yield vs energy for {sup 80}Se ions stopped in a thick Y target. These results, demonstrated that useful detection efficiencies could be obtained for Se ions at energies accessible with our accelerator, and that the count rate from target x rays is small compared to the Se K{alpha} rate. We followed these measurements with a survey of x ray yields for Z = 14-46.
Date: March 1, 1996
Creator: Proctor, I.D.; Roberts, M.L.; McAninch, J.E. & Bench, G.S.
Partner: UNT Libraries Government Documents Department

Viability of long-lived fission products as signatures in forensic radiochemistry

Description: Forensic radiochemistry refers to studies on special nuclear materials, related to nonproliferation and anti-smuggling efforts. AMS (accelerator mass spectroscopy) measurement of long-lived fission products and U and Pu isotopes has the potential to significantly aid the field of forensic radiochemistry by providing new or more sensitive signatures and improving on the speed with which they can be determined. Expanding the suite of signatures obtainable form an illicit sample of special nuclear material increases the likelihood that its point of origin can be positively identified, leveraging LLNL`s impact on policy decisions regarding national security.
Date: January 1, 1997
Creator: McAninch, J.E.; Proctor, I.D.; Stoyer, N.J. & Moody, K.J.
Partner: UNT Libraries Government Documents Department

Measurement of {sup 63}Ni and {sup 59}Ni by accelerator mass spectrometry using characteristic projectile x-rays

Description: The long-lived isotopes of nickel ({sup 59}Ni, {sup 63}Ni) have current and potential use in a number of applications including cosmic radiation studies, biomedical tracing, characterization of low-level radioactive wastes, and neutron dosimetry. Methods are being developed at LLNL for the routine detection of these isotopes by AMS. One intended application is in Hiroshima dosimetry. The reaction {sup 63}Cu(n,p){sup 63}Ni has been identified as one of a small number of reactions which might be used for the direct determination of the fast neutron fluence emitted by the Hiroshima bomb. AMS measurement of {sup 63}Ni(t{sub 1/2} = 100 y) requires the chemical removal of {sup 63}Cu, which is a stable isobar of {sup 63}Ni. Following the electrochemical separation of Ni from gram-sized copper samples, the Cu concentration is further lowered to < 2 x 10{sup -8} (Cu/Ni) using the reaction of Ni with carbon monoxide to form the gas Ni(CO){sub 4}. The Ni(CO){sub 4} is thermally decomposed directly in sample holders for measurement by AMS. After analysis in the AMS spectrometer, the ions are identified using characteristic projectile x-rays, allowing further rejection of remaining {sup 63}Cu. In a demonstration experiment, {sup 63}Ni was measured in Cu wires (2-20 g) which had been exposed to neutrons from a {sup 252}Cf source. We successfully measured {sup 63}Ni at levels necessary for the measurement of Cu samples exposed near the Hiroshima hypocenter. For the demonstration samples, the Cu content was chemically reduced by a factor of 10{sup 12} with quantitative retention of {sup 63}Ni. Detection sensitivity (3{sigma}) was {approximately}20 fg {sup 63}Ni in 1 mg Ni carrier ({sup 63}Ni/Ni {approx} 2 x 10{sup -11}). Significant improvements in sensitivity are expected with planned incremental changes in the methods. Preliminary results indicate that a similar sensitivity is achievable for {sup 59}Ni (t{sub 1/2} = 10{sup 5} ...
Date: May 1996
Creator: McAninch, J. E.; Hainsworth, L. J. & Marchetti, A. A.
Partner: UNT Libraries Government Documents Department

Hydrologic and geochemical controls on the transport of radionuclides in natural undisturbed arid environments as determined by accelerator mass spectrometry measurements. 1997 annual progress report

Description: 'During FY97 this study has developed unique accelerator mass spectrometry (AMS) analytical techniques for measurement of {sup 99}Tc and {sup 129}I, which compliments an improved capability for measurement of {sup 36}Cl. The ability to measure these nuclides in natural soil samples has been demonstrated through analytical results obtained during FY97. Methods to determine the distribution of these nuclides in their natural setting, which will vary depending on site-specific chemical conditions, have also been developed. Spatially well-characterized soil samples have been collected from the vadose zone to a depth of -5 meters at the Nevada Test Site. To do this, a deep trench has been excavated and the geological setting for the soils has been well documented. Physical, chemical, and isotopic analysis of these soil samples during the course of this research project will result in a numerical computer model for moisture and radionuclide migration in arid soils that is valuable to nuclear waste storage, site remediation, and groundwater recharge concerns.'
Date: January 1, 1997
Creator: Nimz, G.J.; Caffee, M.W.; Finkel, R.C. & McAninch, J.E.
Partner: UNT Libraries Government Documents Department

PXAMS -- Projectile X ray AMS: X ray yields and applications

Description: Characteristic x rays have recently been explored as a method for the detection and identification of ions in accelerator mass spectrometry (AMS). After analysis in the AMS spectrometer, the ions stop in an appropriately chosen target and the induced x rays identify the ions by atomic number. For the application of AMS to higher mass isotopes, characteristic x rays allow significantly better discrimination of competing atomic isobars than is possible using energy loss detectors. Characteristic x rays also show promise as a convenient component in hybrid detection systems. Measurements of x ray yields are presented for Si, Fe, Ni, Se, Mo, and Pd ions of 0.5--2 MeV/AMU. The yields rise by more than a factor of 10 over this energy range, and approach 1 x-ray per incident ion at 2 MeV/AMU for the lighter ions. Preliminary work on the application of PXAMS to the detection of {sup 79}Se is described.
Date: October 7, 1994
Creator: McAninch, J. E.; Bench, G. S.; Freeman, S. P. H. T.; Roberts, M. L.; Southon, J. R.; Vogel, J. S. et al.
Partner: UNT Libraries Government Documents Department

Measurement of Beryllium in Biological Samples by Accelerator Mass Spectrometry: Applications for Studying Chronic Beryllium Disease

Description: A method using accelerator mass spectrometry (AMS) has been developed for quantifying attomoles of beryllium (Be) in biological samples. This method provides the sensitivity to trace Be in biological samples at very low doses with the purpose of identifying the molecular targets involved in chronic beryllium disease. Proof of the method was tested by administering 0.001, 0.05, 0.5 and 5.0 {micro}g {sup 9}Be and {sup 10}Be by intraperitoneal injection to male mice and removing spleen, liver, femurs, blood, lung, and kidneys after 24 h exposure. These samples were prepared for AMS analysis by tissue digestion in nitric acid, followed by further organic oxidation with hydrogen peroxide and ammonium persulfate and lastly, precipitation of Be with ammonium hydroxide, and conversion to beryllium oxide at 800 C. The {sup 10}Be/{sup 9}Be ratio of the extracted beryllium oxide was measured by AMS and Be in the original sample was calculated. Results indicate that Be levels were dose-dependent in all tissues and the highest levels were measured in the spleen and liver. The measured {sup 10}Be/{sup 9}Be ratios spanned 4 orders of magnitude, from 10{sup -10} to 10{sup -14}, with a detection limit of 3.0 x 10{sup -14}, which is equivalent to 0.8 attomoles of {sup 10}Be. These results show that routine quantification of nanogram levels of Be in tissues is possible and that AMS is a sensitive method that can be used in biological studies to understand the molecular dosimetry of Be and mechanisms of toxicity.
Date: April 15, 2004
Creator: Chiarappa-Zucca, M L; Finkel, R C; Martinelli, R E; McAninch, J E; Nelson, D O & Turtletaub, K W
Partner: UNT Libraries Government Documents Department

Plutonium measurements by accelerator mass spectrometry at LLNL

Description: Mass spectrometric methods provide sensitive, routine, and cost-effective analyses of long-lived radionuclides. Here the authors report on the status of work at Lawrence Livermore National Laboratory (LLNL) to develop a capability for actinide measurements by accelerator mass spectrometry (AMS) to take advantage of the high potential of AMS for rejection of interferences. This work demonstrates that the LLNL AMS spectrometer is well-suited for providing high sensitivity, robust, high throughput measurements of plutonium concentrations and isotope ratios. Present backgrounds are {approximately}2 x 10{sup 7}atoms per sample for environmental samples prepared using standard alpha spectrometry protocols. Recent measurements of {sup 239+240}Pu and {sup 241}Pu activities and {sup 240}Pu/{sup 239}Pu isotope ratios in IAEA reference materials agree well with IAEA reference values and with alpha spectrometry and recently published ICP-MS results. Ongoing upgrades of the AMS spectrometer are expected to reduce backgrounds below 1 x 10{sup 6} atoms per sample while allowing simplifications of the sample preparation chemistry. These simplifications will lead to lower per-sample costs, higher throughput, faster turn around and, ultimately, to larger and more robust data sets.
Date: October 26, 1999
Creator: McAninch, J E; Hamilton, T F; Broan, T A; Jokela, T A; Knezovich, T J; Ognibene, T J et al.
Partner: UNT Libraries Government Documents Department

Biological sample preparation and {sup 41}Ca AMS measurement at LLNL

Description: Calcium metabolism in biology may be better understood by the use of {sup 41}Ca labels, although detection by accelerator mass spectrometry (AMS) is required. Methodologies for preparation of urine samples and subsequent AMS measurement were investigated. Novel attempts at preparing CaH{sub 2} were unsuccessful, but CaF{sub 2} of sufficient purity could be produced by precipitation of calcium from urine as oxalate, followed by separation of calcium by cation exchange chromatography and washing the CaF{sub 2} precipitate. The presence of some remaining impurities could be compensated for by selecting the appropriate accelerated ion charge state for AMS. The use of projectile x rays for isobar discrimination was explored as an alternative to the conventional dE/dx device.
Date: October 10, 1994
Creator: Freeman, S. P. H. T.; Southon, J. R.; Bench, G. S.; McAninch, J. E.; Serfass, R. E.; Fang, Y. et al.
Partner: UNT Libraries Government Documents Department

Hydrologic resources management program and underground test area FY 1999 progress report

Description: This report presents the results from fiscal year (FY) 1999 technical studies conducted by Lawrence Livermore National Laboratory (LLNL) as part of the Hydrology and Radionuclide Migration Program (HRMP) and Underground Test Area (UGTA) work-for-others project. This report is the latest in a series of annual reports published by LLNL to document the migration of radionuclides and controls of radionuclide movement at the Nevada Test Site. The FY 1999 studies highlighted in this report are: (1) Chapter 1 provides the results from flow-through leaching of nuclear melt glasses at 25 C and near-neutral pH using dilute bicarbonate groundwaters. (2) Chapter 2 reports on a summary of the size and concentration of colloidal material in NTS groundwaters. (3) Chapter 3 discusses the collaboration between LLNL/ANCD (Analytical and Nuclear Chemistry Division) and the Center for Accelerator Mass Spectrometry (CAMS) to develop a technique for analyzing NTS groundwater for 99-Technicium ({sup 99}Tc) using accelerator mass spectrometry (AMS). Since {sup 99}Tc is conservative like tritium in groundwater systems, and is not sorbed to geologic material, it has the potential for being an important tool for radionuclide migration studies. (4) Chapter 4 presents the results of secondary ion mass spectrometry measurements of the in-situ distribution of radionuclides in zeolitized tuffs from cores taken adjacent to nuclear test cavities and chimneys. In-situ measurements provide insight to the distribution of specific radionuclides on a micro-scale, mineralogical controls of radionuclide sorption, and identification of migration pathways (i.e., matrix diffusion, fractures). (5) Chapter 5 outlines new analytical techniques developed in LLNL/ANCD to study hydrologic problems at the NTS using inductively coupled plasma mass spectrometry (ICP-MS). With costs for thermal-ionization mass spectrometry (TIMS) increasing relative to sample preparation time and facility support, ICP-MS technology provides a means for rapidly measuring dilute concentrations of radionuclides with precision and abundance sensitivity comparable ...
Date: July 1, 2000
Creator: Smith, D K; Eaton, G F; Rose, T P; Moran, J E; Brachmann, A; McAninch, J E et al.
Partner: UNT Libraries Government Documents Department

Activation Measurements for Thermal Neutrons, U.S. Measurements of 36Cl in Mineral Samples from Hiroshima and Nagasaki; and Measurement of 63 Ni in Copper Samples From Hiroshima by Accelerator Mass Spectrometry

Description: The present paper presents the {sup 36}Cl measurement effort in the US. A large number of {sup 36}Cl measurements have been made in both granite and concrete samples obtained from various locations and distances in Hiroshima and Nagasaki. These measurements employed accelerator mass spectrometry (AMS) to quantify the number of atoms of {sup 36}Cl per atom of total Cl in the sample. Results from these measurements are presented here and discussed in the context of the DS02 dosimetry reevaluation effort for Hiroshima and Nagasaki atomic-bomb survivors. The production of {sup 36}Cl by bomb neutrons in mineral samples from Hiroshima and Nagasaki was primarily via the reaction {sup 35}Cl(n,{gamma}){sup 36}Cl. This reaction has a substantial thermal neutron cross-section (43.6 b at 0.025 eV) and the product has a long half-life (301,000 y). hence, it is well suited for neutron-activation detection in Hiroshima and Nagasaki using AMS more than 50 years after the bombings. A less important reaction for bomb neutrons, {sup 39}K(n,{alpha}){sup 36}Cl, typically produces less than 10% of the {sup 36}Cl in mineral samples such as granite and concrete, which contain {approx} 2% potassium. In 1988, only a year after the publication of the DS86 final report (Roesch 1987), it was demonstrated experimentally that {sup 36}Cl measured using AMS should be able to detect the thermal neutron fluences at the large distances most relevant to the A-bomb survivor dosimetry. Subsequent measurements in mineral samples from both Hiroshima and Nagasaki validated the experimental findings. The potential utility of {sup 36}Cl as a thermal neutron detector in Hiroshima was first presented by Haberstock et al. who employed the Munich AMS facility to measure {sup 36}Cl/Cl ratios in a gravestone from near the hypocenter. That work subsequently resulted in an expanded {sup 36}Cl effort in Germany that paralleled the US work. More recently, ...
Date: January 14, 2005
Creator: Straume, Tore; Marchetti, Alfredo A.; Egbert, Stephen D.; Roberts, James A.; Men, Ping; Fujita, Shoichiro et al.
Partner: UNT Libraries Government Documents Department