Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization
Abstract
In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixingmore »
- Authors:
-
- Univ. of the Pacific, Stockton, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
- Univ. of California, Davis, CA (United States)
- Stony Brook Univ., Stony Brook, NY (United States); Univ. Claude Bernard Lyon 1, Villeurbanne (France)
- Stony Brook Univ., Stony Brook, NY (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of the Pacific, Stockton, CA (United States)
- Publication Date:
- Research Org.:
- Stony Brook Univ., NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1349679
- Grant/Contract Number:
- SC0008613
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Additional Journal Information:
- Journal Volume: 120; Journal Issue: 18; Journal ID: ISSN 2169-897X
- Publisher:
- American Geophysical Union
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
O'Brien, Rachel E., Wang, Bingbing, Laskin, Alexander, Riemer, Nicole, West, Matthew, Zhang, Qi, Sun, Yele, Yu, Xiao -Ying, Alpert, Peter, Knopf, Daniel A., Gilles, Mary K., and Moffet, Ryan C. Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization. United States: N. p., 2015.
Web. doi:10.1002/2015JD023480.
O'Brien, Rachel E., Wang, Bingbing, Laskin, Alexander, Riemer, Nicole, West, Matthew, Zhang, Qi, Sun, Yele, Yu, Xiao -Ying, Alpert, Peter, Knopf, Daniel A., Gilles, Mary K., & Moffet, Ryan C. Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization. United States. https://doi.org/10.1002/2015JD023480
O'Brien, Rachel E., Wang, Bingbing, Laskin, Alexander, Riemer, Nicole, West, Matthew, Zhang, Qi, Sun, Yele, Yu, Xiao -Ying, Alpert, Peter, Knopf, Daniel A., Gilles, Mary K., and Moffet, Ryan C. 2015.
"Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization". United States. https://doi.org/10.1002/2015JD023480. https://www.osti.gov/servlets/purl/1349679.
@article{osti_1349679,
title = {Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization},
author = {O'Brien, Rachel E. and Wang, Bingbing and Laskin, Alexander and Riemer, Nicole and West, Matthew and Zhang, Qi and Sun, Yele and Yu, Xiao -Ying and Alpert, Peter and Knopf, Daniel A. and Gilles, Mary K. and Moffet, Ryan C.},
abstractNote = {In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.},
doi = {10.1002/2015JD023480},
url = {https://www.osti.gov/biblio/1349679},
journal = {Journal of Geophysical Research: Atmospheres},
issn = {2169-897X},
number = 18,
volume = 120,
place = {United States},
year = {Wed Aug 26 00:00:00 EDT 2015},
month = {Wed Aug 26 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces
journal, October 2013
- Bateman, Adam P.; Belassein, Helene; Martin, Scot T.
- Aerosol Science and Technology, Vol. 48, Issue 1
Light Absorption by Carbonaceous Particles: An Investigative Review
journal, January 2006
- Bond, Tami C.; Bergstrom, Robert W.
- Aerosol Science and Technology, Vol. 40, Issue 1
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
Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon
journal, August 2012
- Cappa, C. D.; Onasch, T. B.; Massoli, P.
- Science, Vol. 337, Issue 6098
Transport and mixing patterns over Central California during the carbonaceous aerosol and radiative effects study (CARES)
journal, January 2012
- Fast, J. D.; Gustafson Jr., W. I.; Berg, L. K.
- Atmospheric Chemistry and Physics, Vol. 12, Issue 4
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
Correlations between optical, chemical and physical properties of biomass burn aerosols
journal, January 2007
- Hopkins, R. J.; Lewis, K.; Desyaterik, Y.
- Geophysical Research Letters, Vol. 34, Issue 18
Organic atmospheric aerosols: Review and state of the science
journal, May 2000
- Jacobson, M. C.; Hansson, H. -C.; Noone, K. J.
- Reviews of Geophysics, Vol. 38, Issue 2
Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols
journal, February 2001
- Jacobson, Mark Z.
- Nature, Vol. 409, Issue 6821
Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area
journal, January 2005
- Johnson, K. S.; Zuberi, B.; Molina, L. T.
- Atmospheric Chemistry and Physics, Vol. 5, Issue 11
Organic aerosol and global climate modelling: a review
journal, January 2005
- Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N.
- Atmospheric Chemistry and Physics, Vol. 5, Issue 4
Interferometer-controlled scanning transmission X-ray microscopes at the Advanced Light Source
journal, February 2003
- Kilcoyne, A. L. D.; Tyliszczak, T.; Steele, W. F.
- Journal of Synchrotron Radiation, Vol. 10, Issue 2
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
Microspectroscopic imaging and characterization of individually identified ice nucleating particles from a case field study: CHARACTERIZATION OF INDIVIDUAL IN
journal, September 2014
- Knopf, D. A.; Alpert, P. A.; Wang, B.
- Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 17
Brown carbon and internal mixing in biomass burning particles
journal, August 2012
- Lack, D. A.; Langridge, J. M.; Bahreini, R.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 37
Time-Resolved Aerosol Collector for CCSEM/EDX Single-Particle Analysis
journal, March 2003
- Laskin, Alexander; Iedema, Martin J.; Cowin, James P.
- Aerosol Science and Technology, Vol. 37, Issue 3
Analysis of individual environmental particles using modern methods of electron microscopy and X-ray microanalysis
journal, February 2006
- Laskin, A.; Cowin, J. P.; Iedema, M. J.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 150, Issue 2-3
Tropospheric chemistry of internally mixed sea salt and organic particles: Surprising reactivity of NaCl with weak organic acids: MIXED SEA SALT/ORGANICS PARTICLES
journal, August 2012
- Laskin, Alexander; Moffet, Ryan C.; Gilles, Mary K.
- Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D15
Optical properties of soot–water drop agglomerates: An experimental study
journal, January 2006
- Mikhailov, E. F.; Vlasenko, S. S.; Podgorny, I. A.
- Journal of Geophysical Research, Vol. 111, Issue D7
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
Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge †
journal, October 2010
- Moffet, Ryan C.; Henn, Tobias; Laskin, Alexander
- Analytical Chemistry, Vol. 82, Issue 19
Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City
journal, January 2010
- Moffet, R. C.; Henn, T. R.; Tivanski, A. V.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 3
Spectro-microscopic measurements of carbonaceous aerosol aging in Central California
journal, January 2013
- Moffet, R. C.; Rödel, T. C.; Kelly, S. T.
- Atmospheric Chemistry and Physics, Vol. 13, Issue 20
Physical properties of ambient and laboratory-generated secondary organic aerosol: PHYSICAL PROPERTIES OF ORGANIC AEROSOL
journal, June 2014
- O'Brien, Rachel E.; Neu, Alexander; Epstein, Scott A.
- Geophysical Research Letters, Vol. 41, Issue 12
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
Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects
journal, November 2005
- Pöschl, Ulrich
- Angewandte Chemie International Edition, Vol. 44, Issue 46
Evaporation of ammonium nitrate particles
journal, January 1987
- Richardson, C. B.; Hightower, R. L.
- Atmospheric Environment (1967), Vol. 21, Issue 4
Quantifying aerosol mixing state with entropy and diversity measures
journal, January 2013
- Riemer, N.; West, M.
- Atmospheric Chemistry and Physics, Vol. 13, Issue 22
Brownness of organics in aerosols from biomass burning linked to their black carbon content
journal, August 2014
- Saleh, Rawad; Robinson, Ellis S.; Tkacik, Daniel S.
- Nature Geoscience, Vol. 7, Issue 9
Absorption amplification of black carbon internally mixed with secondary organic aerosol
journal, January 2005
- Schnaiter, M.
- Journal of Geophysical Research, Vol. 110, Issue D19
Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES
journal, January 2012
- Setyan, A.; Zhang, Q.; Merkel, M.
- Atmospheric Chemistry and Physics, Vol. 12, Issue 17
Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
journal, January 2014
- Setyan, A.; Song, C.; Merkel, M.
- Atmospheric Chemistry and Physics, Vol. 14, Issue 13
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
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
Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)
journal, January 2012
- Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.
- Atmospheric Chemistry and Physics, Vol. 12, Issue 16
Aging induced changes on NEXAFS fingerprints in individual combustion particles
journal, January 2011
- Zelenay, V.; Mooser, R.; Tritscher, T.
- Atmospheric Chemistry and Physics, Vol. 11, Issue 22
Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects
journal, February 2006
- Poeschl, Ulrich
- ChemInform, Vol. 37, Issue 7
Organic aerosol and global climate modelling: a review
journal, January 2004
- Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N.
- Atmospheric Chemistry and Physics Discussions, Vol. 4, Issue 5
Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area
journal, August 2005
- Johnson, K. S.; Zuberi, B.; Molina, L. T.
- Atmospheric Chemistry and Physics Discussions
Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces
text, January 2014
- Bateman, Adam P.; Belassein, Helene; Martin, Scot T.
- Taylor & Francis
Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces
text, January 2014
- Bateman, Adam P.; Belassein, Helene; Martin, Scot T.
- Taylor & Francis
Single particle diversity and mixing state measurements
other, January 2014
- Healy, R. M.; Riemer, N.; Wenger, J. C.
- München : European Geopyhsical Union
Chemistry of new particle growth in mixed urban and biogenic emissions - Insights from CARES
other, January 2014
- Setyan, A.; Song, C.; Merkel, M.
- München : European Geopyhsical Union
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: Measurements, Modeling, and Impacts
journal, May 2019
- Riemer, N.; Ault, A. P.; West, M.
- Reviews of Geophysics, Vol. 57, Issue 2
Methodology for quantifying the volatile mixing state of an aerosol
journal, May 2016
- Dickau, Matthew; Olfert, Jason; Stettler, Marc E. J.
- Aerosol Science and Technology, Vol. 50, Issue 8
A Review of the Representation of Aerosol Mixing State in Atmospheric Models
journal, March 2019
- Stevens, Robin; Dastoor, Ashu
- Atmosphere, Vol. 10, Issue 4
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
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
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
The diverse chemical mixing state of aerosol particles in the southeastern United States
journal, January 2018
- Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.
- Atmospheric Chemistry and Physics, Vol. 18, Issue 16
Quantitative capabilities of STXM to measure spatially resolved organic volume fractions of mixed organic ∕ inorganic particles
journal, January 2019
- Fraund, Matthew; Park, Tim; Yao, Lin
- Atmospheric Measurement Techniques, Vol. 12, Issue 3
X-ray microscopy
journal, July 1965
- Cosslett, V. E.
- Reports on Progress in Physics, Vol. 28, Issue 1