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At least 91 records · Page 5

Signatures of aerosol-cloud interactions in GiOcean: a coupled global reanalysis with two-moment cloud microphysics

Aerosols influence the Earth's radiative balance through direct interactions with radiation and by affecting cloud properties. Anthropogenic aerosols have led to cooling during the industrial era through aerosol–cloud interactions (ACI), including aerosol effects on cloud microphysical properties and the subsequent adjustments. However, large uncertainties remain in Earth system models (ESMs) regarding the magnitude of this cooling. In part, ESMs substantially disagree on cloud properties, thermodynamics, the hydrological cycle, and general circulation. Reanalysis provides a useful avenue for exploring the impact of ACI on clouds and radiation because its atmosphere is forced to match realistic conditions through the assimilation of observations. Here, we explore the impact of ACI on clouds in the GiOcean reanalysis – the first to incorporate aerosol-cloud interactions. We contrast variables important for ACI between GiOcean and satellite observations and develop 2-dimensional lookup tables of ACI for both using a source-sink budget perspective to attribute the changes in cloud droplet number (Nd) and liquid water path (LWP) to aerosol and meteorology. A compositing analysis using lookup tables shows that GiOcean captures key aspects of aerosol–cloud–precipitation interactions, including (1) activation of aerosol into cloud droplets, (2) effective precipitation scavenging of Nd, (3) suppression of precipitation by high Nd in regions with heavy aerosol emissions. In contrast, satellite observations do not exhibit clear patterns for processes (2) and (3). Random Forest analysis shows that interannual variability in Nd and LWP over the Northern Hemisphere ocean in GiOcean is primarily driven by precipitation, consistent with satellite observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Distribution and Sources of Tropospheric Aerosols Over the Western North Atlantic During ACTIVATE (February-March 2020)

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) is a five-year (2019-2023) NASA Earth-Venture Suborbital-3 (EVS-3) mission to robustly characterize aerosol-cloud-meteorology interactions during February-June, with a focus on marine boundary layer clouds. This characterization requires understanding of aerosol composition, distribution, transport pathways, and sources. Here we use the GEOS-Chem chemical transport model driven by the MERRA-2 reanalysis to simulate tropospheric carbon monoxide (CO) and aerosols over the western North Atlantic Ocean (WNAO) during the first field deployment of ACTIVATE (February-March 2020). CO is used as a tracer to diagnose transport pathways for continental pollution outflow to the WNAO. The aerosol simulation represents all major aerosols including sulfate-nitrate-ammonium (SNA), mineral dust, sea salt, black and organic carbon aerosols. Model-simulated mixing ratios of SNA and organic carbon are compared with aircraft observations. We show that intensive aerosol mass measurements in the lower troposphere over the North American outflow region during ACTIVATE provide strong constraints on model aerosol wet scavenging. Comparisons of model aerosol extinctions with the airborne High Spectral Resolution Lidar-2 (HSRL-2) measurements indicate that the model generally captures continental outflow of aerosols and enhanced extinctions associated with sea salt. Simulated aerosol optical depths (AODs) and extinction vertical profiles are also compared with satellite retrievals from MODIS/Aqua and CALIOP/CALIPSO, respectively. CALIOP sometimes observes enhanced aerosol extinction at altitudes between ~1.5km and ~2.0km south of 32°N. The model reproduces this enhancement and attributes it to coarse-mode sea salt associated with high relative humidity. The relative contributions of continental and oceanic sources to the aerosol loading, AOD, and their distributions over the study domain will also be discussed.

aerosols↗

Final report: Insights from ARM observations into aerosol processing and transport by extratropical cyclones and aerosol effects on cyclone clouds

This project advanced understanding of aerosol–cloud interactions in extratropical cyclones using observations from the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory and ACE-ENA field campaigns, along with satellite datasets and numerical modeling. We have quantified the susceptibility of frontal clouds to aerosols, showing that this susceptibility is similar to that in non-frontal clouds despite substantial (factor 2) differences in droplet concentrations between these cloud types, and also significant differences in cloud albedo. A key finding was that Aitken-mode (here, 60-100nm diameter) aerosols play a disproportionately important role in droplet activation in frontal clouds, and concentrations of these particles are frequently strongly biased in climate models. Activation of aerosols depends strongly on updraft speeds, and via collaboration with Argonne National Laboratory we contributed to quantifying these better with the ARM radar wind profiler at the ENA site. Our studies in the North Atlantic have analogs in the Southern Ocean, and to draw these out we examined data from the MARCUS and SOCRATES field campaigns. We identified new particle formation within extratropical cyclones as a potentially important source of cloud condensation nuclei in these pristine marine environments. By combining ARM observations with perturbed parameter ensemble simulations, we demonstrated that surface observations can effectively constrain aerosol–cloud adjustments and reduce uncertainty in simulated cloud liquid water path responses by approximately 15%, yielding stronger constraints on historical aerosol cooling effects. The work further established precipitation processes as a dominant control on aerosol–cloud interactions and Earth system predictability.

Gordon, Hamish [Department of Chemical Engineering↗

Heterogeneous Chemistry of HONO on Liquid Sulfuric Acid: A New Mechanism of Chlorine Activation on Stratospheric Sulfate Aerosols

Heterogeneous chemistry of nitrous acid (HONO) on liquid sulfuric acid (H2SO4) Was investigated at conditions that prevail in the stratosphere. The measured uptake coefficient (gamma) of HONO on H2SO4 increased with increasing acid content, ranging from 0.03 for 65 wt % to about 0.1 for 74 wt %. In the aqueous phase, HONO underwent irreversible reaction with H2SO4 to form nitrosylsulfuric acid (NO(+)HSO4(-). At temperatures below 230 K, NO(+)HSO4(-) was observed to be stable and accumulated in concentrated solutions (less than 70 wt % H2SO4) but was unstable and quickly regenerated HONO in dilute solutions (less than 70 wt %). HCl reacted with HONO dissolved in sulfuric acid, releasing gaseous nitrosyl chloride (ClNO). The reaction probability between HCl and HONO varied from 0.01 to 0.02 for 60-72 wt % H2SO4. In the stratosphere, ClNO photodissociates rapidly to yield atomic chlorine, which catalytically destroys ozone. Analysis of the laboratory data reveals that the reaction of HCl with HONO on sulfate aerosols can affect stratospheric ozone balance during elevated sulfuric acid loadings after volcanic eruptions or due to emissions from the projected high-speed civil transport (HSCT). The present results may have important implications on the assessment of environmental acceptability of HSCT.

Zhang, Renyi↗

Lessons from Earth Bioaerosol Sampling for Venus Habitability & Biosignature Science

Venus’s clouds are often discussed as a potential habitat. Several high-priority science goals – cloud aerosol composition, internal radiative flux, and aerosol residence time and circulation models – will improve our understanding of Venus in an astrobiology context. Lessons from Earth’s aerobiosphere can inform these requirements and interpretation of results. A stable Venus aerobiosphere would need microorganisms to reproduce faster than they settle out due to gravity. This is a joint constraint of the potential nutrients and energy influx, bioenergetic costs such as desiccation and radiation damage, and aerosol dynamics. Though life cycles involving S- and Fe-based redox metabolism have been proposed, at an optimistic estimate of 75% H2SO4, Venus aerosol water activity (aw) is still ~0.02, far below the observed microbial growth limit of ~0.6. Long-term desiccation with brief spurts of repair, growth and reproduction in response to transient water influx (perhaps volcanism) is the most likely model for Earth-like life on Venus – a ‘desert bloom’ scenario. In Earth’s troposphere, clouds can carry 103 – 105 cells/mL, some metabolically active. A better analogue may be Earth’s stratospheric sulfate aerosol layer: supercooled sulfuric acid aerosols (acid weight fraction 0.6 – 0.85, 0.1 – 1 µm diameter, 0.1 – 1 cm-3) with little water activity, long residence times, high UV radiation, and only sporadic influx from surface particle sources. Viable cells isolated from this region are rare (~102 cells/m3), though ‘hot spots’ at tropospheric mixing occur. Cells are primarily in inactive forms such as spores, and it is unclear if any are associated with sulfate aerosols or simply co-located. Given the heterogeneities in Venus clouds and the model of a sparse, largely dormant ecosystem, a single transect on descent would most likely pass through a low-water, inactive region, missing potential signs of habitability or biosignatures. Even a passive aerial platform (balloon) may end up following a single air mass over its lifetime. A better strategy for Venus would target an aerial region with some upwelling from surface sources, and take multiple transects separated in time and space. Earth’s stratospheric bioaerosol population could provide a starting point for estimating the required lower volume and detection limits.

Earth↗

Impact of Urban Pollution on Organic-Mediated New-Particle Formation and Particle Number Concentration in the Amazon Rainforest

A major challenge in assessing the impact of aerosols on climate change is to understand how human activities change aerosol loading and properties relative to the pristine-preindustrial baseline. Here we combine chemical transport simulation and field measurements to investigate the effect of anthropogenic pollution from an isolated metropolis on particle number concentration over the preindustrial-like Amazon rainforest through various new-particle formation (NPF) mechanisms and primary particle emissions. To represent organic-mediated NPF, we employ a state-of-the-art model that systematically simulates the formation chemistry and thermodynamics of extremely low volatility organic compounds as well as their roles in NPF processes, and further update the model to improve organic NPF simulations under human-influenced conditions. Results show that urban pollution from the metropolis increases particle number concentration by a factor of 5–25 over the downwind region (within 200 km from city center) compared to background conditions. Overall, our model indicates that NPF contributes over 70% of the total particle number in the downwind region except immediately adjacent to the sources. Among different NPF mechanisms, the ternary NPF involving organics and sulfuric acid overwhelmingly dominates. The improved understanding of particle formation mechanisms will help better quantify anthropogenic aerosol forcing from pristine-preindustrial times to present day.

54 ENVIRONMENTAL SCIENCES↗

Transport and Chemical Evolution over the Pacific (TRACE-P)Aircraft Mission: Design, Execution, and First Results

The NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission was conducted in February-April 2001 over the NW Pacific (1) to characterize the Asian chemical outflow and relate it quantitatively to its sources and (2) to determine its chemical evolution. It used two aircraft, a DC-8 and a P-3B, operating out of Hong Kong and Yokota Air Force Base (near Tokyo), with secondary sites in Hawaii, Wake Island, Guam, Okinawa, and Midway. The aircraft carried instrumentation for measurements of long-lived greenhouse gases, ozone and its precursors, aerosols and their precursors, related species, and chemical tracers. Five chemical transport models (CTMs) were used for chemical forecasting. Customized bottom-up emission inventories for East Asia were generated prior to the mission to support chemical forecasting and to serve as a priori for evaluation with the aircraft data. Validation flights were conducted for the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument and revealed little bias (6 plus or minus 2%) in the MOPITT measurements of CO columns. A major event of transpacific Asian pollution was characterized through combined analysis of TRACE-P and MOPITT data. The TRACE-P observations showed that cold fronts sweeping across East Asia and the associated warm conveyor belts (WCBs) are the dominant pathway for Asian outflow to the Pacific in spring. The WCBs lift both anthropogenic and biomass burning (SE Asia) effluents to the free troposphere, resulting in complex chemical signatures. The TRACE-P data are in general consistent with a priori emission inventories, lending confidence in our ability to quantify Asian emissions from socioeconomic data and emission factors. However, the residential combustion source in rural China was found to be much larger than the a priori, and there were also unexplained chemical enhancements (HCN, CH3Cl, OCS, alkylnitrates) in Chinese urban plumes. The Asian source of CCl4 was found to be much higher than government estimates. Measurements of HCN and CH3CN indicated a dominant biomass burning source and ocean sink for both gases. Large fractions of sulfate and nitrate were found to be present in dust aerosols. Photochemical activity in the Asian outflow was strongly reduced by aerosol attenuation of UV radiation, with major implications for the concentrations of HOx, radicals. New particle formation, apparently from ternary nucleation involving NH3, was observed in Chinese urban plumes.

Jacob, Daniel J.↗

Improved Cloud Condensation Nucleus Spectrometer

An improved thermal-gradient cloud condensation nucleus spectrometer (CCNS) has been designed to provide several enhancements over prior thermal- gradient counters, including fast response and high-sensitivity detection covering a wide range of supersaturations. CCNSs are used in laboratory research on the relationships among aerosols, supersaturation of air, and the formation of clouds. The operational characteristics of prior counters are such that it takes long times to determine aerosol critical supersaturations. Hence, there is a need for a CCNS capable of rapid scanning through a wide range of supersaturations. The present improved CCNS satisfies this need. The improved thermal-gradient CCNS (see Figure 1) incorporates the following notable features: a) The main chamber is bounded on the top and bottom by parallel thick copper plates, which are joined by a thermally conductive vertical wall on one side and a thermally nonconductive wall on the opposite side. b) To establish a temperature gradient needed to establish a supersaturation gradient, water at two different regulated temperatures is pumped through tubes along the edges of the copper plates at the thermally-nonconductive-wall side. Figure 2 presents an example of temperature and supersaturation gradients for one combination of regulated temperatures at the thermally-nonconductive-wall edges of the copper plates. c) To enable measurement of the temperature gradient, ten thermocouples are cemented to the external surfaces of the copper plates (five on the top plate and five on the bottom plate), spaced at equal intervals along the width axis of the main chamber near the outlet end. d) Pieces of filter paper or cotton felt are cemented onto the interior surfaces of the copper plates and, prior to each experimental run, are saturated with water to establish a supersaturation field inside the main chamber. e) A flow of monodisperse aerosol and a dilution flow of humid air are introduced into the main chamber at the inlet end. The inlet assembly is designed to offer improved (relative to prior such assemblies) laminar-flow performance within the main chamber. Dry aerosols are subjected to activation and growth in the supersaturation field. f) After aerosol activation, at the outlet end of the main chamber, a polished stainless-steel probe is used to sample droplets into a laser particle counter. The probe features an improved design for efficient sampling. The counter has six channels with size bins in the range of 0.5- to 5.0-micron diameter. g) To enable efficient sampling, the probe is scanned along the width axis of the main chamber (thereby effecting scanning along the temperature gradient and thereby, further, effecting scanning along the supersaturation gradient) by means of a computer-controlled translation stage.

Leu, Ming-Taun↗

A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

Bauer, S. E.↗

Surfactants and cloud droplet activation: A systematic extension of Köhler theory based on analysis of droplet stability

The activation of aerosol particles to form cloud droplets, a necessary first step in cloud formation, controls much of the impact that aerosols have on clouds and climate. Recently, there has been a surge of interest in extending the Köhler theory of cloud droplet activation to include surface active (typically organic) as well as water-soluble (typically inorganic) aerosol components, but a systematic framework for doing this has yet to be developed. Here, we apply a droplet stability analysis to this end. Ideal and Szyszkowski–Langmuir surfactant models are analyzed to demonstrate the new approach, but the underlying theoretical framework is fundamental and model free. A key finding is that superficial densities at the cloud activation threshold (Köhler maximum) are significantly sub-monolayer, with fractional coverage ranging from 69% to 85% for the organic compounds and mixtures studied. The result, significant for model inventories of cloud condensation nuclei, is a weakening of the surfactant effect relative to expectations based on bulk sample measurements. Analytical results are obtained for the loci of Köhler maxima and applied to aerosol mixtures containing an arbitrary number of water-soluble and surfactant components.

54 ENVIRONMENTAL SCIENCES↗

Three Years of Airborne Observations During NASA Activate: A Statistical Summary of Chemical, Optical, and Microphysical Aerosol Properties Over the Western North Atlantic Ocean

Airborne observations are critical to understanding Earth’s climate system and surface-level air quality by providing both spatial and vertical information that is not possible through ground measurement networks or satellite observations. Airborne platforms allow assessments of long-range transport, vertical redistribution, boundary-layer dynamics, and cloud-aerosol-interactions that are critical to model evaluation and satellite validation. Still, the high cost and effort of aircraft operations can limit measurement campaigns to short, focused time periods. Multiple deployments are often necessary for seasonal comparisons, and results can be limited if target phenomenon are infrequent. Subsequent analyses typically focus on case studies, especially if deployment conditions are climatologically anomalous. The NASA ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment) mission was designed to overcome these limitations by operating semi-continuously over multiple months during multiple seasons. Flight plans were intentionally simple, repetitive, and systematic to provide a statistically robust dataset that could be utilized similarly to a ground-network. Here, we present an overview of three years (2020-2022) of aerosol measurements from the NASA HU-25 Falcon aircraft supporting the ACTIVATE mission. Data from 179 flights were considered, the majority of which were based at NASA Langley Research Center and flown locally over the Wester North Atlantic Ocean just east of Hampton, VA, USA. Airmass characteristics tended to transition from continental outflow near the coast to mostly marine over the open ocean. Seasonal, diurnal, spatial, and vertical trends in aerosol microphysical, optical, and chemical properties are discussed in the context of synoptic scale meteorology. Statistical benefits of the ACTIVATE sampling strategy are discussed with regard to future model evaluation.

Luke D Ziemba↗

Lessons from Earth Aerobiology for Venus Astrobiology

Venus’s clouds have often suggested as a possible habitat. The constraints governing putative airborne life in such a habitat in turn inform priorities and strategies for remote and in situ exploration, methods by which resulting biosignatures might be detected, exoplanet habitability assessment, and planetary protection concerns. Lessons drawn from studying Earth’s aerobiosphere can help improve this understanding. There are altitude ranges within Venus’s clouds in which temperature, pressure, particle size, and radiation appear to be within the limits of microbial life on Earth, and life cycles involving S- and Fe-based redox metabolism have been proposed. However, given the lack of a habitable surface reservoir, a long-term stable Venus aerobiosphere would require that the reproduction rate of the airborne microbes be faster than the settling rate of airborne microbes due to gravity, or eventually the population would be depleted; put another way, the mean generation time would need to exceed the mean residence time. This creates a joint constraint of aerosol dynamics, potential nutrient availability and energy influx, and bioenergetic costs such as desiccation and radiation damage. Even at an optimistic estimate of 75% H2SO4, Venus aerosol water activity (aw) is still ~0.02, far below the observed microbial growth limit of ~0.6. Long-term desiccation with brief spurts of repair and growth in response to transient water influx, such as from volcanism, is the most likely model for Earth-like life on Venus – a ‘desert bloom’ scenario. Several high-priority science goals – cloud aerosol composition, internal radiative flux, and aerosol residence time and circulation models – thus will also improve our understanding of Venus in an astrobiology context. In Earth’s troposphere, warm water clouds can carry 103 – 105 cells/mL, some metabolically active. However, Earth’s stratospheric sulfate aerosol layer may be a better analogue: supercooled sulfuric acidaerosols (acid weight fraction 0.6 – 0.85, 0.1 – 1 μm diameter, 0.1 – 1 cm-3) with little water activity, long residence times, high UV radiation, and only sporadic influx from surface particle sources. Though ‘hot spots’ can occur associated with tropospheric mixing, viable cells in stratospheric samples are rare (~102 cells/m3), and primarily inactive forms such as spores. It is not yet clear whether such bioaerosols are associated with sulfate aerosols or simply co-located, and reproduction in situ has not yet been observed. In this model of a sparse, largely dormant Venus ecosystem, a single transect on descent is likely to pass through a low-water, inactive region, missing potential signs of habitability or biosignatures. A targeted strategy would sample through an aerial region with some upwelling from surface sources, andtake multiple transects separated in time and space. This is compatible with other in situ science goals seeking to understand the dynamics and heterogeneities of Venus’s clouds.

Lower atmosphere↗

Quantifying long-term seasonal and regional impacts of North American fire activity on continental boundary layer aerosols and cloud condensation nuclei

An intimate knowledge of aerosol transport is essential in reducing the uncertainty of the impacts of aerosols on cloud development. Datasets from the U. S. Department of Energy (DOE) Atmospheric Radiation Measurement platform in the Southern Great Plains region (ARM-SGP) and the NASA Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) showed seasonal increases in aerosol loading and total carbon concentration during the spring and summer months (2008-2016) which was attributed to fire activity and smoke transport within North America. The monthly mean MERRA-2 surface carbonaceous aerosol mass concentration and ARM-SGP total carbon products were strongly correlated (R=0.82, p<0.01) along with a moderate correlation with the ARM-SGP cloud condensation nuclei (N CCN ) product (0.5, p~0.1). The monthly mean ARM-SGP total carbon and N CCN products were strongly correlated (0.7, p~0.01). An additional product denoting fire number and coverage taken from the National Interagency Fire Center (NIFC) showed a moderate correlation with the MERRA-2 carbonaceous product (0.45, p<0.01) during the 1981-2016 warm season months (March-September). With respect to meteorological conditions, the correlation between the NIFC fire product and MERRA-2 850 hPa isobaric height anomalies was lower (0.26, p~0.13) due to the variability in the frequency, intensity, and number of fires in North America. An observed increase in the isobaric height anomaly during the past decade may lead to frequent synoptic ridging and drier conditions with more fires, thereby potentially impacting cloud/precipitation processes and decreasing air quality.

54 ENVIRONMENTAL SCIENCES↗

Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming

The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.

Hofmann, David J.↗

Local Tractor Activity at S2 (Mt. Airy) Site

This dataset documents local tractor activity at the S2 (Mt. Airy) site during CoURAGE. It identifies periods where local tractor activity impacted aerosol measurements using both PM10/PM2.5 ratios and ARM camera data for visual confirmation of tractor. Data flags are as follows: 1 = confirmed no local tractor influence on aerosol measurements 2 = one data indicator is present (extreme PM10/PM2.5 ratio OR visual confirmation of tractor sighting), but not both 3 = both data indicators confirm local tractor influence on aerosol 0 = missing data, no determination possible

Tractor Activity using ARM camera photos and PM10/↗

Calibration correction of an active scattering spectrometer probe to account for refractive index of stratospheric aerosols

The use of the active scattering spectrometer probe (ASAS-X) to measure sulfuric acid aerosols on U-2 and ER-2 research aircraft has yielded results that are at times ambiguous due to the dependence of particles' optical signatures on refractive index as well as physical dimensions. The calibration correction of the ASAS-X optical spectrometer probe for stratospheric aerosol studies is validated through an independent and simultaneous sampling of the particles with impactors; sizing and counting of particles on SEM images yields total particle areas and volumes. Upon correction of calibration in light of these data, spectrometer results averaged over four size distributions are found to agree with similarly averaged impactor results to within a few percent: indicating that the optical properties or chemical composition of the sample aerosol must be known in order to achieve accurate optical aerosol spectrometer size analysis.

Pueschel, R. F.↗

Satellite-Assisted Particulate Matter (SAPM) for the Models, In situ, and Remote Sensing of Aerosols (MIRA) Working Group

Models, In situ, and Remote sensing of Aerosols (MIRA) is an international working group that provides a forum for collaborations amongst these three atmospheric aerosol communities. MIRA consists of a collection of interdisciplinary and independently funded Topic/Project groups with clear goals and generally characterized by requests for additional scientific data. The Satellite-Assisted Particulate Matter (SAPM) Topic group focuses on the study of fine particulate matter (PM2.5), as it is a major contributor to air pollution and negatively impacts human health. Our group aims to provide intercomparisons of various methods and techniques for estimating surface PM2.5 assisted by satellite remote sensors (passive and active), global aerosol models, and in situ aerosol measurements. The overall motivation of our work is to enhance PM2.5 coverage beyond in situ ground stations, which can be limited. In this presentation, we provide an overview of various PM2.5 estimation approaches by current SAPM team members, as each approach has its own strengths and limitations. One approach uses near-surface aerosol extinction retrievals from the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and an assumed value of mass extinction efficiency to derive PM2.5 concentrations (Toth et al 2019). A study using this method found a promising agreement (R=0.60; slope=0.89) with U.S. Environmental Protection Agency (EPA) in situ PM2.5 measurements over the contiguous United States (CONUS) for a 12-year (2007-2018) period (Toth et al 2022). In a different approach combining spaceborne lidar and a model, the Cloud Aerosol Transport System (CATS) lidar and Goddard Earth Observing System (GEOS) model are blended in an ensemble variational assimilation scheme to retrieve aerosol extinction and convert speciated mass concentrations to total PM2.5. A recent study (Matus et al in prep.) found agreement within 2 μg/m3 over the CONUS on the 2016 annual mean when compared to EPA ground-based measurements. Another study explored trends in city aerosol optical depth (AOD) from a spaceborne passive remote sensor, Moderate Resolution Imaging Spectroradiometer (MODIS), and found that these trends agree well with trends in city surface PM2.5, which provides confidence in the use of city AOD for city PM2.5 trend studies (Vohra et al 2021). In a follow-on study, steep and significant trends (~2.5 to 7.8% a-1) in AOD are found for several South Asian cities (e.g., Bangalore and Hyderabad), suggesting rapid growth in PM2.5 (Vohra et al 2022). Also in this presentation, we report results on our current collective SAPM study of India, a country that exhibits high levels of PM2.5 pollution. We show the temporal (i.e., seasonal) and spatial variability of PM2.5 over India using the CALIOP and CATS+model approaches, comparisons between the estimated PM2.5 from the retrieval schemes, and validation with in situ PM2.5 ground-based observations from the Central Pollution Control Board in India. This region provides us with an excellent case study to test our PM2.5 retrievals in heavily polluted scenes and over a complex and varying topography. The SAPM Topic group actively seeks international participants/collaborators in our group, including those working with in situ aerosol measurements (e.g., ACTRIS). We are interested in aerosol datasets in order to either improve our PM2.5 estimates from various approaches (e.g., using in situ mass scattering/absorption coefficient and aerosol hygroscopic properties for various aerosol species) and/or validate the PM2.5 estimates (e.g., using in situ ground-based PM2.5 concentrations).

Travis D Toth↗

Performance characterization of the Radionuclide Aerosol Sampler/Analyzer air sampler during a high-activity release event

The performance of the Radionuclide Aerosol Sampler/Analyzer (RASA) under high-activity conditions has been evaluated to maintain and protect the operations of International Monitoring System (IMS) radionuclide stations. Station measurements following the Fukushima Daichi accident of 11 March 2011 have been combined with laboratory measurements to understand how the quality of the measurements made using the RASA High-Purity Germanium (HPGe) gamma-spectrometer are impacted by increased sample activity and detector dead-time. Detector saturation has been identified to occur at a count rate of 175,000 counts s-1, at which level there are significant impacts to the sample live-time and detector resolution in addition to a system contamination risk. To safeguard against these effects, a dead-time limit of 16.6% is proposed that could be maintained by monitoring the activity collecting on the filter using a Cadmium Zinc Telluride (CZT) detector installed into the particulate collection area of the RASA. This limit would ensure that the IMS technical specifications for measurement time (> 20 h) and detector resolution (2.5 keV at 1332 keV) are met. The CZT would dynamically control the RASA air flow to limit the collection of particulate activity beneath the HPGe dead-time threshold and would also provide measurements useful for CTBT verification purposes and dose assessments.

Burnett, Jonathan L.↗