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At least 163 records · Page 9

FY23 Update: Aerosol Sampling for the Canister Deposition Field Demonstration

This report describes the results of preliminary testing of aerosol monitoring equipment that will be used to continuously monitor the aerosol source term for the multi-year Canister Deposition Field Demonstration (CDFD). These data are required inputs for the development and validation of models for the deposition of dust and potentially corrosive salts on the surface of spent nuclear fuel (SNF) dry storage canisters. Surface salt loads correlate with the extent of corrosion damage on a metal surface, and potentially to the likelihood and timing of initiation of stress corrosion cracks. Aerosols will be monitored at the CDFD site using three instruments. A Dekati ® ELPI+ cascade impactor will be used for real-time monitoring of aerosol particle sizes. It will also collect dust in 14 size bins on impactor targets that can be chemically analyzed to determine the soluble salts present as a function of particle size. However, this instrument can only measure dried aerosols, with a diameter of <10 µm. The second instrument is a Topas laser particle size spectrometer, which provides real-time monitoring of aerosol particle sizes up to ~40 µm in size. It monitors both the ambient (potentially deliquesced) aerosol particle size distributions required for the dust deposition models and the distributions of the equivalent dried particles, allowing correlation with the Dekati ® data. However, it does not discriminate between inert dust particles and salt aerosols, and it does not retain samples of the different particle sizes for later analysis. The third instrument that will monitor aerosols at the CDFD site is a Clean Air Status and Trends Network (CASTNET) tower, which uses a multiple canister system to collect weekly samples for analysis to total suspended aerosol particle compositions and atmospheric gas concentrations. This status report describes work in FY23 to develop the capabilities for using these tools. In two training exercises, the cascade impactor and laser particle sizer were deployed in two different testing environments, one indoor and one outdoor. For the cascade impactor, the tests provided opportunities for the operators to familiarize themselves with impactor substrate preparation, and post-test sample removal and analysis. For the laser particle sizer, the tests were used to evaluate different instrument parameters, to determine the most appropriate settings for capturing transient events. Data and samples were collected for weeks to months for each test, and the results are presented here. In addition to the preliminary testing, contracts were developed with WSP Analytical Labs for sample preparation and analysis of the cascade impactor samples. The impactor tower from outdoor test was delivered to WSP and used to train the staff there in disassembly, sample extraction, sample analysis, and tower reassembly with new target substrates. These are tasks that WSP will be performing routinely for the CDFD project. The CASTNET system cannot be purchased or tested until an actual site has been selected for the CDFD test. Work for this FY has been restricted to preparation of contracts for purchasing the CASTNET tower, and for sample analysis, once the tower is in operation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Estimated Diffusion Out of a TRISO Particle Under Ambient Conditions

Many analyses performing diffusion calculations for tri-structural isotropic (TRISO) fuel focus on either reactor conditions or accident scenarios, both instances of elevated temperatures. However, it is worthwhile to understand the diffusion of different elements out of a TRISO particle at ambient atmospheric temperatures, i.e. atmospheric temperatures that are common on the Earth’s surface. This report will outline the thermal analysis and diffusion calculations and then present the results of a generic TRISO particle.

Ivanusa, Pavlo↗

MOSAiC-Colorado State University Ice Spectrometer

This data set contains atmospheric ice nucleating particle (INP) measurements, using Colorado State University&rsquo;s (CSU) Ice Spectrometer (IS), of filter collections taken at the U.S. DOE ARM AMF2 site onboard the R/V Polarstern P-deck during the Multidisciplinary Drifting Observatory for the Study of Arctic Climate (MOSAiC) field campaign. Samples were collected from October 27, 2019 to September 24, 2020. A filter sampler was mounted approximately 15 m above ground level on a railing in proximity to (and approximately 3 m below) the Aerosol Observation System (AOS) inlet. Single-use filter units open to the atmosphere were pre-cleaned and pre-loaded with 47-mm diameter Nuclepore polycarbonate (0.2 &micro;m pore-diameter) filters. Filters were typically drawn for a three-day period, with an average volume of air filtered of 87,000 standard liters. Total volumes were calculated through recorded daily flow rates using a mass flow meter (TSI). After collection, filters were stored and transported frozen until analysis using CSU&rsquo;s IS instrument (McCluskey et al., 2018). Aerosol particles were first re-suspended in 8 mL of 0.1 &micro;m-filtered deionized (DI) water. Aliquots of each suspension, and corresponding 11-fold dilutions, were dispensed into polymerase chain reaction (PCR) trays and placed into the aluminum blocks of the IS. Samples were cooled at approximately 0.33 &deg;C min -1 and freezing detected optically with corresponding temperatures recorded. Cumulative INP concentrations were determined through calculating the number of INPs per mL of suspension (Vali, 1971) and converting to concentration per standard L of air by accounting for the proportion of liquid used and volume of air collected. All samples were corrected for the number of INPs on the average of four field blanks (cleaned, handled, transported, and analyzed in the same way without air flow). Two-tailed, 95% confidence intervals for binomial sampling are provided (Agresti and Coull, 1998). Select samples were also heat treated (95 &deg;C for 20 min) to denature and deactivate biological INPs present and digested in 10% H 2 O 2 at 95 &deg;C under UV-B for 20 min to remove any organic carbon INPs. Agresti, A, and BA Coull. 1998. "Approximate is better than &ldquo;exact&rdquo; for interval estimation of binomial proportions." American Statistics 52: 119&ndash;126. https://doi.org/10.2307/2685469 McCluskey, CS, J Ovadnevaite, M Rinaldi, J Atkinson, F Belosi, D Ceburnis, &hellip; and PJ DeMott. 2018. "Marine and Terrestrial Organic Ice-Nucleating Particles in Pristine Marine to Continentally Influenced Northeast Atlantic Air Masses." Journal of Geophysical Research: Atmospheres 123 (11): 6196&ndash;6212, https://doi.org/10.1029/2017JD028033 Vali, G. 1971. "Quantitative Evaluation of Experimental Results and the Heterogeneous Freezing Nucleation of Supercooled Liquids." Journal of the Atmospheric Sciences 28: 402-209. https://doi.org/10.1175/1520-0469(1971)028<0402:QEOERA>2.0.CO;2

54 ENVIRONMENTAL SCIENCES↗

High Time Resolution Modelled and Measured New Particle Formation Rates During the 2023 Pittsburgh, PA Campaign

Particle size distributions are used to calculate nucleation rates during new particle formation (NPF). However, the low time resolution and poor sensitivity of instruments deployed to observe particle size distributions can lead to inaccurate estimates of nucleation rates. We calculated nucleation rates in Pittsburgh, PA from particle size distributions measured with the new high time resolution Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM) and from gas precursor concentrations measured with a chemical ionization mass spectrometer. The CPC FARM nucleation rates were calculated by examining the appearance rate of particles in the smallest size bin at 1.6 nm. The nucleation rate of 1.6 nm determined every second resulted in positive and negative rates, indicating the influence of inhomogeneous mixing and advection of precursor gases and clusters. These effects are not currently considered when estimating nucleation rates from measurements. The nucleation rates from the CPC FARM were compared to the nucleation rates determined from a transient acid‐base reaction model using measured sulfuric acid concentration, strong base concentrations, and CPC detection efficiencies. The transient form of the model allowed the advection of heterogeneously mixed precursors to influence the nucleation rate. Good agreement between particle and gas‐based nucleation rates is observed during sulfuric acid‐driven NPF events. This study demonstrates that high time resolution measurements of short‐lived and rapidly formed particles are needed to accurately capture nucleation rates, which are likely influenced by advection of nucleation precursors and clusters in heterogeneous environments such as urban areas.

Cheng, D. [Carnegie Mellon Univ., Pittsburgh, PA (↗

Understanding Biomass Burning Aerosol via Integrated Analyses of Aerosol Mass Spectrometry Data from DOE Campaigns and ACRF Long Term Measurements

Biomass burning (BB) is one of the largest sources of aerosol particles in the atmosphere and a significant source of trace gases important to atmospheric chemistry. Organic aerosols from biomass burning sources (BBOA) are an important but poorly characterized component of the earth’s climate system. BBOA composition and life cycle processes are associated with enormous complexities and contribute significantly to model uncertainties. Hence it is important to improve the ability to simulate the concentration and properties (chemical, optical, and hygroscopic) of BBOA and the atmospheric aging processes that affect these properties. Here, we propose to analyze ambient data collected from the DOE Biomass Burning Observation Project (BBOP) field campaign and from a long term measurement site of the Atmospheric Radiation Measurement (ARM) program – the Southern Great Plains (SGP), where transported BB plumes and elevated BBOA episodes were frequently observed. This project is aimed at 1) gaining detailed, quantitative understanding of the chemical and physical properties of BBOA and their chemical changes during atmospheric aging via advanced analysis of aerosol measurement data acquired at the summit of Mt. Bachelor (MBO) during the BBOP campaign and through integration with concurrent measurements of trace gases, particle properties, and meteorological conditions performed at MBO and from the G-1 aircraft; 2) gaining better understanding of BBOA properties and its roles in radiative forcing via analysis of routine data from the ARM long-term measurement sites; and 3) integrating the results from 1) and 2) into a global database of aerosol mass spectrometry and collaborate with modelers on evaluating and improving numerical model performance as part of the ASR program.

54 ENVIRONMENTAL SCIENCES↗

Data analysis in the ICARUS (SBN FD) Cosmic Ray Tagging system

When a cosmic ray particle collides with the upper atmosphere, it creates a shower of particles that transverse down to the Earth’s surface. These cosmogenic particles provide a challenging background in neutrino experiments. The Short Baseline Neutrino (SBN) Program is composed of three Liquid Argon Time Projection Chambers (LArTPCs) that will help us understand the elusive neutrino. Together with a Cosmic Ray Tagger (CRT) system, the ICARUS detector serves as the Far Detector in the SBN Program. The CRT surrounds the detector medium and tags incoming particles allowing us to combat the high flux of comic rays we experience at ICARUS. In this poster, I will show some of the first data analyses done with the fully commissioned CRT system, including studies using CRT timing information and CRT hit reconstruction.

43 PARTICLE ACCELERATORS↗

Nuclear Waste Tank Emission Contributions to Particle Size Distribution

Pollutants from anthropogenic activities including industrial processes are ubiquitous to the environment. To understand the impact from industrial aerosol on climate and human health, industrial aerosol needs to be better characterized. Here, in this study, particle number concentrations were used as a proxy for atmospheric pollutants, which include both particles and gases. Particle concentration and size distribution were measured using a scanning mobility particle sizer (SMPS) approximately 4.5 km from primary industrial areas at the Savannah River Site in Aiken, SC. Industrial areas include numerous nuclear waste storage and processing tanks. The SMPS data were divided into two groups depending on the wind direction measured onsite to categorize transport from the industrial area or from elsewhere. Industrial contributions were found to have a higher concentration of particles with sizes less than 200 nm, 859 ± 564 cm -3 , in comparison to non-industrial attributed particles, 733 ± 495 cm -3 on average from March-July 2021. For sizes larger than 200 nm, industrial and non-industrial particles have a similar concentration, 89 ± 59 cm -3 and 99 ± 61 cm -3 , with non-industrial concentrations being slightly larger. To confirm that industrial particles could travel to the sampling location, air dispersion modeling was completed for specific case studies during the sampling period. The atmospheric dispersion modeling results confirmed that particles released at the industrial areas reached the sampling location when the wind direction was favorable for transport from the industrial areas. The greater concentration of smaller-sized particles in industrial emissions has implications for typical particulate measurements (PM2.5), heath impacts, and climatological influences.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Cloud Water Chemistry and Aerosol Processing: Assessing the Hydroxyl Radical Burst in Newly Formed Cloud Droplets (Field Campaign Report)

Aerosol particles are tiny liquid or solid particles in the atmosphere, ranging in size from a few nanometers to several micrometers in diameter. Aerosol-cloud interactions are the most uncertain aspect of the climate system, and models routinely underpredict aerosol particle formation. Clouds are well known to alter aerosol size, chemical composition, and radiative properties, but the processes are poorly characterized. Organics and sulfates are the most abundant materials in particles, and for each of these there are significant gaps in the understanding of the role of clouds in their formation and/or aging. Many of the cloud processes are driven by aqueous chemistry that depends on hydroxyl (OH) radicals, the subject of this project.

54 ENVIRONMENTAL SCIENCES↗

Effects of Sucrose on Phase Transitions of Organic/Inorganic Aerosols

Aerosol morphology influences the interactions of particles with light, water uptake, and heterogeneous chemistry. Through these mechanisms, morphology may be important to the role of aerosol particles on the climate system. A factor that impacts morphology is the diverse and complex mixture of organic compounds that make up the aerosol particles in the atmosphere. In this paper, we investigate the effect of sucrose on liquid-liquid phase separation. As the amount of sucrose is increased, the oxygen to carbon ratio (O:C) of the particles increases. We demonstrate that the morphology of the particle changes as O:C is increased with phase separation causing the particle to take on a textured appearance due to large or small inclusions, as opposed to a core-shell particle. As a result of the increased O:C ratio, the separation relative humidity (SRH) of the particles decreases and, in all cases, the SRH can be completely arrested with the addition of a sufficiently large concentration of sucrose. The quantity of sucrose required to arrest phase separation of the particles shows a direct correlation with the SRH of the system without sucrose. The identity of the salt further impacts the amount of sucrose required to arrest phase separation and is controlled more strongly by the identity of the anion. When the mixture contains an organic/inorganic combination that is strongly phase separating, phase separation is observed at an O:C of 0.92 which is a higher O:C value than previously shown (O:C > 0.8). Sucrose is compared with several other high O:C compounds to confirm the influence of the average O:C ratio. In all, these effects could drastically influence aerosol processes in the climate system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Millicharged particles from the heavens: single- and multiple-scattering signatures

For nearly a century, studying cosmic-ray air showers has driven progress in our understanding of elementary particle physics. In this work, we revisit the production of millicharged particles in these atmospheric showers and provide new constraints for XENON1T and Super-Kamiokande and new sensitivity estimates of current and future detectors, such as JUNO. We discuss distinct search strategies, specifically studies of single-energy-deposition events, where one electron in the detector receives a relatively large energy transfer, as well as multiple-scattering events consisting of (at least) two relatively small energy depositions. We demonstrate that these atmospheric search strategies — especially the multiple-scattering signature — provide significant room for improvement beyond existing searches, in a way that is complementary to anthropogenic, beam-based searches for MeV-GeV millicharged particles. Finally, we also discuss the implementation of a Monte Carlo simulation for millicharged particle detection in large-volume neutrino detectors, such as IceCube.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

AEROICESTUDY-Colorado State University Ice Spectrometer

The dataset comprises measures, using Colorado State University's Ice Spectrometer (IS, an immersion freezing device with a range from 0 °C down to -26 to -29 °C) of atmospheric ice nucleating particle (INP) concentrations taken at ARM's Southern Great Plains (SGP) Site Guest Instrument Facility (GIF), in Lamont, Oklahoma, during the Aerosol-Ice Formation Closure Pilot Study (AEROICESTUDY). A filter sampler was mounted approximately 6 m above ground level atop the GIF rooftop platform. Single-use filter units open to the atmosphere fitted with pre-cleaned and pre-sterilized, 47-mm diameter Nuclepore polycarbonate filters were used. Filters were typically drawn for either a full day period (9AM-5PM CDT) or broken up into morning (9AM-12PM CDT) and afternoon (1PM-5PM CDT) periods. Additionally, 4 overnight filters were taken (6PM-8AM CDT). The volume of air filtered was typically between 3000 and 8000 standard liters for daily samples. After collection, filters were stored at -20 °C until processed. Initial processing to obtain spectra of INP number concentration active via the immersion freezing mechanism versus temperature was conducted using CSU's IS instrument (McCluskey et al., 2018). For measurement of INPs, collected aerosol particles were re-suspended in 8 mL of 0.1 µm-filtered deionized (DI) water. Aliquots of each suspension, and serial dilutions, were dispensed into trays which were fit into aluminum blocks in the IS. Samples were cooled at 0.33 °C per min and the freezing temperatures of wells recorded automatically. Cumulative INP concentrations were determined by first calculating the INPs per mL of suspension based on Vali (1971) and then converting to concentration per standard liter of air using the proportion of the total liquid sample dispensed and the air sample volumes. Two-tailed, 95% confidence intervals for binomial sampling were based on Equation 2 from Agresti and Coull (1998). Aliquots of suspensions from selected samples were also heat treated (95 °C for 20 min) to denature and deactiv

54 ENVIRONMENTAL SCIENCES↗

CROCUS Dual Polarization Ceilometer Data at Northeastern Illinois University Rooftop

This dataset is from the Department of Energy Office of Science funded project, CROCUS Urban Integrated Field Laboratory (https://crocus-urban.org/). The dual-polarization ceilometer (Vaisala CL61) is an autonomous lidar system operating at 910 nm wavelength, providing valuable measurements for understanding atmospheric boundary layer evolution, air quality, and cloud-aerosol interactions. The CL61 measures the backscattered signal intensity alternating between parallel- and cross-polarization signals. The unique depolarization measurement capability improves discrimination between different particle types, such as liquid droplets, ice crystals, and aerosols. The depolarization is highly dependent on the scatterer shape and orientation (spherical vs non-spherical particles), with the linear depolarization ratio providing a measure of dominant backscatter signal component from atmospheric particles at various heights, essentially allowing discrimination between liquid and solid particles. With its efficient optical system, CL61’s improved signal-to-noise ratio compared to traditional ceilometers allows studying detailed vertical profiles of aerosols and clouds up to 15 km height.Datasets are stored in a netCDF data format, and we we encourage users to make use of the associated toolkits available from Unidata (https://www.unidata.ucar.edu/software/netcdf/), Project Pythia (https://foundations.projectpythia.org/core/data-formats/netcdf-cf.html), and our “Instrument Cookbooks” (https://crocus-urban.github.io/instrument-cookbooks) for more information on how to process the metadata-rich datasets.

54 ENVIRONMENTAL SCIENCES↗

Sunlight can turn smoldering pine wood smoke into a glass

Wildfires inject biomass burning organic aerosols (BBOA) into the atmosphere. During their lifetimes of weeks to months, they are exposed to ultraviolet (UV) irradiation. Viscosity and phase behaviour are essential properties for understanding their chemical and climate impacts. Here, we quantify changes in viscosity and phase behavior after UV exposure. After an atmospheric equivalent of 8.7 days of boundary layer UV exposure, BBOA develop a highly viscous (glassy) outer phase with a viscosity at least five orders of magnitude higher than unaged BBOA, which persists up to at least 58% relative humidity. High-resolution mass spectrometry indicates that UV-aging increases oxidation and molecular weight. Using our viscosity results, we predict that UV-aged BBOA are frequently glassy above ~2.5 km and can have viscosities up to eight orders of magnitude higher than unaged particles in some atmospheric regions, which may influence lifetimes of pollutants and brown carbon, and impact stratospheric ozone chemistry.

Golay, Zoe↗

A Cellular Automaton Simulation for Predicting Phase Evolution in Solid-State Reactions

New computational tools for solid-state synthesis recipe design are needed in order to accelerate the experimental realization of novel functional materials proposed by high-throughput materials discovery workflows. This work contributes a cellular automaton simulation framework for predicting the time-dependent evolution of intermediate and product phases during solid-state reactions as a function of precursor choice and amount, reaction atmosphere, and heating profile. The simulation captures the effects of reactant particle spatial distribution, particle melting, and reaction atmosphere. Reaction rates based on rudimentary kinetics are estimated using density functional theory data from the Materials Project and machine learning estimators for the melting point and the vibrational entropy component of the Gibbs free energy. The resulting simulation framework allows for the prediction of the likely outcome of a reaction recipe before any experiments are performed. We analyze five experimental solid-state recipes for BaTiO 3 , CaZrN 2 , and YMnO 3 found in the literature to illustrate the performance of the model in capturing reaction selectivity and reaction pathways as a function of temperature and precursor choice. This simulation framework offers an easier way to optimize existing recipes, aid in the identification of intermediates, and design effective recipes for yet unrealized inorganic solids in silico .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

X-ray Spectroscopic Quantification of Phosphorus Transformation in Saharan Dust during Trans-Atlantic Dust Transport

Saharan dust is an important phosphorus (P) supply to remote and oligotrophic parts of the oceans and American lowland tropical rainforests. Phosphorus speciation in aeolian dust ultimately controls the release and bioavailability of P after dust deposition, but the speciation in Saharan dust and its change during the trans-Atlantic transport remains unclear. Here, using P K-edge X-ray absorption near edge structure (XANES) spectroscopy, we showed that with increasing dust traveling distance from the Sahara Desert to Cape Verde and to Puerto Rico, about 570 and 4000 km, respectively, the proportion of Ca-bound P (Ca-P), including both apatite and non-apatite forms, decreased from 68–73% to 50–71% and to 21–37%. The changes were accompanied by increased iron/aluminum-bound P proportion from 14–25% to 23–46% and to 44–73%, correspondingly. Laboratory simulation experiments suggest that the changes in P speciation can be ascribed to increasing degrees of particle sorting and atmospheric acidification during dust transport. The presence of relatively soluble non-apatite Ca-P in the Cape Verde dust but not in the Puerto Rico dust is consistent with the higher P water solubility of the former than the latter. Our findings provide insights into the controls of atmospheric processes on P speciation, solubility, and stability in Saharan dust.

54 ENVIRONMENTAL SCIENCES↗