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1. Influences of Recent Particle Formation on Southern Ocean Aerosol Variability and Low Cloud Properties

   https://doi.org/10.1029/2020JD033529  

   McCoy, Isabel L. ; Bretherton, Christopher S. ; Wood, Robert ; Twohy, Cynthia H. ; Gettelman, Andrew ; Bardeen, Charles G. ; Toohey, Darin W. ( April 2021 , Journal of Geophysical Research: Atmospheres)

   Controls on pristine aerosol over the Southern Ocean (SO) are critical for constraining the strength of global aerosol indirect forcing. Observations of summertime SO clouds and aerosols in synoptically varied conditions during the 2018 SOCRATES aircraft campaign reveal novel mechanisms influencing pristine aerosol‐cloud interactions. The SO free troposphere (3–6 km) is characterized by widespread, frequent new particle formation events contributing to much larger concentrations (≥1,000 mg⁻¹) of condensation nuclei (diameters > 0.01 μm) than in typical sub‐tropical regions. Synoptic‐scale uplift in warm conveyor belts and sub‐polar vortices lifts marine biogenic sulfur‐containing gases to free‐tropospheric environments favorable for generating Aitken‐mode aerosol particles (0.01–0.1 μm). Free‐tropospheric Aitken particles subside into the boundary layer, where they grow in size to dominate the sulfur‐based cloud condensation nuclei (CCN) driving SO cloud droplet number concentrations (N_d ∼ 60–100 cm⁻³). Evidence is presented for a hypothesized Aitken‐buffering mechanism which maintains persistently high summertime SON_dagainst precipitation removal through CCN replenishment from activation and growth of boundary layer Aitken particles. Nudged hindcasts from the Community Atmosphere Model (CAM6) are found to underpredict Aitken and accumulation mode aerosols andN_d, impacting summertime cloud brightness and aerosol‐cloud interactions and indicating incomplete representations of aerosol mechanisms associated with ocean biology.

    

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2. African smoke particles act as cloud condensation nuclei in the wintertime tropical North Atlantic boundary layer over Barbados

   https://doi.org/10.17604/drt6-ys34  

   Royer, Haley ; Pöhlker, Mira ; Krueger, Ovid Oktavian ; Blades, Edmund ; Sealy, Peter ; Lata, Nurun Nahar ; Cheng, Zezhen ; China, Swarup ; Ault, Andrew ; Quinn, Patricia ; et al ( January 2023 , University of Miami Libraries)

   The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygrocopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds-Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN Number concentrations as well as the proportions of dust and smoke particles increased, whereas average κ slightly decreased (κ = 0.46 +/- 0.10) from marine background conditions (κ = 0.52 +/- 0.09) when the particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust in CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean. In the file “Dust_Mass_Conc_Royer2022” dust mass concentrations in grams per meter^3 are provided for each day of sampling. These data were used to generate Figure 2a in the manuscript. The file “Particle_Type_#fract_Royer2022” contains data obtained through CCSEM/EDX analysis and used to generate the temporal chemistry plot (Figure 4) provided in the manuscript. The data contains particle numbers for each particle type identified on stage 3 of the sampler, total particle numbers analyzed for the entire stage 3 sample, as well as particle number fractions in % values. In the file “Size-resolved_chem_Royer2022” we provide particle # and number fraction (%) values used to generate size-resolved chemistry plots in the manuscript (Figures 5a and 5b). The file includes all particle numbers and number fractions for sea salt, aged sea salt, dust+sea salt, dust, dust+smoke, smoke, sulfate, and organic particles in each size bin from 0.1 through 8.058 um during cumulative clean marine periods and CAT Event 1 as described in the manuscript. The file “K_at_0.16S_Royer2022” contains κ values calculated at 0.16% supersaturation (S) throughout the entire sampling period. These data were specifically used to generate the plot in Figure 7a. The file “CCN#_at_0.16S_Royer2022” contains cloud condensation nuclei (CCN) values calculated at 0.16% supersaturation (S) throughout the entire sampling period. These data were used to create the CCN portion of the plot in Figure 7b. 

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3. Measurement report: Cloud processes and the transport of biological emissions affect southern ocean particle and cloud condensation nuclei concentrations

   https://doi.org/10.5194/acp-21-3427-2021  

   Sanchez, Kevin J. ; Roberts, Gregory C. ; Saliba, Georges ; Russell, Lynn M. ; Twohy, Cynthia ; Reeves, Michael J. ; Humphries, Ruhi S. ; Keywood, Melita D. ; Ward, Jason P. ; McRobert, Ian M. ( January 2021 , Atmospheric Chemistry and Physics)

   null (Ed.)

   Abstract. Long-range transport of biogenic emissions from the coastof Antarctica, precipitation scavenging, and cloud processing are the mainprocesses that influence the observed variability in Southern Ocean (SO)marine boundary layer (MBL) condensation nuclei (CN) and cloud condensationnuclei (CCN) concentrations during the austral summer. Airborne particlemeasurements on the HIAPER GV from north–south transects between Hobart,Tasmania, and 62∘ S during the Southern Ocean Clouds, RadiationAerosol Transport Experimental Study (SOCRATES) were separated into fourregimes comprising combinations of high and low concentrations of CCN andCN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCNconcentrations were almost always shown to have crossed the Antarctic coast,a location with elevated phytoplankton emissions relative to the rest of theSO in the region south of Australia. The presence of high CCN concentrationswas also consistent with high cloud fractions over their trajectory,suggesting there was substantial growth of biogenically formed particlesthrough cloud processing. Cases with low cloud fraction, due to the presenceof cumulus clouds, had high CN concentrations, consistent with previouslyreported new particle formation in cumulus outflow regions. Measurementsassociated with elevated precipitation during the previous 1.5 d of theirtrajectory had low CCN concentrations indicating CCN were effectivelyscavenged by precipitation. A coarse-mode fitting algorithm was used todetermine the primary marine aerosol (PMA) contribution, which accounted for<20 % of CCN (at 0.3 % supersaturation) and cloud dropletnumber concentrations. Vertical profiles of CN and large particleconcentrations (Dp>0.07 µm) indicated that particleformation occurs more frequently above the MBL; however, the growth ofrecently formed particles typically occurs in the MBL, consistent with cloudprocessing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols,Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean(CAPRICORN-2) campaign were also conducted during the same period as theSOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia,likely due to continental and coastal biogenic emissions. The Antarcticcoastal source of CCN from the south, CCN sources from the midlatitudes, andenhanced precipitation sink in the cyclonic circulation between the Ferreland polar cells (around 60∘ S) create opposing latitudinalgradients in the CCN concentration with an observed minimum in the SObetween 55 and 60∘ S. The SOCRATES airbornemeasurements are not influenced by Australian continental emissions butstill show evidence of elevated CCN concentrations to the south of60∘ S, consistent with biogenic coastal emissions. In addition, alatitudinal gradient in the particle composition, south of the Australianand Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCNspectra and aerosol particle size distribution. The particles are morehygroscopic to the north, consistent with a greater fraction of sea saltfrom PMA, and less hygroscopic to the south as there is more sulfate andorganic particles originating from biogenic sources in coastal Antarctica. 

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4. Impact of Giant Sea Salt Aerosol Particles on Precipitation in Marine Cumuli and Stratocumuli: Lagrangian Cloud Model Simulations

   https://doi.org/10.1175/JAS-D-21-0041.1  

   ( December 2021 , Journal of the Atmospheric Sciences)

   The impact of giant sea salt aerosols released from breaking waves on rain formation in marine boundary layer clouds is studied using large-eddy simulations (LES). We perform simulations of marine cumuli and stratocumuli for various concentrations of cloud condensation nuclei (CCN) and giant CCN (GCCN). Cloud microphysics are modeled with a Lagrangian method that provides key improvements in comparison to previous LES of GCCN that used Eulerian bin microphysics. We find that GCCN significantly increase precipitation in stratocumuli. This effect is strongest for low and moderate CCN concentrations. GCCN are found to have a smaller impact on precipitation formation in cumuli. These conclusions are in agreement with field measurements. We develop a simple parameterization of the effect of GCCN on precipitation, accretion, and autoconversion rates in marine stratocumuli.

   Breaking sea waves release salt particles into the atmosphere. Cloud droplets formed on these salt particles can grow larger than droplets formed on other smaller particles. Therefore, sea salt particles can be important for rain formation over oceans. To investigate this effect, we performed idealized computer simulations of stratocumulus and cumulus clouds. Sea salt particles were modeled with an unprecedented precision thanks to the use of an emerging modeling method. In our simulations sea salt particles significantly enhance rain formation in stratocumuli, but not in cumuli. Our study has implications for climate models, because stratocumuli are important for Earth’s energy budget and for rain enhancement experiments.

    

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5. Insights of warm-cloud biases in Community Atmospheric Model 5 and 6 from the single-column modeling framework and Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) observations

   https://doi.org/10.5194/acp-23-8591-2023  

   Wang, Yuan ; Zheng, Xiaojian ; Dong, Xiquan ; Xi, Baike ; Yung, Yuk L. ( January 2023 , Atmospheric Chemistry and Physics)

   Abstract. There has been a growing concern that most climate models predict precipitation that is too frequent, likely due to lack of reliable subgrid variabilityand vertical variations in microphysical processes in low-level warm clouds.In this study, the warm-cloud physics parameterizations in the singe-columnconfigurations of NCAR Community Atmospheric Model version 6 and 5 (SCAM6and SCAM5, respectively) are evaluated using ground-based and airborneobservations from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the EasternNorth Atlantic (ACE-ENA) field campaign near the Azores islands during2017–2018. The 8-month single-column model (SCM) simulations show that both SCAM6 and SCAM5 cangenerally reproduce marine boundary layer cloud structure, majormacrophysical properties, and their transition. The improvement in warm-cloud properties from the Community Atmospheric Model 5 and 6 (CAM5 to CAM6) physics can be found through comparison with the observations. Meanwhile, both physical schemes underestimate cloud liquidwater content, cloud droplet size, and rain liquid water content butoverestimate surface rainfall. Modeled cloud condensation nuclei (CCN)concentrations are comparable with aircraft-observed ones in the summer but areoverestimated by a factor of 2 in winter, largely due to the biases in thelong-range transport of anthropogenic aerosols like sulfate. We also testthe newly recalibrated autoconversion and accretion parameterizations thataccount for vertical variations in droplet size. Compared to theobservations, more significant improvement is found in SCAM5 than in SCAM6.This result is likely explained by the introduction of subgrid variationsin cloud properties in CAM6 cloud microphysics, which further suppresses thescheme's sensitivity to individual warm-rain microphysical parameters. Thepredicted cloud susceptibilities to CCN perturbations in CAM6 are within areasonable range, indicating significant progress since CAM5 which produces anaerosol indirect effect that is too strong. The present study emphasizes theimportance of understanding biases in cloud physics parameterizations bycombining SCM with in situ observations.

    

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