Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles
Abstract
Recent observational studies suggest that nucleation-scavenging is the principal path to removing black carbon-containing aerosol from the atmosphere, thus affecting black carbon’s lifetime and radiative forcing. Modeling the process of nucleation-scavenging is challenging, since black carbon (BC) forms complex internal mixtures with other aerosol species. Here, we examined the impacts of black carbon mixing state on nucleation scavenging using the particle-resolved aerosol model PartMC-MOSAIC. This modeling approach has the unique advantage that complex aerosol mixing states can be represented on a per-particle level. For a scenario library that comprised hundreds of diverse aerosol populations, we quantified nucleation-scavenged BC mass fractions. Consistent with measurements, these vary widely, depending on the amount of BC, the amount of coating and coating material, as well as the environmental supersaturation. We quantified the error in the nucleation-scavenged black carbon mass fraction introduced when assuming an internally mixed distribution, and determined its bounds depending on environmental supersaturation and on the aerosol mixing state index χ . For a given χ value, the error decreased at higher supersaturations. For more externally mixed populations (χ <20%), the nucleation-scavenged BC mass fraction could be overestimated by more than 1000% at supersaturations of 0.1%, while for more internally mixed populationsmore »
- Authors:
-
- Meteorological Research Inst. (MRI), Tsukuba (Japan)
- Univ. of Illinois, Urbana-Champaign, IL (United States)
- Publication Date:
- Research Org.:
- Univ. of Illinois at Urbana-Champaign, IL (United States)
- Sponsoring Org.:
- USDOE Atmospheric System Research (ASR)
- OSTI Identifier:
- 1501893
- Grant/Contract Number:
- SC0011771
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Atmosphere (Basel)
- Additional Journal Information:
- Journal Name: Atmosphere (Basel); Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2073-4433
- Publisher:
- MDPI
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; black carbon; nucleation-scavenging; aerosol mixing state; cloud microphysics; particle-resolved model
Citation Formats
Ching, Joseph, West, Matthew, and Riemer, Nicole. Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles. United States: N. p., 2018.
Web. doi:10.3390/atmos9010017.
Ching, Joseph, West, Matthew, & Riemer, Nicole. Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles. United States. https://doi.org/10.3390/atmos9010017
Ching, Joseph, West, Matthew, and Riemer, Nicole. Thu .
"Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles". United States. https://doi.org/10.3390/atmos9010017. https://www.osti.gov/servlets/purl/1501893.
@article{osti_1501893,
title = {Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles},
author = {Ching, Joseph and West, Matthew and Riemer, Nicole},
abstractNote = {Recent observational studies suggest that nucleation-scavenging is the principal path to removing black carbon-containing aerosol from the atmosphere, thus affecting black carbon’s lifetime and radiative forcing. Modeling the process of nucleation-scavenging is challenging, since black carbon (BC) forms complex internal mixtures with other aerosol species. Here, we examined the impacts of black carbon mixing state on nucleation scavenging using the particle-resolved aerosol model PartMC-MOSAIC. This modeling approach has the unique advantage that complex aerosol mixing states can be represented on a per-particle level. For a scenario library that comprised hundreds of diverse aerosol populations, we quantified nucleation-scavenged BC mass fractions. Consistent with measurements, these vary widely, depending on the amount of BC, the amount of coating and coating material, as well as the environmental supersaturation. We quantified the error in the nucleation-scavenged black carbon mass fraction introduced when assuming an internally mixed distribution, and determined its bounds depending on environmental supersaturation and on the aerosol mixing state index χ . For a given χ value, the error decreased at higher supersaturations. For more externally mixed populations (χ <20%), the nucleation-scavenged BC mass fraction could be overestimated by more than 1000% at supersaturations of 0.1%, while for more internally mixed populations (χ >75%), the error was below 100% for the range of supersaturations (from 0.02% to 1%) investigated here. Thus, accounting for black carbon mixing state and knowledge of the supersaturation of the environment are crucial when determining the amount of black carbon that can be incorporated into clouds.},
doi = {10.3390/atmos9010017},
journal = {Atmosphere (Basel)},
number = 1,
volume = 9,
place = {United States},
year = {Thu Jan 11 00:00:00 EST 2018},
month = {Thu Jan 11 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Can Reducing Black Carbon Emissions Counteract Global Warming?
journal, August 2005
- Bond, Tami C.; Sun, Haolin
- Environmental Science & Technology, Vol. 39, Issue 16
Black carbon mixing state impacts on cloud microphysical properties: Effects of aerosol plume and environmental conditions: IMPACTS OF BC MIXING STATE ON CLOUDS
journal, May 2016
- Ching, J.; Riemer, N.; West, M.
- Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 10
Radiative forcing and climate response
journal, March 1997
- Hansen, J.; Sato, M.; Ruedy, R.
- Journal of Geophysical Research: Atmospheres, Vol. 102, Issue D6
Explaining variance in black carbon's aging timescale
journal, January 2015
- Fierce, L.; Riemer, N.; Bond, T. C.
- Atmospheric Chemistry and Physics, Vol. 15, Issue 6
Black carbon (BC) in alpine aerosols and cloud water—concentrations and scavenging efficiencies
journal, October 2001
- Hitzenberger, R.; Berner, A.; Giebl, H.
- Atmospheric Environment, Vol. 35, Issue 30
A key process controlling the wet removal of aerosols: new observational evidence
journal, October 2016
- Ohata, Sho; Moteki, Nobuhiro; Mori, Tatsuhiro
- Scientific Reports, Vol. 6, Issue 1
Metrics to quantify the importance of mixing state for CCN activity
journal, January 2017
- Ching, Joseph; Fast, Jerome; West, Matthew
- Atmospheric Chemistry and Physics, Vol. 17, Issue 12
Wet removal of black carbon in Asian outflow: Aerosol Radiative Forcing in East Asia (A-FORCE) aircraft campaign: REMOVAL OF BLACK CARBON
journal, February 2012
- Oshima, N.; Kondo, Y.; Moteki, N.
- Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D3
Quantifying aerosol mixing state with entropy and diversity measures
journal, January 2013
- Riemer, N.; West, M.
- Atmospheric Chemistry and Physics, Vol. 13, Issue 22
Enhanced haze pollution by black carbon in megacities in China
journal, March 2016
- Ding, A. J.; Huang, X.; Nie, W.
- Geophysical Research Letters, Vol. 43, Issue 6
Will black carbon mitigation dampen aerosol indirect forcing?: BLACK CARBON MITIGATION
journal, May 2010
- Chen, W. -T.; Lee, Y. H.; Adams, P. J.
- Geophysical Research Letters, Vol. 37, Issue 9
Simulating the evolution of soot mixing state with a particle‐resolved aerosol model
journal, January 2009
- Riemer, N.; West, M.; Zaveri, R. A.
- Journal of Geophysical Research, Vol. 114, Issue D9
Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects
journal, November 2005
- Pöschl, Ulrich
- Angewandte Chemie International Edition, Vol. 44, Issue 46
Vertical Profiles of Aerosol and Radiation and the Influence of a Temperature Inversion: Measurements and Radiative Transfer Calculations
journal, October 1996
- Wendisch, M.; Mertes, S.; Ruggaber, A.
- Journal of Applied Meteorology, Vol. 35, Issue 10
Toward Reduced Representation of Mixing State for Simulating Aerosol Effects on Climate
journal, May 2017
- Fierce, Laura; Riemer, Nicole; Bond, Tami C.
- Bulletin of the American Meteorological Society, Vol. 98, Issue 5
Reduction of Tropical Cloudiness by Soot
journal, May 2000
- Ackerman, A. S.
- Science, Vol. 288, Issue 5468
Simulating aerosol chamber experiments with the particle-resolved aerosol model PartMC
journal, March 2017
- Tian, J.; Brem, B. T.; West, M.
- Aerosol Science and Technology, Vol. 51, Issue 7
Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch
journal, January 2007
- Cozic, J.; Verheggen, B.; Mertes, S.
- Atmospheric Chemistry and Physics, Vol. 7, Issue 7
Seasonal variation of the atmospheric aerosol near the top of the marine boundary layer over Spitsbergen related to the Arctic sulphur cycle
journal, January 1994
- Heintzenberg, Jost; Leck, Caroline
- Tellus B: Chemical and Physical Meteorology, Vol. 46, Issue 1
Modeling the formation of secondary organic aerosol within a comprehensive air quality model system
journal, November 2001
- Schell, Benedikt; Ackermann, Ingmar J.; Hass, Heinz
- Journal of Geophysical Research: Atmospheres, Vol. 106, Issue D22
The MESSy aerosol submodel MADE3 (v2.0b): description and a box model test
journal, January 2014
- Kaiser, J. C.; Hendricks, J.; Righi, M.
- Geoscientific Model Development, Vol. 7, Issue 3
Modelled black carbon radiative forcing and atmospheric lifetime in AeroCom Phase II constrained by aircraft observations
journal, January 2014
- Samset, B. H.; Myhre, G.; Herber, A.
- Atmospheric Chemistry and Physics, Vol. 14, Issue 22
Short-term effects of controlling fossil-fuel soot, biofuel soot and gases, and methane on climate, Arctic ice, and air pollution health
journal, January 2010
- Jacobson, Mark Z.
- Journal of Geophysical Research, Vol. 115, Issue D14
Soot climate forcing via snow and ice albedos
journal, December 2003
- Hansen, J.; Nazarenko, L.
- Proceedings of the National Academy of Sciences, Vol. 101, Issue 2
Phase partitioning of aerosol particles in clouds at Kleiner Feldberg
journal, August 1994
- Hallberg, A.; Noone, K. J.; Ogren, J. A.
- Journal of Atmospheric Chemistry, Vol. 19, Issue 1-2
Black carbon semi-direct effects on cloud cover: review and synthesis
journal, January 2010
- Koch, D.; Del Genio, A. D.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 16
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
journal, January 2007
- Petters, M. D.; Kreidenweis, S. M.
- Atmospheric Chemistry and Physics, Vol. 7, Issue 8
Enhanced Absorption of Solar Radiation By Cloud Droplets Containing Soot Particles In Their Surface: NOTES AND CORRESPONDENCE
journal, January 1992
- Chylek, Petr; Hallett, John
- Quarterly Journal of the Royal Meteorological Society, Vol. 118, Issue 503
Present-day climate forcing and response from black carbon in snow
journal, January 2007
- Flanner, Mark G.; Zender, Charles S.; Randerson, James T.
- Journal of Geophysical Research, Vol. 112, Issue D11
Phase partitioning of aerosol constituents in cloud based on single-particle and bulk analysis
journal, August 1997
- Gieray, R.; Wieser, P.; Engelhardt, T.
- Atmospheric Environment, Vol. 31, Issue 16
Estimating black carbon aging time-scales with a particle-resolved aerosol model
journal, January 2010
- Riemer, Nicole; West, Matthew; Zaveri, Rahul
- Journal of Aerosol Science, Vol. 41, Issue 1
Size-dependent scavenging efficiencies of multicomponent atmospheric aerosols in clouds
journal, January 2003
- Sellegri, K.
- Journal of Geophysical Research, Vol. 108, Issue D11
Hygroscopic properties of carbon and diesel soot particles
journal, August 1997
- Weingartner, E.; Burtscher, H.; Baltensperger, U.
- Atmospheric Environment, Vol. 31, Issue 15
Evaluation of black carbon estimations in global aerosol models
journal, January 2009
- Koch, D.; Schulz, M.; Kinne, S.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 22
Size-resolved observations of refractory black carbon particles in cloud droplets at a marine boundary layer site
journal, January 2015
- Schroder, J. C.; Hanna, S. J.; Modini, R. L.
- Atmospheric Chemistry and Physics, Vol. 15, Issue 3
Black carbon solar absorption suppresses turbulence in the atmospheric boundary layer
journal, October 2016
- Wilcox, Eric M.; Thomas, Rick M.; Praveen, Puppala S.
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 42
Model for Simulating Aerosol Interactions and Chemistry (MOSAIC)
journal, January 2008
- Zaveri, Rahul A.; Easter, Richard C.; Fast, Jerome D.
- Journal of Geophysical Research, Vol. 113, Issue D13
A new lumped structure photochemical mechanism for large-scale applications
journal, December 1999
- Zaveri, Rahul A.; Peters, Leonard K.
- Journal of Geophysical Research: Atmospheres, Vol. 104, Issue D23
The growth of atmospheric aerosol particles as a function of the relative humidity—II. An improved concept of mixed nuclei
journal, September 1973
- Winkler, Peter
- Journal of Aerosol Science, Vol. 4, Issue 5
Black carbon absorption at the global scale is affected by particle-scale diversity in composition
journal, September 2016
- Fierce, Laura; Bond, Tami C.; Bauer, Susanne E.
- Nature Communications, Vol. 7, Issue 1
Aerosol black carbon measurements at the South Pole: Initial results, 1986-1987
journal, October 1988
- Hansen, A. D. A.; Bodhaine, B. A.; Dutton, E. G.
- Geophysical Research Letters, Vol. 15, Issue 11
Black carbon and other species at a high-elevation European site (Mount Sonnblick, 3106 m, Austria): Concentrations and scavenging efficiencies
journal, October 2000
- Hitzenberger, R.; Berner, A.; Kromp, R.
- Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D20
Impacts of black carbon mixing state on black carbon nucleation scavenging: Insights from a particle-resolved model: PARTMC-MOSAIC BLACK CARBON MIXING STATE
journal, December 2012
- Ching, J.; Riemer, N.; West, M.
- Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D23
Phase partitioning for different aerosol species in fog
journal, January 1992
- Hallberg, A.; Ogren, J. A.; Noone, K. J.
- Tellus B: Chemical and Physical Meteorology, Vol. 44, Issue 5
A single-column particle-resolved model for simulating the vertical distribution of aerosol mixing state: WRF-PartMC-MOSAIC-SCM v1.0
journal, January 2017
- Curtis, Jeffrey H.; Riemer, Nicole; West, Matthew
- Geoscientific Model Development, Vol. 10, Issue 11
Bounding the role of black carbon in the climate system: A scientific assessment: BLACK CARBON IN THE CLIMATE SYSTEM
journal, June 2013
- Bond, T. C.; Doherty, S. J.; Fahey, D. W.
- Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 11
Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects
journal, February 2006
- Poeschl, Ulrich
- ChemInform, Vol. 37, Issue 7
Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch
journal, January 2006
- Cozic, J.; Verheggen, B.; Mertes, S.
- Atmospheric Chemistry and Physics Discussions, Vol. 6, Issue 6
Evaluation of black carbon estimations in global aerosol models
journal, January 2009
- Koch, D.; Schulz, M.; Kinne, S.
- Atmospheric Chemistry and Physics Discussions, Vol. 9, Issue 4
Simulating aerosol chamber experiments with the particle-resolved aerosol model PartMC
text, January 2017
- Tian, J.; Brem, B. T.; West, M.
- Taylor & Francis
Simulating aerosol chamber experiments with the particle-resolved aerosol model PartMC
text, January 2017
- Tian, J.; Brem, B. T.; West, M.
- Taylor & Francis
Simulating aerosol chamber experiments with the particle-resolved aerosol model PartMC
text, January 2017
- Tian, J.; Brem, B.; West, M.
- Taylor & Francis
Phase partitioning for different aerosol species in fog
journal, November 1992
- Hallberg, A.; Ogren, J. A.; Noone, K. J.
- Tellus B, Vol. 44, Issue 5
Seasonal variation of the atmospheric aerosol near the top of the marine boundary layer over Spitsbergen related to the Arctic sulphur cycle*
journal, February 1994
- Heintzenberg, Jost; Leck, Caroline
- Tellus B, Vol. 46, Issue 1
Simulating the evolution of soot mixing state with a particle-resolved aerosol model
text, January 2008
- Riemer, N.; West, M.; Zaveri, R. A.
- arXiv
Estimating black carbon aging time-scales with a particle-resolved aerosol model
preprint, January 2009
- Riemer, N.; West, M.; Zaveri, R. A.
- arXiv
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
journal, January 2006
- Petters, M. D.; Kreidenweis, S. M.
- Atmospheric Chemistry and Physics Discussions, Vol. 6, Issue 5
Seasonal variation of the atmospheric aerosol near the top of the marine boundary layer over Spitsbergen related to the Arctic sulphur cycle
journal, January 1994
- Heintzenberg, Jost; Leck, Caroline
- Tellus B: Chemical and Physical Meteorology, Vol. 46, Issue 1
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
journal, January 2006
- Petters, M. D.; Kreidenweis, S. M.
- Atmospheric Chemistry and Physics Discussions, Vol. 6, Issue 5
Works referencing / citing this record:
Aerosol mixing state revealed by transmission electron microscopy pertaining to cloud formation and human airway deposition
journal, July 2019
- Ching, Joseph; Adachi, Kouji; Zaizen, Yuji
- npj Climate and Atmospheric Science, Vol. 2, Issue 1
Recent Advances in Quantifying Wet Scavenging Efficiency of Black Carbon Aerosol
journal, April 2019
- Yang, Yuxiang; Fu, Yuzhen; Lin, Qinhao
- Atmosphere, Vol. 10, Issue 4
Preface: Morphology and Internal Mixing of Atmospheric Particles
journal, July 2018
- China, Swarup; Mazzoleni, Claudio
- Atmosphere, Vol. 9, Issue 7
Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state
journal, January 2019
- Motos, Ghislain; Schmale, Julia; Corbin, Joel C.
- Atmospheric Chemistry and Physics, Vol. 19, Issue 4
Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580 m a.s.l.)
journal, January 2019
- Motos, Ghislain; Schmale, Julia; Corbin, Joel C.
- Atmospheric Chemistry and Physics, Vol. 19, Issue 6