Impact of dry intrusion events on the composition and mixing state of particles during the winter Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA)
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Published:2021-12-14
Issue:24
Volume:21
Page:18123-18146
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Tomlin Jay M.ORCID, Jankowski Kevin A., Veghte Daniel P., China SwarupORCID, Wang Peiwen, Fraund MatthewORCID, Weis Johannes, Zheng GuangjieORCID, Wang YangORCID, Rivera-Adorno Felipe, Raveh-Rubin ShiraORCID, Knopf Daniel A.ORCID, Wang JianORCID, Gilles Mary K., Moffet Ryan C.ORCID, Laskin AlexanderORCID
Abstract
Abstract. Long-range transport of continental emissions has a far-reaching
influence over remote regions, resulting in substantial change in the size,
morphology, and composition of the local aerosol population and cloud
condensation nuclei (CCN) budget. Here, we investigate the physicochemical
properties of atmospheric particles collected on board a research aircraft
flown over the Azores during the winter 2018 Aerosol and Cloud Experiment in
the Eastern North Atlantic (ACE-ENA) campaign. Particles were collected
within the marine boundary layer (MBL) and free troposphere (FT) after
long-range atmospheric transport episodes facilitated by dry intrusion (DI)
events. Chemical and physical properties of individual particles were
investigated using complementary capabilities of computer-controlled
scanning electron microscopy and X-ray spectromicroscopy to probe particle
external and internal mixing state characteristics. Furthermore, real-time
measurements of aerosol size distribution, cloud condensation nuclei (CCN)
concentration, and back-trajectory calculations were utilized to help bring
into context the findings from offline spectromicroscopy analysis. While
carbonaceous particles were found to be the dominant particle type in the
region, changes in the percent contribution of organics across the particle
population (i.e., external mixing) shifted from 68 % to 43 % in the MBL
and from 92 % to 46 % in FT samples during DI events. This change in
carbonaceous contribution is counterbalanced by the increase in inorganics
from 32 % to 57 % in the MBL and 8 % to 55 % in FT. The
quantification of the organic volume fraction (OVF) of individual particles
derived from X-ray spectromicroscopy, which relates to the multi-component
internal composition of individual particles, showed a factor of 2.06 ± 0.16 and 1.11 ± 0.04 increase in the MBL and FT, respectively, among DI
samples. We show that supplying particle OVF into the κ-Köhler
equation can be used as a good approximation of field-measured in situ CCN
concentrations. We also report changes in the κ values in the MBL from
κMBL, non-DI=0.48 to κMBL, DI=0.41, while changes in the FT result in κFT, non-DI=0.36 to κFT, DI=0.33, which is consistent with enhancements in OVF followed by the DI
episodes. Our observations suggest that entrainment of particles from
long-range continental sources alters the mixing state population and CCN
properties of aerosol in the region. The work presented here provides field
observation data that can inform atmospheric models that simulate sources
and particle composition in the eastern North Atlantic.
Funder
Biological and Environmental Research Israel Science Foundation
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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