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Title: Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic

Abstract

Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as lowmore » as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.« less

Authors:
ORCiD logo; ; ; ; ORCiD logo; ; ; ; ORCiD logo; ORCiD logo; ORCiD logo; ; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States); Purdue Univ., West Lafayette, IN (United States); Washington Univ., St. Louis, MO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Contributing Org.:
Pacific Northwest National Laboratory (PNNL); Brookhaven National Laboratory (BNL); Argonne National Laboratory (ANL); Oak Ridge National Laboratory (ORNL)
OSTI Identifier:
1864608
Alternate Identifier(s):
OSTI ID: 1864673; OSTI ID: 1866745; OSTI ID: 1869781; OSTI ID: 1958531
Report Number(s):
PNNL-SA-169941
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0016370; SC0021034; SC0018948; SC0020259; AC05-76RL01830; AC02-05CH11231; SC002025
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 22 Journal Issue: 8; Journal ID: ISSN 1680-7324
Publisher:
Copernicus GmbH
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; aerosol, ice nucleation

Citation Formats

Knopf, Daniel A., Charnawskas, Joseph C., Wang, Peiwen, Wong, Benny, Tomlin, Jay M., Jankowski, Kevin A., Fraund, Matthew, Veghte, Daniel P., China, Swarup, Laskin, Alexander, Moffet, Ryan C., Gilles, Mary K., Aller, Josephine Y., Marcus, Matthew A., Raveh-Rubin, Shira, and Wang, Jian. Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic. Germany: N. p., 2022. Web. doi:10.5194/acp-22-5377-2022.
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Knopf, Daniel A., Charnawskas, Joseph C., Wang, Peiwen, Wong, Benny, Tomlin, Jay M., Jankowski, Kevin A., Fraund, Matthew, Veghte, Daniel P., China, Swarup, Laskin, Alexander, Moffet, Ryan C., Gilles, Mary K., Aller, Josephine Y., Marcus, Matthew A., Raveh-Rubin, Shira, & Wang, Jian. Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic. Germany. https://doi.org/10.5194/acp-22-5377-2022
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Knopf, Daniel A., Charnawskas, Joseph C., Wang, Peiwen, Wong, Benny, Tomlin, Jay M., Jankowski, Kevin A., Fraund, Matthew, Veghte, Daniel P., China, Swarup, Laskin, Alexander, Moffet, Ryan C., Gilles, Mary K., Aller, Josephine Y., Marcus, Matthew A., Raveh-Rubin, Shira, and Wang, Jian. Mon . "Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic". Germany. https://doi.org/10.5194/acp-22-5377-2022.
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@article{osti_1864608,
title = {Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic},
author = {Knopf, Daniel A. and Charnawskas, Joseph C. and Wang, Peiwen and Wong, Benny and Tomlin, Jay M. and Jankowski, Kevin A. and Fraund, Matthew and Veghte, Daniel P. and China, Swarup and Laskin, Alexander and Moffet, Ryan C. and Gilles, Mary K. and Aller, Josephine Y. and Marcus, Matthew A. and Raveh-Rubin, Shira and Wang, Jian},
abstractNote = {Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.},
doi = {10.5194/acp-22-5377-2022},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 8,
volume = 22,
place = {Germany},
year = {Mon Apr 25 00:00:00 EDT 2022},
month = {Mon Apr 25 00:00:00 EDT 2022}
}
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Morphology and mixing of black carbon particles collected in central California during the CARES field study
journal, January 2016

  • Moffet, Ryan C.; O'Brien, Rachel E.; Alpert, Peter A.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 22
  • DOI: 10.5194/acp-16-14515-2016

Biological Impacts on Carbon Speciation and Morphology of Sea Spray Aerosol
journal, October 2017

Ice Nucleating Activity and Residual Particle Morphology of Bulk Seawater and Sea Surface Microlayer
journal, July 2021

Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K: ICE NUCLEATION BY ATMOSPHERIC PARTICLES
journal, September 2012

  • Wang, Bingbing; Laskin, Alexander; Roedel, Tobias
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D21
  • DOI: 10.1029/2012JD017446

Sea spray aerosol as a unique source of ice nucleating particles
journal, December 2015

  • DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 21
  • DOI: 10.1073/pnas.1514034112

Stimulation of ice nucleation by marine diatoms
journal, December 2010

  • Knopf, D. A.; Alpert, P. A.; Wang, B.
  • Nature Geoscience, Vol. 4, Issue 2
  • DOI: 10.1038/ngeo1037

A Dynamic Link between Ice Nucleating Particles Released in Nascent Sea Spray Aerosol and Oceanic Biological Activity during Two Mesocosm Experiments
journal, January 2017

  • McCluskey, Christina S.; Hill, Thomas C. J.; Malfatti, Francesca
  • Journal of the Atmospheric Sciences, Vol. 74, Issue 1
  • DOI: 10.1175/JAS-D-16-0087.1

Sea Spray Aerosol: The Chemical Link between the Oceans, Atmosphere, and Climate
journal, March 2017

  • Cochran, Richard E.; Ryder, Olivia S.; Grassian, Vicki H.
  • Accounts of Chemical Research, Vol. 50, Issue 3
  • DOI: 10.1021/acs.accounts.6b00603

Aerosol Composition, Mixing State, and Phase State of Free Tropospheric Particles and Their Role in Ice Cloud Formation
journal, November 2021

The Arm Climate Research Facility: A Review of Structure and Capabilities
journal, March 2013

  • Mather, James H.; Voyles, Jimmy W.
  • Bulletin of the American Meteorological Society, Vol. 94, Issue 3
  • DOI: 10.1175/BAMS-D-11-00218.1

Size-resolved characterization of the polysaccharidic and proteinaceous components of sea spray aerosol
journal, April 2017

Development of Heterogeneous Ice Nucleation Rate Coefficient Parameterizations From Ambient Measurements
journal, November 2021

  • Cornwell, Gavin C.; McCluskey, Christina S.; DeMott, Paul J.
  • Geophysical Research Letters, Vol. 48, Issue 23
  • DOI: 10.1029/2021GL095359

Heterogeneous nucleation of ice on anthropogenic organic particles collected in Mexico City: ICE NUCLEATION ON ANTHROPOGENIC AEROSOL
journal, June 2010

  • Knopf, D. A.; Wang, B.; Laskin, A.
  • Geophysical Research Letters, Vol. 37, Issue 11
  • DOI: 10.1029/2010GL043362

Deposition nucleation viewed as homogeneous or immersion freezing in pores and cavities
journal, January 2014

Soft X-ray microscopy and spectroscopy at the molecular environmental science beamline at the Advanced Light Source
journal, February 2006

  • Bluhm, H.; Andersson, K.; Araki, T.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 150, Issue 2-3
  • DOI: 10.1016/j.elspec.2005.07.005

Acidity across the interface from the ocean surface to sea spray aerosol
journal, December 2020

  • Angle, Kyle J.; Crocker, Daniel R.; Simpson, Rebecca M. C.
  • Proceedings of the National Academy of Sciences, Vol. 118, Issue 2
  • DOI: 10.1073/pnas.2018397118

Size-Dependent Changes in Sea Spray Aerosol Composition and Properties with Different Seawater Conditions
journal, May 2013

  • Ault, Andrew P.; Moffet, Ryan C.; Baltrusaitis, Jonas
  • Environmental Science & Technology, Vol. 47, Issue 11
  • DOI: 10.1021/es400416g

Heterogeneous nucleation of ice on surrogates of mineral dust
journal, January 2006

  • Knopf, Daniel A.; Koop, Thomas
  • Journal of Geophysical Research, Vol. 111, Issue D12
  • DOI: 10.1029/2005JD006894

Automated Single-Particle SEM/EDX Analysis of Submicrometer Particles down to 0.1 μm
journal, January 2001

  • Laskin, Alexander; Cowin, James P.
  • Analytical Chemistry, Vol. 73, Issue 5
  • DOI: 10.1021/ac0009604

Pre-activation of aerosol particles by ice preserved in pores
journal, January 2017

Overview of Ice Nucleating Particles
journal, January 2017

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