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DOE OSTI2022

Gamma Spectrometry Code Rodeo for Uranium Enrichment—FY 2021 Report

In FY22, the participating Department of Energy (DOE) laboratories continued the work on the project “Gamma Spectrometry Code Rodeo for Uranium Enrichment”. Oak Ridge National Laboratory (ORNL) and Lawrence Livermore National Laboratory (LLNL) continued their efforts to acquire spectra using uranium sources. A collimator (with side and back shields) was custom designed and constructed at ORNL. Spectra were acquired at ORNL using the uranium enrichment standards supplied by New Brunswick Laboratory (NBL) and the collimated M400 detector. Spectra were also acquired using steel absorbers of different thickness placed between the source and the collimated M400 detector. The plan was to ship the collimator to LLNL so that spectra could be acquired using the LLNL detector in collimated geometries. This activity was suspended since problems were noticed with the performance of the LLNL M400 detector. Also, it was brought to light to the project team that some of the aspects of the M400 detector had been updated by the vendor H3D in response to requests by the IAEA. In February 2021, the ORNL and LLNL M400 detectors were returned to the H3D factory in order to resolve the problems with the LLNL detector and to update ORNL and LLNL detectors to the same configuration as the M400 supplied to the IAEA. H3D repaired the LLNL M400 and performed the IAEA updates on both the ORNL and LLNL detectors. ORNL and LLNL received the detectors in April 2021. Data acquisition was continued using the upgraded detectors. ORNL re-collected the spectra using point sources and the NBL standards in uncollimated and collimated geometries. The collimator was shipped from ORNL to LLNL. Spectra were acquired at LLNL through Q4 of FY22. When the ORNL spectra were examined closely, it became apparent that there were spurious artifacts present in some of the spectra. This rendered suspect the ORNL spectra collected in June/July 2021 time frame. ORNL contacted H3D and per H3D’s advice, the M400 detector was returned to H3D for repairs in mid-August 2021. H3D diagnosed the problem and established that the root cause was the extra tight packaging that created a strain on the CZT crystals, causing one of them to break down. The repaired M400 was returned to ORNL in early September 2021. ORNL re-started data acquisition for the third time. Data was continued to be acquired at ORNL and LLNL through September 2021. The ORNL and LLNL data will be shared with the principal investigators from the analyzing laboratories. The GADRAS code and FRAM have been developed to have the capability to analyze the M400 spectra. Good quality spectra from FY21 have been analyzed using modified versions of GADRAS and FRAM. The spectra have also been analyzed using the GEM code. The analysis results from GADRAS, FRAM and GEM codes are presented and discussed in this report. Some preliminary results from FRAM and GEM analysis were presented in February 2021 at the U-Pu Isotopics Workshop sponsored by the IAEA. CZTU code is being modified to analyze M400 spectra. Data collection, code development and analysis will be continued in FY22 as per the FY22 Project Work Plan (PWP).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Microreactor Assembly Transportation Cask Model Description for Criticality Safety Validation Basis Assessment (Rev. 3)

Criticality safety analyses are completed on a transportation cask used for microreactor assembly shipment to provide an example of model and analysis to industry for reproducing this type of study on their microreactor fuel shipment. The fuel assembly considered is based on a gas-cooled microreactor (GC-MR), which utilizes HALEU fuel in the form of TRISO particles and utilizes various design options considered in industry designs. Various versions of this GC-MR assembly were studied, with and without YH 2 moderator, providing similar conclusions. The shipment cask design is revised based on an existing ES-3100 design, developed by Y-12 for the transport of highly enriched uranium (HEU), but is enlarged to hold the GC-MR fuel assembly. Criticality safety analysis for the cask/GC-MR fuel assembly package was performed using the CSAS6 sequence of SCALE6.3.2, utilizing the ENDF/B-VII.1 based continuous energy neutron library, and the analysis strictly follows the guideline from NRC reference reports. Different scenarios, e.g. normal operation, undamaged cask with water flooded, damaged cask with optimal water moderation, have been analyzed and it could be concluded the package would always have a large margin of subcriticality even packed in an infinite array. Sensitivity and similarity analyses are also performed using the TSUNAMI sequence of SCALE6.3.2, and the similarity analysis uses all the experiments from the ICSBEP Handbook with Highly Enriched Uranium (HEU), Intermediate and Mixed Enriched Uranium (IEU) and Low Enriched Uranium (LEU) systems, together with additional ones that are sponsored by the DNCSH program, and selected IRPhEP experiments using TRISO fuel and graphite moderator. These similarity analyses indicate that the dry nominal design has no similar benchmark experiments (ck values greater than 0.8), which may become problematic if more assemblies are shipped together (or a fully loaded core is shipped) and margin to criticality is reduced. However, the cask models with flooded assemblies exhibited similarities to many experiments with c k values greater than 0.8.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2026

Memorial Pools Energy Efficiency Retrofits

The National September 11 Memorial & Museum completed a retrofit of the submergible LED lighting fixtures in its North and South Memorial Pools, located at the World Trade Center site in New York City. The two one-acre pools are illuminated nightly by custom LED fixtures set into their base, and the original lights — in place since 2011 — had begun reaching the end of their useful life, leaving sections of the pools dim or dark. Rather than fully replacing the fixtures, the project team worked with the original manufacturer, Acuity Brands, to retrofit and reuse existing components across all eight pool walls (34 fixtures per wall), reducing cost and waste. Fixtures were shipped in custom crates to Minnesota for retrofitting, then reinstalled onsite by Memorial & Museum staff and contractor ABM. The team addressed two key technical challenges during the project: early leakage in retrofitted fixtures, resolved by introducing vacuum-sealing and nitrogen-fill testing before shipment; and chord damage during transit, resolved with custom-designed shipping crates. All eight pool walls were successfully retrofitted and reinstalled by August 27, 2025, ahead of the 25th anniversary of the September 11, 2001 attacks. Sitewide electrical consumption in September 2025 reflected an approximate 7% reduction, contributing to the institution's broader net-zero and LEED Gold sustainability goals.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2010

TANK 40 FINAL SB6 CHEMICAL CHARACTERIZATION RESULTS

A sample of Sludge Batch 6 (SB6) was taken from Tank 40 in order to obtain radionuclide inventory analyses necessary for compliance with the Waste Acceptance Product Specifications (WAPS), and a portion of the sample was designated for SB6 processing studies. The SB6 WAPS sample was also analyzed for chemical composition including noble metals and fissile composition, and these results are reported here. These analyses along with the WAPS radionuclide analyses will help define the composition of the sludge in Tank 40 that is currently being fed to DWPF as SB6. At the Savannah River National Laboratory (SRNL) the 3-L Tank 40 SB6 sample was transferred from the shipping container into a 4-L high density polyethylene vessel and solids were allowed to settle overnight. Supernate was then siphoned off and circulated through the shipping container to complete the transfer of the sample. Following thorough mixing of the 3-L sample, a 485 g sub-sample was removed. This sub-sample was then utilized for all subsequent analytical samples.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2010

TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: MODIFIED MONOSODIUM TITANATE PHASE III FINAL REPORT

This document provides a final report of Phase III testing activities for the development of modified monosodium titanate (mMST), which exhibits improved strontium and actinide removal characteristics compared to the baseline MST material. The activities included characterization of the crystalline phases present at varying temperatures, solids settling characteristics, quantification of the peroxide content; evaluation of the post-synthesis gas release under different conditions; the extent of desorption of {sup 85}Sr, Np, and Pu under washing conditions; and the effects of age and radiation on the performance of the mMST. Key findings and conclusions include the following. The peroxide content of several mMST samples was determined using iodometric titration. The peroxide content was found to decrease with age or upon extended exposure to elevated temperature. A loss of peroxide was also measured after exposure of the material to an alkaline salt solution similar in composition to the simulated waste solution. To determine if the loss of peroxide with age affects the performance of the material, Sr and actinide removal tests were conducted with samples of varying age. The oldest sample (4 years and 8 months) did show lower Sr and Pu removal performance. When compared to the youngest sample tested (1 month), the oldest sample retained only 15% of the DF for Pu. Previous testing with this sample indicated no decrease in Pu removal performance up to an age of 30 months. No loss in Np removal performance was observed for any of the aged samples, and no uptake of uranium occurred at the typical sorbent loading of 0.2 g/L. Additional testing with a uranium only simulant and higher mMST loading (3.0 g/L) indicated a 10% increase of uranium uptake for a sample aged 3 years and 8 months when compared to the results of the same sample measured at an age of 1 year and 5 months. Performance testing with both baseline-MST and mMST that had been irradiated in a gamma source to a total dose of 3.95 x 10{sup 6} R, indicated little to no affect on the performance of the material to remove Sr and actinides. Previous testing established that mMST releases oxygen gas during the synthesis, and continues to off-gas during storage post synthesis. The post-synthesis gas release rate was measured under several conditions, including varying the pH of the wash water and at elevated temperature (49 C, typical of bounding summertime storage without air conditioning). Results indicated that a high pH (basic) wash reduced the initial gas release rate, but after 2 days the release rates from all different pH washed samples were not statistically different. The gas release rate at 49 C, a temperature at which the material may be exposed to during shipping and storage, was consistently about 2.5 times higher than the rate at room temperature. All gas release results indicated that vented containers would be necessary for shipping and storage of large quantities of material. Suspension of sorbate-loaded solids into diluted solutions representing intermediate and final stages of washing for 24-hours revealed no evidence of desorption of Sr, Pu or Np from the mMST solids. Based on the results of the Phase III testing as well as that from earlier studies (Phases I and II), SRNL researchers recommend adopting the use of the mMST material for the removal of strontium and actinides from the SRS HLW supernatant liquids in the Actinide Removal Process and Salt Waste Processing Facility. Given the decrease in Sr and Pu removal performance for the mMST having an age of 4 years and 8 months, we recommend that mMST be used within 30 months of production. Furthermore we recommend that DOE provide funding to conduct pilot-scale testing of the mixing and settling characteristics of the mMST and impact, if any, on the generation of hydrogen during processing in the Defense Waste Processing Facility (DWPF).

08 HYDROGEN↗
DOE OSTI2010

Global Radiological Source Sorting, Tracking, and Monitoring Project: Phase I Final Report

As a proof of concept tested in an operational context, the Global Radiological Source Sorting, Tracking, and Monitoring (GRadSSTraM) Project successfully demonstrated that radio frequency identification (RFID) and Web 2.0* technologies can be deployed to track controlled shipments between the United States and the European Union. Between November 2009 and May 2010, a total of 19 shipments were successfully shipped from Oak Ridge National Laboratory (ORNL) by the U.S. Postal Service (USPS) and tracked to their delivery at England's National Physical Laboratory (NPL) by the United Kingdom Royal Mail. However, the project can only be viewed as a qualified success as notable shortcomings were observed. Although the origin and terminus of all RFID-enabled shipments were recorded and no shipments were lost, not all the waypoints between ORNL and NPL were incorporated into the pilot. Given limited resources, the project team was able to install RFID listeners/actuators at three waypoints between the two endpoints. Although it is likely that all shipments followed the same route between ORNL and NPL, it cannot be determined beyond question that all 19 shipments were routed on identical itineraries past the same three waypoints. The pilot also raises the distinct possibility that unattended RFID tracking alone, without positive confirmation that a tagged item has been properly recorded by an RFID reader, does not meet a rigorous standard for shipping controlled items. Indeed, the proof of concept test strongly suggests that a multifaceted approach to tracking may be called for, including tracking methods that are capable of reading and accepting multiple inputs for individual items [e.g., carrier-provided tracking numbers, Universal Product Codes (UPCs), and RFID tags]. For controlled items, another apparent requirement is a confirmation feature, human or otherwise, which can certify that an item's RFID tag, UPC, or tracking number has been recorded.

42 ENGINEERING↗
DOE OSTI2026

Block Island Survey and Deployment Operations Data

This dataset contains survey, navigation, and platform-design data supporting instrument deployment and positioning during the 2016-2017 RODEO field operations at Block Island. It includes an acoustic localization software toolkit and its Block Island position solutions, R/V Tioga ship navigation and underway data, CTD casts, ship-track charts, and engineering designs for the deployed moorings and arrays.

17 WIND ENERGY↗
DOE OSTI2012

Broadband Acoustic Environment at a Tidal Energy Site in Puget Sound

Admiralty Inlet has been selected as a potential tidal energy site. It is located near shipping lanes, is a highly variable acoustic environment, and is frequented by the endangered southern resident killer whale (SRKW). Resolving environmental impacts is the first step to receiving approval to deploy tidal turbines. Several monitoring technologies are being considered to determine the presence of SRKW near the turbines. Broadband noise level measurements are critical for determining design and operational specifications of these technologies. Acoustic environment data at the proposed site was acquired at different depths using a cabled vertical line array from three different cruises during high tidal period in February, May, and June 2011. The ambient noise level decreases approximately 25 dB re 1 μPa per octave from frequency ranges of 1 kHz to 70 kHz, and increases approximately 20 dB re 1 μPa per octave for the frequency from 70 kHz to 200 kHz. The difference of noise pressure levels in different months varies from 10 to 30 dB re 1 μPa for the frequency range below 70 kHz. Commercial shipping and ferry vessel traffic were found to be the most significant contributors to sound pressure levels for the frequency range from 100 Hz to 70 kHz, and the variation could be as high as 30 dB re 1 μPa. These noise level measurements provide the basic information for designing and evaluating both active and passive monitoring systems proposed for deploying and operating for tidal power generation alert system.

16 TIDAL AND WAVE POWER↗
DOE OSTI2011

Anthropogenic sulfur dioxide emissions: 1850-2005

Sulfur aerosols impact human health, ecosystems, agriculture, and global and regional climate. A new annual estimate of anthropogenic global and regional sulfur dioxide emissions has been constructed spanning the period 1850 2005 using a bottom-up mass balance method, calibrated to country-level inventory data. Global emissions peaked in the early 1970s and decreased until 2000, with an increase in recent years due to increased emissions in China, international shipping, and developing countries in general. An uncertainty analysis was conducted including both random and systemic uncertainties. The overall global uncertainty in sulfur dioxide emissions is relatively small, but regional uncertainties ranged up to 30%. The largest contributors to uncertainty at present are emissions from China and international shipping. Emissions were distributed on a 0.5 grid by sector for use in coordinated climate model experiments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign averaged longitudinal gradients, and highlight differences in model simulations with (W) and without wet (NW) deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptual model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, including the reliability required for policy analysis and geo-engineering applications.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Sources of black carbon aerosols in South Asia and surrounding regions during the Integrated Campaign for Aerosols, Gases and Radiation Budget (ICARB)

This study examines differences in the surface black carbon (BC) aerosol loading between the Bay of Bengal (BoB) and the Arabian Sea (AS) and identifies dominant sources of BC in South Asia and surrounding regions during March–May 2006 (Integrated Campaign for Aerosols, Gases and Radiation Budget, ICARB) period. A total of 13 BC tracers are introduced in the Weather Research and Forecasting Model coupled with Chemistry to address these objectives. The model reproduced the temporal and spatial variability of BC distribution observed over the AS and the BoB during the ICARB ship cruise and captured spatial variability at the inland sites. In general, the model underestimates the observed BC mass concentrations. However, the model–observation discrepancy in this study is smaller compared to previous studies. Model results show that ICARB measurements were fairly well representative of the AS and the BoB during the pre-monsoon season. Elevated BC mass concentrations in the BoB are due to 5 times stronger influence of anthropogenic emissions on the BoB compared to the AS. Biomass burning in Burma also affects the BoB much more strongly than the AS. Results show that anthropogenic and biomass burning emissions, respectively, accounted for 60 and 37% of the average ± standard deviation (representing spatial and temporal variability) BC mass concentration (1341 ± 2353 ng m -3 ) in South Asia. BC emissions from residential (61%) and industrial (23%) sectors are the major anthropogenic sources, except in the Himalayas where vehicular emissions dominate. We find that regional-scale transport of anthropogenic emissions contributes up to 25% of BC mass concentrations in western and eastern India, suggesting that surface BC mass concentrations cannot be linked directly to the local emissions in different regions of South Asia.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Russia's black carbon emissions: focus on diesel sources

Black carbon (BC) is a significant climate forcer with a particularly pronounced forcing effect in polar regions such as the Russian Arctic. Diesel combustion is a major global source of BC emissions, accounting for 25–30 % of all BC emissions. While the demand for diesel is growing in Russia, the country's diesel emissions are poorly understood. This paper presents a detailed inventory of Russian BC emissions from diesel sources. Drawing on a complete Russian vehicle registry with detailed information about vehicle types and emission standards, this paper analyzes BC emissions from diesel on-road vehicles. We use the COPERT emission model (COmputer Programme to calculate Emissions from Road Transport) with Russia-specific emission factors for all types of on-road vehicles. On-road diesel vehicles emitted 21 Gg of BC in 2014: heavy-duty trucks account for 60% of the on-road BC emissions, while cars represent only 5% (light commercial vehicles and buses account for the remainder). Using Russian activity data and fuel-based emission factors, the paper also presents BC emissions from diesel locomotives and ships, off-road engines in industry, construction and agriculture, and generators. The study also factors in the role of superemitters in BC emissions from diesel on-road vehicles and off-road sources. The total emissions from diesel sources in Russia are estimated to be 49 Gg of BC and 17 Gg of organic carbon (OC) in 2014. Off-road diesel sources emitted 58% of all diesel BC in Russia.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

The efficacy of aerosol–cloud radiative perturbations from near-surface emissions in deep open-cell stratocumuli

Aerosol–cloud radiative effects are determined and quantified in simulationsof deep open-cell stratocumuli observed during the VAMOS Ocean-Cloud-Atmosphere-LandStudy Regional Experiment (VOCALS-REx) campaign offthe west coast of Chile. The cloud deck forms in a boundarylayer 1.5 km deep, with cell sizes reaching 50 km in diameter. Global databases of shiptracks suggest that these linear structures are seldom found in boundarylayers this deep. Here, we quantify the changes in cloud radiative propertiesto a continuous aerosol point source moving along a fixed emission linereleasing 10 17 particles per second. We show that a spatially coherentcloud perturbation is not evident along the emission line. Yet our modelsimulates an increase in domain-mean all-sky albedo of 0.05, corresponding toa diurnally averaged cloud radiative effect of 20 W m -2 , given theannual mean solar insolation at the VOCALS-REx site. Therefore, markedchanges in cloud radiative properties in precipitating deep open cells may bedriven by anthropogenic near-surface aerosol perturbations, such as thosegenerated by ships.Furthermore, we demonstrate that these changes in cloud radiative propertiesare masked by the naturally occurring variability within the organised cloudfield. A clear detection and attribution of cloud radiative effects to aperturbation in aerosol concentrations becomes possible when sub-filtering ofthe cloud field is applied, using the spatio-temporal distribution of theaerosol perturbation. Therefore, this work has implications for the detectionand attribution of effective cloud radiative forcing in marine stratocumuli,which constitutes one of the major physical uncertainties within the climatesystem. Our results suggest that ships may sometimes have a substantialradiative effect on marine clouds and albedo, even when ship tracks are notreadily visible.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Opportunistic experiments to constrain aerosol effective radiative forcing

Aerosol–cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide “opportunistic experiments” (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)

The MIXv2 Asian emission inventory is developed under the framework of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase IV and produced from a mosaic of up-to-date regional emission inventories. We estimated the emissions for anthropogenic and biomass burning sources covering 23 countries and regions in East, Southeast and South Asia and aggregated emissions to a uniform spatial and temporal resolution for seven sectors: power, industry, residential, transportation, agriculture, open biomass burning and shipping. Compared to MIXv1, we extended the dataset to 2010–2017, included emissions of open biomass burning and shipping, and provided model-ready emissions of SAPRC99, SAPRC07, and CB05. A series of unit-based point source information was incorporated covering power plants in China and India. A consistent speciation framework for non-methane volatile organic compounds (NMVOCs) was applied to develop emissions by three chemical mechanisms. The total Asian emissions for anthropogenic/open biomass sectors in 2017 are estimated as follows: 41.6/1.1 Tg NO x , 33.2/0.1 Tg SO 2 , 258.2/20.6 Tg CO, 61.8/8.2 Tg NMVOC, 28.3/0.3 Tg NH 3 , 24.0/2.6 Tg PM 10 , 16.7/2.0 Tg PM 2.5 , 2.7/0.1 Tg BC (black carbon), 5.3/0.9 Tg OC (organic carbon), and 18.0/0.4 Pg CO 2 . The contributions of India and Southeast Asia were emerging in Asia during 2010–2017, especially for SO 2 , NH 3 and particulate matter. Gridded emissions at a spatial resolution of 0.1° with monthly variations are now publicly available. This updated long-term emission mosaic inventory is ready to facilitate air quality and climate model simulations, as well as policymaking and associated analyses.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

The sources and diurnal variations of submicron aerosols in a coastal–rural environment near Houston, US

Aerosol properties were characterized at a rural site southwest of Houston from May to September 2022 during the intensive operation periods (IOPs) of the Tracking Aerosol Convection Interactions ExpeRiment (TRACER). Backward trajectory analysis reveals three major air mass types: marine air mass from the Gulf, urban air mass influenced by urban emissions, and regional air mass. Marine aerosols typically show a bimodal size distribution and have the lowest particle number and mass concentrations of PM 1 (particulate matter with an aerodynamic diameter of less than 1 µm), while aerosols from air masses strongly influenced by urban emissions exhibit the highest concentrations. Organic aerosol (OA) accounts for more than 50 % of PM 1 for urban and regional air masses, whereas sulfate is comparable to OA in marine air masses. Positive matrix factorization (PMF) analysis of aerosol mass spectra identifies 6 OA factors: hydrocarbon-like OA (HOA), OA from the oxidation of monoterpenes (MT-SOA), OA from the reactive uptake of isoprene epoxydiols by acidic sulfate particles (isoprene-SOA), oxygenated OA arising from shipping emissions (shipping-OOA), and two oxygenated OA factors with high O : C ratios (OOA1 and OOA2). OOA2 has the highest O : C ratio and exhibits elevated mass concentration in the afternoon. Similar diurnal variation of highly oxidized OA factors was commonly observed in the Houston area during previous studies and attributed to the SOA formation by photochemistry and mixing from aloft. Here, using air mass backward trajectories and a 1-D box model, we show the diurnal trend of OOA2 mass concentration is instead driven by changes in air mass arriving at the rural site. The air mass changes are likely caused by the shift between land breezes and sea/bay breezes. Within the same air mass type (e.g., either urban or marine air mass), OOA2 mass concentration is largely independent of wind direction and shows essentially no diurnal variation, suggesting OOA2 is related to aged OA with minimal influence by local emissions. This study helps identify the major sources of OA in the Houston region and highlights the impacts of both atmospheric chemistry and meteorology on aerosol properties in the coastal–rural environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2011

Anthropogenic Sulfur Dioxide Emissions: 1850-2005

Sulfur aerosols impact human health, ecosystems, agriculture, and global and regional climate. A new annual estimate of anthropogenic global and regional sulfur dioxide emissions has been constructed spanning the period 1850 - 2005. A combination of mass balance and best available inventory data was used in order to achieve the most accurate estimate possible. Global emissions peaked in the early 1970s and decreased until 2000, with an increase in recent years due to increased emissions in China, international shipping, and developing countries in general. An uncertainty analysis was conducted including both random and systemic uncertainties. The overall global uncertainty in sulfur dioxide emissions is relatively small, but regional uncertainties of up to 30% were found. The largest contributors to uncertainty at present are emissions from China and international shipping.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Aircraft measurements of BrO, IO, glyoxal, NO 2 , H 2 O, O 2 –O 2 and aerosol extinction profiles in the tropics: comparison with aircraft-/ship-based in situ and lidar measurements

Here, tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO 2 ), water vapor (H 2 O) and O 2 –O 2 collision complexes (O 4 ) were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAX-DOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H 2 O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O 4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O 4 -inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCD REF , maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2–0.55 pptv IO and 32–36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and aircraft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6° N; 101.2 to 97.4° W). At 14.5 km, 5–10 pptv NO 2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO 2 and BrO). Our profile retrievals have 12–20 degrees of freedom (DoF) and up to 500 m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 × 10 13 molec cm –2 (RF12) and at least 0.5 × 10 13 molec cm –2 (RF17, 0–10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 × 10 12 molec cm –2 (RF12) and 2.5 × 10 12 molec cm –2 (RF17) and glyoxal VCDs of 2.6 × 10 14 molec cm –2 (RF12) and 2.7 × 10 14 molec cm –2 (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 ± 5%, 0.1–0.2 pptv; glyoxal: 52 ± 5%, 3–20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗