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DOE OSTI2021

Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere

The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about -1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R 2 < 0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15–39%.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Transportation Energy Data Book (Edition 40)

The Transportation Energy Data Book: Edition 40 is a statistical compendium prepared and published by Oak Ridge National Laboratory (ORNL) under contract with the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. Designed for use as a desk-top reference, the Data Book represents an assembly and display of statistics and information that characterize transportation activity and presents data on other factors that influence transportation energy use. The purpose of this document is to present relevant statistical data in the form of tables and graphs. The latest edition of the Data Book is available via the Internet (tedb.ornl.gov).This edition of the Data Book has 13 chapters which focus on various aspects of the transportation industry. Chapter 1 focuses on petroleum; Chapter 2 – energy; Chapter 3 – highway vehicles; Chapter 4 – light vehicles; Chapter 5 – heavy vehicles; Chapter 6 – alternative fuel vehicles; Chapter 7 – transit and other shared mobility; Chapter 8 – fleet vehicles; Chapter 9 – household vehicles; Chapter 10 – nonhighway modes; Chapter 11 – transportation and the economy; Chapter 12 – greenhouse gas emissions; and Chapter 13 – criteria pollutant emissions. The sources used represent the latest available data. There are also two appendices which include detailed source information for some tables and measures of conversion. A glossary of terms is also included for the reader’s convenience.

02 PETROLEUM↗

DOE OSTI2025

Long-Range Transport of Biomass Burning Aerosols from Southern Africa: A Case Study Using Layered Atlantic Smoke Interactions with Clouds Observations

A case study of an incoming biomass burning aerosol plume at Ascension Island is analyzed for the peak of the 2017 fire season using satellites, reanalysis and in situ observations. Measurements from the Atmospheric Radiation Measurement Mobile Facility 1 reveal an abrupt change from relatively clean conditions (~70 parts per billion by volume of carbon monoxide) to a more polluted state (~150 parts per billion by volume of carbon monoxide). Corresponding changes in aerosol size reveal a broadening of size distributions toward larger optical diameters, consistent with the arrival of aged aerosols. Within a 24 h period, black carbon fraction increases ~500% from ~300 ng m e to ~1500 ng m 3 , while light absorption coefficients increase ~300%. Long-range transport of these aerosols is primarily confined between 2 and 5 km above sea level along the northwesterly trade winds. Our results show that the primary driver of increases in aerosol loading over Ascension Island is an intensification of the St. Helena high-pressure system (anticyclone) that leads to a weakening of trade winds and increases westward transport on its northern flank. A better understanding of the complex interactions between air quality, meteorology and long-range aerosol transport is important for future modeling studies focused on aerosol–cloud–radiation interactions over the open ocean and reducing its associated uncertainties.

aerosol size distribution↗

NASA NTRS1974

Aerodynamic size distribution of suspended particulate matter in the ambient air in the city of Cleveland, Ohio

The City of Cleveland Division of Air Pollution Control and NASA jointly investigated the chemical and physical characteristics of the suspended particulate matter in Cleveland, and as part of the program, measurements of the particle size distribution of ambient air samples at five urban locations during August and September 1972 were made using high-volume cascade impactions. The distributions were evaluated for lognormality, and the mass median diameters were compared between locations and as a function of resultant wind direction. Junge-type distributions were consistent with dirty continental aerosols. About two-thirds of the suspended particulate matter observed in Cleveland is less than 7 microns in diameter.

Leibecki, H. F.↗

NASA NTRS1980

A global biogeocenotical biosphere simulation

This model of the D. Forrester type, constructed in differential equations, predicts the food and mineral supply for the factors biosphere population, depending on two socio-economic factors, until about the year 2500. If contemporary rates of natural resources utilization are maintained and there is no management of the environment, food resources will begin to limit human population growth after 2200, and mineral resources will after 2300. A decrease in the biosphere pollution, increase in effective agricultural production, and discovery of new energy sources may forestall or completely avert the onset of a crisis situation. Conservation measures, according to the model, are to a considerable extent realizable only if carried out simultaneously in both areas.

Moiseyev, N. N.↗

NASA NTRS1981

A diagnostic model for studying daytime urban air quality trends

A single cell Eulerian photochemical air quality simulation model was developed and validated for selected days of the 1976 St. Louis Regional Air Pollution Study (RAPS) data sets; parameterizations of variables in the model and validation studies using the model are discussed. Good agreement was obtained between measured and modeled concentrations of NO, CO, and NO2 for all days simulated. The maximum concentration of O3 was also predicted well. Predicted species concentrations were relatively insensitive to small variations in CO and NOx emissions and to the concentrations of species which are entrained as the mixed layer rises.

Brewer, D. A.↗

NASA NTRSDate not supplied

NASA DEVELOP’s Approach to Building Individual and Institutional Capacity to Use Earth Observations for Atmospheric Monitoring and Decision Making

NASA DEVELOP, an Applied Sciences’ Capacity Building program, introduces individuals and institutions to the applications of NASA Earth observation data in an effort to help inform decision making. The program employs early career professionals to conduct rapid feasibility studies tailored specific to partner needs. Each year, DEVELOP conducts 50-60 feasibility studies that highlight the capabilities of Earth observations for measuring and monitoring a wide range of environmental phenomena. For this presentation, example projects will be highlighted that focus on monitoring air quality and pollution, wildfire emissions, and greenhouse gasses such as methane. An overview of example projects, the user communities involved, satellite data used, and lessons learned will be shared.

Capacity Building↗

NASA NTRS2021

Chemical Transport Models Often Underestimate Inorganic Atmospheric Aerosol Acidity in Remote Regions of the Atmosphere

The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about -1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R(exp 2) < 0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15-39%.

Chemical transport model↗

NASA NTRS2022

Sources, Transport and Visibility Impact of Ambient Submicrometer Particle Size Distributions in an Urban Area of Central Taiwan

This study applied positive matrix factorization (PMF) to identify the sources of size-resolved submicrometer (10–1000 nm) particles and quantify their contributions to impaired visibility based on the particle number size distributions (PNSDs), aerosol light extinction (b p ), air pollutants (PM 10 , PM 2.5 , SO 2 , O 3 , and NO), and meteorological parameters (temperature, relative humidity, wind speed, wind direction, and ultraviolet index) measured hourly over an urban basin in central Taiwan between 2017 and 2021. The transport of source-specific PNSDs was evaluated with wind and back trajectory analyses. The PMF revealed six sources to the total particle number (TPN), surface (TPS), volume (TPV), and b p . Factor 1 (F1), the key contributor to TPN (35.0 %), represented nucleation (<25 nm) particles associated with fresh traffic emission and secondary new particle formation, which were transported from the west-southwest by stronger winds (>2.2 m s -1 ). F2 represented the large Aitken (50–100 nm) particles transported regionally via northerly winds, whereas F3 represented large accumulation (300–1000 nm) particles, which showed elevated concentrations under stagnant conditions (<1.1 m s −1 ). F4 represented small Aitken (25–50 nm) particles arising from the growth and transport of the nucleation particles (F1) via west-southwesterly winds. F5 represented large Aitken particles originating from combustion-related SO 2 sources and carried by west-northwesterly winds. F6 represented small accumulation (100–300 nm) particles emitted both by local sources and by the remote SO 2 sources found for F5. Overall, large accumulation particles (F3) played the greatest role in determining the TPV (66.4 %) and TPS (34.8 %), and their contribution to bp increased markedly from 17.3 % to 40.7 % as visibility decreased, indicating that TPV and TPS are better metrics than TPN for estimating b p . Furthermore, slow-moving air masses—and therefore stagnant conditions—facilitate the build-up of accumulation mode particles (F3 + F6), resulting in the poorest visibility.

source apportionment↗

NASA NTRS1977

A theoretical/experimental program to develop active optical pollution sensors

Light detection and ranging (LIDAR) technology was applied to the assessment of air quality, and its usefulness was evaluated by actual field tests. Necessary hardware was successfully constructed and operated in the field. Measurements of necessary physical parameters, such as SO2 absorption coefficients were successfully completed and theoretical predictions of differential absorption performance were reported. Plume modeling improvements were proposed. A full scale field test of equipment, data analysis and auxiliary data support was conducted in Maryland during September 1976.

Mills, F. S.↗

NASA NTRS2000

Ozone and Water Vapor Measurements by Raman Lidar in the Planetary Boundary Layer: Error Sources and Field Measurements

Why do we need time series of ozone and water vapor profiles at low altitude? The degradation of air quality is a very serious environmental problem that affects urban and industrial areas worldwide. Air pollution injures human health and ecosystems, diminishes crop yield, and spoils patrimony and materials. The phenomena involved in air pollution are very complex. Once emitted into the atmosphere, (primary) pollutants are transported, dispersed, transformed by gas/solid phase change and chemical reaction, and finally removed by dry and wet deposition. Most challenging is the fact that the health and environmental impacts of secondary pollutants (formed in the atmosphere) are frequently more severe than those of their precursors (primary pollutants). This is the case of ozone and other photochemical pollutants, such as peroxyacetil nitrate (PAN) and secondary particles, produced in the atmosphere by the photo-oxidation volatile organic compounds (VOC) catalyzed by nitrogen oxides (NO(sub x)). Photochemical air pollution is a complex science because of the non-linearity of its response to changes in primary emission.

Lazzarotto, Benoit↗

DOE OSTI2023

Comparing measurements of the mixing layer height to modeled values

The mixing layer height (MLH) is the top layer of turbulent mixing within the lower atmosphere, above the Earth’s surface. Estimates of the mixing layer height allow us to determine the volume available for the dispersion of pollutants throughout the atmosphere. Our goal is to identify the most suitable mixing layer height input for our dispersion modeling tool (AERMOD). For this project we evaluated two different methods of estimating the local mixing layer height. First, we use 3 estimates of the mixing layer height obtained from a ceilometer, each height estimate corresponds to a different gradient in aerosol backscatter which is used as a proxy for mixing layer height identification. Second, we use AERMET, our AERMOD modeling system preprocessor for meteorological data, which estimates the mixing layer height using several equations combined with measured meteorological data. We evaluate the ceilometer and AERMET estimates over a 5-year period (2015-2019) to see how well aligned the estimated mixing layer heights are. Our results suggest that our model, AERMET, is on average, aligned with ceilometer estimates during the daytime hours. However, daily maximum MLH estimates by AERMET occur earlier in the day than those estimated by the ceilometer. We believe that the ceilometer struggles with accurately measuring the MLH during nighttime hours as a result of sensor limitations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Intercomparison of airborne and surface-based measurements during the CLARIFY, ORACLES and LASIC field experiments

Data are presented from intercomparisons between two research aircraft, the FAAM BAe-146 and the NASA Lockheed P3, and between the BAe-146 and the surface-based DOE (Department of Energy) ARM (Atmospheric Radiation Monitoring) Mobile Facility at Ascension Island (8 S, 14.5W, a remote island in the mid-Atlantic). These took place from 17 August to 5 September 2017, during the African biomass burning season. The primary motivation was to give confidence in the use of data from multiple platforms with which to evaluate numerical climate models. The three platforms were involved in the CLouds-Aerosol-Radiation Interaction and Forcing for Year 2017 (CLARIFY-2017), ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), and Layered Atlantic Smoke and Interactions with Clouds (LASIC) field experiments. Comparisons from flight segments on six days where the BAe-146 flew alongside the ARM facility on Ascension Island are presented, along with comparisons from wing-tip to wing-tip flight of the P3 and BAe-146 on 18 th August 2017. The intercomparison flight sampled a relatively clean atmosphere overlying a moderately polluted boundary layer, while the 6 fly-bys of the ARM site sampled both clean and polluted conditions 2–4 km upwind. We compare and validate characterisations of aerosol physical, chemical, and optical properties, atmospheric radiation, and cloud microphysics between platforms. We assess the performance of measurement instrumentation in the field, under conditions where sampling conditions are not tightly controlled as in laboratory measurements where calibrations are performed. Solar radiation measurements compared well between airborne platforms. Optical absorption coefficient measurements compared well across all three platforms, even though absolute magnitudes were often low (< 10 Mm -1 ) and close to the sensitivity limits of measurement instrumentation thereby confounding assessments of the comparability of absorption Ångström exponent characterisations. Aerosol absorption measurements from airborne platforms were more comparable than aircraft-to-ground observations. Scattering coefficient observations compared well between airborne platforms, but agreement with ground-based measurements was worse, potentially caused by small differences in sampling conditions or actual aerosol population differences. Chemical composition measurements followed a similar pattern, with better comparisons between the airborne platforms. Thermodynamics, aerosol, and cloud microphysical properties generally compared well.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2000

Clear-Sky Closure Studies of Tropospheric Aerosol and Water Vapor During ACE-2 Using Airborne Sunphotometer, Airborne In-Situ, Space-Borne, and Ground-Based Measurements

We report on clear-sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE-2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in-situ (a differential mobility analyzer, three optical particle counters, three nephelometers, and one absorption photometer) measurements taken aboard the Pelican aircraft, space-borne NOAA/AVHRR data and ground-based lidars. A wide range of aerosol types was encountered throughout the ACE-2 area, including background Atlantic marine, European pollution-derived, and (although less frequently than expected) African mineral dust. During the two days discussed here, vertical profiles flown in cloud free air masses revealed three distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. Based on size-resolved composition information we have established an aerosol model that allows us to compute optical properties of the ambient aerosol using the optical particle counter results. In the dust, the agreement in layer AOD (lambda=380-1060 nm) is 3-8%. In the MBL there is a tendency for the in-situ results to be slightly lower than the sunphotometer measurements (10-17% at lambda=525 nm), but these differences are within the combined error bars of the measurements and computations. Aerosol size-distribudon closure based on in-situ size distributions and inverted sunphotometer extinction spectra has been achieved in the MBL (total surface area and volume agree within 0.2, and 7%, respectively) but not in the dust layer. The fact that the three nephelometers operated at three different relative humidities (RH) allowed to parameterize hygroscopic growth and to therefore estimate optical properties at ambient RH. The parameters derived for different aerosol types are themselves useful for the aerosol modeling community. The fact that the nephelometers and the absorption photometer sampled the aerosol through a cyclone make those measurements less useful for thee closure study carried out here. Large corrections (especially in the dust) had to be applied. Therefore, it is not surprising that closure with the sunphotometer was not always achieved. Agreement within 0.02 in AOD was achieved in the dust layer when the airorne sunphotometer extinction or AOD was compared to ground-based lidar measurements. We found that the presence of the elevated dust layers removes the good agreement between satellite and sunphotometer AOD usually found in the absence of the dust layer. We still compare the scattering phase functions used in the satellite retrieval with those obtained from the aerosol or the sunphotometer measurements.

Schmid, Beat↗

NASA NTRS2018

Investigation of NO2 Measurements Made During DISCOVER-AQ and KORUS-AQ Campaigns in Conjunction with NO2 Tropospheric Column from the Ozone Monitoring Instrument (OMI) and High-Resolution Community Multi-Scale Air Quality (CMAQ) Model Simulation

Atmospheric NO2 is produced by combustion, lightning, and in soil. NO2 affects ozone production and criteria pollutant itself.It also has indirect radiative impacts in the troposphere, since ozone has largest warming effect in upper troposphere. Tropospheric vertical column densities (VCD) of NO2 are available from satellites (GOME, OMI, SCIAMACHY, GOME-2). DISCOVER-AQ and KORUS-AQ aircraft campaigns we reconducted to improve the use of satellites to monitor air quality for public health and environmental benefit in United States and South Korea. In this study, we investigate 1) How do these measurements compare? 2) What is the best way to make comparisons of space- and ground-based measurements?

multi-scale air quality↗

NASA NTRSDate not supplied

Illustrating the Spatiotemporal Complexity of No2 Columns Using A Multi-Perspective Observing System: Moving Toward Geostationary Product Validation and Applications

As a precursor to secondary pollutants like ozone and PM2.5, nitrogen dioxide (NO2) is crucial to understand when addressing air quality issues. However, due to NO2’s short lifetime during the daytime and complexity of emission sources in urbanized regions, interpreting datasets from ground or satellite perspectives alone are challenged by variance in spatial and temporal resolutions. High resolution airborne mapping (< 1 km) of NO2 column densities across morning, midday, and afternoon add a unique perspective toward interpreting satellite data with respect to ground-measurements. This presentation focuses on the interpretation of spatiotemporal complexity of NO2 columns from the Synergistic TEMPO Air Quality Science Study (STAQS). The mission’s goal is to integrate geostationary observations from Tropospheric Emissions: Monitoring of Pollution (TEMPO) with traditional and enhanced air quality monitoring to improve the understanding of air quality science for increased societal benefit. We will demonstrate the interweaved perspective of NO2 columns from ground-based Pandora spectrometers and satellite-based observations (e.g., TROPOMI) as compared to high spatial resolution airborne observations from the GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS). This includes the evaluation of each dataset through comparison to each other to identify potential biases in data products and the impact of heterogeneity on these comparisons. Airborne data will also be used as a proxy for geostationary observations with morning, midday, and afternoon raster maps collected over four cities (Los Angeles, Chicago, Toronto, and New York City). Finally, recent research outcomes will be presented to demonstrate how airborne and geostationary observations can be used to evaluate emission inventories and air quality models.

Laura Judd↗

DOE OSTI2020

Feedback on Forty-year Long Clean-up Operations of a Contaminated Soil for Environmental Purpose - 20026

One of the CEA facilities in France is the place of miscellaneous mapping and clean-up operations since the 1980's. The final purpose of the conducted work deals with the environmental remediation of the building. In France, the absence of a regulatory framework for the management of sites polluted by radioactive substances, especially as the lack of release thresholds, has led to develop different approaches of soil radiological characterization. The geostatistical approach is part of them. Preliminary investigations are an unavoidable step prior to clearance and remediation. First, historical analysis enables to define site perimeters to investigate as well as to precisely locate expected contaminated parts. For radioactive pollutants, the media (water, soil, air) and transfer routes participate in the definition of the investigation perimeter and thus also need to be identified through a geological study. At the same time, functional analysis leads to choose the best measurement means which could provide useful information when combined with visual inspection. An equipment well adapted to easy-to-measure radionuclides as gamma emitters, such as gamma probe or on-site gamma spectrometry, is usually selected as a non-destructive assay. Coupled with spatial positions, processed on-site radiological data can be mapped. Data processing consists in mapping and kriging before a geostatistical analysis in order to identify the zones of interest to be targeted. Selected zones are not only linked to high level count rates but also to low level ones so that a pollution-free reference is known in the area. This data processing also enables to categorize waste types according to their origin and contamination levels. An expected volume of different waste then follows as well as the waste characterization equipments. In-depth investigations, e.g. core drillings and samplings, naturally ensue to aim at remediation optimization through the assessment of environmental impact. After clean-up operations, non-destructive assays as well as destructive samplings enable to check the effective clearance. Following this methodology in the present remediation work, results of the first non-destructive assay campaign highlighted a long-lived transuranic radionuclides contamination in the concrete flagstone. Successive non-destructive assays were then performed in the defined zones of interest. Count rates measured with a surface probe were first mapped. The best localization of destructive assays, i.e. core drillings at a 1 meter depth, came from this surface mapping followed by a geostatistical analysis. The concrete flagstone was totally removed. Then, the depth of soil to remove under the flagstone was optimized from the results of radiological activities measured in core drillings samples. A new surface mapping was then drawn after this partial soil excavation. The sand and demolition rubble samples, homogeneously constituted from the flagstone fragments, were analyzed by gamma spectrometry. Meanwhile, waste drums and other containers were also measured by gamma spectrometry and passive neutron measurement devices. All these results have brought miscellaneous pieces of information. In this context, major issues appear in terms of physical constraints such as the premises tininess as well as of soil sampling techniques and in terms of measurement performances assessment and the representativeness of homogeneous samples. The choice of radiological soil and waste characterization devices is described in the light of enhanced performances by keeping in mind radiation protection requirements and a willing to always optimize waste categories (very low level waste) and volume. The improvement of the characterization methods appears through this forty-year long work while sharing the feedback of encountered difficulties. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRSDate not supplied

Sub-City-Scale Air Quality Forecasts Combining Models, Satellites, and Surface Measures

Poor air quality is a global major concern, especially in cities with their higher emissions and large numbers of exposed people. Air quality monitoring has traditionally relied on ground-based measurements from a few accurate but expensive regulatory-grade monitors, leading to limited spatial data coverage. More recently, these have been supplemented with other data sources, including satellite observations of pollutants, atmospheric chemistry model simulations, and low-cost monitors allowing for denser spatial data collection at the expense of lower accuracy compared to regulatory-grade monitors. Each of these air quality data sources have their own benefits and drawbacks, and so there is an opportunity to combine these data together while respecting their relative strengths and weaknesses in order to generate a more comprehensive and detailed picture of local air quality. I will present our current work towards such a combination, with a focus on producing higher spatial resolution estimates and near-term forecasts of Nitrogen Dioxide in urban areas in the United States. Our method combines data from the GEOS Composition Forecasting (GEOS-CF) model system, TROPOMI tropospheric NO2 satellite data products, and ground measurements from the EPA regulatory monitoring network using a combination of simple intuitive relationships and machine learning techniques. I will show the performance of this proposed method in several urban areas in the United States, comparing it with baseline approaches using single data sources separately. Overall, we find that combining these disparate datasets together leads to more accurate air quality forecasts in the target areas than is possible using each data source separately.

Air quality↗