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Title: Metrics to quantify the importance of mixing state for CCN activity

Abstract

It is commonly assumed that models are more prone to errors in predicted cloud condensation nuclei (CCN) concentrations when the aerosol populations are externally mixed. In this work we investigate this assumption by using the mixing state index (χ) proposed by Riemer and West (2013) to quantify the degree of external and internal mixing of aerosol populations. We combine this metric with particle-resolved model simulations to quantify error in CCN predictions when mixing state information is neglected, exploring a range of scenarios that cover different conditions of aerosol aging. We show that mixing state information does indeed become unimportant for more internally mixed populations, more precisely for populations with χ larger than 75 %. For more externally mixed populations (χ below 20 %) the relationship of χ and the error in CCN predictions is not unique and ranges from lower than -40 % to about 150 %, depending on the underlying aerosol population and the environmental supersaturation. We explain the reasons for this behavior with detailed process analyses.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Sciences and Global Change Division
  2. University of Illinois at Urbana–Champaign, Urbana (United States). Department of Mechanical Science and Engineering
  3. University of Illinois at Urbana–Champaign, Urbana (United States). Department of Atmospheric Sciences
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1367378
Report Number(s):
PNNL-SA-122612
Journal ID: ISSN 1680-7324; KP1701000
Grant/Contract Number:  
AC05-76RL01830; SC0011771
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 17; Journal Issue: 12; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; CCN; mixing state; aerosol; particles

Citation Formats

Ching, Joseph, Fast, Jerome, West, Matthew, and Riemer, Nicole. Metrics to quantify the importance of mixing state for CCN activity. United States: N. p., 2017. Web. doi:10.5194/acp-17-7445-2017.
Ching, Joseph, Fast, Jerome, West, Matthew, & Riemer, Nicole. Metrics to quantify the importance of mixing state for CCN activity. United States. https://doi.org/10.5194/acp-17-7445-2017
Ching, Joseph, Fast, Jerome, West, Matthew, and Riemer, Nicole. Wed . "Metrics to quantify the importance of mixing state for CCN activity". United States. https://doi.org/10.5194/acp-17-7445-2017. https://www.osti.gov/servlets/purl/1367378.
@article{osti_1367378,
title = {Metrics to quantify the importance of mixing state for CCN activity},
author = {Ching, Joseph and Fast, Jerome and West, Matthew and Riemer, Nicole},
abstractNote = {It is commonly assumed that models are more prone to errors in predicted cloud condensation nuclei (CCN) concentrations when the aerosol populations are externally mixed. In this work we investigate this assumption by using the mixing state index (χ) proposed by Riemer and West (2013) to quantify the degree of external and internal mixing of aerosol populations. We combine this metric with particle-resolved model simulations to quantify error in CCN predictions when mixing state information is neglected, exploring a range of scenarios that cover different conditions of aerosol aging. We show that mixing state information does indeed become unimportant for more internally mixed populations, more precisely for populations with χ larger than 75 %. For more externally mixed populations (χ below 20 %) the relationship of χ and the error in CCN predictions is not unique and ranges from lower than -40 % to about 150 %, depending on the underlying aerosol population and the environmental supersaturation. We explain the reasons for this behavior with detailed process analyses.},
doi = {10.5194/acp-17-7445-2017},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 12,
volume = 17,
place = {United States},
year = {Wed Jun 21 00:00:00 EDT 2017},
month = {Wed Jun 21 00:00:00 EDT 2017}
}

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Cited by: 25 works
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Works referenced in this record:

Weighted Flow Algorithms (WFA) for stochastic particle coagulation
journal, September 2011

  • DeVille, R. E. L.; Riemer, N.; West, M.
  • Journal of Computational Physics, Vol. 230, Issue 23
  • DOI: 10.1016/j.jcp.2011.07.027

Modeling the evolution of aerosol particles in a ship plume using PartMC-MOSAIC
journal, January 2014


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
  • DOI: 10.1002/2016JD024851

Explaining variance in black carbon's aging timescale
journal, January 2015


Methodology for quantifying the volatile mixing state of an aerosol
journal, May 2016


The effect of physical and chemical aerosol properties on warm cloud droplet activation
journal, January 2006

  • McFiggans, G.; Artaxo, P.; Baltensperger, U.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 9
  • DOI: 10.5194/acp-6-2593-2006

Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols
journal, February 2001


Quantifying aerosol mixing state with entropy and diversity measures
journal, January 2013


Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain
journal, January 2011


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
  • DOI: 10.1029/2008JD011073

In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates
journal, July 2009

  • Moffet, R. C.; Prather, K. A.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 29
  • DOI: 10.1073/pnas.0900040106

Binning for Efficient Stochastic Multiscale Particle Simulations
journal, January 2013

  • Michelotti, M. D.; Heath, M. T.; West, M.
  • Multiscale Modeling & Simulation, Vol. 11, Issue 4
  • DOI: 10.1137/130908038

CCN closure study: Effects of aerosol chemical composition and mixing state
journal, January 2015

  • Bhattu, Deepika; Tripathi, S. N.
  • Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 2
  • DOI: 10.1002/2014JD021978

The aerosol-climate model ECHAM5-HAM
journal, January 2005

  • Stier, P.; Feichter, J.; Kinne, S.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 4
  • DOI: 10.5194/acp-5-1125-2005

MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models
journal, January 2008

  • Bauer, S. E.; Wright, D. L.; Koch, D.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 20
  • DOI: 10.5194/acp-8-6003-2008

CCN predictions using simplified assumptions of organic aerosol composition and mixing state: a synthesis from six different locations
journal, January 2010

  • Ervens, B.; Cubison, M. J.; Andrews, E.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 10
  • DOI: 10.5194/acp-10-4795-2010

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
  • DOI: 10.1029/2001JD000384

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
  • DOI: 10.5194/gmd-7-1137-2014

Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model
journal, January 2010

  • Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.
  • Geoscientific Model Development, Vol. 3, Issue 2
  • DOI: 10.5194/gmd-3-519-2010

Inference of population structure using multilocus genotype data: dominant markers and null alleles: TECHNICAL ARTICLE
journal, March 2007


Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model
journal, January 2016


Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization
journal, September 2015

  • O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander
  • Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 18
  • DOI: 10.1002/2015JD023480

A new method for multicomponent activity coefficients of electrolytes in aqueous atmospheric aerosols
journal, January 2005


Single particle diversity and mixing state measurements
journal, January 2014

  • Healy, R. M.; Riemer, N.; Wenger, J. C.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 12
  • DOI: 10.5194/acp-14-6289-2014

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
  • DOI: 10.5194/acp-7-1961-2007

Estimating black carbon aging time-scales with a particle-resolved aerosol model
journal, January 2010


Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements
journal, January 2013

  • Healy, R. M.; Sciare, J.; Poulain, L.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 18
  • DOI: 10.5194/acp-13-9479-2013

MADE-in: a new aerosol microphysics submodel for global simulation of insoluble particles and their mixing state
journal, January 2011

  • Aquila, V.; Hendricks, J.; Lauer, A.
  • Geoscientific Model Development, Vol. 4, Issue 2
  • DOI: 10.5194/gmd-4-325-2011

Hygroscopic properties of carbon and diesel soot particles
journal, August 1997


Evaluation of black carbon estimations in global aerosol models
journal, January 2009


Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions
journal, April 2016

  • Che, H. C.; Zhang, X. Y.; Wang, Y. Q.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep24497

A computationally efficient Multicomponent Equilibrium Solver for Aerosols (MESA)
journal, January 2005

  • Zaveri, Rahul A.; Easter, Richard C.; Peters, Leonard K.
  • Journal of Geophysical Research, Vol. 110, Issue D24
  • DOI: 10.1029/2004JD005618

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
  • DOI: 10.1029/2007JD008782

Characterization of the Single Particle Mixing State of Individual Ship Plume Events Measured at the Port of Los Angeles
journal, March 2010

  • Ault, Andrew P.; Gaston, Cassandra J.; Wang, Ying
  • Environmental Science & Technology, Vol. 44, Issue 6
  • DOI: 10.1021/es902985h

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
  • DOI: 10.1029/1999JD900876

Local and Regional Components of Aerosol in a Heavily Trafficked Street Canyon in Central London Derived from PMF and Cluster Analysis of Single-Particle ATOFMS Spectra
journal, February 2015

  • Giorio, Chiara; Tapparo, Andrea; Dall’Osto, Manuel
  • Environmental Science & Technology, Vol. 49, Issue 6
  • DOI: 10.1021/es506249z

Improving our fundamental understanding of the role of aerosol−cloud interactions in the climate system
journal, May 2016

  • Seinfeld, John H.; Bretherton, Christopher; Carslaw, Kenneth S.
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 21
  • DOI: 10.1073/pnas.1514043113

Entropy and Information in Neural Spike Trains
journal, January 1998

  • Strong, S. P.; Koberle, Roland; de Ruyter van Steveninck, Rob R.
  • Physical Review Letters, Vol. 80, Issue 1
  • DOI: 10.1103/PhysRevLett.80.197

The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols
journal, January 2010

  • Wang, J.; Cubison, M. J.; Aiken, A. C.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 15
  • DOI: 10.5194/acp-10-7267-2010

Droplet activation properties of organic aerosols observed at an urban site during CalNex-LA: CCN ACTIVITY OF ORGANIC AEROSOLS
journal, April 2013

  • Mei, Fan; Hayes, Patrick L.; Ortega, Amber
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 7
  • DOI: 10.1002/jgrd.50285

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
  • DOI: 10.1029/2012JD018269

When is cloud condensation nuclei activity sensitive to particle characteristics at emission?: CCN ACTIVITY OF PRIMARY AEROSOL
journal, December 2013

  • Fierce, Laura; Riemer, Nicole; Bond, Tami C.
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 24
  • DOI: 10.1002/2013JD020608

Evolution and Measurement of Species Diversity
journal, May 1972


Single Particle Characterization of Ultrafine and Accumulation Mode Particles from Heavy Duty Diesel Vehicles Using Aerosol Time-of-Flight Mass Spectrometry
journal, June 2006

  • Toner, Stephen M.; Sodeman, David A.; Prather, Kimberly A.
  • Environmental Science & Technology, Vol. 40, Issue 12
  • DOI: 10.1021/es051455x

A three-dimensional sectional representation of aerosol mixing state for simulating optical properties and cloud condensation nuclei: Aerosol Mixing State Representation
journal, May 2016

  • Ching, Joseph; Zaveri, Rahul A.; Easter, Richard C.
  • Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 10
  • DOI: 10.1002/2015JD024323

Aerosol Properties and Processes: A Path from Field and Laboratory Measurements to Global Climate Models
journal, July 2007

  • Ghan, Steven J.; Schwartz, Stephen E.
  • Bulletin of the American Meteorological Society, Vol. 88, Issue 7
  • DOI: 10.1175/BAMS-88-7-1059

Particle-resolved simulation of aerosol size, composition, mixing state, and the associated optical and cloud condensation nuclei activation properties in an evolving urban plume
journal, January 2010

  • Zaveri, Rahul A.; Barnard, James C.; Easter, Richard C.
  • Journal of Geophysical Research, Vol. 115, Issue D17
  • DOI: 10.1029/2009JD013616

MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models
journal, January 2008

  • Bauer, S. E.; Wright, D.; Koch, D.
  • Atmospheric Chemistry and Physics Discussions, Vol. 8, Issue 3
  • DOI: 10.5194/acpd-8-9931-2008

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
  • DOI: 10.5194/acpd-9-15769-2009

CCN predictions using simplified assumptions of organic aerosol composition and mixing state: a synthesis from six different locations
journal, January 2009

  • Ervens, B.; Cubison, M. J.; Andrews, E.
  • Atmospheric Chemistry and Physics Discussions, Vol. 9, Issue 5
  • DOI: 10.5194/acpd-9-21237-2009

Functional Groups of Metazoan Parasites of the Dusky Flounder (Syacium papillosum) as Bioindicators of Environmental Health of the Yucatan Shelf
journal, April 2021

  • Vidal-Martínez, Víctor M.; Ocaña, Frank A.; Soler-Jiménez, Lilia C.
  • Bulletin of Environmental Contamination and Toxicology
  • DOI: 10.1007/s00128-021-03177-9

The effect of physical and chemical aerosol properties on warm cloud droplet activation
text, January 2006


Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model
journal, January 2010

  • Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.
  • Geoscientific Model Development Discussions, Vol. 3, Issue 2
  • DOI: 10.5194/gmdd-3-651-2010

Single particle diversity and mixing state measurements
other, January 2014

  • Healy, R. M.; Riemer, N.; Wenger, J. C.
  • München : European Geopyhsical Union
  • DOI: 10.34657/1248

Estimating black carbon aging time-scales with a particle-resolved aerosol model
preprint, January 2009


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
  • DOI: 10.5194/acpd-6-8435-2006

Works referencing / citing this record:

Effects of Aerosols on the Precipitation of Convective Clouds: A Case Study in the Yangtze River Delta of China
journal, July 2019

  • Liu, Chong; Wang, Ti‐Jian; Chen, Pu‐Long
  • Journal of Geophysical Research: Atmospheres, Vol. 124, Issue 14
  • DOI: 10.1029/2018jd029924

Aerosol mixing state matters for particles deposition in human respiratory system
journal, June 2018


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
  • DOI: 10.1038/s41612-019-0081-9

A Review of the Representation of Aerosol Mixing State in Atmospheric Models
journal, March 2019


Machine Learning to Predict the Global Distribution of Aerosol Mixing State Metrics
journal, January 2018

  • Hughes, Michael; Kodros, John; Pierce, Jeffrey
  • Atmosphere, Vol. 9, Issue 1
  • DOI: 10.3390/atmos9010015

Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles
journal, January 2018

  • Ching, Joseph; West, Matthew; Riemer, Nicole
  • Atmosphere, Vol. 9, Issue 1
  • DOI: 10.3390/atmos9010017