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

Report on 240Am(n,x) surrogate cross section test measurement

The main goal of the test measurement was to determine the feasibility of the {sup 243}Am(p,t) reaction as a surrogate for {sup 240}Am(n,f). No data cross section data exists for neutron induced reactions on {sup 240}Am; the half-life of this isotope is only 2.1 days making direct measurements difficult, if not impossible. The 48-hour experiment was conducted using the STARS/LIBERACE experimental facility located at the 88 Inch Cyclotron at Lawrence Berkeley National Laboratory in August 2011. A description of the experiment and results is given. The beam energy was initially chosen to be 39 MeV in order to measure an equivalent neutron energy range from 0 to 20 MeV. However, the proton beam was not stopped in the farady cup and the beam was deposited in the surrounding shielding material. The shielding material was not conductive, and a beam current, needed for proper tuning of the beam as well as experimental monitoring, could not be read. If the {sup 240}Am(n,f) surrogate experiment is to be run at LBNL, simple modifications to the beam collection site will need to be made. The beam energy was reduced to 29 MeV, which was within an energy regime of prior experiments and tuning conditions at STARS/LIBERACE. At this energy, the beam current was successfully tuned and measured. At 29 MeV, data was collected with both the {sup 243}Am and {sup 238}U targets. An example particle identification plot is shown in Fig. 1. The triton-fission coincidence rate for the {sup 243}Am target and {sup 238}U target were measured. Coincidence rates of 0.0233(1) cps and 0.150(6) cps were observed for the {sup 243}Am and {sup 238}U targets, respectively. The difference in count rate is largely attributed to the available target material - the {sup 238}U target contains approximately 7 times more atoms than the {sup 243}Am. A proton beam current of {approx}0.7 nA was used for measurements on both targets. Assuming a full experimental run under similar conditions, an estimate for the run time needed was made. Figure 2 shows the number of days needed as a function of acceptable uncertainty for a measurement of 1-20 MeV equivalent neutron energy, binned into 200 keV increments. A 5% measurement will take 3 days for U, but 20 days for Am. It may be difficult to be the sole user of the LBNL cyclotron, or another facility, for such an extended period. However, a 10% measurement will take 19 hours for U, and 5 days for Am. Such a run period is more reasonable and will allow for the first ever measurement of the {sup 240}Am(n,f) cross section. We also anticipate 40% more beam time being available at Texas A&M Cyclotron Institute compared to LBNL in FY2012. The increased amount of beam time will allow us to accumulate better statistics then what would have been available at LBNL

Surrogate Measurement of the \u3csup\u3e238\u3c/sup\u3ePu(\u3cem\u3en,f\u3c/em\u3e\u3c/em\u3e) Cross Section

The neutron-induced fission cross section of 238Pu was determined using the surrogate ratio method. The (n,f) cross section over an equivalent neutron energy range 5–20 MeV was deduced from inelastic α-induced fission reactions on 239Pu, with 235U(α,α′f) and 236U(α,α′f) used as references. These reference reactions reflect 234U(n,f) and 235U(n,f) yields, respectively. The deduced 238Pu(n,f) cross section agrees well with standard data libraries up to ~10 MeV, although larger values are seen at higher energies. The difference at higher energies is less than 20%

Solid Collection Efforts: Ta Collimator Evaluation

Ta collimator sets that were part of the gated x-ray detector diagnostic (GXD) at NIF were analyzed for debris distribution and damage in 2011. These disks (ranging in thickness from 250 to 750 {mu}m) were fielded approximately 10 cm from target chamber center (TCC) on various symcap, THD and re-emit shots. The nose cone holder and forward Ta collimator (facing target chamber center, TCC) from all shots show evidence of surface melt. Non-destructive analysis techniques such as optical microscopy, surface profilometry, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and x-ray fluorescence (XRF) were used to determine debris composition and degree of deformation associated with each Ta disk. Molten debris from the stainless steel nose cone contaminated the surface of the collimators along with other debris associated with the target assembly (Al, Si, Cu, Au and In). Surface elemental analysis of the forward collimator Ta disks indicates that Au hohlraum debris is less concentrated on these samples versus those fielded 50 cm from TCC in the wedge range filter (WRF) assembly. It is possible that the Au is distributed below or within the stainless steel melt layer covering the disk, as most of the foreign debris is captured in the melted coating. The other disks (fielded directly behind the forward collimator in a sandwiched configuration) have visible forms of deformation and warping. The degree of warping increases as the shock wave penetrates the assembly with the most damage sustained on the back collimator. In terms of developing a solid collection capability, the collimator analyses suggests that close proximity may cause more interference with capsule debris collection and more damage to the surface of the collector diagnostic. The analyses of the Ta collimators were presented to the Target and Laser Interaction Sphere (TaLIS) group; a representative presentation is attached to this document

Solid Collection Efforts: Ta Collimator Evaluation

Ta collimator sets that were part of the gated x-ray detector diagnostic (GXD) at NIF were analyzed for debris distribution and damage in 2011. These disks (ranging in thickness from 250 to 750 {mu}m) were fielded approximately 10 cm from target chamber center (TCC) on various symcap, THD and re-emit shots. The nose cone holder and forward Ta collimator (facing target chamber center, TCC) from all shots show evidence of surface melt. Non-destructive analysis techniques such as optical microscopy, surface profilometry, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and x-ray fluorescence (XRF) were used to determine debris composition and degree of deformation associated with each Ta disk. Molten debris from the stainless steel nose cone contaminated the surface of the collimators along with other debris associated with the target assembly (Al, Si, Cu, Au and In). Surface elemental analysis of the forward collimator Ta disks indicates that Au hohlraum debris is less concentrated on these samples versus those fielded 50 cm from TCC in the wedge range filter (WRF) assembly. It is possible that the Au is distributed below or within the stainless steel melt layer covering the disk, as most of the foreign debris is captured in the melted coating. The other disks (fielded directly behind the forward collimator in a sandwiched configuration) have visible forms of deformation and warping. The degree of warping increases as the shock wave penetrates the assembly with the most damage sustained on the back collimator. In terms of developing a solid collection capability, the collimator analyses suggests that close proximity may cause more interference with capsule debris collection and more damage to the surface of the collector diagnostic. The analyses of the Ta collimators were presented to the Target and Laser Interaction Sphere (TaLIS) group; a representative presentation is attached to this document

Electrodeposition of U and Pu on Thin C and Ti Substrates

Physics experiments aimed at deducing key parameters for use in a variety of programs critical to the mission of the National Laboratories require actinide targets placed onto various substrates. The target material quantity and the substrate desired depend upon the type of experiment being designed. The physicist(s) responsible for the experimental campaign will consult with the radiochemistry staff as to the feasibility of producing a desired target/substrate combination. In this report they discuss the production of U and Pu targets on very thin C and Ti substrates. The techniques used, plating cells designed for, tips, and limits is discussed

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

Effectiveness of traveller screening for emerging pathogens is shaped by epidemiology and natural history of infection.

During outbreaks of high-consequence pathogens, airport screening programs have been deployed to curtail geographic spread of infection. The effectiveness of screening depends on several factors, including pathogen natural history and epidemiology, human behavior, and characteristics of the source epidemic. We developed a mathematical model to understand how these factors combine to influence screening outcomes. We analyzed screening programs for six emerging pathogens in the early and late stages of an epidemic. We show that the effectiveness of different screening tools depends strongly on pathogen natural history and epidemiological features, as well as human factors in implementation and compliance. For pathogens with longer incubation periods, exposure risk detection dominates in growing epidemics, while fever becomes a better target in stable or declining epidemics. For pathogens with short incubation, fever screening drives detection in any epidemic stage. However, even in the most optimistic scenario arrival screening will miss the majority of cases