Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols

Li, Xiaohan; Wolf, Martin; Shen, Xiaoli; Steinke, Isabelle; Lai, Zhenli; Niu, Sining; China, Swarup; Shrivastava, Manish; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.; Bourg, Ian C.; Cziczo, Daniel J.; Burrows, Susannah M.; Zhang, Yue

doi:10.1021/acs.est.4c06285

Title: Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols

Journal Article · 09 December 2024 · Environmental Science & Technology

DOI: https://doi.org/10.1021/acs.est.4c06285 · OSTI ID:2483758

^[1]; Wolf, Martin ^[2]; Shen, Xiaoli ^[3]; Steinke, Isabelle ^[4];

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^[6];

^[7];

^[1]; Cziczo, Daniel J. ^[3];

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^[5]

Princeton University, NJ (United States)
Yale University, New Haven, CT (United States)
Purdue University, West Lafayette, IN (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Delft University (Netherlands)
Texas A&M University, College Station, TX (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
University of North Carolina at Chapel, NC (United States)

Organic aerosols (OAs) may serve as ice-nucleating particles (INPs), impacting the formation and properties of cirrus clouds when their phase state and viscosity are in the semisolid to glassy range. However, there is a lack of direct parameterization between aerosol viscosity and their ice nucleation capabilities. In this study, we experimentally measured the ice nucleation rate of 2-methyltetrols (2-MT) aerosols, a key component of isoprene-epoxydiol-derived secondary organic aerosols (IEPOX-SOA), at different viscosities. These results demonstrate that the phase state has a significant impact on the ice nucleation abilities of OA under typical cirrus cloud conditions, with the ice nucleation rate increasing by 2 to 3 orders of magnitude when the phase state changes from liquid to semisolid. An innovative parametric model based on classical nucleation theory was developed to directly quantify the impact of viscosity on the heterogeneous nucleation rate. This model accurately represents our laboratory measurement and can be implemented into climate models due to its simple, equation-based form. Based on data collected from the ACRIDICON-CHUVA field campaign, our model predicts that the INP concentration from IEPOX-SOA can reach the magnitude of 1 to tens per liter in the cirrus cloud region impacted by the Amazon rainforest, consistent with recent field observations and estimations. This novel parameterization framework can also be applied in regional and global climate models to further improve representations of cirrus cloud formation and associated climate impacts.

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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); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); Princeton University, NJ (United States); Texas A&M University, College Station, TX (United States)

Sponsoring Organization:: EMSL; National Science Foundation (NSF); U.S. National Science Foundation (NSF); 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), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Grant/Contract Number:: AC05-76RL01830; SC0018419; SC0024034

OSTI ID:: 2483758

Report Number(s):: PNNL-SA-200294

Journal Information:: Environmental Science & Technology, Journal Name: Environmental Science & Technology Journal Issue: 51 Vol. 58; ISSN 1520-5851; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions Li, Ying; Day, Douglas A.; Stark, Harald Atmospheric Chemistry and Physics, Vol. 20, Issue 13 https://doi.org/10.5194/acp-20-8103-2020	journal	January 2020
Ice nucleation on surrogates of boreal forest SOA particles: effect of water content and oxidative age Piedehierro, Ana A.; Welti, André; Buchholz, Angela Atmospheric Chemistry and Physics, Vol. 21, Issue 14 https://doi.org/10.5194/acp-21-11069-2021	journal	January 2021
The contribution of Saharan dust to the ice-nucleating particle concentrations at the High Altitude Station Jungfraujoch (3580 m a.s.l.), Switzerland Brunner, Cyril; Brem, Benjamin T.; Collaud Coen, Martine Atmospheric Chemistry and Physics, Vol. 21, Issue 23 https://doi.org/10.5194/acp-21-18029-2021	journal	December 2021
The seasonal cycle of ice-nucleating particles linked to the abundance of biogenic aerosol in boreal forests Schneider, Julia; Höhler, Kristina; Heikkilä, Paavo Atmospheric Chemistry and Physics, Vol. 21, Issue 5 https://doi.org/10.5194/acp-21-3899-2021	journal	January 2021
Ice-nucleating particles near two major dust source regions Beall, Charlotte M.; Hill, Thomas C. J.; DeMott, Paul J. Atmospheric Chemistry and Physics, Vol. 22, Issue 18 https://doi.org/10.5194/acp-22-12607-2022	journal	September 2022
Predicting atmospheric background number concentration of ice-nucleating particles in the Arctic Li, Guangyu; Wieder, Jörg; Pasquier, Julie T. Atmospheric Chemistry and Physics, Vol. 22, Issue 21 https://doi.org/10.5194/acp-22-14441-2022	journal	November 2022
Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic Knopf, Daniel A.; Charnawskas, Joseph C.; Wang, Peiwen Atmospheric Chemistry and Physics, Vol. 22, Issue 8 https://doi.org/10.5194/acp-22-5377-2022	journal	April 2022
Microphysics of liquid water in sub-10 nm ultrafine aerosol particles Li, Xiaohan; Bourg, Ian C. Atmospheric Chemistry and Physics, Vol. 23, Issue 4 https://doi.org/10.5194/acp-23-2525-2023	journal	February 2023
Organic aerosol and global climate modelling: a review Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N. Atmospheric Chemistry and Physics, Vol. 5, Issue 4 https://doi.org/10.5194/acp-5-1053-2005	journal	January 2005
Some ice nucleation characteristics of Asian and Saharan desert dust Field, P. R.; Möhler, O.; Connolly, P. Atmospheric Chemistry and Physics, Vol. 6, Issue 10 https://doi.org/10.5194/acp-6-2991-2006	journal	January 2006
Efficiency of the deposition mode ice nucleation on mineral dust particles Möhler, O.; Field, P. R.; Connolly, P. Atmospheric Chemistry and Physics, Vol. 6, Issue 10 https://doi.org/10.5194/acp-6-3007-2006	journal	January 2006
The formation, properties and impact of secondary organic aerosol: current and emerging issues Hallquist, M.; Wenger, J. C.; Baltensperger, U. Atmospheric Chemistry and Physics, Vol. 9, Issue 14 https://doi.org/10.5194/acp-9-5155-2009	journal	January 2009
The SPectrometer for Ice Nuclei (SPIN): an instrument to investigate ice nucleation Garimella, Sarvesh; Kristensen, Thomas Bjerring; Ignatius, Karolina Atmospheric Measurement Techniques, Vol. 9, Issue 7 https://doi.org/10.5194/amt-9-2781-2016	journal	January 2016
Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods Petters, M. D.; Kreidenweis, S. M.; Ziemann, P. J. Geoscientific Model Development, Vol. 9, Issue 1 https://doi.org/10.5194/gmd-9-111-2016	journal	January 2016

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54 ENVIRONMENTAL SCIENCES
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