More Like this

1. Cloud Processes and the Transport of Biological Emissions Regulate Southern Ocean Particle and Cloud Condensation Nuclei Concentrations

   Sanchez, K. J.; Roberts, G. C.; Saliba, G.; Russell, L. M.; Twohy, C.; Reeves, M.; Humphries, R. S.; Keywood, M. D.; Ward, J. P.; McRobert, I. M. (January 2021, Atmospheric chemistry and physics)

   null (Ed.)

   Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north-south transects between Hobart, Tasmania and 62°S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5-day HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO in the region south of Australia. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5-days of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A coarse-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution which accounted for < 20% of CCN (at 0.3% supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations (Dp > 0.07µm) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. 

   more » « less
2. 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. 

   more » « less
3. Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements

   https://doi.org/10.5194/acp-23-10713-2023  

   Zhang, Chupeng; Hai, Shangfei; Gao, Yang; Wang, Yuhang; Zhang, Shaoqing; Sheng, Lifang; Zhao, Bin; Wang, Shuxiao; Jiang, Jingkun; Huang, Xin; et al (January 2023, Atmospheric Chemistry and Physics)

   Abstract. New particle formation (NPF) and subsequent particle growth are importantsources of condensation nuclei (CN) and cloud condensation nuclei (CCN).While many observations have shown positive contributions of NPF to CCN atlow supersaturation, negative NPF contributions were often simulated inpolluted environments. Using the observations in a coastal city of Qingdao,Beijing, and Gucheng in north China, we thoroughly evaluate the simulatednumber concentrations of CN and CCN using an NPF-explicit parameterizationembedded in the WRF-Chem model. For CN, the initial simulation shows largebiases of particle number concentrations at 10–40 and 40–100 nm. Byadjusting the process of gas–particle partitioning, including the massaccommodation coefficient (MAC) of sulfuric acid, the phase changes in primary organic aerosol emissions, and the condensational amount of nitric acid, the improvement of the particle growth process yields substantially reduced overestimation of CN. Regarding CCN, secondary organic aerosol (SOA) formed from the oxidation of semi-volatile and intermediate-volatility organic compounds (S/IVOCs) is called SI-SOA, the yield of which is an important contributor. At default settings, the SI-SOA yield is too high without considering the differences in precursor oxidation rates. Lowering the SI-SOA yield under linear H2SO4 nucleation scheme results in much-improved CCN simulations compared to observations. On the basis of the bias-corrected model, we find substantially positive contributions of NPF to CCN at low supersaturation (∼ 0.2 %) over broad areas of China, primarily due to competing effects of increasing particle hygroscopicity, a result of reductions in SI-SOA amount, surpassing that of particle size decreases. The bias-corrected model is robustly applicable to other schemes, such as the quadratic H2SO4 nucleation scheme, in terms of CN and CCN, though the dependence of CCN on SI-SOA yield is diminished likely due to changes in particle composition. This study highlights potentially much larger NPF contributions to CCN on a regional and even global basis. 

   more » « less
4. 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. 

   more » « less
5. Ion-induced cloud modulation through new particle formation and runaway cloud condensation nuclei production

   https://doi.org/10.1093/oxfclm/kgae018  

   Chandrakar, Kamal_Kant; Cantrell, Will; Shaw, Raymond_A (September 2024, Oxford Open Climate Change)

   Abstract Cloud formation in the Pi Convection–Cloud Chamber is achieved via ionization in humid conditions, without the injection of aerosol particles to serve as cloud condensation nuclei (CCN). Abundant ions, turbulence, and supersaturated water vapor combine to produce new particles, which grow to become CCN sized and eventually are activated to form clouds. Coupling between the new particle formation and cloud droplets causes predator-prey type oscillations in aerosol and droplet concentrations under turbulent conditions. Leading terms are identified in the budgets for Aitken and accumulation mode aerosols and for cloud droplets. The cloud coupling is proposed to be a result of cloud-induced runaway CCN production through aerosol scavenging. The experiments suggest potential applications to marine cloud brightening, in which ions rather than sea-salt aerosols are generated. 

   more » « less