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NASA NTRS2019

Observation of absorbing aerosols above clouds over the south-east Atlantic Ocean from the geostationary satellite SEVIRI – Part 1: Method description and sensitivity

High-temporal-resolution observations from satellites have a great potential for studying the impact of biomass burning aerosols and clouds over the south-east Atlantic Ocean (SEAO). This paper presents a method developed to simultaneously retrieve aerosol and cloud properties in aerosol above-cloud conditions from the geostationary instrument Meteosat Second Generation/Spinning Enhanced Visible and Infrared Imager (MSG/SEVIRI). The above-cloud aerosol optical thickness (AOT), the cloud optical thickness (COT) and the cloud droplet effective radius (CER) are derived from the spectral contrast and the magnitude of the signal measured in three channels in the visible to shortwave infrared region. The impact of the absorption from atmospheric gases on the satellite signal is corrected by applying transmittances calculated using the water vapour profiles from a Met Office forecast model. The sensitivity analysis shows that a 10 % error on the humidity profile leads to an 18.5 % bias on the above-cloud AOT, which highlights the importance of an accurate atmospheric correction scheme. In situ measurements from the CLARIFY-2017 airborne field campaign are used to constrain the aerosol size distribution and refractive index that is assumed for the aforementioned retrieval algorithm. The sensitivities in the retrieved AOT, COT and CER to the aerosol model assumptions are assessed. Between 09:00 and 15:00 UTC, an uncertainty of 40 % is estimated on the above-cloud AOT, which is dominated by the sensitivity of the retrieval to the single-scattering albedo. The absorption AOT is less sensitive to the aerosol assumptions with an uncertainty generally lower than 17 % between 09:00 and 15:00 UTC. Outside of that time range, as the scattering angle decreases, the sensitivity of the AOT and the absorption AOT to the aerosol model increases. The retrieved cloud properties are only weakly sensitive to the aerosol model assumptions throughout the day, with biases lower than 6 % on the COT and 3 % on the CER. The stability of the retrieval over time is analysed. For observations outside of the backscattering glory region, the time series of the aerosol and cloud properties are physically consistent, which confirms the ability of the retrieval to monitor the temporal evolution of aerosol above-cloud events over the SEAO.

cloud properties↗

NASA NTRS2021

Present and future aerosol impacts on Arctic climate change in the GISS-E2.1 Earth system model

The Arctic is warming 2 to 3 times faster than the global average, partly due to changes in short-lived climate forcers (SLCFs) including aerosols. In order to study the effects of atmospheric aerosols in this warming, recent past (1990–2014) and future (2015–2050) simulations have been carried out using the GISS-E2.1 Earth system model to study the aerosol burdens and their radiative and climate impacts over the Arctic (>60°N), using anthropogenic emissions from the Eclipse V6b and the Coupled Model Intercomparison Project Phase 6 (CMIP6) databases, while global annual mean greenhouse gas concentrations were prescribed and kept fixed in all simulations. Results showed that the simulations have underestimated observed surface aerosol levels, in particular black carbon (BC) and sulfate (SO2−4), by more than 50 %, with the smallest biases calculated for the atmosphere-only simulations, where winds are nudged to reanalysis data. CMIP6 simulations performed slightly better in reproducing the observed surface aerosol concentrations and climate parameters, compared to the Eclipse simulations. In addition, simulations where atmosphere and ocean are fully coupled had slightly smaller biases in aerosol levels compared to atmosphere-only simulations without nudging. Arctic BC, organic aerosol (OA), and SO2−4 burdens decrease significantly in all simulations by 10 %–60 % following the reductions of 7 %–78 % in emission projections, with the Eclipse ensemble showing larger reductions in Arctic aerosol burdens compared to the CMIP6 ensemble. For the 2030–2050 period, the Eclipse ensemble simulated a radiative forcing due to aerosol–radiation interactions (RFARI) of −0.39 ± 0.01 W/sq. m, which is −0.08 W/sq. m larger than the 1990–2010 mean forcing (−0.32 W/sq. m), of which −0.24 ± 0.01 W/sq. m was attributed to the anthropogenic aerosols. The CMIP6 ensemble simulated a RFARI of −0.35 to −0.40 W/sq. m for the same period, which is −0.01 to −0.06 W/sq. m larger than the 1990–2010 mean forcing of −0.35 W/sq. m. The scenarios with little to no mitigation (worst-case scenarios) led to very small changes in the RFARI, while scenarios with medium to large emission mitigations led to increases in the negative RFARI, mainly due to the decrease in the positive BC forcing and the decrease in the negative SO2−4 forcing. The anthropogenic aerosols accounted for −0.24 to −0.26 W/sq. m of the net RFARI in 2030–2050 period, in Eclipse and CMIP6 ensembles, respectively. Finally, all simulations showed an increase in the Arctic surface air temperatures throughout the simulation period. By 2050, surface air temperatures are projected to increase by 2.4 to 2.6 °C in the Eclipse ensemble and 1.9 to 2.6 °C in the CMIP6 ensemble, compared to the 1990–2010 mean. Overall, results show that even the scenarios with largest emission reductions leads to similar impact on the future Arctic surface air temperatures and sea-ice extent compared to scenarios with smaller emission reductions, implying reductions of greenhouse emissions are still necessary to mitigate climate change.

Aerosols↗

NASA NTRS2021

Spectral Derivatives of Optical Depth for Partitioning Aerosol Type and Loading

Quantifying aerosol compositions (e.g., type, loading) from remotely sensed measurements by spaceborne, suborbital and ground-based platforms is a challenging task. In this study, the first and second-order spectral derivatives of aerosol optical depth (AOD) with respect to wavelength are explored to determine the partitions of the major components of aerosols based on the spectral dependence of their particle optical size and complex refractive index. With theoretical simulations from the Second Simulation of a Satellite Signal in the Solar Spectrum (6S) model, AOD spectral derivatives are characterized for collective models of aerosol types, such as mineral dust (DS) particles, biomass-burning (BB) aerosols and anthropogenic pollutants (AP), as well as stretching out to the mixtures among them. Based on the intrinsic values from normalized spectral derivatives, referenced as the Normalized Derivative Aerosol Index (NDAI), a unique pattern is clearly exhibited for bounding the major aerosol components; in turn, fractions of the total AOD (fAOD) for major aerosol components can be extracted. The subtlety of this NDAI method is examined by using measurements of typical aerosol cases identified carefully by the ground-based Aerosol Robotic Network (AERONET) sun–sky spectroradiometer. The results may be highly practicable for quantifying fAOD among mixed-type aerosols by means of the normalized AOD spectral derivatives.

aerosol partition↗

NASA NTRS2022

Vertical structure of biomass burning aerosol transported over the southeast Atlantic Ocean

Biomass burning in southwestern Africa produces smoke plumes that are transported over the Atlantic Ocean and overlie vast regions of stratocumulus clouds. This aerosol layer contributes to direct and indirect radiative forcing of the atmosphere in this region particularly during the months of August, September, and October. There was a multi-year international campaign to study this aerosol and its interactions with clouds. Here, we report on the evolution of aerosol distributions and properties as measured by the airborne high spectral resolution lidar (HSRL-2) during the ORACLES (Observations of Aerosols above Clouds and their intEractionS) campaign in September 2016. The NASA Langley HSRL-2 instrument was flown on the NASA ER-2 aircraft for several days in September 2016. Data were aggregated at two pairs of 2° × 2° grid boxes to examine the evolution of the vertical profile of aerosol properties during transport over the ocean. Results showed that the structure of the profile of aerosol extinction and microphysical properties is maintained over a 1 to 2 d timescale. In the 3–5 km altitude range, 95 % of the aerosol extinction was contributed by particles in the 0.05–0.50 µm radius size range with the aerosol in this size range having an average effective radius of 0.16 µm. This indicates that there is essentially no scavenging or dry deposition at these altitudes. Moreover, there is very little day-to-day variation in these properties, such that time sampling as happens in such campaigns may be representative of longer periods such as monthly means. Below 3 km, there is considerable mixing with larger aerosol, most likely continental source near land. Furthermore, these measurements indicated that there was often a distinct gap between the bottom of the aerosol layer and cloud tops at the selected locations as evidenced by a layer of several hundred meters that contained relatively low aerosol extinction values above the clouds.

lidar↗

NASA NTRS2022

Circular Polarization in Atmospheric Aerosols

Recent technological advances have demonstrated the feasibility of deploying spaceborne optical detectors with full polarimetric capabilities. The measurement of all four Stokes coefficients opens significant new opportunities for atmospheric aerosol studies and applications. While considerable amounts of attention have been dedicated to sensors with sensitivity to the total intensity and linear polarization (represented by Stokes coefficients I, U, Q), there has been less attention to the additional information brought by measuring circular polarization (coefficient V). This report fills this gap in knowledge by providing an overview of aerosol sources of circular polarization in the atmosphere and discusses possible remote sensing signatures. In this manuscript, circularly polarized radiation that results from the interaction of incident unpolarized radiation are considered in three physical settings: optical activity originating in biogenic aerosols, alignment of non-spherical particles in the presence of electrical fields (such as dust, smoke, and volcanic ash) and aerosol multiple scattering effects. Observational and theoretical evidence of, and the settings and conditions for non-zero aerosol circular polarization generated from incident unpolarized radiation are here gathered and discussed. In addition, novel radiative transfer simulations are shown to illustrate notable spectral and other features where circular polarization may provide additional information that is possibly independent from total intensity and linear polarization only observations. Current techniques for detection of aerosol composition (also referred as aerosol type) from space provide limited information. Remote identification of aerosols such as smoke, volcanic ash, and dust particles can only be accomplished with some degree of confidence for moderate to high concentrations. When the same aerosols are found at lower concentrations (but still high enough to be of importance for air quality and cloud formation), these methods often produce ambiguous results. The circular polarization of aerosols is rarely utilized, and we explore its value for improved determination aerosol composition. This study is presented as an overview with a goal to provide a new perspective on an overlooked optical property and to trigger interest in further exploration of this subject.

Aerosol type↗

NASA NTRS2023

Dispersion and Aging of Volcanic Aerosols after the La Soufriere Eruption in April 2021

Volcanic aerosols change the atmospheric composition and thereby affect weather and climate. Aerosol dynamic processes such as nucleation, condensation, and coagulation modify the shape, size, and mass of aerosol particles, which influence their atmospheric lifetime and radiative properties. Nevertheless, most models omit these processes for ash particles. In this work, we explore the ash aerosol aging and sulfate production during the first 4 days following the 2021 La Soufrière (St. Vincent) eruption with the ICON-ART model (ICOsahedral Nonhydrostatic model with Aerosol and Reactive Trace gases). Online coupling of ICON-ART with a one-dimensional volcanic plume model calculates volcanic emission, which makes it possible to resolve the different eruption phases of the noncontinuous La Soufrière eruption. We compared our simulated aerosol distribution and composition with observations from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument, the Multiangle Imaging SpectroRadiometer (MISR) Research Aerosol (RA) Algorithm, and the Barbados Cloud Observatory (BCO). We show that online coupling is essential to adequately model the emissions and plume development close to the volcano. The modeled aerosol aging is in very good agreement with observations from MISR near the emission source and with CALIOP at larger distances. Furthermore, particle aging occurs faster in the troposphere than in the stratosphere due to the availability of water vapor and OH, but a layer of coated ash appears at the plume top due to faster oxidation of SO2 and lofting by aerosol-radiation interaction. This paper gives the first direct comparison of aerosol aging in volcanic eruption plumes between simulations and observations

volcanic aerosols↗

NASA NTRS2026

South Asian Monsoon Response to Regional Aerosol Emission Reductions: Insights From RAMIP

Anthropogenic aerosol and associated precursor gas emissions are already declining in many regions and are likely to decline significantly by 2050, with major implications for regional climate. Unlike greenhouse gases, aerosol impacts are spatially heterogeneous and can influence climate both near emission sources and through remote teleconnections. This is particularly important for the South Asian monsoon system, where both local and remote aerosol changes can significantly affect precipitation patterns. Using simulations from the Regional Aerosol Model Intercomparison Project, we examine how local and remote aerosol emission reductions influence South Asian climate across both pre-monsoon and monsoon seasons, including weakening of the elevated heat pump (EHP) mechanism during pre-monsoon months. Our analysis employs 10-member ensembles from 10 CMIP6-era models to compare three experiments with global, South Asian, and East Asian aerosol reductions relative to a high-emission baseline (SSP3-7.0). This experimental design allows us to isolate and quantify the distinct impacts of regional emission changes. Results reveal that global aerosol reductions produce a larger all-India precipitation increase (+0.28 mm day −1 ) than South Asian reductions alone (+0.19 mm day −1 ), with the strongest regional responses over the northern Bay of Bengal, the Western Ghats and Indo-Gangetic Plains. East Asian reductions show uncertain but modest precipitation reductions of 0.2-0.6 mm day −1 over parts of west-central and eastern Indian regions. Pre-monsoon carbonaceous aerosol reductions systematically weaken the EHP, cooling the mid-troposphere over the Himalayan foothills by up to 0.4 K and producing localised anomalous descent that opposes the climatological pre-monsoon ascent. Substantial inter-model diversity exists in the spatial patterns and magnitudes of these responses, highlighting key uncertainties in aerosol–monsoon interactions. The South Asian precipitation response is driven by enhanced land–sea thermal contrast, while the pre-monsoon EHP weakening is attributable exclusively to local South Asian carbonaceous aerosol forcing rather than remote teleconnections. These findings have direct implications for air quality and climate adaptation planning across South Asia as regional aerosol emissions diverge under different development pathways.

cmip6↗

NASA NTRSDate not supplied

MISR Level 2 Aerosol parameters (MIL2ASAE_V1)

The Aerosol data contain aerosol optical depth, aerosol physical model, ancillary meteorological data, and related parameters. The aerosol data include tropospheric aerosol optical depth, Angstrom exponent and single scattering albedo on 17.6 km centers, aerosol mixture identifier and retrieval residuals, and ancillary data including assumed ozone optical depth and retrieval flags. For complete information about the aerosol mixtures, the user will need to order the MISR Aerosol Climatology Product (MIANACP) to obtain Aerosol Physical and Optical Properties (APOP) and the Mixture files. The Mixture files list up to 3 component models used in each mixture, with their relative compositional fractions, and includes ancillary information such as single scattering albedo. The APOP gives detailed information for the component particle models. [Location=GLOBAL] [Temporal_Coverage: Start_Date=2000-02-24; Stop_Date=] [Spatial_Coverage: Southernmost_Latitude=-90; Northernmost_Latitude=90; Westernmost_Longitude=-180; Easternmost_Longitude=180] [Data_Resolution: Latitude_Resolution=1.1 km - 17.6 km; Longitude_Resolution=1.1 km - 17.6 km; Horizontal_Resolution_Range=1 km - < 10 km or approximately .01 degree - < .09 degree; Temporal_Resolution=about 15 orbits/day].

CIRRUS OPTICAL DEPTH↗

NASA NTRSDate not supplied

MISR Level 2 Aerosol parameters (MIL2ASAE_V2)

EOSDIS↗

DOE OSTI2024

Quantifying the Diversity of an Atmospheric Aerosol Population in an Arctic Oil Field on a Single‐Particle Level

As the Arctic rapidly warms, sea ice extent is decreasing and oil and gas extraction activities are expanding. Local combustion emissions affect the Arctic atmospheric aerosol chemical mixing state (the distribution of chemical species across the aerosol population), which impacts climate-relevant properties. Bulk and single-particle measurements of submicron aerosols were conducted at Oliktok Point, Alaska within the North Slope of Alaska oil fields. In this work, we quantify aerosol diversity using online single-particle mass spectrometry data (32,880 individual particles), offline single-particle microscopy data (20,912 individual particles), and online bulk aerosol mass spectrometry and aethalometer data. This method was used to derive individual particle mass fractions for both refractory and non-refractory material within distinct particle types. Single-particle, average single-particle, and bulk population diversities (D i , D α , D γ , respectively) and mixing state indices (χ) were calculated for the data set. Calculated D i values were generally low (2.2 ± 0.6), as individual particle masses were dominated by a few chemical species of interest. Aged aerosol particles (those internally mixed with nitrate and/or sulfate) exhibited higher D i values (>3) compared to recently emitted (fresh) aerosol particles. During oil field plume periods, D α values approached three due to the abundance of diesel combustion particles, which were rich in sulfate, black carbon, and organic aerosol. Overall, the submicron aerosol population within the Arctic oil fields was found to be relatively externally mixed (χ < 50%), due to the constant local emissions within oil fields combining with background aerosol and locally emitted sea spray aerosol at the coastal site.

Wu, J.↗

DOE OSTI2021

Aerosol Chemical Speciation Monitor (ACSM) Composition-Dependent Collection Efficiency (CDCE) Value-Added Product Report

Aerosol particles influence the Earth’s radiation balance directly by absorbing and scattering light and indirectly by influencing cloud formation, properties, and lifetimes. Measurements of aerosol particle optical properties, mass loading, size distributions, microphysical properties, cloud formation properties, and chemical composition are important for understanding the aerosol life cycle and for validating earth system models that predict these quantities. The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Aerosol Observing System (AOS) is a highly instrumented platform that measures many of these aerosol properties in situ. The Aerodyne aerosol chemical speciation monitor (ACSM) is a baseline instrument deployed in the AOS. The ACSM provides a quantitative measurement of aerosol particle chemical composition for non-refractory (operationally defined as components that evaporate on the 600ºC vaporizer) aerosol components in real time. Standard output is the mass concentration of particulate organics, nitrate, sulfate, chloride, and ammonium. One well-known limitation to the accuracy of the ACSM data is in evaluating the fraction of the ambient aerosol particles that are detected by the instrument. This quantity is referred to as the collection efficiency (CE) and is often less than unity. This is attributed to particles rebounding after impaction onto the heated vaporizer rather than being trapped, volatilized rapidly, and detected. Other factors, such as divergence of the aerosol particle beam, may also impact CE, but the particle rebound effect is the dominant factor. Scientists will sometimes assume CE = 0.5 (i.e., one half of sampled particles are detected) for ambient particles collected during field missions. However, parameterizations have been developed that express CE as a function of the measured chemical composition, referred to as the composition-dependent collection efficiency (CDCE). The physical explanation for a CDCE, supported by laboratory studies, is that rebound from the vaporizer is a function of the particle phase, with liquid-like particles “sticking” to the vaporizer and solid-like or crystalline particles “bouncing” from the vaporizer. Thus, particles with compositions are liquids-like under the measurement conditions (e.g., certain organics, acidic particles, particles enriched in nitrate) have CE close to unity while crystalline or solid particles (e.g., deliquesced ammonium sulfate) have lower CE. This value-added product (VAP) implements the procedure described by Middlebrook et al. (2012) to correct the ACSM data for the composition-dependent collection efficiency. Applying this parameterization improves the accuracy of the ACSM data and brings them into better agreement with other co-located aerosol measurements.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Are Marine Low Cloud Droplet Concentrations Buffered by Entrained Aitken‐Mode Aerosol (Final Technical Report)

During the summertime, the high-latitude oceans come to life with green phytoplankton, which gain their energy from sunlight and are food for sea creatures small and large. When the phytoplankton are eaten or die, sulfur-rich gases are released under the ocean surface and mix into the air. Observations suggest that, over the Southern Ocean, frequent storms lift this air high into the atmosphere while raining out particulates like salt. As a result, the sulfur-rich air then spawns high concentrations of small ‘Aitken-mode’ aerosol particles. We hypothesize that these particles work their way down into the marine boundary layer, where they can replenish the supply of cloud-condensation nuclei scavenged by frequent precipitation. Further, this process maintains high concentrations of liquid cloud droplets in austral summer, promoting more sunlight to be reflected to space. We call this ‘Aitken buffering’. The primary objective of this project has been to document and test what role Aitken-mode aerosols play in clouds over the Southern Ocean and elsewhere. This effort has included three main components: 1) developing a computer model that realistically simulates the aerosol processes and the small-scale turbulent air motions that move aerosols around and create the clouds, 2) using that model to interpret and extend these observations for process understanding, by allowing different factors that contribute to the aerosol budget, such as surface wind speed, precipitation, surface gas exchange, etc. to be separated, and 3) studying Aitken-mode aerosol and its variability with a focus over the Southern Ocean and Antarctica, using data from Atmospheric Radiation Measurement (ARM) sites and other available observations. Initial computer studies in more idealized conditions found that elevated concentrations of Aitken-mode aerosols above the clouds could help prevent the breakup of those clouds by acting as cloud-condensation nuclei after they were entrained into the cloudy boundary layer. Simulations of a day during the ACE-ENA field campaign showed that Aitken-mode aerosols could also prevent cloud breakup under more realistic conditions. A new method that extracts information about Aitken-mode aerosols from measurements of aerosols onto which cloud droplets can form finds that Aitken-mode aerosols do vary seasonally over the Southern Ocean, with a peak in summertime, as described above. Other work during this project has focused on understanding how patterns of water vapor, clouds and precipitation are coupled within low-lying clouds over the oceans, and also on how cloud droplets cluster within clouds and how the distribution of cloud droplet sizes change as dry air is mixed into clouds, with the latter studies also using observations from ACE-ENA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Characterization of Organosulfates and Organonitrates in Vertically Resolved Aerosols over the Southern Great Plains Field Campaign Report

Aerosol is the largest individual source of uncertainty in assessing the Earth’s radiative balance due to poorly understood aerosol processes and aerosol-cloud interactions. Thus, to constrain aerosol’s climate impacts, it is critical to understand aerosol compositions at high elevations. Organic material accounts for about 20-80% of total aerosol mass in the atmosphere and is known to play a key role in aerosol processes and cloud formation. In prior research, characterization of aerosol molecular composition has been mostly carried out at ground level. In these ground-level measurements, total speciated organosulfates and organonitrates may contribute significantly to organic aerosol mass on the order of 10-40%, most of which are from abundant biogenic volatile organic compounds such as isoprene and monoterpenes. Organosulfates and organonitrates have also been shown to be present in substantial amounts in cloud water, suggesting that they can be transported and/or directly formed at high elevations. On the other hand, the less common and more expensive aircraft studies have performed high-altitude measurements, but were often limited in the number of different altitudes sampled and in sample collection under consistent conditions. Therefore, the vertical distributions of key aerosol components such as organosulfates and organonitrates are not well understood and have not been extensively studied. Nevertheless, it is important to understand how organosulfates and organonitrates in aerosols are distributed, transformed, participate in aqueous-phase processes, and interact with high-altitude clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Aerosol Hygroscopic Growth, Mixing State, and Cloud Condensation Nuclei Activity during TRACER (Field Campaign Report)

Convective clouds play a critical role in the Earth’s climate system. Recent research has shown that a realistic representation of convective processes is critical to constraining climate sensitivity in global climate models. Theoretical and modeling studies showed that aerosols could have strong dynamic feedback to convection in warm and humid environments through enhancing ice-related processes and condensational growth. A few observation-based studies also suggested the influence of aerosols on convective cloud and precipitation properties. However, robust observational quantification of an aerosol effect on convective clouds isolated from other factors remains elusive. Understanding the impact of aerosol on convective clouds requires knowledge of the cloud condensation nuclei (CCN) spectrum, which represents the number of particles that uptake water and form cloud droplets as a function of supersaturation. The water uptake by aerosol is also of critical importance for the direct interaction of aerosol with radiation (i.e., aerosol direct effect) due to light scattering and absorption by aerosol. While both droplet activation under supersaturated conditions (i.e., relative humidity RH > 100%) and the hygroscopic growth under sub-saturated conditions (i.e., RH < 100%) are strongly influenced by particle hygroscopicity, the thermodynamic regimes and measurement methods are quite different. Aerosol particles, especially organic particles, can exhibit higher hygroscopicity for droplet activation than that for hygroscopic growth. In the subsaturated regime, the hygroscopicity of organic particles can also vary strongly with RH. However, global climate models usually treat organic species in aerosols with a constant hygroscopicity, potentially introducing substantial uncertainties in the quantification of aerosol radiative effects.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

The CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) measurement campaign

The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

On the differences in the vertical distribution of modeled aerosol optical depth over the southeastern Atlantic

Abstract. The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Observations of high-time-resolution and size-resolved aerosol chemical composition and microphysics in the central Arctic: implications for climate-relevant particle properties

Abstract. Aerosols play a critical role in the Arctic's radiative balance, influencing solar radiation and cloud formation. Limited observations in the central Arctic leave gaps in understanding aerosol dynamics year-round, affecting model predictions of climate-relevant aerosol properties. Here, we present the first annual high-time-resolution observations of submicron aerosol chemical composition in the central Arctic during the Arctic Ocean 2018 (AO2018) and the 2019–2020 Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expeditions. Seasonal variations in the aerosol mass concentrations and chemical composition in the central Arctic were found to be driven by typical Arctic seasonal regimes and resemble those of pan-Arctic land-based stations. Organic aerosols dominated the pristine summer, while anthropogenic sulfate prevailed in autumn and spring under haze conditions. Ammonium, which impacts aerosol acidity, was consistently less abundant, relative to sulfate, in the central Arctic compared to lower latitudes of the Arctic. Cyclonic (storm) activity was found to have a significant influence on aerosol variability by enhancing emissions from local sources and the transport of remote aerosol. Local wind-generated particles contributed up to 80 % (20 %) of the cloud condensation nuclei population in autumn (spring). While the analysis presented herein provides the current central Arctic aerosol baseline, which will serve to improve climate model predictions in the region, it also underscores the importance of integrating short-timescale processes, such as seasonal wind-driven aerosol sources from blowing snow and open leads/ocean in model simulations. This is particularly important, given the decline in mid-latitude anthropogenic emissions and the increase in local ones.

Heutte, Benjamin (ORCID:0000000173727460)↗

NASA NTRS1987

SAGE aerosol measurements. Volume 3: January 1, 1981 to November 18, 1981

The Stratospheric Aerosol and Gas Experiment (SAGE) satellite system, launched February 18, 1979, obtained profiles of aerosol extinction at 1.00 micron and 0.45 micron ozone concentration, and nitrogen dioxide concentration. Data taken during sunset events are presented in the form of zonal and seasonal averages of aerosol extinction of 1.00 micron and 0.45 micron, ratios of aerosol extinction to molecular extinction at 1.00 micron and ratios of aerosol extinction at 0.45 micron to aerosol extinction at 1.00 micron. Averages for 1981 are shown in tables, and in profile and contour plots (as a function of altitude and latitude). In addition, temperature data provided by NOAA for the time and location of each SAGE measurement are averaged and shown in a similar format. The stratospheric aerosol distribution for 1981 shows effects of volcanically injected material from eruptions of Ulawun, Alaid, and Pagan. Peak values of aerosol extinction at 0.45 micron and 1.00 micron were 2 to 4 times higher than typical peak values observed during near background conditions. Stratospheric aerosol optical depth values at 1.00 microns increased by a factor of about 2 from near background levels in regions of volcanic activity. During the year, these values ranged from between 0.001 and 0.006. The largest were near the location of a recent eruption. The distribution of the ratio of aerosol to molecular extinction at 1.00 microns also showed that maximum values are found in the vicinity of an eruption. These maximums varied in altitude, but remained below a height of about 25 km. No attempt has been made to give detailed explanations or interpretations of these data. The intent is to provide, in a ready-to-use visual format, representative zonal and seasonal averages of aerosol extinction data for the third calendar year of the SAGE data set to facilitate atmospheric and climatic studies.

Mccormick, M. Patrick↗