Influence of Arctic Microlayers and Algal Cultures on Sea Spray Hygroscopicity and the Possible Implications for Mixed‐Phase Clouds

Christiansen, Sofus; Ickes, Luisa; Bulatovic, Ines; Leck, Caroline; Murray, Benjamin J.; Bertram, A. K.; Wagner, Robert; Gorokhova, Elena; Salter, Matthew; Ekman, Annica M. L.; Bilde, Merete

doi:10.1029/2020jd032808

Cited by 18 publications

(14 citation statements)

References 126 publications

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“…3 show that fresh NaCl particles (a, blue line) are activated slightly earlier (SS crit = 0.32) than fresh sea salt (b, blue line; SS crit = 0.33). The results for fresh NaCl and sea salt are consistent with previously published data of SS crit,NaCl = 0.32–0.33 58 , 59 and SS crit,sea salt = 0.34–0.36 59 , 60 . After three hours of ageing by and UV lights, the SS crit needed to activate the particles is increased for both types of salts reaching values of SS crit = 0.39 (a, red line) and SS crit = 0.41 (b, red line), for NaCl and sea salt, respectively.…”

Section: Resultssupporting

confidence: 92%

The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol

Rosati

Christiansen

Dinesen

et al. 2021

Sci Rep

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Sea spray aerosol (SSA) contributes significantly to natural aerosol particle concentrations globally, in marine areas even dominantly. The potential changes of the omnipresent inorganic fraction of SSA due to atmospheric ageing is largely unexplored. In the atmosphere, SSA may exist as aqueous phase solution droplets or as dried solid or amorphous particles. We demonstrate that ageing of liquid NaCl and artificial sea salt aerosol by exposure to ozone and UV light leads to a substantial decrease in hygroscopicity and cloud activation potential of the dried particles of the same size. The results point towards surface reactions on the liquid aerosols that are more crucial for small particles and the formation of salt structures with water bound within the dried aerosols, termed hydrates. Our findings suggest an increased formation of hydrate forming salts during ageing and the presence of hydrates in dried SSA. Field observations indicate a reduced hygroscopic growth factor of sub-micrometre SSA in the marine atmosphere compared to fresh laboratory generated NaCl or sea salt of the same dry size, which is typically attributed to organic matter or sulphates. Aged inorganic sea salt offers an additional explanation for such a measured reduced hygroscopic growth factor and cloud activation potential.

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Section: Resultssupporting

confidence: 92%

The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol

Rosati

Christiansen

Dinesen

et al. 2021

Sci Rep

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“…The current study is novel in that the aerosolized SML samples were analyzed to determine κ values directly from aerosols generated by SML samples, and it must be noted that the difference in techniques may contribute to different values of κ. To our knowledge, the only previous study on κ values of SML samples was that by Christiansen et al (2020). They report κ values of 1.03-1.16, though these were taken in the Arctic Ocean unlike our own.…”

Section: Ccn Measurementsmentioning

confidence: 73%

“…Rasmussen et al (2017) determined the critical diameters of aerosolized SML to be 70.9 nm at 0.2% SS and 30.6 nm at 0.76% SS. Christiansen et al (2020) found the critical diameters of aerosolized SML to be 100 nm at 0.11% SS and 50 nm at 0.32% SS. The DSML critical diameters ranged from 73.9 ± 5.7 nm at 0.32% SS to 27.9 ± 1.0 nm at 1.24% SS.…”

Section: Ccn Measurementsmentioning

confidence: 96%

“…However, previous studies have also relied on SML samples (Rasmussen et al, 2017;Irish et al, 2019;Christiansen et al, 2020;Ickes et al, 2020;Wolf et al, 2020) and even on surface water samples (Mason et al, 2016;Irish et al, 2017;Wilbourn et al, 2020) to understand the warm and ice cloud nucleating behavior of materials contained in aerosol. Christiansen et al (2020) observed that the CCN activity of SML samples collected in the North Atlantic and Arctic Ocean was the same as artificial seawater containing only salt, within experimental error. Although seawater rather than SML samples were analyzed, Rasmussen et al (2017) did not observe significant changes in CCN properties due to marine organics.…”

Section: Introductionmentioning

confidence: 99%

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Role of Sea Surface Microlayer Properties in Cloud Formation

et al. 2021

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To date, the relative contribution of primary marine organic matter to the subset of atmospheric particles that nucleate cloud droplets is highly uncertain. Here, cloud condensation nuclei (CCN) measurements were conducted on aerosolized sea surface microlayer (SML) samples collected from the North Atlantic Ocean during the NASA North Atlantic Aerosols and Marine Ecosystems Study (NAAMES), κ values were predicted for three representative high molecular weight (HMW) organic components of marine aerosol: 6-glucose, humic acid, and ribulose-1,5-bisphosphate carboxylase/oxygenase (RuBisCO). The predicted κ values for pure organic aerosols varied by only ±0.01 across all of the organics chosen. For the desalted SML samples, calculations assuming an organic composition of entirely RuBisCO provided the closest predicted κ values for the desalted SML samples with a mean κ value of 0.53 ± 0.10. These results indicate that it is the sea salt in the SML which drives the cloud formation potential of marine aerosols. While the presence of organic material from the ocean surface waters may increase aerosol mass due to enrichment processes, cloud formation potential of mixed organic/salt primary marine aerosols will be slightly weakened or unchanged compared to sea spray aerosol.

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“…High concentrations of aerosol particles in the MBL can be formed during NPF events in the FT and subsequently entrained downward into the MBL (Bates et al, 1998a;Clarke et al, 1996Clarke et al, , 2013Korhonen et al, 2008;Pirjola et al, 2000;De Reus et al, 2000;Russell et al, 1998;Thornton et al, 1997;Yoon and Brimblecombe, 2002). The nucleation of new aerosol particles often occurs in the FT owing to the low total condensational sink and cold temperatures (Raes et al, 1997;Yue and Deepak, 1982).…”

Section: Vertical Transportmentioning

confidence: 99%

Measurement report: Cloud Processes and the Transport of Biological Emissions Regulate Southern Ocean Particle and Cloud Condensation Nuclei Concentrations

Sanchez¹,

Roberts²,

Saliba³

et al. 2020

Preprint

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Abstract. 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. 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 course-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution which accounted for 0.07 µm) 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. 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 the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south as well as CCN sources from the mid-latitudes create a latitudinal gradient in CCN concentration with an observed minimum in the SO between 55° S and 60° S. The SOCRATES airborne measurements are not influenced by Australian continental emissions, but still show evidence of elevated CCN concentrations to the south of 60° S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition is observed; more hygroscopic particles to the north, consistent with a greater fraction of sea salt from PMA, and more sulfate and organic particles to the south, which are likely from biogenic sources in coastal Antarctica.

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Influence of Arctic Microlayers and Algal Cultures on Sea Spray Hygroscopicity and the Possible Implications for Mixed‐Phase Clouds

Cited by 18 publications

References 126 publications

The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol

The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol

Role of Sea Surface Microlayer Properties in Cloud Formation

Measurement report: Cloud Processes and the Transport of Biological Emissions Regulate Southern Ocean Particle and Cloud Condensation Nuclei Concentrations

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