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NASA NTRSDate not supplied

Investigation of the Potential for Lidar & Polarimeter Combined Aerosol Retrievals Using Various Instrument Combinations

As a scientific community, we are motivated to achieve better observational capabilities for aerosols, to reduce uncertainties about aerosol’s role in climate. Encouraged by the National Academies Decadal Survey, many are looking to the synergy of lidar and polarimeter as a means of achieving improved measurements. Polarimetric observations of total-column radiances have excellent sensitivity to aerosol size distribution and absorption properties. Active lidar measurements have fewer wavelengths and view angles and therefore more limited sensitivity to aerosol microphysical properties such as complex refractive index. Yet the advantage of vertically resolved profiles is game-changing, especially given that models contain significant uncertainty about the vertical distribution of aerosol and that polarimeter and other passive retrievals must make assumptions about vertical distribution which can impact performance. To optimize the synergy, a joint polarimeter + lidar mission requires a joint retrieval. However, the exact instruments that will be launched on a future satellite are unknown, and the capabilities of polarimeters and lidars cover a large range. In this study, we perform information content analysis for a range of nominal instrument combinations. The methodology is ideal for assessing the impact of measurements and a priori information (assumptions and constraints) with respect to the desired retrieval products, and for comparing measurement systems. It has advantages that make it useful in advance of or in parallel with retrieval development, such as producing quantitatively useful comparisons even for retrieval scenarios that are significantly underdetermined and therefore impossible to retrieve without significant assumptions, and it is not impacted by retrieval-specific sources of error such as incomplete or incorrect convergence which can complicate the interpretation of a retrieval performance analysis. Here, we will derive the expected uncertainty in retrieved aerosol concentration, effective radius, fine mode fraction and single scattering albedo, for a combination of a polarimeter with various grades of lidar, from an elastic backscatter lidar, similar to the pathfinder CALIOP on the CALIPSO satellite, to a multi-wavelength high spectral resolution lidar.

Sharon P Burton↗

NASA NTRS2019

Validation, Comparison, and Integration of GOCI, AHI, MODIS, MISR, and VIIRS Aerosol Optical Depth Over East Asia During the 2016 KORUS-AQ Campaign

Recently launched multichannel geostationary Earth orbit (GEO) satellite sensors, such as the Geostationary Ocean Color Imager (GOCI) and the Advanced Himawari Imager (AHI), provide aerosol products over East Asia with high accuracy, which enables the monitoring of rapid diurnal variations and the transboundary transport of aerosols. Most aerosol studies to date have used low Earth orbit (LEO) satellite sensors, such as the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging Spectroradiometer (MISR), with a maximum of one or two overpass daylight times per day from midlatitudes to low latitudes. Thus, the demand for new GEO observations with high temporal resolution and improved accuracy has been significant. In this study the latest versions of aerosol optical depth (AOD) products from three LEO sensors – MODIS (Dark Target, Deep Blue, and MAIAC), MISR, and the Visible/Infrared Imager Radiometer Suite (VIIRS), along with two GEO sensors (GOCI and AHI), are validated, compared, and integrated for a period during the Korea–United States Air Quality Study (KORUS-AQ) field campaign from 1 May to 12 June 2016 over East Asia. The AOD products analyzed here generally have high accuracy with high R (0.84–0.93) and low RMSE (0.12–0.17), but their error characteristics differ according to the use of several different surface-reflectance estimation methods. High-accuracy near-real-time GOCI and AHI measurements facilitate the detection of rapid AOD changes, such as smoke aerosol transport from Russia to Japan on 18–21 May 2016, heavy pollution transport from China to the Korean Peninsula on 25 May 2016, and local emission transport from the Seoul Metropolitan Area to the Yellow Sea in South Korea on 5 June 2016. These high-temporal-resolution GEO measurements result in more representative daily AOD values and make a greater contribution to a combined daily AOD product assembled by median value selection with a 0.5∘×0.5∘ grid resolution. The combined AOD is spatially continuous and has a greater number of pixels with high accuracy (fraction within expected error range of 0.61) than individual products. This study characterizes aerosol measurements from LEO and GEO satellites currently in operation over East Asia, and the results presented here can be used to evaluate satellite measurement bias and air quality models.

Myungje Choi↗

NASA NTRS2021

Air Pollution Scenario over Pakistan: Characterization and Ranking of Extremely Polluted Cities using Long-Term Concentrations of Aerosols and Trace Gases

Pakistan ranks third in the world in terms of mortality attributable to air pollution, with aerosol mass concentrations (PM2.5) consistently well above WHO (World Health Organization) air quality guidelines (AQG). However, regulation is dependent on a sparse network of air quality monitoring stations and insufficient ground data. This study utilizes long-term observations of aerosols and trace gases to characterize and rank the air pollution scenarios and pollution characteristics of 80 selected cities in Pakistan. Datasets used include (1) the Aqua and Terra (AquaTerra) MODIS (Moderate Resolution Imaging Spectroradiometer) Level 2 Collection 6.1 merged Dark Target and Deep Blue (DTB) aerosol optical depth (AOD) retrieval products; (2) the CAMS (Copernicus Atmosphere Monitoring Service) reanalysis PM1, PM2.5, and PM10 data; (3) the MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, Version 2) reanalysis PM2.5 data, (4) the OMI (Ozone Monitoring Instrument) tropospheric vertical column density (TVCD) of nitrogen dioxide (NO2), and VCD of sulfur dioxide (SO2) in the Planetary Boundary Layer (PBL), (5) the VIIRS (Visible Infrared Imaging Radiometer Suite) Nighttime Lights data, (6) MODIS Collection 6 Version 2 global monthly fire location data (MCD14ML), (7) population density, (8) MODIS Level 3 Collection 6 land cover types, (9) AERONET (AErosol RObotic NETwork) Version 3 Level 2.0 data, and (10) ground-based PM2.5 concentrations from air quality monitoring stations. Potential Source Contribution Function (PSCF) analyses were performed by integrating with ground-based PM2.5 concentrations and the NOAA (National Oceanic and Atmospheric Administration) HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) air parcel back trajectories to identify potential pollution source areas which are responsible for extreme air pollution in Pakistan. Results show that the ranking of the top polluted cities depends on the type of pollutant considered and the metric used. For example, Jhang, Multan, and Vehari were characterized as the top three polluted cities in Pakistan when considering AquaTerra DTB AOD products; for PM1, PM2.5, and PM10 Lahore, Gujranwala, and Okara were the top three; for tropospheric NO2 VCD Lahore, Rawalpindi, and Islamabad and for PBL SO2 VCD Lahore, Mirpur, and Gujranwala. The results demonstrate that Pakistan’s entire population has been exposed to high PM2.5 concentrations for many years, with a mean annual value of 54.7 μg/cu. m, over all Pakistan from 2003 to 2020. This value exceeds Pakistan’s National Environmental Quality Standards (Pak-NEQS, i.e., <15 μg/cu. m annual mean) for ambient air defined by the Pakistan Environmental Protection Agency (Pak-EPA) as well as the WHO Interim Target-1 (i.e., mean annual PM2.5 <35 μg/cu. m). The spatial analyses of the concentrations of aerosols and trace gases in terms of population density, nighttime lights, land cover types, and fire location data, and the PSCF analysis indicate that Pakistan’s air quality is strongly affected by anthropogenic sources inside of Pakistan, with contributions from surrounding countries. Statistically significant positive (increasing) trends in PM1, PM2.5, PM10, tropospheric NO2 VCD, and SO2 VCD were observed in ~89%, ~67%, ~48%, 91%, and ~88% of the Pakistani cities (80 cities), respectively. This comprehensive analysis of aerosol and trace gas levels, their characteristics in spatio-temporal domains, and their trends over Pakistan, is the first of its kind. Results will be helpful to the Ministry of Climate Change (Government of Pakistan), Pak-EPA, SUPARCO (Pakistan Space and Upper Atmosphere Research Commission), policymakers, and the local research community to mitigate air pollution and its effects on human health.

Muhammad Bilal↗

NASA NTRS2021

Polarimetric sensitivity of light-absorbing carbonaceous aerosols over ocean: A theoretical assessment

Visible-light-absorbing carbonaceous aerosols within the boundary layer affect the radiance and polarization states of the radiation at the top of the atmosphere. Remote sensing from suborbital and satellite-based platforms utilizes these radiance and polarization signals to retrieve the key properties of these aerosols. Recent retrieval algorithms have shown a progressive trend toward including multi-angular and multi-spectral polarimetric measurements to produce better retrieval accuracy in comparison to those using measurements based on a single viewing angle. Here, we perform a theoretical investigation of the top of atmosphere (TOA) radiance-related reflectance factor (bidirectional reflectance factor (BRF)) and the two types of polarimetry-related factors (polarized bidirectional reflectance factor (pBRF) and the degree of linear polarization (DoLP)) for different types of atmospheric light-absorbing carbonaceous aerosols as a function of particle size distribution. We selected three polarimetric bands corresponding to those utilized by NASA's Airborne Multiangle SpectroPolarimetric Imager (AirMSPI)—near-UV (470 nm), visible (660 nm), and near-infrared (865 nm)—for our simulations which were performed over ocean surface using the successive order of scattering (SOS) algorithm coupled to a Lorenz-Mie aerosol optics model. The analysis of particle phase matrix elements indicates a close relationship between the angular dependencies of DoLP and associated phase matrix components at the shortest polarimetric band (470 nm). Using Jacobian analysis, we find that the radiance- and polarimetry-related reflectance factors of weakly light-absorbing aerosols, such as brown carbon, are more sensitive to changes in particle size and imaginary refractive index in comparison with those of black carbon, which is strongly light-absorbing. Our results suggest that the DoLP data could be used by future retrieval algorithms for reliably estimating microphysical properties of absorbing carbonaceous aerosols with imaginary refractive index less than 0.4.

refractive index↗

NASA NTRSDate not supplied

Open Source Application of Fusing Aerosol Products from GEO and LEO Satellites

Retrieving aerosol optical depths (AODs) from sun-synchronous polar orbiting (aka low earth orbit, LEO) satellites, such as MODISs, and VIIRSs, OMI, TROPOMI, etc, has become well-established as a tool for extracting information on particulate matter (PM) and related processes in the atmosphere. However, with recently launched geostationary satellites (GEO), such as GOES-16/17/18, and Himawari-8/9, and Meteosat Third Generation (MTG) they provide a much higher temporal resolution (order of 10 minutes), typically an image once or more per hour during daylight compared to LEO once per day. By combining these observations, we may be able to characterize the diurnal cycle of global AOD at the local, regional and global scale. While the science community is still exploring the new data from GEO observations, we have been thinking about how to properly combine/merge/fuse those data considering differences in their spatial and temporal resolutions. However, this poses a “Big Data” challenge. The big data challenge is not just about data storage, but also about data discoverability, and accessibility, and even more, about data migration/mirroring in the cloud-computing environment. This paper is merely showing some of the efforts and approaches we have attempted in fusing six satellites’ Level 2 aerosol data (three are from GEO (GOES-16/17 and Himawari-8), and the other three are from LEO (TERRA/MODIS, AQUA/MODIS, SNPP-VIIRS) from Dark Target (DT) aerosol retrieval algorithm. Having the on-demand capability of fusing remote sensing products onto the desired temporal and spatial domain enables researchers and application practitioners to better manipulate and work with satellite and sensor data. It is our hopeWe hope that by making such an open-source package, and the accompanying functionality, the scientific community will be granted easier access to aerosol data processing resources. The MEaSUREs Program (Making Earth System Data Records for Use in Research Environments) expands our understanding of the Earth's current system through atmospheric and surface measurements. In an effort to aid the scientific research component and improve open source methods, this project developed Python code for fusing six satellite Level 2 aerosol data (three are from geostationary satellites (GEO), and the other three are from low earth orbital satellites (LEO)) from Dark Target Aerosol Retrieval Algorithm.

Jennifer Wei↗

NASA NTRS2023

Virus Infection of Phytoplankton Increases Average Molar Mass and Reduces Hygroscopicity of Aerosolized Organic Matter

Viral infection of phytoplankton is a pervasive mechanism of cell death and bloom termination, which leads to the production of dissolved and colloidal organic matter that can be aerosolized into the atmosphere. Earth-observing satellites can track the growth and death of phytoplankton blooms on weekly time scales but the impact of viral infection on the cloud forming potential of associated aerosols is largely unknown. Here, we determine the influence of viral-derived organic matter, purified viruses, and marine hydrogels on the cloud condensation nuclei activity of their aerosolized solutions, compared to organic exudates from healthy phytoplankton. Dissolved organic material derived from exponentially growing and infected cells of well-characterized eukaryotic phytoplankton host-virus systems, including viruses from diatoms, coccolithophores and chlorophytes, was concentrated, desalted, and nebulized to form aerosol particles composed of primarily of organic matter. Aerosols from infected phytoplankton cultures resulted in an increase in critical activation diameter and average molar mass in three out of five combinations evaluated, along with a decrease in organic kappa (hygroscopicity) compared to healthy cultures and seawater controls. The infected samples also displayed evidence of increased surface tension depression at realistic cloud water vapor supersaturations. Amending the samples with xanthan gum to simulate marine hydrogels increased variability in organic kappa and surface tension in aerosols with high organic to salt ratios. Our findings suggest that the pulses of increased dissolved organic matter associated with viral infection in surface waters may increase the molar mass of dissolved organic compounds relative to surface waters occupied by healthy phytoplankton or low phytoplankton biomass.

Atmospheric science↗

NASA NTRSDate not supplied

Models, In Situ, and Remote Sensing of Aerosols (MIRA)

There is a natural partitioning of scientific interest amongst three focus areas of aerosol research: modeling, in situ measurements, and remote sensing observations. The community benefits when these groups interact, with overall benefits towards advancing our understanding of climate, weather, and air quality. To this end, MIRA seeks to foster international collaborations across disciplines and regional boundaries and offers a complementary association with established international working groups. Within the present framework, MIRA has identified four initial focus areas, with opportunities to add more by the working group. One effort advances knowledge of the aerosol lidar ratio for different aerosol compositions and locations to improve backscatter lidar retrievals from satellites and ground-based instruments. Another effort seeks to improve aerosol optical parameters used by climate and radiative transfer models. A third effort focuses on harmonizing aerosol assimilation models with satellite measurement retrievals, and a fourth interest seeks to develop retrievals of aerosol Particulate Matter from remote sensing measurements. The presentation will provide an overview of MIRA and ways for the community to engage.

Chip Trepte↗

NASA NTRSDate not supplied

The Plankton, Aerosol, Cloud, Ocean Ecosystem (Pace) Mission Overview: From Concept to Launch

Abstract for Technical Review: The Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) mission is a strategic climate continuity mission that was defined in the 2010 document Responding to the Challenge of Climate and Environmental Change: NASA’s Plan for Climate-Centric Architecture for Earth Observations and Applications from Space (referred to as the “Climate Initiative”). Launched in February 2024, the PACE mission represents NASA’s next investment in ocean biology, clouds, and aerosol data records. PACE will extend the high quality ocean ecological, ocean biogeochemical, cloud, and aerosol particle data records begun by NASA in the 1990s, building on the exceptional heritages of the Sea-Viewing Wide Field-of-View Sensor (SeaWiFS), the Moderate Resolution Imaging Spectroradiometer (MODIS), the Multi-angle Imaging SpectroRadiometer (MISR), and the Visible Infrared Imaging Radiometer Suite (VIIRS). NASA Headquarters directed the mission development and implementation to the NASA Goddard Space Flight Center (GSFC) with guidance to utilize a Design-to-Cost (DTC) process. Mission studies were conducted to define appropriate approaches within and across elements while maximizing science capabilities at a high cost confidence. Mission baseline requirements development is also embedded within the DTC process, as these requirements were not established at the onset of the mission concept development. The PACE project office at NASA’s GSFC was responsible for the satellite development, launch and commissioning. The NASA Headquarters PACE Program Science office is responsible for supporting the science data processing system and assembling competed community science teams, which includes field-based vicarious calibration and data product validation efforts to support the PACE Project Science team. The PACE observatory is comprised of three instruments, the Ocean Color Instrument (OCI) and two polarimeters, the Hyper-Angular Rainbow Polarimeter 2 (HARP2) and the Spectro-Polarimeter for Exploration (SPEXone) and the PACE spacecraft. The observatory has been commissioned and is performing on-orbit science data collection operations. Summary for Program: The Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) mission is a strategic climate continuity mission that was defined in the 2010 document Responding to the Challenge of Climate and Environmental Change: NASA’s Plan for Climate-Centric Architecture for Earth Observations and Applications from Space (referred to as the “Climate Initiative”). Launched in February 2024 under the leadership of the NASA Goddard Space Flight Center (GSFC), the PACE mission represents NASA’s next investment in ocean biology, clouds, and aerosol data records. PACE will extend the high quality ocean ecological, ocean biogeochemical, cloud, and aerosol particle data records begun by NASA in the 1990s. The PACE observatory is comprised of the Ocean Color Instrument (OCI), the Hyper-Angular Rainbow Polarimeter 2 (HARP2) and the Spectro-Polarimeter for Exploration (SPEXone), along with the PACE spacecraft.

Robert H Estep, Jr↗

NASA NTRSDate not supplied

Tracking the Hunga Tonga-Hunga Ha’apai Eruption Stratospheric Aerosol and Trace Gas Plumes Using Machine Learning

The Hunga Tonga-Hunga Ha’apai (HTHH) submarine volcano had an explosive eruption phase on January 15, 2022, that thrusted ash, gases, and water vapor through the troposphere and into the stratosphere. The stratospheric volcanic plume included aerosol precursor gases such as SO2 and H2S as well as anomalously high water vapor concentrations due to the submarine oceanic origin. With these atmospheric constituents, the sulfuric gases and water vapor formed sulfate (SO4) particles via gas-to-particle reactions and these aerosols likely increased in size due to hygroscopic growth within anomalously humid regions. Strong easterlies and gravity waves propagated the volcanic impacts throughout the stratosphere. Orbital and suborbital passive sensor retrievals detected changes in the aerosol and trace gas characteristics within the atmospheric column for cloud-free regions over the southern hemisphere. While the CALIPSO lidar can detect aerosol layers in the stratosphere, passive sensors such as MODIS retrieved the total column aerosol abundance and characteristics. Previous studies used manual tracking methods to determine volcanic plume positions and compared them to ground observations. In this study, we examine the machine learning (ML) approaches including segmentation, object detection, and object tracking to identify and track aerosol and trace gas plumes using orbital and suborbital sensor data. This ML implementation strives to provide a more systematic approach to separate total column effects from those of the stratosphere. Similar ML tracking may be useful for stratospheric impact events observed historically by CALIPSO and in the future with EarthCare and the Atmosphere Observing System (AOS) lidar-capable missions.

Rhys Leahy↗

NASA NTRS2024

Long-Term Trends in Aerosols, Low Clouds, and Large-scale Meteorology over the Western North Atlantic from 2003 to 2020

A continuous decrease of aerosol over the western North Atlantic Ocean (WNAO) on decadal timescales provides a long-term experiment to evaluate how other natural and anthropogenic processes affect the manifestation of aerosol-cloud interactions in this region. Furthermore, the WNAO is a natural laboratory with diverse aerosol sources, marine boundary layer clouds that are more variable than marine stratocumulus deck regions, and unique flow regimes set up by the Gulf Stream and semi-permanent Bermuda High. We investigate how satellite-retrieved macrophysical and microphysical properties of low clouds and the surface shortwave irradiance changed from 2003 to 2020, in tandem with this aerosol decrease. The decadal changes in large-scale meteorology relating to the North Atlantic Oscillation (NAO) are also examined. We find no significant changes in low-cloud fraction but a widespread reduction in low-cloud optical depth attributed to fewer and larger cloud droplets with almost no change in cloud liquid water path. Despite robust signals in low-cloud optical properties together with aerosol decrease, a corresponding increase in the surface shortwave irradiance trends, also called surface brightening, is lacking. This absence of brightening is potentially due to concomitant changes found in large-scale meteorology associated with NAO— a Bermuda High strengthening, sea surface warming, and atmospheric moistening— as well as an increase in high cloud fraction that can counteract the surface brightening. Ultimately, our findings suggest that spatial patterns in the decadal meteorological variability, likely set up by NAO, contribute more to the surface cloud radiative effect over the WNAO than aerosol-cloud interactions.

J Minnie Park↗

NASA NTRS2023

Satellite characterization of global stratospheric sulfate aerosols released by Tonga volcano

Large volcanic eruptions create an enhanced layer of sulfate aerosols in the stratosphere. These sulfuric acid droplets persist for many months, altering the climate and stratospheric chemistry. Sulfate aerosols scatter sunlight back to space, cooling the surface of the Earth and absorb outgoing thermal radiation, heating the stratosphere. The calculation of the climate impact of sulfate aerosols depends on their physical properties such as droplet size and chemical composition. These properties are not well known, and this uncertainty contributes to the errors in climate model predictions. Here we derive the first empirical formula that predicts the composition of stratospheric sulfate aerosols from volcanic eruptions from the air temperature and water vapor pressure. Measurements of atmospheric infrared transmittance of the Hunga Tonga-Hunga Ha'apai sulfate aerosol plume by the Atmospheric Chemistry Experiment (ACE) satellite were analyzed to determine composition (weight percent of sulfuric acid) and median particle radius. These data are supplemented by measurements of the Raikoke and Nabro eruptions. Our analysis allows the properties of volcanic aerosols in the stratosphere to be predicted reliably in atmospheric models.

P Bernath↗

DOE OSTI2025

Analysis of contrasting aerosol indirect effects in liquid water clouds over the northern part of Arabian Sea

The extensive daily statistics of aerosol properties, cloud properties, and their mutual correlations provide crucial information for better assessing future climate change. Here, in this paper, 14 years (2010–2023) of data from the Moderate Resolution Imaging Spectroradiometer (MODIS) are analyzed over the northern part of Arabian Sea (Latitude: 21°–25° N and Longitude: 62°–68° E) to assess the characteristics of aerosols and clouds and their relationships under different meteorological conditions. When aerosol optical depth (AOD) is less than ~0.7, the observations exhibit a positive correlation between AOD and cloud droplet effective radius (CDR) but negative correlations between AOD and cloud droplet number concentration (CDNC), between AOD and cloud optical depth (COD), between AOD and cloud liquid water path (CLWP), and between AOD and cloud geometrical thickness (H). The corresponding aerosol-cloud correlations change signs when the AOD values are larger than 0.7. However, the single folded positive AOD-cloud fraction (CF) relationship is observed in both AOD regimes. Similar correlations are also observed between precipitable water vapor (PWV) and CDR, CDNC, COD, H, CF and CLWP, together with a positive correlation between PWV and AOD. Further isolation of the environmental effects from aerosol effects by stratifying AOD and cloud data into different LTS and PWV bins shows that the signature of the well-known Twomey effect is observed under high LTS-high PWV conditions, while an opposite effect (anti-Twomey) is observed under low PWV conditions, regardless of LTS values. Additionally, negative correlations between AOD and COD, AOD and CLWP, and AOD and H are observed under low LTS, regardless of PWV conditions, with a slight positive correlation when AOD >0.4 under high LTS and PWV conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Fast response of global monsoon area and precipitation to regional carbonaceous aerosols

Monsoon exerts a significant social and economic impact on billions of people around the world. Changes in global monsoon (GM) rainfall under global warming have been well studied; however, the understanding of GM connection with regional aerosol emissions is limited. Using an atmospheric general circulation model (AGCM), we attempt to quantify the response of global monsoon area and precipitation to the removal of carbonaceous aerosols over North America (AM), North Africa (AF), Europe (EU), and Asia (AS). Response to the emission removal, the global average aerosol optical depths (AOD) are reduced by 2.21%, 1.8%, 1.16%, and 3.8% respectively. Additionally, a southward shift in the GM domain is observed, responding to changes in magnitude and position of the Inter-Tropical Convergence Zone, when carbonaceous aerosols are removed over these regions in the Northern Hemisphere. The percentage departure in the area-averaged GM precipitation is found to be 4-fold in magnitude for the removal of emissions over EU when compared to that of AM and AF. A shrinkage in the GM area is also observed, which is maximum for EU (~-30%) compared to AM and AF (~-25%). The change in GM precipitation and area are found to be the least and opposite in nature for AS emissions. This study provides insight into the regional nature of carbonaceous aerosol effects on global precipitation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Formation of Inorganic Sulfate and Volatile Nonsulfated Products from Heterogeneous Hydroxyl Radical Oxidation of 2-Methyltetrol Sulfate Aerosols: Mechanisms and Atmospheric Implications

Chemical transformation of 2-methyltetrol sulfates (2-MTS), key isoprene-derived secondary organic aerosol (SOA) constituents, through heterogeneous hydroxyl radical ( • OH) oxidation can result in the formation of previously unidentified atmospheric organosulfates (OSs). However, detected OSs cannot fully account for the sulfur content released from reacted 2-MTS, indicating the existence of sulfur in forms other than OSs, such as inorganic sulfates. This work investigated the formation of inorganic sulfates through heterogeneous • OH oxidation of 2-MTS aerosols. Remarkably, high yields of inorganic sulfates, defined as the moles of inorganic sulfates produced per mole of reacted 2-MTS, were observed in the range from 0.48 ± 0.07 to 0.68 ± 0.07. These could be explained by the production of sulfate (SO 4 •- ) and sulfite (SO 3 •- ) radicals through the cleavage of C-O(S) and (C)O-S bonds, followed by aerosol-phase reactions. Additionally, non-sulfated products resulting from bond cleavage were likely volatile and evaporated into gas phase, as evidenced by observed aerosol mass loss (up to 25%) and concurrent size reduction upon oxidation. This investigation highlights the significant transformation of sulfur from its organic to inorganic forms during the heterogeneous oxidation of 2-MTS aerosols, potentially influencing the physicochemical properties and environmental impacts of isoprene-derived SOA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Aircraft Measurements from a U.S. Western Wildfire Demonstrating Day and Night Differences in the Chemical Composition and Optical Properties of Biomass Burning Aerosols and Their Atmospheric Evolution

The composition and transformations of biomass burning aerosols (BBA) have been measured onboard the NOAA Twin Otter research aircraft during the Fire Influence on Regional to Global Environments and Air Quality field study. Here, we analyze real-time aerosol mass spectrometry measurements across three flights during the afternoon, late afternoon, and night of August 28, 2019, for one midsized wildfire. Analysis of several metrics showed that the aerosol composition and optical properties varied depending on the burning conditions at the fire zone and the time of day the BBA was emitted, with substantial variations in the available sunlight. The total aerosol mass loadings were dominated by organic components with a much smaller contribution from inorganic species. A gradual buildup of organic material was observed during the afternoon as the plume aged, indicating the condensation of photochemically formed low-volatility oxidized organic compounds. Highly hygroscopic ammonium nitrate was the main inorganic component, suggesting potential water content in BBA particles and the likelihood of their aqueous-phase reactivity. Depletions of particle-phase NO 3 – and Cl – relative to carbon monoxide were observed in the late afternoon and nighttime plumes, respectively, aligning with known gas-particle partitioning thermodynamics and the heterogeneous chemistry of dissolved nitrate and chloride. The wavelength-dependent light absorption by aerosol species was higher for the plume sampled at night and showed no significant changes with plume age, despite observed trends in composition and mass downwind. These differences in particle composition and optical properties demonstrate that the processes involved in BBA aging are not uniform for the same wildfire over the course of the day and depend highly on when the BBA was emitted, as well as the burning phase at the emissions source.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

TAMU TRACER: Targeted Mobile Measurements to Isolate the Impacts of Aerosols and Meteorology on Deep Convection

Difficulty in using observations to isolate the impacts of aerosols from meteorology on deep convection often stems from inability to resolve the spatiotemporal variations in the environment serving as the storm’s inflow region. During the DOE TRacking Aerosol Convection interactions ExpeRiment (TRACER) in June-September 2022, a Texas A&M University (TAMU) team conducted a mobile field campaign to characterize the meteorological and aerosol variability in airmasses that serve as inflow to convection across the ubiquitous mesoscale boundaries associated with the sea- and bay-breezes in the Houston, Texas, region. These boundaries propagate inland over the fixed DOE Atmospheric Radiation Measurement (ARM) sites. However, convection occurs on either or both the continental or maritime sides or along the boundary. The maritime and continental airmasses serving as convection inflow may be quite distinct, with different meteorological and aerosol characteristics that fixed-site measurements cannot simultaneously sample. Thus, a primary objective of TAMU TRACER was to provide mobile measurements similar to those at the fixed sites, but in the opposite airmass across these moving mesoscale boundaries. TAMU TRACER collected radiosonde, lidar, aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) measurements on 29 enhanced operations days covering a variety of maritime, continental, outflow, and pre-frontal airmasses. This paper summarizes the TAMU TRACER deployment and measurement strategy, instruments, available datasets, and provides sample cases highlighting differences between these mobile measurements and those made at the ARM sites. We also highlight the exceptional TAMU TRACER undergraduate student participation in high impact learning activities through forecasting and field deployment opportunities.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Moving beyond the Aerosol Climatology of WRF-Solar: A Case Study over the North China Plain

Numerical weather prediction (NWP), when accessible, is a crucial input to short-term solar power forecasting. WRF-Solar, the first NWP model specifically designed for solar energy applications, has shown promising predictive capability. Nevertheless, few attempts have been made to investigate its performance under high aerosol loading, which attenuates incoming radiation significantly. The North China Plain is a polluted region due to industrialization, which constitutes a proper testbed for such investigation. Here, in this paper, aerosol direct radiative effect (DRE) on three surface shortwave radiation components (i.e., global, beam, and diffuse) during five heavy pollution episodes is studied within the WRF-Solar framework. Results show that WRF-Solar overestimates instantaneous beam radiation up to 795.3 W m -2 when the aerosol DRE is not considered. Although such overestimation can be partially offset by an underestimation of the diffuse radiation of about 194.5 W m -2 , the overestimation of the global radiation still reaches 160.2 W m -2 . This undesirable bias can be reduced when WRF-Solar is powered by Copernicus Atmosphere Monitoring Service (CAMS) aerosol forecasts, which then translates to accuracy improvements in photovoltaic (PV) power forecasts. This work also compares the forecast performance of the CAMS-powered WRF-Solar with that of the European Centre for Medium-Range Weather Forecasts model. Under high aerosol loading conditions, the irradiance forecast accuracy generated by WRF-Solar increased by 53.2% and the PV power forecast accuracy increased by 6.8%.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Aerosol Inlets for a Mid-Sized Uncrewed Aerial System (UAS)

The purpose of this technical report is to document the efforts to design and test two inlet systems for aerosol sampling suitable for deployment on a medium-sized fixed-wing Uncrewed Aerial System (UAS). This work, which was supported by the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) user facility, was conducted at the Pacific Northwest National Laboratory (PNNL) for the ARM Aircraft Facility (AAF) starting in November 2017. The current work is a part of AAF efforts to instrument the ArcticShark (a mid-sized UAS owned and operated by the AAF) for atmospheric research and develop a scientific payload for deployment on a similar-sized UAS with minimal adaptation and integration. An aerosol inlet system is necessary to sample and transport ambient air sample to the scientific instrumentation with minimal distortions to the aerosols. Two isokinetic aerosol inlets were designed: the first is a simple passive system for a single instrument suitable to be installed in a wing pylon; the second is a system with active control designed to sample and distribute air among several heterogeneous instruments and to provide basic humidity control of the air sample so that the measured aerosol parameters should correspond to “dry” conditions (a common requirement). Both systems could be easily adapted for deployment on another platform and/or with a different set of instrumentation. Several conducted flight tests showed that the inlets’ performance met our design goals.

42 ENGINEERING↗