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Exploring the Elevated Water Vapor Signal Associated With the Free Tropospheric Biomass Burning Plume Over the Southeast Atlantic Ocean

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol–cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6–7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume–vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ∼5–6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (∼6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

Kristina Pistone↗

Biomass Burning Smoke and Coincident Water Vapor Over the Southeast Atlantic Stratocumulus Region: Results from Observations and Models

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the Southeast Atlantic (SEA) Ocean. We present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA. Using multiple airborne datasets, we observe a strongly linear correlation between biomass burning indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. This relationship was particularly strong in the 2016 observations, but was also present in the 2017 and 2018 deployments. Using ECMWF and MERRA-2 reanalyses and specialized WRF-Chem simulations, we trace the plume-vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper-tropospheric air and then is subjected to conditions of strong westward advection, namely the South African Easterly Jet (AEJ-S). Our analysis indicates that airmasses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ~5-6km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. The smoky, humid mixed air is then subjected to strong zonal winds and advected over the SEA following largely isentropic trajectories. HYSPLIT back trajectories support this interpretation. With better understanding of this relationship, and its spatial and temporal variations, we are working towards accurately quantifying the radiative and dynamical effects of both aerosol and water vapor over this region.

Kristina Pistone↗

Direct and semi-direct radiative forcing of biomass-burning aerosols over the southeast Atlantic (SEA) and its sensitivity to absorbing properties: a regional climate modeling study

Simulations are performed for the period 2000-2015 by two different regional climate models, ALADIN and RegCM, to quantify the direct and semi-direct radiative effects of biomass-burning aerosols (BBAs) in the southeast Atlantic (SEA) region. Different simulations have been performed using strongly absorbing BBAs in accordance with recent in situ observations over the SEA. For the July-August-September (JAS) season, the single scattering albedo (SSA) and total aerosol optical depth (AOD) simulated by the ALADIN and RegCM models are consistent with the MACv2 climatology and MERRA-2 and CAMS-RA reanalyses near the biomass-burning emission sources. However, the above-cloud AOD is slightly underestimated compared to satellite (MODIS and POLDER) data during the transport over the SEA. The direct radiative effect exerted at the continental and oceanic surfaces by BBAs is significant in both models and the radiative effects at the top of the atmosphere indicate a remarkable regional contrast over SEA (in all-sky conditions), with a cooling (warming) north (south) of 10°S, which is in agreement with the recent MACv2 climatology. In addition, the two models indicate that BBAs are responsible for an important shortwave radiative heating of ~0.5-1K per day over SEA during JAS with maxima between 2 and 4 km a.m.s.l. (above mean sea level). At these altitudes, BBAs increase air temperature by ~0.2-0.5 K, with the highest values being co-located with low stratocumulus clouds. Vertical changes in air temperature limit the subsidence of air mass over SEA, creating a cyclonic anomaly. The opposite effect is simulated over the continent due to the increase in lower troposphere stability. The BBA semi-direct effect on the lower troposphere circulation is found to be consistent between the two models. Changes in the cloud fraction are moderate in response to the presence of smoke, and the models differ over the Gulf of Guinea. Finally, the results indicate an important sensitivity of the direct and semi-direct effects to the absorbing properties of BBAs. Over the stratocumulus (Sc) region, DRE varies from +0.94 W m -2 (scattering BBAs) to +3.93 W m -2 (most absorbing BBAs).

54 ENVIRONMENTAL SCIENCES↗

Direct and Semi-Direct Radiative Forcing of Biomass-Burning Aerosols Over the Southeast Atlantic (SEA) And Its Sensitivity to Absorbing Properties: A Regional Climate Modeling Study

Simulations are performed for the period 2000–2015 by two different regional climate models, ALADIN and RegCM, to quantify the direct and semi-direct radiative effects of biomass-burning aerosols (BBAs) in the southeast Atlantic (SEA) region. Different simulations have been performed using strongly absorbing BBAs in accordance with recent in situ observations over the SEA. For the July–August–September (JAS) season, the single scattering albedo (SSA) and total aerosol optical depth (AOD) simulated by the ALADIN and RegCM models are consistent with the MACv2 climatology and MERRA-2 and CAMS-RA reanalyses near the biomass-burning emission sources. However, the above-cloud AOD is slightly underestimated compared to satellite (MODIS and POLDER) data during the transport over the SEA. The direct radiative effect exerted at the continental and oceanic surfaces by BBAs is significant in both models and the radiative effects at the top of the atmosphere indicate a remarkable regional contrast over SEA (in all-sky conditions), with a cooling (warming) north (south) of 10 ∘S, which is in agreement with the recent MACv2 climatology. In addition, the two models indicate that BBAs are responsible for an important shortwave radiative heating of ∼0.5–1 K per day over SEA during JAS with maxima between 2 and 4 km a.m.s.l. (above mean sea level). At these altitudes, BBAs increase air temperature by ∼0.2–0.5 K, with the highest values being co-located with low stratocumulus clouds. Vertical changes in air temperature limit the subsidence of air mass over SEA, creating a cyclonic anomaly. The opposite effect is simulated over the continent due to the increase in lower troposphere stability. The BBA semi-direct effect on the lower troposphere circulation is found to be consistent between the two models. Changes in the cloud fraction are moderate in response to the presence of smoke, and the models differ over the Gulf of Guinea. Finally, the results indicate an important sensitivity of the direct and semi-direct effects to the absorbing properties of BBAs. Over the stratocumulus (Sc) region, DRE varies from +0.94 W m−2 (scattering BBAs) to +3.93 W m−2 (most absorbing BBAs).

Marc Mallet↗

Impacts of Aerosol and Cloud Variability on Satellite-Derived All-skies Direct Aerosol Radiative Effects (DARE) over the North and Southeast Atlantic

The Top-of-Atmosphere (TOA) Shortwave (SW) Direct Aerosol Radiative Effect (DARE) in all-sky conditions (i.e., aerosols in clear skies and aerosols above and below all types of clouds) is the global change in upwelling radiative flux due to aerosols. It is one of the strongest indicators of global climate change due to aerosols. SW DARE at TOA depends on the Earth’s surface albedo, cloud fraction, cloud optical properties, and aerosol optical properties, which are all challenging to accurately characterize from space. The overarching goals of our project are to provide state-of-the-art observational all-sky TOA SW DARE, along with guidance on which aerosol and/or cloud properties are the most important to measure, and at which spatio-temporal scales, for accurate DARE observations. We compute all-sky DARE based on state-of-the-art cloud and aerosol retrieval algorithms from CALIOP (Cloud–Aerosol Lidar with Orthogonal Polarization) and MODIS (Moderate Resolution Imaging spectroradiometer) satellite sensors, as well as aerosol intensive properties from MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, version 2) simulations over three specific regions of the Atlantic Ocean from 2012 to 2016. In this symposium, we present a characterization of the cloud and aerosol optical and physical properties and the observational TOA SW DARE along three individual satellite tracks in the Southeast Atlantic region -- on September 18 and 20, 2016 and August 13, 2017. We then quantify the impact of assuming homogeneous cloud or aerosol fields in space-based TOA SW DARE calculations. And, finally, the resulting space-based all-skies aerosol vertical distribution and DARE calculations are evaluated using remote sensing observations from coincident suborbital flights from the NASA ORACLES (the ObseRvations of Aerosols above CLouds and their intEractionS, ORACLES field campaign) field campaign. The NASA Atmospheric Observing System (AOS) mission addresses the NASA Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables and proposes, as one of its aerosol objectives, to reduce uncertainties in estimates of global mean all-sky SW DARE at TOA. Well characterizing clouds, aerosol vertical distributions, aerosol types and associated all-skies DARE over the Atlantic Ocean will inform the AOS community on where, when, how, and how often the satellite retrievals should be performed to estimate DARE and reduce all-skies DARE uncertainties most accurately. These comprehensive characterizations will also identify the key regions and times when the AOS (or other ACCP-related) suborbital missions should be conducted to evaluate and improve the AOS space-based observations and retrievals.

aerosol↗

Exploring the Elevated Water Vapor Signal Associated with Biomass Burning Aerosol over the Southeast Atlantic Ocean

The quantification of radiative forcing due to the cumulative effects of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in our understanding of the physical climate. How the magnitude of these effects may be modified by meteorological conditions is an important aspect of this question. The Southeast Atlantic Ocean (SEA), with seasonal biomass burning (BB) smoke plumes overlying a persistent stratocumulus cloud deck, offers a perfect natural observatory in which to study the complexities of aerosol-cloud interactions. The NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign consists of three field deployments over three years (2016-2018) with the goal of gaining a better understanding of the complex processes (direct and indirect) by which BB aerosols affect clouds. We present results from the first ORACLES field deployment, which took place in September 2016 out of Walvis Bay, Namibia. Two NASA aircraft were flown with a suite of aerosol, cloud, radiation, and meteorological instruments for remote-sensing and in-situ observations. A strong correlation was observed between the aircraft-measured pollution indicators (carbon monoxide and aerosol properties) and atmospheric water vapor content, at all altitudes. Atmospheric reanalysis indicates that convective dynamics over the continent, near likely contribute to this elevated signal. Understanding the mechanisms by which water vapor covaries with plume strength is important to quantifying the magnitude of the aerosol direct and semi-direct effects in the region.

Pistone, Kristina↗

Radiative Heating from Biomass Burning Aerosol and its Impact on Cloud Structure in the Southeast Atlantic

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. In many cases, the complex physical relationships between marine boundary cloud morphology and the environmental conditions in which the clouds exist are not well understood. Such uncertainties arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean. It is likely that the absorbing and heating properties of these aerosols influence the microphysical composition and macrophysical arrangement of marine stratocumulus and trade cumulus in this region; however, this has yet to be quantified. The deployment of the Atmospheric Radiation Measurement Mobile Facility #1 (AMF1) in support of LASIC (Layered Atlantic Smoke Interactions with Clouds) provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96 S, 14.35 W). Thermodynamic profiles will be analyzed through the unique combination of sounding data from radiosonde launches and microwave profiling radiometers, giving observations of additional quantities important for cloud development such as CAPE and CIN at a fine temporal resolution. The thermodynamic profiles will be presented in conjunction with detailed observations of the cloud structure over the site from a K-band cloud radar, micropulse lidar, and laser ceilometer. The observed thermodynamic and cloud profiles will be used as input forcing, alongside aerosols from the Modern Era Retrospective analysis for Research and Applications, version 2 (MERRA-2), for the Rapid Radiative Transfer Model (RRTM) to gain information regarding the radiative heating profiles. Idealized experiments using RRTM with and without aerosols will be used to quantify the impact of biomass burning carbonaceous aerosol plumes as they pass over the site. Due to documented discrepancies in the single scatter albedo (SSA) between models and observations, further sensitivity experiments will demonstrate the importance of the optical properties of biomass burning aerosol in accurately representing heating within the column. Finally, the heating rates will be put into context of the cloud structure over the site from the perspective of the mass flux closure from the University of Washington shallow convective scheme.

Collow, Allison↗

Aerosol Above Cloud Optical Depth in the Southeast Atlantic and Its Use in Continuity NASA Products

When aerosol overlie bright clouds, their radiative impact on the incident light can be either positive or negative. This difference in radiative impact promotes difficulties in remote sensing aerosol properties, which have shown biases in aerosol optical depth (AOD) retrievals when clouds are underneath. To better constrain this quantity, we have measured aerosols above clouds over the course of 3 years in the southeast Atlantic as part of the ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES). These directly measured AOD above clouds are used to build and improve upon the current Near-Real-Time MODACAERO algorithm for above cloud AOD from MODIS, into a continuity product for NASA EOS/SNPP/JPSS. Here we present a summary of the above cloud aerosol optical depth measured during ORACLES, and that will be used for porting the MODACAERO algorithm to the continuity product. We use aerosol optical depth measured directly from sunlight attenuation using the Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) and compare it to the active remote sensing, High Spectral Resolution Lidar-2 (HSRL-2). We present a combination of all 3 years of measurements during peak biomass burning season. We have observed average above cloud aerosol optical depth at 500 nm ranging from 0.28 to 0.37, with the maximum in August 2017. We emphasize the use of improved aerosol absorption and scattering models based on airborne measurements during ORACLES.

aerosol optical depth (AOD)↗

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

Jens Redemann↗

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3-5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

54 ENVIRONMENTAL SCIENCES↗

Aerosol hygroscopicity over the southeast Atlantic Ocean during the biomass burning season – Part 1: From the perspective of scattering enhancement​​​​​​​

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f(RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f(80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f(80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f(80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κ OA ) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κ OA at lower altitudes. We propose a parameterization that quantifies f(RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH 4 ) 2 SO 4 –BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH 4 ) 2 SO 4 –BC internal mixture with respect to the f(RH) prediction. The sensitivity of f(RH) to κ OA indicates that applying a constant κ OA is only suitable when the OA fraction is low and κ OA shows limited variation. However, in situations deviating these two criteria, κ OA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κ OA variability is recommended.

54 ENVIRONMENTAL SCIENCES↗

Estimating the Direct Radiative Effect of Absorbing Aerosols Overlying Marine Boundary Layer Clouds in the Southeast Atlantic Using MODIS and CALIOP

Absorbing aerosols such as smoke strongly absorb solar radiation, particularly at ultraviolet and visible/near-infrared (VIS/NIR) wavelengths, and their presence above clouds can have considerable implications. It has been previously shown that they have a positive (i.e., warming) direct aerosol radiative effect (DARE) when overlying bright clouds. Additionally, they can cause biased passive instrument satellite retrievals in techniques that rely on VIS/NIR wavelengths for inferring the cloud optical thickness (COT) and effective radius (re) of underlying clouds, which can in turn yield biased above-cloud DARE estimates. Here we investigate Moderate Resolution Imaging Spectroradiometer (MODIS) cloud optical property retrieval biases due to overlying absorbing aerosols observed by Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and examine the impact of these biases on above-cloud DARE estimates. The investigation focuses on a region in the southeast Atlantic Ocean during August and September (2006-2011), where smoke from biomass burning in southern Africa overlies persistent marine boundary layer stratocumulus clouds. Adjusting for above-cloud aerosol attenuation yields increases in the regional mean liquid COT (averaged over all ocean-only liquid clouds) by roughly 6%; mean re increases by roughly 2.6%, almost exclusively due to the COT adjustment in the non-orthogonal retrieval space. It is found that these two biases lead to an underestimate of DARE. For liquid cloud Aqua MODIS pixels with CALIOP-observed above-cloud smoke, the regional mean above-cloud radiative forcing efficiency (DARE per unit aerosol optical depth (AOD)) at time of observation (near local noon for Aqua overpass) increases from 50.9Wm(sup-2)AOD(sup-1) to 65.1Wm(sup-2)AOD(sup -1) when using bias-adjusted instead of nonadjusted MODIS cloud retrievals.

aerosols↗

Connecting the Radiative Influences of Aerosol upon the Mass Flux Profiles of Shallow Cumuli across the Southeast Atlantic Ocean Basin and its Boundaries (Final Report)

The Atlantic Ocean covers approximately 25% of Earth’s surface and the atmosphere above it is home to a complex array of clouds and aerosols that have important influences on regional and global weather and climate. These influences must be accurately depicted in short range, medium range, seasonal, and climate forecast models. Conditions over the tropical Atlantic are particularly complex due to continental scale plumes of dust from the Sahara Desert and smoke from agricultural burning in Africa that drift across the Atlantic Ocean basin toward the Americas. These plumes are often found meandering in the lower atmosphere above shallow tropical clouds that form above the ocean surface, presumably mingling with these clouds on occasion due to convective mixing processes. Elevated dust and smoke particles absorb incoming sunlight and substantially warm the marine atmosphere in the layer in which they are present. This warming may alter the thermal stability of the marine atmosphere and may throttle or enhance the development of clouds, change their internal structure and the rate at which they precipitate. Alternatively, it may isolate the lower atmosphere from drier layers above enabling water vapor to accumulate near the ocean surface potentially leading to the development of deeper convection. Our study was organized around the principal concept of determining the impact of African smoke and dust plumes upon cloud development at ASI and understanding how a popular shallow convection parameterization used in models responds to the presence of this aerosol. We analyzed observations collected during the US Department of Energy (DOE) Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign using the Atmospheric Radiation Measurement Program’s Mobile Facility #1 (AMF-1), which was deployed to Ascension Island (ASI) in Southeastern Atlantic for a one-year period. Ascension Island is immediately downwind from an African source of these plumes, but far enough removed to enable the lower atmosphere to have reacted to their presence. A main goal of our study was to compute radiative heating rate profiles over Ascension Island and along the trajectory from the biomass burning regions along coastal Africa to Ascension Island. To compute the radiative heating rate due to aerosols and clouds, we employed observed profiles of temperature, humidity, and clouds from LASIC alongside aerosol optical properties from the Modern-era Retrospective analysis for Research and Applications Version 2 (MERRA-2), as input for the Rapid Radiation Transfer Model (RRTM). Radiative heating was also assessed across the southeast Atlantic Ocean using an ensemble of back trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. We were successful in this effort and the resulting publication is already being cited despite its relatively short lifetime in the literature. The second part of our study involved the process-level representation of the clouds observed over the Southeastern Atlantic in models. Our initial task, upon which the balance of this portion of the study depended, was to evaluate the representativeness of the clouds observed by AMF-1. What orographic influence did Ascension Island have on the measured cloud structure? We set out to answer this question by trying to separate observations that were clearly indicative of orographic forcing from those that were representative of open ocean. The siting of AMF-1, which was 340-m above sea-level on the slope of a steep escarpment, proved demonstrably problematic for cloud process measurements. Despite considerable effort using multiple approaches including artificial intelligence (AI), we were unable to successfully compensate for the orographic forcing present at the AMF-1 site on ASI and, hence, produce process-level summaries of the convective mass flux representative of open ocean over the Southeastern Atlantic. Even though the project has officially ended, we are making a final attempt using two new types of clustering algorithm (i.e., AI) on the recommendation of a former student, who is an expert in this area. Since we have only recently begun to test these new AI schemes, the recommendations from the second part of our project outlined below are based on our experience at the time of this report.

54 ENVIRONMENTAL SCIENCES↗

Biomass burning and marine aerosol processing over the southeast Atlantic Ocean: a TEM single-particle analysis

This study characterizes single-particle aerosol composition from filters collected during the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) and CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) campaigns. In particular the study describes aged biomass burning aerosol (BBA), its interaction with the marine boundary layer and the influence of biomass burning (BB) air on marine aerosol. The study finds evidence of BBA influenced by marine boundary layer processing as well as sea salt influenced by BB air. Secondary chloride aerosols were observed in clean marine air as well as in BB-influenced air in the free troposphere. Higher-volatility organic aerosol appears to be associated with increased age of biomass burning plumes, and photolysis or oxidation may be a mechanism for the apparent increased volatility. Aqueous processing and interaction with the marine boundary layer air may be a mechanism for the presence of sodium on many aged potassium salts. By number, biomass burning potassium salts and modified sea salts are the most observed particles on filter samples. The most commonly observed BC coatings are inorganic salts. These results suggest that atmospheric processes such as photolysis, oxidation and cloud processing are key drivers in the elemental composition and morphology of aged BBA. Fresh BBA inorganic salt content, as it has an important role in the particles' ability to uptake water, may be a key driver in how aqueous processing and atmospheric aging proceed.

54 ENVIRONMENTAL SCIENCES↗

Bottom Pressure Tides Along a Line in the Southeast Atlantic Ocean and Comparisons with Satellite Altimetry

Seafloor pressure records, collected at 11 stations aligned along a single ground track of the Topex/Poseidon and Jason satellites, are analyzed for their tidal content. With very low background noise levels and approximately 27 months of high-quality records, tidal constituents can be estimated with unusually high precision. This includes many high-frequency lines up through the seventh-diurnal band. The station deployment provides a unique opportunity to compare with tides estimated from satellite altimetry, point by point along the satellite track, in a region of moderately high mesoscale variability. That variability can significantly corrupt altimeter-based tide estimates, even with 17 years of data. A method to improve the along-track altimeter estimates by correcting the data for nontidal variability is found to yield much better agreement with the bottom-pressure data. The technique should prove useful in certain demanding applications, such as altimetric studies of internal tides.

Ray, Richard D.↗

Swelling of Transported Smoke from Savanna fires over the Southeast Atlantic Ocean

We use the recently released Version 4 (V4) lidar data products from CALIPSO to study the smoke plumes transported from Southern African biomass burning areas. The significant improvements in CALIPSO V4 Level 1 calibration and the V4 Level 2 aerosol subtyping algorithms, the latter being particularly relevant to biomass burning smoke over this area, lead to a better representation of their optical properties. For the first time, we show evidence of smoke particles increasing in size, evidenced in their particulate color ratios, as they are transported over the South Atlantic Ocean from the source regions over Southern Africa. This is likely due to hygroscopic swelling of the smoke particles and is reflected in the higher relative humidity in the middle troposphere for profiles with smoke. This finding may have implications for radiative forcing estimates over this area and is relevant to the ORACLES field mission that is currently underway.

Kar, J.↗

Swelling of Transported Smoke from Savanna Fires over the Southeast Atlantic Ocean

We use the recently released Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Version 4.1 (V4) lidar data to study the smoke plumes transported from Southern African biomass burning areas. Significant improvements in the CALIPSO V4 Level 1 calibration and V4 Level 2 algorithms lead to a better representation of their optical properties, with the aerosol subtype improvements being particularly relevant to smoke over this area. For the first time, we show evidence of smoke particles increasing in size, evidenced in their particulate color ratios, as they are transported over the South Atlantic Ocean from the source regions over Southern Africa. We hypothesize that this is due to hygroscopic swelling of the smoke particles and is reflected in the higher relative humidity in the middle troposphere for profiles with smoke. This finding may have implications for radiative forcing estimates over this area and is also relevant to the ORACLES field mission.

Kar, J.↗

Swelling of Transported Smoke from Savanna Fires over the Southeast Atlantic Ocean

We use the recently released Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Version 4.1 (V4) lidar data to study the smoke plumes transported from Southern African biomass burning areas. Significant improvements in the CALIPSO V4 Level 1 calibration and V4 Level 2 algorithms lead to a better representation of their optical properties, with the aerosol subtype improvements being particularly relevant to smoke over this area. For the first time, we show evidence of smoke particles increasing in size, as demonstrated by their particulate color ratios, as they are transported over the South Atlantic Ocean from the source regions over Southern Africa. We hypothesize that this is due to hygroscopic swelling of the smoke particles and is reflected in the higher relative humidity in the middle troposphere for profiles with smoke. This finding may have implications for radiative forcing estimates over this area and is also relevant to the ORACLES field mission.

J. Kar↗