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DOE OSTI2014

pH and Amphiphilic Structure Direct Supramolecular Behavior in Biofunctional Assemblies

Supramolecular self-assembly offers promising new ways to control nanostructure morphology and respond to external stimuli. A pH-sensitive self-assembled system was developed to both control nanostructure shape and respond to the acidic microenvironment of tumors using self-assembling peptide amphiphiles (PAs). Here, by incorporating an oligo-histidine H 6 sequence, we developed two PAs that self-assembled into distinct morphologies on the nanoscale, either as nanofibers or spherical micelles, based on the incorporation of the aliphatic tail on the N-terminus or near the C-terminus, respectively. Both cylinder and sphere-forming PAs demonstrated reversible disassembly between pH 6.0 and 6.5 upon protonation of the histidine residues in acidic solutions. These PAs were then characterized and assessed for their potential to encapsulate hydrophobic chemotherapies. The H 6 -based nanofiber assemblies encapsulated camptothecin (CPT) with up to 60% efficiency, a 7-fold increase in CPT encapsulation relative to spherical micelles. Additionally, pH-sensitive nanofibers showed improved tumor accumulation over both spherical micelles and nanofibers that did not change morphologies in acidic environments. We have demonstrated that the morphological transitions upon changes in pH of supramolecular nanostructures affect drug encapsulation and tumor accumulation. Lastly, our findings also suggest that these supramolecular events can be tuned by molecular design to improve the pharmacologic properties of nanomedicines.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Universal Approach for the Depolymerization of Polyamides via Photothermal Conversion

Polyamides (PAs) exhibit excellent chemical stability and mechanical resistance, yet these same characteristics lead to their widespread accumulation in the environment as pollution. In this work, we developed an inclusive and operationally simple photothermal strategy to recycle PAs, overcoming the high energy barriers necessary to break down these materials. PAs can be depolymerized using photothermally mediated ring-closing depolymerization and acidic hydrolysis to afford cyclic and linear monomers using carbon black as a photothermal agent (PTA) under visible light irradiation. We showed that polyamide 6 is efficiently depolymerized to ε-caprolactam with 74% yield in 10 min. Similarly, in 1 h, the photothermal acidic hydrolysis of polyamide 6,6 afforded hexamethylene diamine and adipic acid with 97 and 96% yields, respectively. This method was further applied to a variety of aliphatic and aromatic PAs and mixed PA waste. Both photothermally promoted processes effectively depolymerize pigment-containing postconsumer waste by leveraging existing black pigments as PTAs. Here, photothermal conversion provided a general and rapid route for PA depolymerization under visible light irradiation, enabling high monomer yields with inexpensive reagents and a general tolerance to additives, demonstrating this approach’s potential for a circular plastic economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2013

Analysis of Resistant Starches in Rat Cecal Contents Using Fourier Transform Infrared Photoacoustic Spectroscopy

Fourier transform infrared photoacoustic spectroscopy (FTIR-PAS) qualitatively and quantitatively measured resistant starch (RS) in rat cecal contents. Fisher 344 rats were fed diets of 55% (w/w, dry basis) starch for 8 weeks. Cecal contents were collected from sacrificed rats. A corn starch control was compared against three RS diets. The RS diets were high-amylose corn starch (HA7), HA7 chemically modified with octenyl succinic anhydride, and stearic-acid-complexed HA7 starch. To calibrate the FTIR-PAS analysis, samples from each diet were analyzed using an enzymatic assay. A partial least-squares cross-validation plot generated from the enzymatic assay and FTIR-PAS spectral results for starch fit the ideal curve with a R2 of 0.997. A principal component analysis plot of components 1 and 2 showed that spectra from diets clustered significantly from each other. This study clearly showed that FTIR-PAS can accurately quantify starch content and identify the form of starch in complex matrices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Panoscopic approach for high-performance Te-doped skutterudite

One-step plasma-activated sintering (OS-PAS) fabrication of single-phase high-performance CoSb 3 -based skutterudite thermoelectric material with a hierarchical structure on a time scale of a few minutes is first reported here. The formation mechanism of the CoSb 3 phase and the effects of the current and pressure fields on the phase transformation and microstructure evolution are studied in the one-step PAS process. The application of the panoscopic approach to this system and its effect on the transport properties are investigated. The results show that the hierarchical structure forms during the formation of the skutterudite phase under the effects of both current and sintering pressure. The samples fabricated by the OS-PAS technique have defined hierarchical structures, which scatter phonons more intensely over a broader range of frequencies and significantly reduce the lattice thermal conductivity. High-performance bulk Te-doped skutterudite with the maximum ZT of 1.1 at 820 K for the composition CoSb 2.875 Te 0.125 was obtained. Such high ZT values rival those obtained from single filled skutterudites. As a result, this newly developed OS-PAS technique enhances the thermoelectric performance, dramatically shortens the synthesis period and provides a facile method for obtaining hierarchical thermoelectric materials on a large scale.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Water Ordering Controls the Dynamic Equilibrium of Micelle-Fiber Formation in Self-Assembly of Peptide Amphiphiles

Understanding the role of water in governing the kinetics of the self-assembly processes of amphiphilic peptides has still remained elusive. Here, using a multi-stage atomistic-coarse-grained approach, complemented by circular dichroism/infra-red spectroscopy and dynamic light scattering experiments, we highlight the dual nature of water in dictating the mechanism and dynamics of self-assembly of peptide amphiphiles (PAs). Our computational study shows that (i) Water cage formation and breakage near the hydrophobic groups controls the fusion dynamics and aggregation of PAs in the micellar stage, and (ii) Enhanced structural ordering of vicinal water near the hydrophilic amino acids shifts the equilibrium towards the fiber phase and stimulates structure and order in the PAs when they assemble into a hexagonal nanofiber architecture. Finally, spectroscopy and microscopy studies authenticate our computational observation that water ordering near the PAs increases with increase in time. The measured infra-red O-H bond stretch frequency reminiscent of ice-like suggests that the solvated water becomes increasingly solid-like with increased structural order in the assembled peptide network – thus shedding light on the role of water in a self-assembly process.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2015

Molecular design for growth of supramolecular membranes with hierarchical structure

Membranes with hierarchical structure exist in biological systems, and bio-inspired building blocks have been used to grow synthetic analogues in the laboratory through self-assembly. The formation of these synthetic membranes is initiated at the interface of two aqueous solutions, one containing cationic peptide amphiphiles (PA) and the other containing the anionic biopolymer hyaluronic acid (HA). The membrane growth process starts within milliseconds of interface formation and continues over much longer timescales to generate robust membranes with supramolecular PA–HA nanofibers oriented orthogonal to the interface. Computer simulation indicates that formation of these hierarchically structured membranes requires strong interactions between molecular components at early time points in order to generate a diffusion barrier between both solutions. Experimental studies using structurally designed PAs confirm simulation results by showing that only PAs with high ζ potential are able to yield hierarchically structured membranes. Furthermore, the chemical structure of such PAs must incorporate residues that form β-sheets, which facilitates self-assembly of long nanofibers. In contrast, PAs that form low aspect ratio nanostructures interact weakly with HA and yield membranes that exhibit non-fibrous fingering protrusions. Furthermore, experimental results show that increasing HA molecular weight decreases the growth rate of orthogonal nanofibers. Overall, this result is supported by simulation results suggesting that the thickness of the interfacial contact layer generated immediately after initiation of self-assembly increases with polymer molecular weight.

36 MATERIALS SCIENCE↗

DOE OSTI2022

The miniJPAS survey: White dwarf science with 56 optical filters

We analyze the white dwarf population in miniJPAS, the first square degree observed with 56 medium-band, 145 Å in width optical filters by the Javalambre Physics of the accelerating Universe Astrophysical Survey (J-PAS), to provide a data-based forecast for the white dwarf science with low-resolution ($R$ ~ 50) photo-spectra. We define the sample of the bluest point-like sources in miniJPAS with $r$ < 21.5 mag, a point-like probability larger than 0.5, ($u$ - $r$)< 0.80 mag, and ($g$ - $i$)< 0.25 mag. This sample comprises 33 sources with spectroscopic information: 11 white dwarfs and 22 quasi-stellar objects (QSOs). We estimate the effective temperature ($T$ eff ), the surface gravity, and the composition of the white dwarf population by a Bayesian fitting to the observed photo-spectra. The miniJPAS data are sensitive to the Balmer series and the presence of polluting metals. Our results, combined with those from the Javalambre Photometric Local Universe Survey (J-PLUS) which has a lower spectral resolution but has already observed thousands of white dwarfs, suggest that J-PAS photometry would permit – down to $r$ ~ 21.5 mag and at least for sources with 7000 < $T$ eff < 22 000 K – both the classification of the observed white dwarfs into H-dominated and He-dominated with 99% confidence and the detection of calcium absorption for equivalent widths larger than 15 Å. The effective temperature is estimated with a 2% uncertainty, which is close to the 1% from spectroscopy. A precise estimation of the surface gravity depends on the available parallax information. In addition, the white dwarf population at $T$ eff > 7000 K can be segregated from the bluest extragalactic QSOs, providing a clean sample based on optical photometry alone. The J-PAS low-resolution photo-spectra would produce precise effective temperatures and atmospheric compositions for white dwarfs, complementing the data from Gaia. J-PAS will also detect and characterize new white dwarfs beyond the Gaia magnitude limit, providing faint candidates for spectroscopic follow-up.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

The miniJPAS survey: A search for extreme emission-line galaxies

Context. Galaxies with extreme emission lines (EELGs) may play a key role in the evolution of the Universe, as well as in our understanding of the star formation process itself. For this reason an accurate determination of their spatial density and fundamental properties in different epochs of the Universe will constitute a unique perspective towards a comprehensive picture of the interplay between star formation and mass assembly in galaxies. In addition to this, EELGs are also interesting in order to explain the reionization of the Universe, since their interstellar medium (ISM) could be leaking ionizing photons, and thus they could be low z, analogous of extreme galaxies at high z . Aims. This paper presents a method to obtain a census of EELGs over a large area of the sky by detecting galaxies with rest-frame equivalent widths ≥300 Å in the emission lines [O II]λλ3727,3729Å, [O III]λ5007Å, and Hα. For this, we aim to use the J-PAS survey, which will image an area of ≈8000 deg 2 with 56 narrow band filters in the optical. As a pilot study, we present a methodology designed to select EELGs on the miniJPAS images, which use the same filter dataset as J-PAS, and thus will be exportable to this larger survey. Methods. We make use of the miniJPAS survey data, conceived as a proof of concept of J-PAS, and covering an area of ≈1 deg 2 . Objects were detected in the r SDSS images and selected by imposing a condition on the flux in a given narrow-band J-PAS filter with respect to the contiguous ones, which is analogous to requiring an observed equivalent width larger than 300 Å in a certain emission line within the filter bandwidth. The selected sources were then classified as galaxies or quasi-stellar objects (QSOs) after a comparison of their miniJPAS fluxes with those of a spectral database of objects known to present strong emission lines. This comparison also provided a redshift for each source, which turned out to be consistent with the spectroscopic redshifts when available (|Δz/(1 + z spec )| ≤ 0.01). Results. The selected candidates were found to show a compact appearance in the optical images, some of them even being classified as point-like sources according to their stellarity index. After discarding sources classified as QSOs, a total of 17 sources turned out to exhibit EW 0 ≥ 300 Å in at least one emission line, thus constituting our final list of EELGs. Our counts are fairly consistent with those of other samples of EELGs in the literature, although there are some differences, which were expected due to biases resulting from different selection criteria.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2016

Detection of ethylene gas in exhaled breath of people living in landfill using CO{sub 2} laser photoacoustic spectroscopy with multicomponent analysis

The photoacoustic spectrometer (PAS) had been built and the performance had been determined. The research was based on the conversion of the absorbed middle infra red (IR) radiation by gas confined in a closed PAS cell into standing acoustic wave, which could be detected by a suitable electroacoustic transducer such as a microphone. The lowest detection limit for this setup was (57,1 ± 0,3) ppb and quality factor was (14,5 ± 0,6) for ethylene gas in 10P14 CO{sub 2} laser line. Then, this PAS was used to measure of ethylene gas concentration in breath sample of people living in near the Piyungan Bantul Yogyakarta landfill. The result from multicomponent analysis showed that PAS enable to measure the lowest concentration of volatile organic compound (VOC), such as ethylene, which occured on ambien air in Piyungan landfill. Variaty of distance area applied in this research. In the range of ±0,5 km from landfill, we obtained the concentration of ethylene gas concentration for human breath was (1,520 ± 0,002) ppm, while in the range of ±45 km, the ethylene gas concentration for human breath was (0,424 ± 0,002) ppm. Ethylene gas concentrations in exhaled gas decreased along with increasing distance variation of the landfill.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Genetic analysis of Physcomitrella patens identifies ABSCISIC ACID NON-RESPONSIVE , a regulator of ABA responses unique to basal land plants and required for desiccation tolerance

The anatomically simple plants that first colonized land must have acquired molecular and biochemical adaptations to drought stress. Abscisic acid (ABA) coordinates responses leading to desiccation tolerance in all land plants. We identified ABA nonresponsive mutants in the model bryophyte Physcomitrella patens and genotyped a segregating population to map and identify the ABA NON-RESPONSIVE (ANR) gene encoding a modular protein kinase comprising an N-terminal PAS domain, a central EDR domain, and a C-terminal MAPKKK-like domain. anr mutants fail to accumulate dehydration tolerance-associated gene products in response to drought, ABA, or osmotic stress and do not acquire ABA-dependent desiccation tolerance. The crystal structure of the PAS domain, determined to 1.7-Å resolution, shows a conserved PAS-fold that dimerizes through a weak dimerization interface. Targeted mutagenesis of a conserved tryptophan residue within the PAS domain generates plants with ABA nonresponsive growth and strongly attenuated ABA-responsive gene expression, whereas deleting this domain retains a fully ABA-responsive phenotype. ANR orthologs are found in early-diverging land plant lineages and aquatic algae but are absent from more recently diverged vascular plants. Lastly, we propose that ANR genes represent an ancestral adaptation that enabled drought stress survival of the first terrestrial colonizers but were lost during land plant evolution.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2011

Integrated Genome-Based Studies of Shewanella Ecophysiology

We have constructed in-frame deletions of 7 of the 10 PAS-GGDEF-EAL proteins in Shewanella oneidensis MR-1. We are currently in the process of characterizing the deletion mutants under a wide range of growth conditions. In addition to characterizing growth, we will also examine the biofilm formation of the deletion mutants. In addition to the genetic analyses of the mutants, we are also interested in comparing the activities of the various PAS-GGDEF-EAL proteins. Proteins containing PAS, GGDEF and EAL amino acid sequence motifs may play an important role in regulating c-di-GMP signaling in response to environmental conditions. A genetic and biochemical analysis into the roles of these proteins is underway. PDE activity was observed for several PAS-GGDEF-EAL proteins. One of these proteins, SO0427, also demonstrates possible DGC activity in vitro. Currently, we are studying the growth, motility and biofilm formation characteristics of deletion mutants, as well as the activity of the purified proteins.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2013

Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada: Review of the Performance Assessments and Composite Analyses (2012 Annual Summary Report)

The Maintenance Plan for the Performance Assessments and Composite Analyses for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada Test Site (National Security Technologies, LLC 2007a) requires an annual review to assess the adequacy of the performance assessments (PAs) and composite analyses (CAs), with the results submitted to the U.S. Department of Energy (DOE) Office of Environmental Management. The Disposal Authorization Statements for the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) also require that such reviews be made and that secondary or minor unresolved issues be tracked and addressed as part of the maintenance plan (DOE 1999a, 2000). The U.S. Department of Energy, National Nuclear Security Administration Nevada Site Office performed an annual review of the Area 3 and Area 5 RWMS PAs and CAs for fiscal year (FY) 2012. This annual summary report presents data and conclusions from the FY 2012 review, and determines the adequacy of the PAs and CAs. Operational factors (e.g., waste forms and containers, facility design, and waste receipts), closure plans, monitoring results, and research and development (RD) activities were reviewed to determine the adequacy of the PAs. Likewise, the environmental restoration activities at the Nevada National Security Site (NNSS) relevant to the sources of residual radioactive material that are considered in the CAs, the land-use planning, and the results of the environmental monitoring and RD activities were reviewed to determine the adequacy of the CAs. Important developments in FY 2012 include the following: Release of a special analysis for the Area 3 RWMS assessing the continuing validity of the PA and CA; Development of a new Area 5 RWMS closure inventory estimate based on disposals through FY 2012; Evaluation of new or revised waste streams by special analysis; and Development of version 4.114 of the Area 5 RWMS GoldSim PA model. The Area 3 RWMS has been in inactive status since July 1, 2006, with the last shipment received in April 2006. The FY 2012 review of operations, facility design, closure plans, monitoring results, and RD results for the Area 3 RWMS indicates no changes that would impact PA validity. A special analysis using the Area 3 RWMS v2.102 GoldSim PA model was prepared to update the PA results for the Area 3 RWMS in FY 2012. The special analysis concludes that all performance objectives can be met and the Area 3 RWMS PA remains valid. There is no need to the revise the Area 3 RWMS PA. Review of Area 5 RWMS operations, design, closure plans, monitoring results, and RD activities indicates no significant changes other than an increase in the inventory disposed. The FY 2012 PA results, generated with the Area 5 RWMS v4.114 GoldSim PA model, indicate that there continues to be a reasonable expectation of meeting all performance objectives. The results and conclusions of the Area 5 RWMS PA are judged valid, and there is no need to the revise the PA. A review of changes potentially impacting the CAs indicates that no significant changes occurred in FY 2012. The continuing adequacy of the CAs was evaluated with the new models, and no significant changes that would alter CA results or conclusions were found. The revision of the Area 3 RWMS CA, which will include the Underground Test Area source term (Corrective Action Unit [CAU] 97), is scheduled for FY 2024, following the completion of the Yucca Flat CAU 97 Corrective Action Decision Document/Corrective Action Plan in FY 2016. Inclusion of the Frenchman Flat CAU 98 results in the Area 5 RWMS CA is scheduled for FY 2016, pending the completion of the CAU 98 closure report in FY 2015. Near-term RD efforts will focus on continuing development of the Area 3 and Area 5 RWMS GoldSim PA/CA and inventory models.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

2013 Annual Summary Report for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada: Review of the Performance Assessments and Composite Analyses

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2017

2016 Annual Summary Report for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada: Review of the Performance Assessments and Composite Analyses

The Maintenance Plan for the Performance Assessments and Composite Analyses for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada Test Site (National Security Technologies, LLC 2007a) requires an annual review to assess the adequacy of the performance assessments (PAs) and composite analyses (CAs), with the results submitted to the U.S. Department of Energy (DOE) Office of Environmental Management. The Disposal Authorization Statements for the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) also require that such reviews be made and that secondary or minor unresolved issues be tracked and addressed as part of the maintenance plan.The U.S. Department of Energy, National Nuclear Security Administration Nevada Field Office (NNSA/NFO) performed an annual review of the Area 3 and Area 5 RWMS PAs and CAs for federal fiscal year (FY) 2016. This annual summary report presents results and conclusions of the FY 2016 review, and determines the adequacy of the PAs and CAs. Operational factors (e.g., waste forms and containers, facility design, and waste receipts), closure plans, monitoring results, and research and development (R&D) activities were reviewed to determine the adequacy of the PAs. Likewise, the environmental restoration activities at the Nevada National Security Site (NNSS) relevant to the sources of residual radioactive material that are considered in the CAs, the land-use planning, and the results of the environmental monitoring and R&D activities were reviewed to determine the adequacy of the CAs. Important developments in FY 2016 include the following: Development of a new Area 5 RWMS closure inventory estimate based on disposals through FY 2016, Evaluation of new or revised waste streams by special analysis, and Development and acceptance of version 4.200 of the Area 5 RWMS GoldSim PA/CA model. The Area 3 RWMS has been in inactive status since July 1, 2006, with the last shipment received in April 2006. The FY 2016 review of operations, facility design, closure plans, monitoring results, and R&D results for the Area 3 RWMS indicates no changes that would impact PA validity. The conclusion of the annual review is that all performance objectives can be met and the Area 3 RWMS PA remains valid. There is no need to revise the Area 3 RWMS PA. Review of Area 5 RWMS operations, design, closure plans, monitoring results, and R&D activities indicates that no significant changes have occurred. The FY 2016 PA results, generated with the Area 5 RWMS v4.200 GoldSim PA model, indicate that there continues to be a reasonable expectation of meeting all performance objectives. All results remain less than 50% of their performance objectives. The results and conclusions of the Area 5 RWMS PA are judged valid, and there is no need to the revise the PA. A review of changes potentially impacting the CAs indicates that no significant changes occurred in FY 2016. A new Corrective Action Unit (CAU), CAU 576, with corrective action sites near the Area 3 RWMS and Area 5 RWMS was identified in FY 2016. The sites are currently under investigation and not expected to be important sources for the CA. The continuing adequacy of the CAs was evaluated with the new models, and no significant changes that would alter the CAs’ results or conclusions were found. The revision of the Area 3 RWMS CA, which will include the Yucca Flat Underground Test Area (CAU 97) source, is scheduled for FY 2024, following the completion of the Corrective Action Decision Document/Corrective Action Plan. Inclusion of the Frenchman Flat Underground Test Area (CAU 98) source in the Area 5 RWMS CA is planned pending the completion of the CAU 98 Closure Report in FY 2017. Near-term R&D efforts will focus on continuing development of the PA, CA, and inventory models for the Area 3 and Area 5 RWMSs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Impact of GSA2018 Flow Update, Alternative Dispersion Model, and Increased Grid Resolution on Tank Closure Performance Assessments

The F-Area Tank Farm (FTF) and H-Area Tank Farm (HTF) Performance Assessments (PAs) involve simulations of radionuclide and chemical waste migration through groundwater to exposure points. These solute transport simulations are based on a circa 2004 “GSA/PORFLOW” flow model [WSRC-TR-2004-00106]. The GSA/PORFLOW model was significantly updated in 2016-2017 [SRNL-STI-2017-00008 Rev. 1]. Impacts of the “GSA2016” flow model on the F- and H-Tank Farm PAs were assessed in SRNL-STI-2017-00445, Impacts of Updated GSA Groundwater Flow Models on the FTF, HTF and SDF PAs. Since then (2018-2019) further revisions resulted in a “GSA2018” flow model [SRNL-STI-2018-00643], which has been adopted for the 2019 Saltstone PA revision [SRR-CWDA-2019-00001 Revision A]. This study assesses the impacts of the GSA2018 flow model on the FTF and HTF PAs. Also assessed are the impacts of an alternative plume dispersion model and increased grid resolution that have been incorporated in the 2019 Saltstone PA.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

TRACER Carbonaceous Aerosols Thrust – University of California, Davis Field Campaign Report

The broader U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign aims to increase our understanding of convective cloud life cycles and aerosol-convection interactions. Our TRACER Carbonaceous Aerosols Thrust-University of California, Davis (TRACER-CAT-UCDavis) study complemented these broader aims by characterizing and quantifying the optical properties and composition of carbonaceous aerosols during part of the TRACER intensive sampling period (July 1- July 31, 2022) at the first ARM Mobile Facility (AMF1) main site (M1) in La Porte, Texas. Our measurements complemented the suite of instrumentation already provided by the AMF1, expanding the capabilities through deployment of unique, state-of-the-science instrumentation. The instrumentation included: (i) two cavity-attenuated phase shift spectroscopy single-scatter albedo (CAPS-SSA) instruments operating at 530 nm and 630 nm, and that were modified to characterize particle light absorption, extinction, and scattering at elevated humidities; (ii) the UC Davis dual-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS), which characterizes dry particle extinction and absorption at 405 nm and 532 nm; (iii) a soot particle aerosol mass spectrometer (SP-AMS) that operated in “laser only” mode that characterized the size-dependent compositions of black carbon (BC)-containing particles; (v) a thermal denuder, to remove coatings on particles; and (vi) a scanning electrical mobility sizer (SEMS), to characterize particle mobility diameters from 10-1300 nm. Our measurements occurred alongside complementary observations made by Los Alamos National Laboratory (LANL) during the TRACER-CAT-LANL study, including a humidified CAPS-SSA instrument operating at 450 nm. Our primary scientific interest is in understanding the relationship between particle composition and light absorption, with a particular focus on the influence of water uptake. While it is known that coatings on BC can enhance absorption, the extent to which this occurs in the atmosphere and the specific role that water plays as a coating remain unclear. The TRACER-CAT-UCDavis measurements were made with near-complete coverage for the CRD-PAS, SP-AMS, and SEMS throughout the intensive period. The UC Davis humidified CAPS-SSA instruments had significant challenges with operation owing to the demanding conditions (large temperature fluctuations, high humidity), exacerbated by supply chain issues that delayed resolution of these challenges. However, the humidified CAPS-SSA instrument operated by LANL operated throughout the intensive period with near-complete coverage. The dry light extinction measurements from the CRD-PAS measurements and the LANL CAPS-SSA exhibited a good correlation, although the CAPS-SSA systematically measured greater extinction values than expected. While all instruments, with the exception of an aerodynamic particle sizer (APS), measured behind a common particulate matter (PM)2.5 μm cyclone, the greater extinction measured by the LANL CAPS-SSA compared to the CRD-PAS may have resulted from different losses of larger particles in the sampling lines from the cyclone to the instruments; the tubing length was shorter from the cyclone to the LANL CAPS-SSA, consistent with this idea. A summary of the TRACER-CAT-UCDavis measurements, along with some of the TRACER-CAT-LANL measurements, are shown in the figure below. Notably, there were periods when the contributions of presumed dust were substantial and even dominated the observed light extinction and absorption. Also, there was a clear shift in the behavior of submicron particles from before July 16, 2022 to after, with the prior period exhibiting regular episodes of new particle formation and the latter period exhibiting rapid variations in the concentrations of small particles.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020) (Rev. 2)

This document provides an updated Hanford Site composite analysis (CA). A Hanford Site CA was prepared and issued in 1998 (PNNL-11800) with an addendum provided in 2002 (PNNL-11800 Addendum 1). The CA was approved in 2002 (Frei, 2002) and has been maintained (DOE/RL-2000-29 and subsequent revisions) to support low-level waste disposal performance assessments (PAs) and disposal authorizations for facilities at the Hanford Site, including the following: Continued operation of the Environmental Restoration Disposal Facility (ERDF) and the 200 East and 200 West Low-Level Burial Grounds; Construction of the Integrated Disposal Facility (IDF); Forthcoming closure of tank residual waste systems such as Waste Management Area (WMA) C. The CA maintenance program resulted in a determination in 2015 (DOE/RL-2015-66) that the Hanford Site CA needed an update for the following reasons: While the initial Hanford Site CA has been maintained since 2001, the accumulation of basis changes reported in the annual summary reports over the succeeding 14 years merit evaluation in an updated analysis; The U.S. Department of Energy (DOE) Headquarters requested in a memorandum in 2015 (Gilbertson and Marcinowski, 2015) that “as soon as the relevant PAs are complete, the CA will be revised to account for all of the new information.” This updated Hanford Site CA accounts for the following new information: 1. Inclusion of a detailed Hanford Site baseline disposition that projects remedial activities through site closure. There have been significant changes through decision making in the Comprehensive Environmental Response, Compensation, and Liability Act of 1980 (CERCLA) process that were not available when the original CA was produced; 2. Inclusion of an updated inventory basis, new modeling capabilities, and new decisions reached in the associated record of decision (ROD) that was provided by issuance of DOE/EIS-0391 in fiscal year (FY) 2013. Development of a Hanford Site groundwater model from the baseline provided in a technical transfer of models for the Final Tank Closure and Waste Management Environmental Impact Statement (DOE/EIS-0391) commenced in FY 2014 and resulted in the plateau-to-river (P2R) groundwater flow model that is used in this updated Hanford Site CA; 3. Accounting for pump and treat systems, which were not evaluated in the initial CA. Pump and treat systems have had significant impact on groundwater flow system behavior, contaminant transport, and contaminant removal from Hanford Site groundwater. This process is accounted for in the use of the P2R model for this updated Hanford Site CA; 4. Inclusion of water-level data collected since the initial CA was completed. Data collected as the unconfined aquifer water levels continue to recede since the cessation of large liquid discharges in the late 1990s have led to marked improvement in understanding of the flow system for future conditions, particularly regarding northward flow potential in the critical Gable Gap area. The calibration in the latest version of the P2R model accounts for this information; 5. Inclusion of results from the revised ERDF PA completed in 2013 (WCH-5209) that account for updated inventory and expansion of the ERDF facility to about twice the size that was evaluated in the original CA; 6. Use of updated geoframeworks to provide the structural basis for numerical fate and transport models in the groundwater pathway of this updated CA. The geologic basis for groundwater models has continued to improve with additional data collection and interpretation with the creation and maintenance of the Hanford South Geoframework and the Central Plateau Vadose Zone Geoframework tools; 7. Incorporation of updated tank residual inventory estimates. Tank residual inventory estimates have improved with the incorporation of tank retrieval inventory data for those tanks that have completed retrieval. The CA inventory data package includes this updated information; 8. Incorporation of WMA C PA results. Two additional PAs for tank farm closure decisions are in preparation during the period required to prepare an updated Hanford Site CA: WMA C (FY 2016) and WMA A-AX (in preparation). The WMA C PA results are incorporated into the updated Hanford Site CA, and its grouted residuals model is used as the basis for a release model to account for the other tank farm systems modeling in this updated CA; 9. An update to the IDF PA was submitted in FY 2017 and has been reviewed and approved. The results of the IDF PA are incorporated into this updated CA; 10. Updated risk assessment scenarios. The risk assessment scenarios currently in use for Hanford Site CERCLA and Resource Conservation and Recovery Act of 1976 (RCRA) analyses differ from those evaluated in the initial Hanford Site CA. The representative person exposure scenario evaluated in this updated Hanford Site CA is consistent with recent PAs and CERCLA and RCRA analyses as the Hanford Site. This updated Hanford Site CA provides the following: A comparison of the updated Hanford Site CA all-pathway dose results with the performance measures during the compliance period, which is assumed to begin with site closure in calendar 2070 with the last scheduled disposal action and continue for 1,000 years postclosure (to calendar year 3069); A comparison of Hanford Site CA all-pathway dose results with the performance measures during the postcompliance period to address potential peaks beyond the compliance period. This is accomplished by evaluating dose in the period for 9,000 years following the compliance period (i.e., from calendar year 3070 to 12070).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1993

NASA pyrotechnically actuated systems program

The Office of Safety and Mission Quality initiated a Pyrotechnically Actuated Systems (PAS) Program in FY-92 to address problems experienced with pyrotechnically actuated systems and devices used both on the ground and in flight. The PAS Program will provide the technical basis for NASA's projects to incorporate new technological developments in operational systems. The program will accomplish that objective by developing/testing current and new hardware designs for flight applications and by providing a pyrotechnic data base. This marks the first applied pyrotechnic technology program funded by NASA to address pyrotechnic issues. The PAS Program has been structured to address the results of a survey of pyrotechnic device and system problems with the goal of alleviating or minimizing their risks. Major program initiatives include the development of a Laser Initiated Ordnance System, a pyrotechnic systems data base, NASA Standard Initiator model, a NASA Standard Linear Separation System and a NASA Standard Gas Generator. The PAS Program sponsors annual aerospace pyrotechnic systems workshops.

Schulze, Norman R.↗