Marine aerosol chemistry gradients: Elucidating primary and secondary processes and fluxes

Čeburnis, Darius; O’Dowd, Colin; Jennings, Gerard; Facchini, M. C.; Emblico, L.; Decesari, Stefano; Fuzzi, S.; Šakalys, J.

doi:10.1029/2008gl033462

Cited by 100 publications

(104 citation statements)

References 14 publications

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“…SC and CR activation curves converge at high s, likely because the WSOC concentration is high enough to notably decrease surface depression, more for organics in SC than for CR (Figure 3). The difference in CCN activity is consistent with studies to date (e.g., [16,56]), showing that hygroscopic components tend to be incorporated in cloud droplets where their less hygroscopic counterparts prefer to remain in the interstitial air. It is also noted that the CR samples excluded droplets <5 μm diameter thus the excluded smaller droplets may potentially contain less hygroscopic materials.…”

Section: Surface Tensionsupporting

confidence: 79%

“…; Table 4), possibly long-chained aliphatic compounds within primary organic matter transferred to the aerosol from bubble bursting at the seawater surface [16,34,54,59,60]. The marine nature of the SC sample is further supported by its inferred surface tension depression (Figure 3, which is remarkably consistent with dissolved organic matter [34].…”

Section: Inferred Molar Volumes and Uncertaintiessupporting

confidence: 64%

“…POMA can exhibit low hygroscopic growth factors but maintain high CCN activity [13] or vice versa [14]. Secondary organic marine aerosol (SOMA) can be produced during cloud processing [15][16][17][18][19]; perhaps the most studied chemical pathway for SOMA is glyoxylic acid oxidation [20] via several aqueous phase intermediates [21][22][23]. Continental biogenic emissions can also contribute to organic mass in marine clouds at high altitudes [24].…”

Section: Introductionmentioning

confidence: 99%

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CCN Properties of Organic Aerosol Collected Below and within Marine Stratocumulus Clouds near Monterey, California

et al. 2015

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Abstract:The composition of aerosol from cloud droplets differs from that below cloud. Its implications for the Cloud Condensation Nuclei (CCN) activity are the focus of this study. Water-soluble organic matter from below cloud, and cloud droplet residuals off the coast of Monterey, California were collected; offline chemical composition, CCN activity and surface tension measurements coupled with Köhler Theory Analysis are used to infer the molar volume and surfactant characteristics of organics in both samples. Based on the surface tension depression of the samples, it is unlikely that the aerosol contains strong surfactants. The activation kinetics for all samples examined are consistent with rapid (NH4)2SO4 calibration aerosol. This is consistent with our current understanding of droplet kinetics for ambient CCN. However, the carbonaceous material in cloud drop residuals is OPEN ACCESSAtmosphere 2015, 6 1591 far more hygroscopic than in sub-cloud aerosol, suggestive of the impact of cloud chemistry on the hygroscopic properties of organic matter.

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Section: Surface Tensionsupporting

confidence: 79%

Section: Inferred Molar Volumes and Uncertaintiessupporting

confidence: 64%

Section: Introductionmentioning

confidence: 99%

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CCN Properties of Organic Aerosol Collected Below and within Marine Stratocumulus Clouds near Monterey, California

et al. 2015

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“…The same authors also reported the results of principal component analysis, eddy-correlation flux measurements and Aerosol Mass Spectrometry gradient measurements, confirming a very low contribution of the shoreline to aerosol number concentration at Mace Head. In a subsequent experiment, Ceburnis et al (2008) estimated that coastal-generated aerosol might contribute between 5-20% of the aerosol particle mass concentration at Mace Head in the 3-30 m surface layer, but argued that the effect on chemical composition and subsequent chemical fluxes was not significant.…”

Section: Introductionmentioning

confidence: 99%

On the representativeness of coastal aerosol studies to open ocean studies: Mace Head – a case study

et al. 2009

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Abstract.A unique opportunity arose during the MAP project to compare open ocean aerosol measurements with those undertaken at the Mace Head Global Atmosphere Watch Station, a station used for decades for aerosol process research and long-term monitoring. The objective of the present study is to demonstrate that the key aerosol features and processes observed at Mace Head are characteristic of the open ocean, while acknowledging and allowing for spatial and temporal gradients. Measurements were conducted for a 5-week period at Mace Head and offshore, on the Research Vessel Celtic Explorer, in generally similar marine air masses, albeit not in connected-flow scenarios. The results of the study indicate, in terms of aerosol number size distribution, higher nucleation mode particle concentrations at Mace Head than offshore, pointing to a strong coastal source of new particles that is not representative of the open ocean. The Aitken mode exhibited a large degree of similarity, with no systematic differences between Mace Head and the open ocean, while the accumulation mode showed averagely 35% higher concentrations at Mace Head. The higher accumulation mode concentration can be attributed equally to cloud processing and to a coastal enhancement in concentration. Chemical analysis showed similar or even higher offshore concentrations for dominant species, such as nss-SO −2 4 , WSOC, WIOC and MSA. Sea salt concentration differences determined a 40% higher supermicron mass at Mace Head, although this difference can be attributed to a higher Correspondence to: M. Rinaldi (m.rinaldi@isac.cnr.it) wind speed at Mace Head during the comparison period. Moreover, the relative chemical composition as a function of size illustrated remarkable similarity. While differences to varying degrees were observed between offshore and coastal measurements, no convincing evidence was found of local coastal effects, apart from nucleation mode aerosol, thus confirming the integrity of previously reported marine aerosol characterisation studies at Mace Head.

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“…This result may suggest a minor contribution of water-soluble organic matter in summer due to a negligible contribution of aged continental air masses and/or significant contribution from marine biota. Based on the gradient flux measurements, Ceburnis et al (2008) found that water-insoluble organic matter (WIOM) exhibited an upward flux, whereas water-soluble organic matter (WSOM) exhibited a downward flux, suggesting a primary production for WIOM and a secondary formation for WSOM. In this study, WIOM/WSOM ratios were higher in summer (mean: 1.45 ± 0.17) and autumn (0.35 ± 0.57) than in winter (0.19 ± 0.67) as shown in Fig.…”

Section: Monthly/seasonal Variationsmentioning

confidence: 99%

Long-term (2001–2012) trends of carbonaceous aerosols from a remote island in the western North Pacific: an outflow region of Asian pollutants

2018

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Abstract. The present study reports on long-term trends of carbonaceous aerosols in total suspended particulate (TSP) samples collected at Chichijima in the western North Pacific during [2001][2002][2003][2004][2005][2006][2007][2008][2009][2010][2011][2012]. Seasonal variations of elemental carbon (EC), organic carbon (OC), and water-soluble organic carbon (WSOC) concentrations showed maxima in winter to spring and minima in summer. These seasonal differences in the concentrations of carbonaceous aerosols were associated with the outflows of polluted air masses from East Asia, which are clearly distinguishable from pristine air masses from the central Pacific. The higher concentrations of carbonaceous aerosols during winter to spring are associated with long-range atmospheric transport of East Asian continental polluted air masses, whereas lower concentrations may be due to pristine air masses from the central Pacific in summer. The annual trends of OC / EC (+0.46 % yr −1 ), WSOC (+0.18 % yr −1 ) and WSOC / OC (+0.08 % yr −1 ) showed significant (p < 0.05) increases during the period of 2001-2012, suggesting that photochemical formation of WSOC and its contributions to secondary organic aerosols (SOAs) have increased over the western North Pacific via long-range atmospheric transport. We found a significant increase (+0.33 % yr −1 ) in nss-K + / EC ratios, demonstrating that concentrations of biomass-burning-derived carbonaceous aerosols have increased, while those of primary fossilfuel-derived aerosols have decreased over the western North Pacific. Further, secondary biogenic emissions are also important over the western North Pacific as inferred from a significant increase (+0.14 % yr −1 ) in the concentrations of methanesulfonate (MSA − , a tracer for biogenic sources). This point was further supported by a moderate correlation (r = 0.40) between WSOC and MSA − . We also found a significant increase in OC / TC (total carbon) and WSOC / TC ratios, further suggesting that photochemical formation of WSOC and its contributions to SOAs have increased over the western North Pacific during 2001-2012 via long-range atmospheric transport from East Asia.

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Marine aerosol chemistry gradients: Elucidating primary and secondary processes and fluxes

Cited by 100 publications

References 14 publications

CCN Properties of Organic Aerosol Collected Below and within Marine Stratocumulus Clouds near Monterey, California

CCN Properties of Organic Aerosol Collected Below and within Marine Stratocumulus Clouds near Monterey, California

On the representativeness of coastal aerosol studies to open ocean studies: Mace Head – a case study

Long-term (2001–2012) trends of carbonaceous aerosols from a remote island in the western North Pacific: an outflow region of Asian pollutants

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