Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

Knopf, Daniel A.; Wang, Peiwen; Wong, Benny; Tomlin, Jay M.; Veghte, Daniel P.; Lata, Nurun N.; China, Swarup; Laskin, Alexander; Moffet, Ryan C.; Aller, Josephine Y.; Marcus, Matthew A.; Wang, Jian

doi:10.5194/acp-23-8659-2023

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

Journal Article · Tue Aug 08 00:00:00 EDT 2023 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-23-8659-2023· OSTI ID:1994225

; Wang, Peiwen; Wong, Benny; ; Veghte, Daniel P.; Lata, Nurun N.; ; ; ; Aller, Josephine Y.; Marcus, Matthew A.;

Abstract. Atmospheric ice nucleation impacts the hydrological cycle and climate by modifying the radiative properties of clouds. To improve our predictive understanding of ice formation, ambient ice-nucleating particles (INPs) need to be collected and characterized. Measurements of INPs at lower latitudes in a remote marine region are scarce. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign, in the region of the Azores islands, provided the opportunity to collect particles in the marine boundary layer (MBL) and free troposphere (FT) by aircraft during the campaign's summer and winter intensive operation period. The particle population in samples collected was examined by scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy. The identified INPs were analyzed by scanning electron microscopy with energy-dispersive X-ray analysis. We observed differences in the particle population characteristics in terms of particle diversity, mixing state, and organic volume fraction between seasons, mostly due to dry intrusion events during winter, as well as between the sampling locations of the MBL and FT. These differences are also reflected in the temperature and humidity conditions under which water uptake, immersion freezing (IMF), and deposition ice nucleation (DIN) proceed. Identified INPs reflect typical particle types within the particle population on the samples and include sea salt, sea salt with sulfates, and mineral dust, all associated with organic matter, as well as carbonaceous particles. IMF and DIN kinetics are analyzed with respect to heterogeneous ice nucleation rate coefficients, Jhet, and ice nucleation active site density, ns, as a function of the water criterion Δaw. DIN is also analyzed in terms of contact angles following classical nucleation theory. Derived MBL IMF kinetics agree with previous ACE-ENA ground-site INP measurements. FT particle samples show greater ice nucleation propensity compared to MBL particle samples. This study emphasizes that the types of INPs can vary seasonally and with altitude depending on sampling location, thereby showing different ice nucleation propensities, which is crucial information when representing mixed-phase cloud and cirrus cloud microphysics in models.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Stony Brook University, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Contributing Organization:: Argonne National Laboratory (ANL); Brookhaven National Laboratory (BNL); Oak Ridge National Laboratory (ORNL); Pacific Northwest National Laboratory (PNNL)

Grant/Contract Number:: AC02-05CH11231; AC05-76RL01830; SC0016370; SC0020259; SC0021017; SC0021034; SC0021977

OSTI ID:: 1994225

Alternate ID(s):: OSTI ID: 1994253
OSTI ID: 1994254
OSTI ID: 1994819
OSTI ID: 1996761

Report Number(s):: PNNL-SA-183695

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 15 Vol. 23; ISSN 1680-7324

Publisher:: Copernicus GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

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54 ENVIRONMENTAL SCIENCES
aerosol
ice nucleation

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

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