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DOE OSTI2021

Review of Wind–Wave Coupling Models for Large-Eddy Simulation of the Marine Atmospheric Boundary Layer

Abstract We present a review of existing wind–wave coupling models and parameterizations used for large-eddy simulation of the marine atmospheric boundary layer. The models are classified into two main categories: (i) the wave-phase-averaged, sea surface–roughness models and (ii) the wave-phase-resolved models. Both categories are discussed from their implementation, validity, and computational efficiency viewpoints, with emphasis given on their applicability in offshore wind energy problems. In addition to the various models discussed, a review of laboratory-scale and field-measurement databases is presented thereafter. The majority of the presented data have been gathered over many decades of studying air–sea interaction phenomena, with the most recent ones compiled to reflect an offshore wind energy perspective. Both provide valuable data for model validation. We also discuss the modeling knowledge gaps and computational challenges ahead.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

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↗
DOE OSTI2020

Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

The southeast Atlantic is home to well-defined smoke outflow from Africa coinciding vertically with extensive marine boundary-layer cloud decks, both reaching their climatological maxima in spatial extent around September. A framework is put forth for evaluating the performance of a range of global and regional aerosol models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. The sparse airborne observations are first aggregated into 2o grid boxes and into three vertical layers: the cloud-topped marine boundary layer (MBL), the layer from cloud top to 3 km, and the 3-6 km layer. Aerosol extensive properties simulated for the entire study region for all September suggest that the 2016 ORACLES observations are reasonably representative of the regional monthly average, with systematic deviations of 30% or less. All six models typically place the bottom of the smoke layer at lower altitudes than do the airborne lidar observations by 300-1400 m, whereas model aerosol top heights are within 0-500 m of the observations. All but one of the models that report carbonaceous aerosol masses underestimate the ratio of particulate extinction to the masses, a proxy for mass extinction efficiency, in 3-6 km. Notable findings on individual models include that WRF-CAM5 predicts the mass of black carbon and organic aerosols with minor (~10% or less) biases. GEOS-5 overestimates the carbonaceous particle masses in the MBL by a factor of 3-6. Extinction coefficients in the free troposphere (FT) and above-cloud aerosol optical depth (ACAOD) are 10-30% lower in WRF-CAM5, 30-50% lower in GEOS-5, 10-40% higher in GEOS-Chem, 10-20% higher in EAM-E3SM except for the practically unbiased 3-6 km extinction, and 20-70% lower in the Unified Model, than the airborne in situ, lidar and sunphotometer measurements. ALADIN-Climate also underestimates the ACAOD, by 30%. GEOS-5 and GEOS-Chem predict carbon monoxide in the MBL with small (10% or less) negative biases, despite their overestimates of carbonaceous aerosol masses. Overall, this study highlights a new approach to utilizing airborne aerosol measurements for model diagnosis.

Shinozuka, Yohei↗
DOE OSTI2023

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Observations of the Marine Atmospheric Boundary Layer’s Response to a Solar Eclipse

The atmospheric response to the solar eclipse of 8 April 2024 in North America is investigated with a specific focus on the marine atmospheric boundary layer (MABL). We leverage measurements collected during the Third Wind Forecast Improvement Project (WFIP3), including Doppler lidars, sonic anemometers, and thermodynamic profiler data to investigate the atmospheric response across sites that experienced partial eclipse conditions with nearly 90% obscuration. Using these measurements, we examine eclipse-induced changes in key meteorological parameters, such as temperature, wind speed, and turbulent fluxes. Most previous eclipse studies have been conducted over land, whereas this study provides new observations for both coastal and marine environments, offering additional insight into eclipse-driven variability in the MABL. The findings confirm a notable decrease in downwelling shortwave radiation during the eclipse, which results in rapid cooling of surface air. The temperature reduction ranges from $1.2^\circ \text {C}$ to $1.4^\circ \text {C}$ in coastal regions and from $0.3^\circ \text {C}$ to $0.5^\circ \text {C}$ over the ocean. This analysis suggests that the MABL’s higher thermal inertia compared to coastal regions moderates the temperature decrease during the eclipse. Wind speed exhibits a more complex behavior, as it is influenced by both the MABL and preexisting synoptic conditions. Although a reduction in wind speed is observable up to approximately 140 m above ground level (AGL) at more inland sites, at other locations closer to the coast, this reduction is constrained to the lowest 100 m AGL. Turbulence parameters retrieved from sonic anemometers, such as turbulence kinetic energy, turbulent heat flux, and friction velocity, decrease during the eclipse at coastal sites, accompanied by a brief transition of atmospheric stability from unstable to neutral or weakly stable conditions. For the open-ocean sites, the variability in turbulence statistics and atmospheric stability is minimal during the occurrence of the eclipse.

16 TIDAL AND WAVE POWER↗
DOE OSTI2025

A Review of Offshore Methane Quantification Methodologies

Since pre-industrial times, anthropogenic methane emissions have increased and are partly responsible for a changing global climate. Natural gas and oil extraction activities are one significant source of anthropogenic methane. While methods have been developed and refined to quantify onshore methane emissions, the ability of methods to directly quantify emissions from offshore production facilities remains largely unknown. Here, we review recent studies that have directly measured emissions from offshore production facilities and critically evaluate the suitability of these measurement strategies for emission quantification in a marine environment. The average methane emissions from production platforms measured using downwind dispersion methods were 32 kg h−1 from 188 platforms; 118 kg h−1 from 104 platforms using mass balance methods; 284 kg h−1 from 151 platforms using aircraft remote sensing; and 19,088 kg h−1 from 10 platforms using satellite remote sensing. Upon review of the methods, we suggest the unusually large emissions, or zero emissions observed could be caused by the effects of a decoupling of the marine boundary layer (MBL). Decoupling can happen when the MBL becomes too deep or when there is cloud cover and results in a stratified MBL with air layers of different depths moving at different speeds. Decoupling could cause: some aircraft remote sensing observations to be biased high (lower wind speed at the height of the plume); the mass balance measurements to be biased high (narrow plume being extrapolated too far vertically) or low (transects miss the plume); and the downwind dispersion measurements much lower than the other methods or zero (plume lofting in a decoupled section of the boundary layer). To date, there has been little research on the marine boundary layer, and guidance on when decoupling happens is not currently available. We suggest an offshore controlled release program could provide a better understanding of these results by explaining how and when stratification happens in the MBL and how this affects quantification methodologies.

Riddick, Stuart N. (ORCID:0000000316841843)↗
DOE OSTI2023

COMBLE Radar b1 Processing: Corrections, Calibrations, and Processing Report

The U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility recently concluded its Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE), with its campaign emphasis on marine boundary-layer clouds and mixed-phase clouds during cold-air outbreaks. The COMBLE campaign featured the deployment of the first ARM Mobile Facility (AMF1) to northern Scandinavia (Andenes, Norway), including its standard complement of ARM cloud radars. In keeping with user demands stemming from the previous AMF Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign in Argentina, a post-campaign radar mentor effort was initiated for COMBLE. This activity was intended to improve the usability of the ARM cloud radar data sets in response to overall demands for calibrated, corrected data sets for downstream studies and retrieval applications. In addition to the terrain complexities previously important to CACTI data sets (e.g., clutter designation and/or removal), COMBLE presented new challenges to existing ARM radar mentor capabilities. These included the extension of existing methodologies (e.g., relative calibration adjustment [RCA] target techniques) to frozen environments and the potential issues with their applicability when considering mixed-phase precipitation conditions. As in the previous CACTI documentation (Hardin et al. 2020), the overall calibration and conditioning process in ARM nomenclature is referred to as generating a “b1” datastream. For the radars, these “b1” standards refer to a datastream that has been calibrated (and cross-calibrated), with effort to deliver the highest-quality (well-characterized) data possible. The “b1” radar mentor reporting (this current document) is intended to detail (i) the status/quality of the original “a1” (raw) data sets during the COMBLE AMF campaign, (ii) the corrections and calibrations that are applied to generate the b1 datastreams available on ARM’s Data Discovery, and (iii) the details of the applied methods, e.g., how radar offset/calibration numbers were determined.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Fine Aerosol Acidity and Water during Summer in the Eastern North Atlantic

Aerosol pH governs many important atmospheric processes that occur in the marine boundary layer, including regulating halogen and sulfur chemistries, and nutrient fertilization of surface ocean waters. In this study, we investigated the acidity of PM1 over the eastern North Atlantic during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) aircraft campaign. The ISORROPIA-II thermodynamic model was used to predict PM1 pH and water. We first investigated the sensitivities of PM1 pH and water predictions to gas-phase NH3 and HNO3 concentrations. Our sensitivity analysis indicated that even though NH3 and HNO3 were present at very low concentrations in the eastern North Atlantic during the campaign, PM1 pH calculations can still be sensitive to NH3 concentrations. Specifically, NH3 was needed to constrain the pH of populations of PM1 that had low mass concentrations of NH4+ and non-volatile cations (NVCs). We next assumed that gas-phase NH3 and HNO3 concentrations during the campaign were 0.15 and 0.09 µg m−3, respectively, based on previous measurements conducted in the eastern North Atlantic. Using the assumption that PM1 were internally mixed (i.e., bulk PM1), we determined that PM1 pH ranged from 0.3–8.6, with a mean pH of 5.0 ± 2.3. The pH depended on both Hair+ and Wi. Hair+ was controlled primarily by the NVCs/SO42− molar ratio, while Wi was controlled by the SO42− mass concentration and RH. Changes in pH with altitude were driven primarily by changes in SO42−. Since aerosols in marine atmospheres are rarely internally mixed, the scenario where non-sea salt species and sea-salt species were present in two separate aerosol modes in the PM1 (i.e., completely externally mixed) was also considered. Smaller pH values were predicted for the aerosol mode comprised only of non-sea salt species compared to the bulk PM1 (difference of around 1 unit on average). This was due to the exclusion of sea-salt species (especially hygroscopic alkaline NVCs) in this aerosol mode, which led to increases in Hair+ values and decreases in Wi values. This result demonstrated that assumptions of aerosol mixing states can impact aerosol pH predictions substantially, which will have important implications for evaluating the nature and magnitude of pH-dependent atmospheric processes that occur in the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Observed Relationships Between Cloud Droplet Effective Radius and Biogenic Gas Concentrations in Summertime Marine Stratocumulus Over the Eastern North Atlantic

Abstract Biogenic gases are a prominent component of the summertime marine boundary layer (MBL) over the Eastern North Atlantic. One of these gases, dimethyl sulfide (DMS), can produce sulfate cloud condensation nuclei (CCN) that, in theory, can brighten clouds through photolysis, and produces a reaction product, methane sulfonic acid (MSA). It is also possible that DMS can interact with sea‐salt or other marine aerosols changing their CCN activation spectrum, which could also modify cloud microphysical structure. Data collected aboard the G1 aircraft during the Aerosol Cloud Experiment Eastern North Atlantic (ACE‐ENA) in well‐mixed and decoupled marine boundary layers (MBLs) were used to examine relationships between the cloud droplet effective radii, , and the concentrations of DMS and MSA in constant cloud liquid water content (LWC) bins. A weak but statistically significant negative correlation was observed between CCN concentration and in most LWC bins, regardless of the source of the CCN, while a weak but statistically significant positive correlation between and DMS was observed. No correlation between the cloud droplet number concentration and DMS was found. The presence of MSA indicated that DMS‐to‐sulfate photolysis was likely occurring, but data sparsity prevented a statistically significant conclusion regarding the relationship between MSA and . Data sparsity in decoupled conditions also prevented statistically significant conclusions. To properly address biogenic gas impacts on cloud microphysics, it is recommended that aircraft data be supplemented by long‐term biogenic gas measurements at the surface in marine locations with appropriate remote and in‐situ cloud sensing capabilities, and the analysis limited to well‐mixed MBL's.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

COMBLE ARM Mobile Facility (AMF) Measurements of Ice Nucleating Particles Field Campaign Report

During the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE), a project with the overarching goal to shed light on the dynamics and microphysical properties of clouds and precipitation in the high-latitude marine boundary layer during cold-air outbreaks (CAOs), we were tasked with providing and assisting the collection of aerosol filter samples for measuring ice nucleating particle (INP) concentrations. Little is known about the properties of CAO cloud systems, how they vary with surface, environmental, and aerosol conditions, the role of cold-air outbreaks in the global atmospheric and ocean circulation, and the accuracy of the treatment of this atmospheric regime in climate models. Uncertainties in climate projections for the arctic and sub-arctic region are large, in part due to the lack of observational guidance to constrain the treatment of aerosol-cloud-precipitation linkages in climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Albedo susceptibility of northeastern Pacific stratocumulus: the role of covarying meteorological conditions

Abstract. Quantification of the radiative adjustment of marine low clouds to aerosol perturbations, regionally and globally, remains the largest source of uncertainty in assessing current and future climate. One of the important steps towards quantifying the role of aerosol in modifying cloud radiative properties is to quantify the susceptibility of cloud albedo and liquid water path (LWP) to perturbations in cloud droplet number concentration (Nd). We use 10 years of spaceborne observations from the polar-orbiting Aqua satellite to quantify the albedo susceptibility of marine low clouds to Nd perturbations over the northeast (NE) Pacific stratocumulus (Sc) region. Mutual information analysis reveals a dominating control of cloud state (e.g., LWP and Nd) on low-cloud albedo susceptibility, relative to the meteorological states that drive these cloud states. Through a LWP–Nd space decomposition of albedo susceptibilities, we show clear separation among susceptibility regimes (brightening or darkening), consistent with previously established mechanisms through which aerosol modulates cloud properties. These regimes include (i) thin non-precipitating clouds (LWP < 55 g m−2) that exhibit brightening (occurring 37 % of the time), corresponding to the Twomey effect; (ii) thicker non-precipitating clouds, corresponding to entrainment-driven negative LWP adjustments that manifest as a darkening regime (36 % of the time); and (iii) another brightening regime (22 % of the time) consisting of mostly precipitating clouds, corresponding to precipitation-suppression LWP positive adjustments. Overall, we find an annual-mean regional low-cloud brightening potential of 20.8±2.68 W m−2 ln(Nd)−1, despite an overall negative LWP adjustment for non-precipitating marine stratocumulus, owing to the high occurrence of the Twomey–brightening regime. Over the NE Pacific, clear seasonal covariabilities among meteorological factors related to the large-scale circulation are found to play an important role in grouping conditions favorable for each susceptibility regime. When considering the covarying meteorological conditions, our results indicate that for the northeastern Pacific stratocumulus, clouds that exhibit the strongest brightening potential occur most frequently within shallow marine boundary layers over a cool ocean surface with a stable atmosphere and a dry free troposphere above. Clouds that exhibit a darkening potential associated with negative LWP adjustments occur most frequently within deep marine boundary layers in which the atmospheric instability and the ocean surface are not strong and warm enough to produce frequent precipitation. Cloud brightening associated with warm-rain suppression is found to preferably occur either under unstable atmospheric conditions or humid free-tropospheric conditions that co-occur with a warm ocean surface.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Contrasting characteristics of open- and closed-cellular stratocumulus cloud in the eastern North Atlantic

Abstract. Extensive regions of marine boundary layer cloud impact the radiative balance through their significant shortwave albedo while having little impact on outgoing longwave radiation. Despite this importance, these cloud systems remain poorly represented in large-scale models due to difficulty in representing the processes that drive their life cycle and coverage. In particular, the mesoscale organization and cellular structure of marine boundary clouds have important implications for the subsequent cloud feedbacks. In this study, we use long-term (2013–2018) observations from the Atmospheric Radiation Measurement (ARM) Facility's Eastern North Atlantic (ENA) site on Graciosa Island, Azores, Portugal, to identify cloud cases with open- or closed-cellular organization. More than 500 h of each organization type are identified. The ARM observations are combined with reanalysis and satellite products to quantify the cloud, precipitation, aerosol, thermodynamic, and large-scale synoptic characteristics associated with these cloud types. Our analysis shows that both cloud organization populations occur during similar sea surface temperature conditions, but the open-cell cases are distinguished by stronger cold-air advection and large-scale subsidence compared to the closed-cell cases, consistent with their formation during cold-air outbreaks. We also find that the open-cell cases were associated with deeper boundary layers, stronger low-level winds, and higher rain rates compared to their closed-cell counterparts. Finally, raindrops with diameters larger than 1 mm were routinely recorded at the surface during both populations, with a higher number of large drops during the open-cellular cases. The similarities and differences noted herein provide important insights into the environmental and cloud characteristics during varying marine boundary layer cloud mesoscale organization and will be useful for the evaluation of model simulations for ENA marine clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

New insights on the prevalence of drizzle in marine stratocumulus clouds based on a machine learning algorithm applied to radar Doppler spectra

Abstract. The detection of the early growth of drizzle particles in marine stratocumulus clouds is important for studying the transition from cloud water to rainwater. Radar reflectivity is commonly used to detect drizzle; however, its utility is limited to larger drizzle particles. Alternatively, radar Doppler spectrum skewness has proven to be a more sensitive quantity for the detection of drizzle embryos. Here, a machine learning (ML)-based technique that uses radar reflectivity and skewness for detecting small drizzle particles is presented. Aircraft in situ measurements are used to develop and validate the ML algorithm. The drizzle detection algorithm is applied to three Atmospheric Radiation Measurement (ARM) observational campaigns to investigate the drizzle occurrence in marine boundary layer clouds. It is found that drizzle is far more ubiquitous than previously thought; the traditional radar-reflectivity-based approach significantly underestimates the drizzle occurrence, especially in thin clouds with liquid water paths lower than 50 g m−2. Furthermore, the drizzle occurrence in marine boundary layer clouds differs among the three ARM campaigns, indicating that the drizzle formation, which is controlled by the microphysical process, is regime dependent. A complete understanding of the drizzle distribution climatology in marine stratocumulus clouds calls for more observational campaigns and continuing investigations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Evaluation of four ground-based retrievals of cloud droplet number concentration in marine stratocumulus with aircraft in situ measurements

Abstract. Cloud droplet number concentration (Nd) is crucial for understanding aerosol–cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based Nd retrievals based on comprehensive datasets from the Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The Nd retrieval methods use ARM ENA observatory ground-based remote sensing observations from a micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP (Droplet Number Concentration) value-added product (VAP), all of which also retrieve cloud effective radius (re). The retrievals are compared against aircraft measurements from the fast cloud droplet probe (FCDP) and the cloud and aerosol spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the Nd and cloud re retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to 4 years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that Nd (re) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify Nd retrieval uncertainties and identify reliable Nd retrieval scenarios. Of the retrieval methods, we recommend using the micropulse lidar-based method. This method has good agreement with in situ measurements, less sensitivity to issues arising from precipitation and low cloud LWP and/or optical depth, and broad applicability by functioning for both daytime and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Evaluation of Four Ground-based Retrievals of Cloud Droplet Number Concentration in Marine Stratocumulus with Aircraft In Situ Measurements

Cloud droplet number concentration (N d ) is crucial for understanding aerosol-cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based N d retrievals based on comprehensive datasets from the Atmospheric Radiation Measurements (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The N d retrieval methods use ARM ENA observatory ground-based remote sensing observations from a Micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP Value-added Product (VAP), all of which also retrieve cloud effective radius (r e ). The retrievals are compared against aircraft measurements from the Fast-Cloud Droplet Probe (FCDP) and the Cloud and Aerosol Spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the N d and cloud r e retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to four years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that N d (r e ) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify N d retrieval uncertainties and identify reliable N d retrieval scenarios. Of the retrieval methods, we recommend using the using the Micropulse lidar-based method given its good agreement with in situ measurements, it has less sensitivity to issues arising from precipitation and low cloud LWP/optical depth, and it has broad applicability by functioning for both day and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

54 ENVIRONMENTAL SCIENCES↗