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Title: Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol

Abstract

Abstract. Soot and black carbon (BC) particles are generated in the incomplete combustion of fossil fuels, biomass, and biofuels. These airborne particles affect air quality, human health, aerosol–cloud interactions, precipitation formation, and climate. At present, the climate effects of BC particles are not well understood. Their role in cloud formation is obscured by their chemical and physical variability and by the internal mixing states of these particles with other compounds. Ice nucleation in field studies is often difficult to interpret. Nonetheless, most field studies seem to suggest that BC particles are not efficient ice-nucleating particles (INPs). On the other hand, laboratory measurements show that in some cases, BC particles can be highly active INPs under certain conditions. By working with well-characterized BC particles, our aim is to systematically establish the factors that govern the ice nucleation activity of BC. The current study focuses on laboratory measurements of the effectiveness of BC-containing aerosol in the formation of ice crystals in temperature and ice supersaturation conditions relevant to cirrus clouds. We examine ice nucleation on BC particles under water-subsaturated cirrus cloud conditions, commonly understood as deposition-mode ice nucleation. We study a series of well-characterized commercial carbon black particles with varying morphologies andmore » surface chemistries as well as ethylene flame-generated combustion soot. The carbon black particles used in this study are proxies for atmospherically relevant BC aerosols. These samples were characterized by electron microscopy, mass spectrometry, and optical scattering measurements. Ice nucleation activity was systematically examined in temperature and saturation conditions in the ranges of 217≤T≤235 K and 1.0≤Sice≤1.5 and 0.59≤Swater≤0.98, respectively, using a SPectrometer for Ice Nuclei (SPIN) instrument, which is a continuous-flow diffusion chamber coupled with instrumentation to measure light scattering and polarization. To study the effect of coatings on INPs, the BC-containing particles were coated with organic acids found in the atmosphere, namely stearic acid, cis-pinonic acid, and oxalic acid. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the BC particles. The measured ice nucleation activity dependencies on temperature, supersaturation conditions, and the physicochemical properties of the BC particles are consistent with an ice nucleation mechanism of pore condensation followed by freezing. Coatings and surface oxidation modify the initial formation efficiency of pristine ice crystals on BC-containing aerosol. Depending on the BC material and the coating, both inhibition and enhancement in INP activity were observed. Our measurements at low temperatures complement published data and highlight the capability of some BC particles to nucleate ice under low ice supersaturation conditions. These results are expected to help refine theories relating to soot INP activation in the atmosphere.« less

Authors:
ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo;
Publication Date:
Research Org.:
Boston College, Chestnut Hill, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1568917
Alternate Identifier(s):
OSTI ID: 1802289
Grant/Contract Number:  
SC0011935
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 19 Journal Issue: 19; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Nichman, Leonid, Wolf, Martin, Davidovits, Paul, Onasch, Timothy B., Zhang, Yue, Worsnop, Doug R., Bhandari, Janarjan, Mazzoleni, Claudio, and Cziczo, Daniel J.. Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol. Germany: N. p., 2019. Web. https://doi.org/10.5194/acp-19-12175-2019.
Nichman, Leonid, Wolf, Martin, Davidovits, Paul, Onasch, Timothy B., Zhang, Yue, Worsnop, Doug R., Bhandari, Janarjan, Mazzoleni, Claudio, & Cziczo, Daniel J.. Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol. Germany. https://doi.org/10.5194/acp-19-12175-2019
Nichman, Leonid, Wolf, Martin, Davidovits, Paul, Onasch, Timothy B., Zhang, Yue, Worsnop, Doug R., Bhandari, Janarjan, Mazzoleni, Claudio, and Cziczo, Daniel J.. Tue . "Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol". Germany. https://doi.org/10.5194/acp-19-12175-2019.
@article{osti_1568917,
title = {Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol},
author = {Nichman, Leonid and Wolf, Martin and Davidovits, Paul and Onasch, Timothy B. and Zhang, Yue and Worsnop, Doug R. and Bhandari, Janarjan and Mazzoleni, Claudio and Cziczo, Daniel J.},
abstractNote = {Abstract. Soot and black carbon (BC) particles are generated in the incomplete combustion of fossil fuels, biomass, and biofuels. These airborne particles affect air quality, human health, aerosol–cloud interactions, precipitation formation, and climate. At present, the climate effects of BC particles are not well understood. Their role in cloud formation is obscured by their chemical and physical variability and by the internal mixing states of these particles with other compounds. Ice nucleation in field studies is often difficult to interpret. Nonetheless, most field studies seem to suggest that BC particles are not efficient ice-nucleating particles (INPs). On the other hand, laboratory measurements show that in some cases, BC particles can be highly active INPs under certain conditions. By working with well-characterized BC particles, our aim is to systematically establish the factors that govern the ice nucleation activity of BC. The current study focuses on laboratory measurements of the effectiveness of BC-containing aerosol in the formation of ice crystals in temperature and ice supersaturation conditions relevant to cirrus clouds. We examine ice nucleation on BC particles under water-subsaturated cirrus cloud conditions, commonly understood as deposition-mode ice nucleation. We study a series of well-characterized commercial carbon black particles with varying morphologies and surface chemistries as well as ethylene flame-generated combustion soot. The carbon black particles used in this study are proxies for atmospherically relevant BC aerosols. These samples were characterized by electron microscopy, mass spectrometry, and optical scattering measurements. Ice nucleation activity was systematically examined in temperature and saturation conditions in the ranges of 217≤T≤235 K and 1.0≤Sice≤1.5 and 0.59≤Swater≤0.98, respectively, using a SPectrometer for Ice Nuclei (SPIN) instrument, which is a continuous-flow diffusion chamber coupled with instrumentation to measure light scattering and polarization. To study the effect of coatings on INPs, the BC-containing particles were coated with organic acids found in the atmosphere, namely stearic acid, cis-pinonic acid, and oxalic acid. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the BC particles. The measured ice nucleation activity dependencies on temperature, supersaturation conditions, and the physicochemical properties of the BC particles are consistent with an ice nucleation mechanism of pore condensation followed by freezing. Coatings and surface oxidation modify the initial formation efficiency of pristine ice crystals on BC-containing aerosol. Depending on the BC material and the coating, both inhibition and enhancement in INP activity were observed. Our measurements at low temperatures complement published data and highlight the capability of some BC particles to nucleate ice under low ice supersaturation conditions. These results are expected to help refine theories relating to soot INP activation in the atmosphere.},
doi = {10.5194/acp-19-12175-2019},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 19,
volume = 19,
place = {Germany},
year = {2019},
month = {10}
}

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  • Atmospheric Chemistry and Physics, Vol. 9, Issue 8
  • DOI: 10.5194/acp-9-2805-2009

Global Phase Diagram of Water Confined on the Nanometer Scale
journal, August 2010

  • Kyakuno, Haruka; Matsuda, Kazuyuki; Yahiro, Hitomi
  • Journal of the Physical Society of Japan, Vol. 79, Issue 8
  • DOI: 10.1143/JPSJ.79.083802

Pre-activation of ice-nucleating particles by the pore condensation and freezing mechanism
journal, January 2016

  • Wagner, Robert; Kiselev, Alexei; Möhler, Ottmar
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 4
  • DOI: 10.5194/acp-16-2025-2016

Pore condensation and freezing is responsible for ice formation below water saturation for porous particles
journal, April 2019

  • David, Robert O.; Marcolli, Claudia; Fahrni, Jonas
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 17
  • DOI: 10.1073/pnas.1813647116

Insights into the role of soot aerosols in cirrus cloud formation
journal, January 2007

  • Kärcher, B.; Möhler, O.; DeMott, P. J.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 16
  • DOI: 10.5194/acp-7-4203-2007

Carboxylic acids in the troposphere, occurrence, sources, and sinks: A review
journal, December 1996


Laboratory studies of ice formation via deposition mode nucleation onto mineral dust and n-hexane soot samples
journal, January 2006

  • Kanji, Zamin A.; Abbatt, Jonathan P. D.
  • Journal of Geophysical Research, Vol. 111, Issue D16
  • DOI: 10.1029/2005JD006766

Historical record of carbonaceous particle concentrations from a European high-alpine glacier (Colle Gnifetti, Switzerland)
journal, September 1999

  • Lavanchy, V. M. H.; Gäggeler, H. W.; Schotterer, U.
  • Journal of Geophysical Research: Atmospheres, Vol. 104, Issue D17
  • DOI: 10.1029/1999JD900408

On the role of ice‐nucleating aerosol in the formation of ice particles in tropical mesoscale convective systems
journal, February 2017

  • Ladino, Luis A.; Korolev, Alexei; Heckman, Ivan
  • Geophysical Research Letters, Vol. 44, Issue 3
  • DOI: 10.1002/2016GL072455

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


Pore structure of soot deposits from several combustion sources
journal, October 2000


Adsorption of Gases in Multimolecular Layers
journal, February 1938

  • Brunauer, Stephen; Emmett, P. H.; Teller, Edward
  • Journal of the American Chemical Society, Vol. 60, Issue 2, p. 309-319
  • DOI: 10.1021/ja01269a023

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


Low-Molecular-Weight Dicarboxylic Acids in an Urban and Rural Atmosphere
journal, March 2000


Kinetically controlled glass transition measurement of organic aerosol thin films using broadband dielectric spectroscopy
journal, January 2018

  • Zhang, Yue; Katira, Shachi; Lee, Andrew
  • Atmospheric Measurement Techniques, Vol. 11, Issue 6
  • DOI: 10.5194/amt-11-3479-2018

Dissociative Adsorption of Water at Vacancy Defects in Graphite
journal, December 2007

  • Cabrera-Sanfelix, Pepa; Darling, George R.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 49
  • DOI: 10.1021/jp076241b

Overview of Ice Nucleating Particles
journal, January 2017