Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean

Cheng, Zezhen; Morgenstern, Megan; Henning, Silvia; Zhang, Bo; Roberts, Gregory C.; Fraund, Matthew; Marcus, Matthew A.; Lata, Nurun Nahar; Fialho, Paulo; Mazzoleni, Lynn; Wehner, Birgit; Mazzoleni, Claudio; China, Swarup

doi:10.1016/j.scitotenv.2023.166865

Title: Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean

Journal Article · Sat Sep 09 00:00:00 EDT 2023 · Science of the Total Environment

DOI:https://doi.org/10.1016/j.scitotenv.2023.166865· OSTI ID:2222437

Cheng, Zezhen ^[1]; Morgenstern, Megan ^[2]; Henning, Silvia ^[3]; Zhang, Bo ^[4]; Roberts, Gregory C. ^[5]; Fraund, Matthew ^[6]; Marcus, Matthew A. ^[7]; Lata, Nurun Nahar ^[1]; Fialho, Paulo ^[8]; Mazzoleni, Lynn ^[2];

^[3]; Mazzoleni, Claudio ^[2];

^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)
Michigan Technological Univ., Houghton, MI (United States)
Leibniz Inst. for Tropospheric Research (ITR), Leipzig (Germany)
National Institute for Aerospace, Hampton, VA (United States)
Centre National de la Recherche Scientifique (CNRS) (France); Univ. of Toulouse (France); Univ. of California, San Diego, CA (United States). Scripps Inst. of Oceanography
Sonoma Technology, Inc., Petaluma, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Institute of Volcanology and Risk Assessment (IVAR), Ponta Delgada (Portugal)

Here, this study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud condensation nuclei (CCN) activities of long-range transported free tropospheric (FT) particles. FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) simulations reveal that most air masses that arrived at the OMP during the sampling period originated in North America and were highly aged (average plume age > 10 days). We probed size-resolved chemical composition, mixing state, and hygroscopicity parameter ($$\mathcal{κ}$$) of individual particles using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX). Based on the estimated individual particle mass from elemental composition, we calculated the mixing state index, $$χ$$. During our study, FT particle populations were internally mixed ($$χ$$ of samples are between 53% and 87%), owing to the long atmospheric aging time. We used data from a miniature Cloud Condensation Nucleus Counter (miniCCNC) to derive the hygroscopicity parameter, $$\mathcal{κ}$$_CCNC. Combining $$\mathcal{κ}$$_CCNC and FLEXPART, we found that air masses recirculated above the North Atlantic Ocean with lower mean altitude had higher $$\mathcal{κ}$$_CCNC due to the higher contribution of sea salt particles. We used CCSEM-EDX and phase state measurements to predict single-particle $$\mathcal{κ}$$ ($$\mathcal{κ}$$_CCSEM-EDX) values, which overlap with the lower range of $$\mathcal{κ}$$_CCNC measured below 0.15 % SS. Therefore, CCSEM-EDX measurements can be useful in predicting the lower bound of $$\mathcal{κ}$$, which can be used in climate models to predict CCN activities, especially in remote locations where online CCN measurements are unavailable.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Environmental Molecular Sciences Laboratory (EMSL), Richland, WA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)

Grant/Contract Number:: AC05-76RL01830; AC02-05CH11231; SC0006941; SC0020053; AGS-1110059

OSTI ID:: 2222437

Report Number(s):: PNNL-SA-185635

Journal Information:: Science of the Total Environment, Vol. 904; ISSN 0048-9697

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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The free troposphere as a potential source of arctic boundary layer aerosol particles: Free Troposphere and Boundary Layer Arctic Aerosol Igel, Adele L.; Ekman, Annica M. L.; Leck, Caroline Geophysical Research Letters, Vol. 44, Issue 13 https://doi.org/10.1002/2017GL073808	journal	July 2017
Calibration and measurement uncertainties of a continuous-flow cloud condensation nuclei counter (DMT-CCNC): CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment Rose, D.; Gunthe, S. S.; Mikhailov, E. Atmospheric Chemistry and Physics, Vol. 8, Issue 5 https://doi.org/10.5194/acp-8-1153-2008	journal	January 2008
Physical Properties of Aerosol Internally Mixed With Soot Particles in a Biogenically Dominated Environment in California Sharma, Noopur; China, Swarup; Bhandari, Janarjan Geophysical Research Letters, Vol. 45, Issue 20 https://doi.org/10.1029/2018GL079404	journal	October 2018
Water Vapor Depletion in the DMT Continuous-Flow CCN Chamber: Effects on Supersaturation and Droplet Growth Lathem, Terry L.; Nenes, Athanasios Aerosol Science and Technology, Vol. 45, Issue 5 https://doi.org/10.1080/02786826.2010.551146	journal	March 2011
Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume Dzepina, K.; Mazzoleni, C.; Fialho, P. Atmospheric Chemistry and Physics, Vol. 15, Issue 9 https://doi.org/10.5194/acp-15-5047-2015	journal	January 2015
Size-dependent hygroscopicity parameter ( κ ) and chemical composition of secondary organic cloud condensation nuclei: SIZE-DEPENDENT κ AND COMPOSITION OF SOA Zhao, D. F.; Buchholz, A.; Kortner, B. Geophysical Research Letters, Vol. 42, Issue 24 https://doi.org/10.1002/2015GL066497	journal	December 2015
Organic composition of three different size ranges of aerosol particles over the Southern Ocean Saliba, G.; Sanchez, K. J.; Russell, L. M. Aerosol Science and Technology, Vol. 55, Issue 3 https://doi.org/10.1080/02786826.2020.1845296	journal	December 2020
Improving our fundamental understanding of the role of aerosol−cloud interactions in the climate system Seinfeld, John H.; Bretherton, Christopher; Carslaw, Kenneth S. Proceedings of the National Academy of Sciences, Vol. 113, Issue 21 https://doi.org/10.1073/pnas.1514043113	journal	May 2016
Organic Coating Reduces Hygroscopic Growth of Phase-Separated Aerosol Particles Li, Weijun; Teng, Xiaome; Chen, Xiyao Environmental Science & Technology, Vol. 55, Issue 24 https://doi.org/10.1021/acs.est.1c05901	journal	December 2021
Aerosol Mixing State: Measurements, Modeling, and Impacts Riemer, N.; Ault, A. P.; West, M. Reviews of Geophysics, Vol. 57, Issue 2 https://doi.org/10.1029/2018RG000615	journal	May 2019
The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols Wang, J.; Cubison, M. J.; Aiken, A. C. Atmospheric Chemistry and Physics, Vol. 10, Issue 15 https://doi.org/10.5194/acp-10-7267-2010	journal	January 2010
Establishing the impact of model surfactants on cloud condensation nuclei activity of sea spray aerosol mimics Forestieri, Sara D.; Staudt, Sean M.; Kuborn, Thomas M. Atmospheric Chemistry and Physics, Vol. 18, Issue 15 https://doi.org/10.5194/acp-18-10985-2018	journal	January 2018
Molecular and physical characteristics of aerosol at a remote free troposphere site: implications for atmospheric aging Schum, Simeon K.; Zhang, Bo; Džepina, Katja Atmospheric Chemistry and Physics, Vol. 18, Issue 19 https://doi.org/10.5194/acp-18-14017-2018	journal	January 2018
Long-term trends of black carbon and particle number concentration in the lower free troposphere in Central Europe Sun, Jia; Hermann, Markus; Yuan, Ye Environmental Sciences Europe, Vol. 33, Issue 1 https://doi.org/10.1186/s12302-021-00488-w	journal	April 2021
A large source of cloud condensation nuclei from new particle formation in the tropics Williamson, Christina J.; Kupc, Agnieszka; Axisa, Duncan Nature, Vol. 574, Issue 7778 https://doi.org/10.1038/s41586-019-1638-9	journal	October 2019
Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2 Stohl, A.; Forster, C.; Frank, A. Atmospheric Chemistry and Physics, Vol. 5, Issue 9 https://doi.org/10.5194/acp-5-2461-2005	journal	January 2005
Review of Aerosol–Cloud Interactions: Mechanisms, Significance, and Challenges Fan, Jiwen; Wang, Yuan; Rosenfeld, Daniel Journal of the Atmospheric Sciences, Vol. 73, Issue 11 https://doi.org/10.1175/JAS-D-16-0037.1	journal	November 2016

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