Measurement of fission gas release from irradiated U Mo dispersion fuel samples
Not Available
Burkes, Douglas E.↗
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Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples
To mimic the reactions that have occurred between plutonium dioxide (PuO2) and degraded polyvinyl chloride during prolonged storage, batches of PuO2 powders with varying specific surface area (4-38m2 g1) were exposed to dry hydrogen chloride gas forming a surface-sorbed exchangeable chloride species that was readily leached by dilute caustic solution. One batch was also humidified under a 95% relative humidity atmosphere. Heat treatment at temperatures between 100 and 950 C steadily reduced the leachable chloride content at least when the initial leachable chloride surface coverage was calculated to be > 0.5 monolayer (ML). Variations between samples are attributed to differences in surface area as well as production route and period of interim storage in air or humidified atmospheres. The data are consistent with surface species and reactions proposed in the literature for HCl adsorption on to TiO2. This indicates that it is interactions between hydrogen chloride/chloride and water/hydroxyl species on the PuO2 surface that are key to understanding the behaviour of these materials when heated in a furnace. These data will inform the design of a future thermal stabilisation process for chloride-contaminated PuO2.
Sutherland-Harper, Sophie↗
Combined Force-Frequency Sampling for Simulation of Systems Having Rugged Free Energy Landscapes.
An adaptive, machine learning-based sampling method is presented for simulation of systems having rugged, multidimensional free energy landscapes. The method's main strength resides in its ability to learn both from the frequency of visits to distinct states and the generalized force estimates that arise in a system as it evolves in phase space. This is accomplished by introducing a self-integrating artificial neural network, which generates an estimate of the free energy directly from its derivatives. The usefulness of the proposed combined approach is examined in the context of two concrete examples, namely, an alanine dipeptide molecule in water and a polymer diffusing through a narrow pore. This new method is found to be robust, faster, and more accurate than approaches that rely only on frequency-based or generalized force-based estimations. After combining the proposed approach with overfill protection and support for sparse data storage and training, the method is shown to be more effective than comparable, previously available techniques and capable of scaling efficiently to larger numbers of collective variables.
Sevgen, Emre↗
Physical and Chemical Morphology of Passively Sampled Environmental Films
Environmental surface films are important mediators in the fate and transport of persistent organic pollutants (POP) via largely uncharacterized mechanisms. This work presents the first analysis of the physical and chemical morphology of passively sampled environmental films. The films are developed in urban, sub-urban, and metropolitan locations for timescales ranging from 1 to 52 weeks by exposing polished silicon wafers to collect passively deposited tropospheric particulate matter. The time-dependent spatial morphology of the films is analyzed by bright-field, scanning electron, and atomic force microscopies. Time-of-flight secondary ion mass spectrometry (ToF-SIMS) imaging data are analyzed to report the film’s chemical morphology and speciation. We find that the film matrix presents an extremely complex physical and chemical system. Deposited PM sizes span six orders of magnitude (millimeter to nanometer regimes), and surface coverages range from ca. 5 % for one week films and ca. 98 % for 52 week films. We observe significant amounts of mineral dust, biogenic organics, and occasional indications of flora growth (i.e., spores). The films exhibit nanoscale surface features indicative of small particulate depositions as well as films of (semi)volatile molecules. SIMS imaging reveals diverse and sometimes segregated chemical domains of hydrocarbons, inorganics, metals, and proteinaceous macromolecules. This work presents the first spatially resolved physical and chemical surface characterization of native environmental films, beginning a study of mechanisms by which these films form, persist, and mature in the environment.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Advancing Aerosol Chemical Characterization and Vertical Profiling over the Southern Great Plains Using Uncrewed Aerial Sampling and Offline Aerosol Mass Spectrometry
Recent advancements in uncrewed aerial systems (UASs) and particulate matter (PM) analytical techniques have provided opportunities for atmospheric research. In this study, we deployed the Department of Energy’s fixed-wing ArcticShark UAS to examine PM 2.5 composition at varying altitudes─within and above the planetary boundary layer (PBL)─over the Southern Great Plains atmospheric observatory (SGP). A total of 22 flights were conducted across March, June, and August 2023. Composite filter samples were collected during each flight and analyzed with offline aerosol mass spectrometry (AMS), complemented by on-board real-time sensors and ground-based instrumentation, to provide a comprehensive view of regional aerosol characteristics. Results show clear vertical and seasonal differences in the aerosol composition. Relative to ground-level measurements, aloft samples exhibited shifts in the distribution of organic and inorganic PM, with the organic composition varying distinctly across seasons. Particulate organic nitrogen (ON) was elevated, with bulk compositions similar in March and June but strongly altered in August, likely driven by biomass burning and enhanced photochemical activity. Combined AMS and chemical ionization mass spectrometry analyses detected amines, amides, and amino acids. PM above the planetary boundary layer was enriched in oxidized organic aerosols, while ground-level PM contained higher nitrate and sulfate. Seasonal differences in aqueous-phase processing were also observed, which were strongest in March during persistent cloud cover and weaker in the drier August period, suggesting a shift from aqueous- to gas-phase SOA formation. In conclusion, these findings highlight the value of UAS in advancing PM measurements and vertical profiling of aerosol composition.
54 ENVIRONMENTAL SCIENCES↗
Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation
The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here in this study, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.
36 MATERIALS SCIENCE↗
Midlatitude Oceanic Cloud and Precipitation Properties as Sampled By the ARM Eastern North Atlantic Observatory
Marine low clouds are critical to the climate system because of their extensive coverage and associated controls on boundary layer dynamics and radiative energy balance. The primary foci for this study are marine low cloud observations over a heavily instrumented site on the Azores archipelago in the eastern North Atlantic (ENA) and their associated raindrop size distribution (DSD) properties, relative low-cloud contributions to the precipitation, and additional sampling (instrument, environmental) considerations. The contribution from low clouds (e.g., cloud top < 4 km) to the overall precipitation over midlatitude oceans is poorly understood, in part because of the lack of coupled, high-quality measurements of precipitation and low-cloud properties. Cloud regime and precipitation breakdowns performed for a multi-year record emphasize the diurnal precipitation cycle and DSD characteristics for both low and deeper clouds. Results demonstrate that marine low clouds over this ENA location account for a significant (45%) contribution to the total rainfall and exhibit a diurnal cycle in cloud (thickness, top, base) and precipitation characteristics similar to satellite records. Additional controls on observed surface rainfall characteristics of low clouds allowed by the extended ground-based facility datasets are also explored. From those analyses, it is suggested that the synoptic state exerts a significant control on low-cloud and surface precipitation properties.
Giangrande, Scott↗
Fast temperature spectrometer for samples under extreme conditions
We have developed a multi-wavelength Fast Temperature Readout (FasTeR) spectrometer to capture a sample’s transient temperature fluctuations, and reduce uncertainties in melting temperature determination. Without sacrificing accuracy, FasTeR features a fast readout rate (about 100 Hz), high sensitivity, large dynamic range, and a well-constrained focus. Complimenting a charge-coupled device spectrometer, FasTeR consists of an array of photomultiplier tubes and optical dichroic filters. The temperatures determined by FasTeR outside of the vicinity of melting are, generally, in good agreement with results from the charge-coupled device spectrometer. Near melting, FasTeR is capable of capturing transient temperature fluctuations, at least on the order of 300 K/s. A software tool, SIMFaster, is described and has been developed to simulate FasTeR and assess design configurations. FasTeR is especially suitable for temperature determinations that utilize ultra-fast techniques under extreme conditions. Working in parallel with the laser-heated diamond-anvil cell, synchrotron Mössbauer spectroscopy, and X-ray diffraction, we have applied the FasTeR spectrometer to measure the melting temperature of {sup 57}Fe{sub 0.9}Ni{sub 0.1} at high pressure.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Spatially Resolved Proteome Mapping of Laser Capture Microdissected Tissue with Automated Sample Transfer to Nanodroplets
Not Available
59 BASIC BIOLOGICAL SCIENCES↗
THE SL2S GALAXY-SCALE LENS SAMPLE. V. DARK MATTER HALOS AND STELLAR IMF OF MASSIVE EARLY-TYPE GALAXIES OUT TO REDSHIFT 0.8
We investigate the cosmic evolution of the internal structure of massive early-type galaxies over half of the age of the universe. We perform a joint lensing and stellar dynamics analysis of a sample of 81 strong lenses from the Strong Lensing Legacy Survey and Sloan ACS Lens Survey and combine the results with a hierarchical Bayesian inference method to measure the distribution of dark matter mass and stellar initial mass function (IMF) across the population of massive early-type galaxies. Lensing selection effects are taken into account. We find that the dark matter mass projected within the inner 5 kpc increases for increasing redshift, decreases for increasing stellar mass density, but is roughly constant along the evolutionary tracks of early-type galaxies. The average dark matter slope is consistent with that of a Navarro-Frenk-White profile, but is not well constrained. The stellar IMF normalization is close to a Salpeter IMF at log M {sub *} = 11.5 and scales strongly with increasing stellar mass. No dependence of the IMF on redshift or stellar mass density is detected. The anti-correlation between dark matter mass and stellar mass density supports the idea of mergers being more frequent in more massive dark matter halos.
79 ASTRONOMY AND ASTROPHYSICS↗
Exploring cosmic homogeneity with the BOSS DR12 galaxy sample
In this study, we probe the transition to cosmic homogeneity in the Large Scale Structure (LSS) of the Universe using the CMASS galaxy sample of BOSS spectroscopic survey which covers the largest effective volume to date, 3 h -3 Gpc 3 at 0.43 ≤ z ≤ 0.7. We study the scaled counts-in-spheres, N( 2 (r), to assess the homogeneity scale of the universe using a Landy & Szalay inspired estimator. Defining the scale of transition to homogeneity as the scale at which D 2 (r) reaches 3 within 1%, i.e. D 2 (r)>2.97 for r>R H , we find R H = (63.3±0.7) h -1 Mpc, in agreement at the percentage level with the predictions of the ΛCDM model R H =62.0 h -1 Mpc. Thanks to the large cosmic depth of the survey, we investigate the redshift evolution of the transition to homogeneity scale and find agreement with the ΛCDM prediction. Finally, we find that D 2 is compatible with 3 at scales larger than 300 h -1 Mpc in all redshift bins. These results consolidate the Cosmological Principle and represent a precise consistency test of the ΛCDM model.
79 ASTRONOMY AND ASTROPHYSICS↗
Baryon content in a sample of 91 galaxy clusters selected by the South Pole Telescope at 0.2 <z < 1.25
We estimate total mass (M-500), intracluster medium (ICM) mass (M-ICM), and stellar mass (M-star) in a Sunyaev-Zel'dovich effect (SZE) selected sample of 91 galaxy clusters with masses M-500 greater than or similar to 2.5 x 10(14) M-circle dot and redshift 0.2 < z < 1.25 from the 2500 deg(2) South Pole Telescope SPT-SZ survey. The total masses M-500 are estimated from the SZE observable, the ICM masses M-ICM are obtained from the analysis of Chandra X-ray observations, and the stellar masses M-star are derived by fitting spectral energy distribution templates to Dark Energy Survey griz optical photometry and WISE or Spitzer near-infrared photometry. We study trends in the stellar mass, the ICM mass, the total baryonic mass, and the cold baryonic fraction with cluster halo mass and redshift. We find significant departures from self-similarity in the mass scaling for all quantities, while the redshift trends are all statistically consistent with zero, indicating that the baryon content of clusters at fixed mass has changed remarkably little over the past approximate to 9 Gyr. We compare our results to the mean baryon fraction (and the stellar mass fraction) in the field, finding that these values lie above (below) those in cluster virial regions in all but the most massive clusters at low redshift. Using a simple model of the matter assembly of clusters from infalling groups with lower masses and from infalling material from the low-density environment or field surrounding the parent haloes, we show that the measured mass trends without strong redshift trends in the stellar mass scaling relation could be explained by a mass and redshift dependent fractional contribution from field material. Similar analyses of the ICM and baryon mass scaling relations provide evidence for the so-called 'missing baryons' outside cluster virial regions.
galaxies: clusters: stellar masses: ICM masses: ba↗
Sample Results from the Interim Salt Disposition Program Macrobatch 8 Tank 21H Qualification Samples
Savannah River National Laboratory (SRNL) analyzed samples from Tank 21H in support of qualification of Macrobatch (Salt Batch) 8 for the Interim Salt Disposition Program (ISDP). An Actinide Removal Process (ARP) and several Extraction-Scrub- Strip (ESS) tests were also performed. This document reports characterization data on the samples of Tank 21H as well as simulated performance of ARP and the Modular Caustic Side Solvent Extraction (CSSX) Unit (MCU). No issues with the projected Salt Batch 8 strategy are identified. A demonstration of the monosodium titanate (MST) (0.2 g/L) removal of strontium and actinides provided acceptable average decontamination factors for plutonium of 2.62 (4 hour) and 2.90 (8 hour); and average strontium decontamination factors of 21.7 (4 hour) and 21.3 (8 hour). These values are consistent with results from previous salt batch ARP tests. The two ESS tests also showed acceptable performance with extraction distribution ratios (D(Cs)) values of 52.5 and 50.4 for the Next Generation Solvent (NGS) blend (from MCU) and NGS (lab prepared), respectively. These values are consistent with results from previous salt batch ESS tests. Even though the performance is acceptable, SRNL recommends that a model for predicting extraction behavior for cesium removal for the blended solvent and NGS be developed in order to improve our predictive capabilities for the ESS tests.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Sample results from the Interim Salt Disposition Program Macrobatch 8 Tank 21H qualification samples
Savannah River National Laboratory (SRNL) analyzed samples from Tank 21H in support of qualification of Macrobatch (Salt Batch) 8 for the Interim Salt Disposition Program (ISDP). An Actinide Removal Process (ARP) and several Extraction-Scrub-Strip (ESS) tests were also performed. This document reports characterization data on the samples of Tank 21H as well as simulated performance of ARP and the Modular Caustic Side Solvent Extraction (CSSX) Unit (MCU). No issues with the projected Salt Batch 8 strategy are identified. A demonstration of the monosodium titanate (MST) (0.2 g/L) removal of strontium and actinides provided acceptable average decontamination factors for plutonium of 2.62 (4 hour) and 2.90 (8 hour); and average strontium decontamination factors of 21.7 (4 hour) and 21.3 (8 hour). These values are consistent with results from previous salt batch ARP tests. The two ESS tests also showed acceptable performance with extraction distribution ratios (D (Cs) ) values of 52.5 and 50.4 for the Next Generation Solvent (NGS) blend (from MCU) and NGS (lab prepared), respectively. These values are consistent with results from previous salt batch ESS tests. Even though the performance is acceptable, SRNL recommends that a model for predicting extraction behavior for cesium removal for the blended solvent and NGS be developed in order to improve our predictive capabilities for the ESS tests.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Sample results from the interim salt disposition program macrobatch 9 tank 21H qualification samples
Savannah River National Laboratory (SRNL) analyzed samples from Tank 21H in support of qualification of Macrobatch (Salt Batch) 9 for the Interim Salt Disposition Program (ISDP). This document reports characterization data on the samples of Tank 21H.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Storm Water Sampling results for 1-16-19 Sampling Event
In the California lndustrial General Permit (IGP) 2014-0057-DWQ for storm water monitoring, effective July 1, 2015, there are 21 contaminants that have been assigned NAL (Numeric Action Level) values, both annual and instantaneous. For annual NALs, an exceedance occurs when the average of all analytical results from all samples taken at a facility during a reporting year for a given parameter exceeds an annual NAL value listed in Table 2 of the General Permit. For instantaneous maximum NALs, an exceedance occurs when two or more analytical results from samples taken for any parameter within a reporting year exceed the instantaneous maximum NAL value (for TSS and O&G), or are outside of the instantaneous maximum NAL range (for pH) listed in Table 2.
54 ENVIRONMENTAL SCIENCES↗
Spectral evolution in high redshift quasars from the final Baryon Oscillation Spectroscopic Survey sample
We report on the diversity in quasar spectra from the Baryon Oscillation Spectroscopic Survey. After filtering the spectra to mitigate selection effects and Malmquist bias associated with a nearly flux-limited sample, we create high signal-to-noise ratio composite spectra from 58,656 quasars (2.1⩽z⩽3.5), binned by luminosity, spectral index, and redshift. With these composite spectra, we confirm the traditional Baldwin effect (BE, i.e., the anti-correlation of C iv equivalent width (EW) and luminosity) that follows the relation W{sub λ}∝L{sup β{sub w}} with slope β{sub w}=−0.35±0.004, −0.35 ± 0.005, and −0.41 ± 0.005 for z = 2.25, 2.46, and 2.84, respectively. In addition to the redshift evolution in the slope of the BE, we find redshift evolution in average quasar spectral features at fixed luminosity. The spectroscopic signature of the redshift evolution is correlated at 98% with the signature of varying luminosity, indicating that they arise from the same physical mechanism. At a fixed luminosity, the average C iv FWHM decreases with increasing redshift and is anti-correlated with C iv EW. The spectroscopic signature associated with C iv FWHM suggests that the trends in luminosity and redshift are likely caused by a superposition of effects that are related to black hole mass and Eddington ratio. The redshift evolution is the consequence of a changing balance between these two quantities as quasars evolve toward a population with lower typical accretion rates at a given black hole mass.
79 ASTRONOMY AND ASTROPHYSICS↗