Calculation of Transactinide Homolog Isotope Production Reactions Possible with the Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory

The LLNL heavy element group has been investigating the chemical properties of the heaviest elements over the past several years. The properties of the transactinides (elements with Z > 103) are often unknown due to their low production rates and short half-lives, which require lengthy cyclotron irradiations in order to make enough atoms for statistically significant evaluations of their chemistry. In addition, automated chemical methods are often required to perform consistent and rapid chemical separations on the order of minutes for the duration of the experiment, which can last from weeks to months. Separation methods can include extraction chromatography, liquid-liquid extraction, or gas-phase chromatography. Before a lengthy transactinide experiment can be performed at an accelerator, a large amount of preparatory work must be done both to ensure the successful application of the chosen chemical system to the transactinide chemistry problem being addressed, and to evaluate the behavior of the lighter elemental homologs in the same chemical system. Since transactinide chemistry is literally performed on one single atom, its chemical properties cannot be determined from bulk chemical matrices, but instead must be inferred from the behavior of the lighter elements that occur in its chemical group and in those of its neighboring elements. By first studying the lighter group homologs in a particular chemical system, when the same system is applied to the transactinide element under investigation, its decay properties can be directly compared to those of the homologues, thereby allowing an inference of its own chemistry. The Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory (LLNL) includes a 1 MV Tandem accelerator, capable of accelerating light ions such as protons to energies of roughly 15 MeV. By using the CAMS beamline, tracers of transactinide homolog elements can be produced both for development of chemical systems and for evaluation of homolog chemical properties. CAMS also offers an environment for testing these systems 'online' by incorporating automated chemical systems into the beamline so that tracers can be created, transported, and chemically separated all on the shorter timescales required for transactinide experiments. Even though CAMS is limited in the types and energies of ions they can accelerate, there are still a wide variety of reactions that can be performed there with commercially available target materials. The half-lives of these isotopes vary over a range that could be used for both online chemistry (where shorter half-lives are required) and benchtop tracers studies (where longer lived isotopes are preferred). In this document, they present a summary of tracer production reactions that could be performed at CAMS, specifically for online, automated chemical studies. They are from chemical groups four through seven, 13, and 14, which would be appropriate for studies of elements 104-107, 113, and 114. Reactions were selected that had (a) commercially available target material, (b) half-lives long enough for transport from a target chamber to an automated chemistry system, and (c) cross-sections at CAMS available projectile energies that were large enough to produce enough atoms to result in a statistically relevant signal after losses for transport and chemistry were considered. In addition, the resulting product atoms had to decay with an observable gamma-ray using standard Ge gamma-ray detectors. The table includes calculations performed for both metal targets and their corresponding oxides

Calculation of Transactinide Homolog Isotope Production Reactions Possible with the Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory

The LLNL heavy element group has been investigating the chemical properties of the heaviest elements over the past several years. The properties of the transactinides (elements with Z > 103) are often unknown due to their low production rates and short half-lives, which require lengthy cyclotron irradiations in order to make enough atoms for statistically significant evaluations of their chemistry. In addition, automated chemical methods are often required to perform consistent and rapid chemical separations on the order of minutes for the duration of the experiment, which can last from weeks to months. Separation methods can include extraction chromatography, liquid-liquid extraction, or gas-phase chromatography. Before a lengthy transactinide experiment can be performed at an accelerator, a large amount of preparatory work must be done both to ensure the successful application of the chosen chemical system to the transactinide chemistry problem being addressed, and to evaluate the behavior of the lighter elemental homologs in the same chemical system. Since transactinide chemistry is literally performed on one single atom, its chemical properties cannot be determined from bulk chemical matrices, but instead must be inferred from the behavior of the lighter elements that occur in its chemical group and in those of its neighboring elements. By first studying the lighter group homologs in a particular chemical system, when the same system is applied to the transactinide element under investigation, its decay properties can be directly compared to those of the homologues, thereby allowing an inference of its own chemistry. The Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory (LLNL) includes a 1 MV Tandem accelerator, capable of accelerating light ions such as protons to energies of roughly 15 MeV. By using the CAMS beamline, tracers of transactinide homolog elements can be produced both for development of chemical systems and for evaluation of homolog chemical properties. CAMS also offers an environment for testing these systems 'online' by incorporating automated chemical systems into the beamline so that tracers can be created, transported, and chemically separated all on the shorter timescales required for transactinide experiments. Even though CAMS is limited in the types and energies of ions they can accelerate, there are still a wide variety of reactions that can be performed there with commercially available target materials. The half-lives of these isotopes vary over a range that could be used for both online chemistry (where shorter half-lives are required) and benchtop tracers studies (where longer lived isotopes are preferred). In this document, they present a summary of tracer production reactions that could be performed at CAMS, specifically for online, automated chemical studies. They are from chemical groups four through seven, 13, and 14, which would be appropriate for studies of elements 104-107, 113, and 114. Reactions were selected that had (a) commercially available target material, (b) half-lives long enough for transport from a target chamber to an automated chemistry system, and (c) cross-sections at CAMS available projectile energies that were large enough to produce enough atoms to result in a statistically relevant signal after losses for transport and chemistry were considered. In addition, the resulting product atoms had to decay with an observable gamma-ray using standard Ge gamma-ray detectors. The table includes calculations performed for both metal targets and their corresponding oxides

Summary of Blast Shield and Material Testing for Development of Solid Debris Collection at the National Ignition Facility (NIF)

The ability to collect solid debris from the target chamber following a NIF shot has application for both capsule diagnostics, particularly for fuel-ablator mix, and measuring cross sections relevant to the Stockpile Stewardship program and nuclear astrophysics. Simulations have shown that doping the capsule with up to 10{sup 15} atoms of an impurity not otherwise found in the capsule does not affect its performance. The dopant is an element that will undergo nuclear activations during the NIF implosion, forming radioactive species that can be collected and measured after extraction from the target chamber. For diagnostics, deuteron or alpha induced reactions can be used to probe the fuel-ablator mix. For measuring neutron cross sections, the dopant should be something that is sensitive to the 14 MeV neutrons produced through the fusion of deuterium and tritium. Developing the collector is a challenge due to the extreme environment of the NIF chamber. The collector surface is exposed to a large photon flux from x-rays and unconverted laser light before it is exposed to a debris wind that is formed from vaporized material from the target chamber center. The photons will ablate the collector surface to some extent, possibly impeding the debris from reaching the collector and sticking. In addition, the collector itself must be mechanically strong enough to withstand the large amount of energy it will be exposed to, and it should be something that will be easy to count and chemically process. In order to select the best material for the collector, a variety of different metals have been tested in the NIF chamber. They were exposed to high-energy laser shots in order to evaluate their postshot surface characterization, morphology, degree of melt, and their ability to retain debris from the chamber center. The first set of samples consisted of 1 mm thick pieces of aluminum that had been fielded in the chamber as blast shields protecting the neutron activation diagnostic. Ten of these pieces were fielded at the equator and one was fielded on the pole. The shields were analyzed using a combination of scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), x-ray fluorescence (XRF), neutron activation analysis (NAA) and chemical leaching followed by mass spectrometry. On each shield, gold debris originating from the gold hohlraum was observed, as well as large quantities of debris that were present in the center of the target chamber at the time of the shot (i.e., stainless steel, indium, copper, etc.) Debris was visible in the SEM as large blobs or splats of material that had encountered the surface of the aluminum and stuck. The aluminum itself had obviously melted and condensed, and some of the large debris splats arrived after the surface had already hardened. Melt depth was determined by cross sectioning the pieces and measuring the melted surface layers via SEM. After the SEM analysis was completed, the pieces were sent for NAA at the USGS reactor and were analyzed by U. Greife at the Colorado School of Mines. The NAA showed that the majority of gold mass present on the shields was not in the form of large blobs and splats, but was present as small particulates that had most likely formed as condensed vapor. Further analysis showed that the gold was entrained in the melted aluminum surface layers and did not extend down into the bulk of the aluminum. Once the gold mass was accounted for from the NAA, it was determined that the aluminum fielded at the equator was collecting a fraction of the total gold hohlraum mass equivalent to 120% {+-} 10% of the solid angle subtended by the shield. The attached presentation has more information on the results of the aluminum blast shield analysis. In addition to the information given in the presentation, the surfaces of the shields have been chemically leached and submitted for mass spectrometric analysis. The results from that analysis are expected to arrive after the due date of this report and will be written up at a later time. Based on the results of the aluminum blast shield analysis, it was determined that additional materials needed to be tested as potential collectors in the NIF chamber. 1-2 mm thick pieces of tantalum, niobium, vanadium, silver, titanium, molybdenum, and graphite foil were fielded in the Wedge Range Filter (WRF) mount at a distance of 50 cm from target chamber center during the shock timing campaign. The pieces were subsequently removed and analyzed in a similar fashion to the aluminum shields. As of this writing, the pieces are still under analysis, but initial results indicate that gold debris was collected on the various materials. Currently, the pieces are being cross-sectioned so that the melt depths of each material can be compared. In addition, NAA and/or mass spectrometry will be performed in order to determine the total gold mass that was collected on each surface

DEVELOPMENT OF SOLID COLLECTION DIAGNOSTICS ON NIF THROUGH BLAST SHIELD ANALYSIS

Radiochemical analysis of post-shot debris inside the National Ignition Facility (NIF) target chamber can help determine various diagnostic parameters associated with the implosion efficiency of the fusion capsule. This capability is limited by the amount of target isotope that can be loaded inside the capsule ablator without affecting performance and the collection efficiency of the capsule debris after implosion. Prior to designing a collection system, the chemical nature and distribution of the debris inside the chamber must be determined and analysis methods developed. The focus of our current work has been on determining the elemental composition and distribution of debris on various blast shields and witness plates that were exposed to the chamber during ignition shots that occurred in 2009. These passive collection plates were used to develop both non-destructive and chemical analysis techniques to determine debris composition and melt depth at various shot energy profiles. A summary of these data will be presented along with our current strategy for the 2011 campaign

Summary of Blast Shield and Material Testing for Development of Solid Debris Collection at the National Ignition Facility (NIF)

The ability to collect solid debris from the target chamber following a NIF shot has application for both capsule diagnostics, particularly for fuel-ablator mix, and measuring cross sections relevant to the Stockpile Stewardship program and nuclear astrophysics. Simulations have shown that doping the capsule with up to 10{sup 15} atoms of an impurity not otherwise found in the capsule does not affect its performance. The dopant is an element that will undergo nuclear activations during the NIF implosion, forming radioactive species that can be collected and measured after extraction from the target chamber. For diagnostics, deuteron or alpha induced reactions can be used to probe the fuel-ablator mix. For measuring neutron cross sections, the dopant should be something that is sensitive to the 14 MeV neutrons produced through the fusion of deuterium and tritium. Developing the collector is a challenge due to the extreme environment of the NIF chamber. The collector surface is exposed to a large photon flux from x-rays and unconverted laser light before it is exposed to a debris wind that is formed from vaporized material from the target chamber center. The photons will ablate the collector surface to some extent, possibly impeding the debris from reaching the collector and sticking. In addition, the collector itself must be mechanically strong enough to withstand the large amount of energy it will be exposed to, and it should be something that will be easy to count and chemically process. In order to select the best material for the collector, a variety of different metals have been tested in the NIF chamber. They were exposed to high-energy laser shots in order to evaluate their postshot surface characterization, morphology, degree of melt, and their ability to retain debris from the chamber center. The first set of samples consisted of 1 mm thick pieces of aluminum that had been fielded in the chamber as blast shields protecting the neutron activation diagnostic. Ten of these pieces were fielded at the equator and one was fielded on the pole. The shields were analyzed using a combination of scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), x-ray fluorescence (XRF), neutron activation analysis (NAA) and chemical leaching followed by mass spectrometry. On each shield, gold debris originating from the gold hohlraum was observed, as well as large quantities of debris that were present in the center of the target chamber at the time of the shot (i.e., stainless steel, indium, copper, etc.) Debris was visible in the SEM as large blobs or splats of material that had encountered the surface of the aluminum and stuck. The aluminum itself had obviously melted and condensed, and some of the large debris splats arrived after the surface had already hardened. Melt depth was determined by cross sectioning the pieces and measuring the melted surface layers via SEM. After the SEM analysis was completed, the pieces were sent for NAA at the USGS reactor and were analyzed by U. Greife at the Colorado School of Mines. The NAA showed that the majority of gold mass present on the shields was not in the form of large blobs and splats, but was present as small particulates that had most likely formed as condensed vapor. Further analysis showed that the gold was entrained in the melted aluminum surface layers and did not extend down into the bulk of the aluminum. Once the gold mass was accounted for from the NAA, it was determined that the aluminum fielded at the equator was collecting a fraction of the total gold hohlraum mass equivalent to 120% {+-} 10% of the solid angle subtended by the shield. The attached presentation has more information on the results of the aluminum blast shield analysis. In addition to the information given in the presentation, the surfaces of the shields have been chemically leached and submitted for mass spectrometric analysis. The results from that analysis are expected to arrive after the due date of this report and will be written up at a later time. Based on the results of the aluminum blast shield analysis, it was determined that additional materials needed to be tested as potential collectors in the NIF chamber. 1-2 mm thick pieces of tantalum, niobium, vanadium, silver, titanium, molybdenum, and graphite foil were fielded in the Wedge Range Filter (WRF) mount at a distance of 50 cm from target chamber center during the shock timing campaign. The pieces were subsequently removed and analyzed in a similar fashion to the aluminum shields. As of this writing, the pieces are still under analysis, but initial results indicate that gold debris was collected on the various materials. Currently, the pieces are being cross-sectioned so that the melt depths of each material can be compared. In addition, NAA and/or mass spectrometry will be performed in order to determine the total gold mass that was collected on each surface

Summary of Disposable Debris Shields (DDS) Analysis for Development of Solid Debris Collection at NIF

Collection of solid debris from the National Ignition Facility (NIF) is being developed both as a diagnostic tool and as a means for measuring nuclear reaction cross sections relevant to the Stockpile Stewardship Program and nuclear astrophysics. The concept is straightforward; following a NIF shot, the debris that is produced as a result of the capsule and hohlraum explosion would be collected and subsequently extracted from the chamber. The number of nuclear activations that occurred in the capsule would then be measured through a combination of radiation detection and radiochemical processing followed by mass spectrometry. Development of the catcher is challenging due to the complex environment of the NIF target chamber. The collector surface is first exposed to a large photon flux, followed by the debris wind that is produced. The material used in the catcher must be mechanically strong in order to withstand the large amount of energy it is exposed to, as well as be chemically compatible with the form and composition of the debris. In addition, the location of the catcher is equally important. If it is positioned too close to the center of the target chamber, it will be significantly ablated, which could interfere with the ability of the debris to reach the surface and stick. If it is too far away, the fraction of the debris cloud collected will be too small to result in a statistically significant measurement. Material, geometric configuration, and location must all be tested in order to design the optimal debris collection system for NIF. One of the first ideas regarding solid debris collection at NIF was to use the disposable debris shields (DDS), which are fielded over the final optics assemblies (FOA) 7 m away from the center of the target chamber. The DDS are meant to be replaced after a certain number of shots, and if the shields could be subsequently analyzed after removal, it would serve as a mechanism for fielding a relatively large collection area through the use of a part meant to be replaced regularly. The solid angle covered by one of the shields is roughly 10{sup -4} of 4{pi}. If several shields were analyzed at once, it would increase the solid angle of the collection area accordingly. The glass shields consist of ammonia hardened silica with a sol gel coating and kapton tape around the edge. The square sheets are 14-inch on each side. The original shields were 1 mm thick, but it was determined that a thicker shield (3.3 mm) was more effective in preventing debris from reaching the FOA. The Solid Radchem group received two sets of DDS as part of our evaluation of the potential use of the DDS as solid debris collectors. The first set consisted of two 3.3 mm shields, one each from the top and bottom of the chamber (the '3mm set'). The second set consisted of four 1mm shields, one from the top of the chamber and the other three from the bottom (the 'IFSA set'). For each set, the shields were cut into smaller subsamples, which were then imaged using scanning electron microscopy (SEM) followed by chemical leaching and mass spectrometry. The purpose was to evaluate both the quantity and identity of the debris that was present on the DDS surfaces, and to determine if any of the capsule debris was reaching the chamber walls. In addition, potential enhancement due to gravity in the chamber was evaluated by directly comparing shields fielded in the top and bottom of the chamber. Based on the results, the use of the DDS as debris collectors would be evaluated. The results from both sets were presented to the DDS Working Group. The slides are attached to this document. The 3mm set results are presented first, followed by the results from the IFSA set. In both cases it was determined that a small fraction of the overall debris field was collected on the DDS. This means that the debris that is formed during a NIF shot is condensing out of the plasma and depositing on surfaces closer to the target chamber center, or else it is simply falling to the bottom of the chamber. In either case, it was determined that using the DDS, or fielding a debris collector at the chamber wall, was not feasible for solid debris collection at NIF due to the small amount of debris that had been collected. In addition, since the glass shields suffered quite a bit of damage from particles impacting the surface, glass was ruled out as a collection medium