Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

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.

doi:10.1002/2015JD023480

Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

Journal Article · Wed Aug 26 00:00:00 EDT 2015 · Journal of Geophysical Research: Atmospheres

DOI:https://doi.org/10.1002/2015JD023480· OSTI ID:1349679

O'Brien, Rachel E. ^[1]; Wang, Bingbing ^[2]; Laskin, Alexander ^[2]; Riemer, Nicole ^[3]; West, Matthew ^[3]; Zhang, Qi ^[4]; Sun, Yele ^[4]; Yu, Xiao -Ying ^[2]; Alpert, Peter ^[5]; ^[6]; Gilles, Mary K. ^[7]; Moffet, Ryan C. ^[8]

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); Stony Brook University
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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Stony Brook Univ., Stony Brook, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: SC0008613

OSTI ID:: 1349679

Alternate ID(s):: OSTI ID: 1229980

Journal Information:: Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Journal Issue: 18 Vol. 120; ISSN 2169-897X

Publisher:: American Geophysical UnionCopyright Statement

Country of Publication:: United States

Language:: English

References (44)

Physical properties of ambient and laboratory-generated secondary organic aerosol: PHYSICAL PROPERTIES OF ORGANIC AEROSOL O'Brien, Rachel E.; Neu, Alexander; Epstein, Scott A. Geophysical Research Letters, Vol. 41, Issue 12 https://doi.org/10.1002/2014GL060219	journal	June 2014
Microspectroscopic imaging and characterization of individually identified ice nucleating particles from a case field study: CHARACTERIZATION OF INDIVIDUAL IN Knopf, D. A.; Alpert, P. A.; Wang, B. Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 17 https://doi.org/10.1002/2014JD021866	journal	September 2014
Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects Pöschl, Ulrich Angewandte Chemie International Edition, Vol. 44, Issue 46 https://doi.org/10.1002/anie.200501122	journal	November 2005
Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects Poeschl, Ulrich ChemInform, Vol. 37, Issue 7 https://doi.org/10.1002/chin.200607299	journal	February 2006
Bounding the role of black carbon in the climate system: A scientific assessment: BLACK CARBON IN THE CLIMATE SYSTEM Bond, T. C.; Doherty, S. J.; Fahey, D. W. Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 11 https://doi.org/10.1002/jgrd.50171	journal	June 2013
Evaporation of ammonium nitrate particles Richardson, C. B.; Hightower, R. L. Atmospheric Environment (1967), Vol. 21, Issue 4 https://doi.org/10.1016/0004-6981(87)90092-8	journal	January 1987
Analysis of individual environmental particles using modern methods of electron microscopy and X-ray microanalysis Laskin, A.; Cowin, J. P.; Iedema, M. J. Journal of Electron Spectroscopy and Related Phenomena, Vol. 150, Issue 2-3 https://doi.org/10.1016/j.elspec.2005.06.008	journal	February 2006
Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge ^† Moffet, Ryan C.; Henn, Tobias; Laskin, Alexander Analytical Chemistry, Vol. 82, Issue 19 https://doi.org/10.1021/ac1012909	journal	October 2010
Organic atmospheric aerosols: Review and state of the science Jacobson, M. C.; Hansson, H. -C.; Noone, K. J. Reviews of Geophysics, Vol. 38, Issue 2 https://doi.org/10.1029/1998RG000045	journal	May 2000
Absorption amplification of black carbon internally mixed with secondary organic aerosol Schnaiter, M. Journal of Geophysical Research, Vol. 110, Issue D19 https://doi.org/10.1029/2005JD006046	journal	January 2005
Optical properties of soot–water drop agglomerates: An experimental study Mikhailov, E. F.; Vlasenko, S. S.; Podgorny, I. A. Journal of Geophysical Research, Vol. 111, Issue D7 https://doi.org/10.1029/2005JD006389	journal	January 2006
Correlations between optical, chemical and physical properties of biomass burn aerosols Hopkins, R. J.; Lewis, K.; Desyaterik, Y. Geophysical Research Letters, Vol. 34, Issue 18 https://doi.org/10.1029/2007GL030502	journal	January 2007
Heterogeneous nucleation of ice on anthropogenic organic particles collected in Mexico City: ICE NUCLEATION ON ANTHROPOGENIC AEROSOL Knopf, D. A.; Wang, B.; Laskin, A. Geophysical Research Letters, Vol. 37, Issue 11 https://doi.org/10.1029/2010GL043362	journal	June 2010
Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K: ICE NUCLEATION BY ATMOSPHERIC PARTICLES Wang, Bingbing; Laskin, Alexander; Roedel, Tobias Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D21 https://doi.org/10.1029/2012JD017446	journal	September 2012
Tropospheric chemistry of internally mixed sea salt and organic particles: Surprising reactivity of NaCl with weak organic acids: MIXED SEA SALT/ORGANICS PARTICLES Laskin, Alexander; Moffet, Ryan C.; Gilles, Mary K. Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D15 https://doi.org/10.1029/2012JD017743	journal	August 2012
Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols Jacobson, Mark Z. Nature, Vol. 409, Issue 6821 https://doi.org/10.1038/35055518	journal	February 2001
Brownness of organics in aerosols from biomass burning linked to their black carbon content Saleh, Rawad; Robinson, Ellis S.; Tkacik, Daniel S. Nature Geoscience, Vol. 7, Issue 9 https://doi.org/10.1038/ngeo2220	journal	August 2014
In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates Moffet, R. C.; Prather, K. A. Proceedings of the National Academy of Sciences, Vol. 106, Issue 29 https://doi.org/10.1073/pnas.0900040106	journal	July 2009
Brown carbon and internal mixing in biomass burning particles Lack, D. A.; Langridge, J. M.; Bahreini, R. Proceedings of the National Academy of Sciences, Vol. 109, Issue 37 https://doi.org/10.1073/pnas.1206575109	journal	August 2012
Time-Resolved Aerosol Collector for CCSEM/EDX Single-Particle Analysis Laskin, Alexander; Iedema, Martin J.; Cowin, James P. Aerosol Science and Technology, Vol. 37, Issue 3 https://doi.org/10.1080/02786820300945	journal	March 2003
Light Absorption by Carbonaceous Particles: An Investigative Review Bond, Tami C.; Bergstrom, Robert W. Aerosol Science and Technology, Vol. 40, Issue 1 https://doi.org/10.1080/02786820500421521	journal	January 2006
Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces Bateman, Adam P.; Belassein, Helene; Martin, Scot T. Aerosol Science and Technology, Vol. 48, Issue 1 https://doi.org/10.1080/02786826.2013.853866	journal	October 2013
Interferometer-controlled scanning transmission X-ray microscopes at the Advanced Light Source Kilcoyne, A. L. D.; Tyliszczak, T.; Steele, W. F. Journal of Synchrotron Radiation, Vol. 10, Issue 2 https://doi.org/10.1107/S0909049502017739	journal	February 2003
Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon Cappa, C. D.; Onasch, T. B.; Massoli, P. Science, Vol. 337, Issue 6098 https://doi.org/10.1126/science.1223447	journal	August 2012
Single particle diversity and mixing state measurements Healy, R. M.; Riemer, N.; Wenger, J. C. München : European Geopyhsical Union https://doi.org/10.34657/1248	other	January 2014
Chemistry of new particle growth in mixed urban and biogenic emissions - Insights from CARES Setyan, A.; Song, C.; Merkel, M. München : European Geopyhsical Union https://doi.org/10.34657/828	other	January 2014
The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols Wang, J.; Cubison, M. J.; Aiken, A. C. Atmospheric Chemistry and Physics, Vol. 10, Issue 15 https://doi.org/10.5194/acp-10-7267-2010	journal	January 2010
Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City Moffet, R. C.; Henn, T. R.; Tivanski, A. V. Atmospheric Chemistry and Physics, Vol. 10, Issue 3 https://doi.org/10.5194/acp-10-961-2010	journal	January 2010
Aging induced changes on NEXAFS fingerprints in individual combustion particles Zelenay, V.; Mooser, R.; Tritscher, T. Atmospheric Chemistry and Physics, Vol. 11, Issue 22 https://doi.org/10.5194/acp-11-11777-2011	journal	January 2011
Transport and mixing patterns over Central California during the carbonaceous aerosol and radiative effects study (CARES) Fast, J. D.; Gustafson Jr., W. I.; Berg, L. K. Atmospheric Chemistry and Physics, Vol. 12, Issue 4 https://doi.org/10.5194/acp-12-1759-2012	journal	January 2012
Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J. Atmospheric Chemistry and Physics, Vol. 12, Issue 16 https://doi.org/10.5194/acp-12-7647-2012	journal	January 2012
Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES Setyan, A.; Zhang, Q.; Merkel, M. Atmospheric Chemistry and Physics, Vol. 12, Issue 17 https://doi.org/10.5194/acp-12-8131-2012	journal	January 2012
Spectro-microscopic measurements of carbonaceous aerosol aging in Central California Moffet, R. C.; Rödel, T. C.; Kelly, S. T. Atmospheric Chemistry and Physics, Vol. 13, Issue 20 https://doi.org/10.5194/acp-13-10445-2013	journal	January 2013
Quantifying aerosol mixing state with entropy and diversity measures Riemer, N.; West, M. Atmospheric Chemistry and Physics, Vol. 13, Issue 22 https://doi.org/10.5194/acp-13-11423-2013	journal	January 2013
Single particle diversity and mixing state measurements Healy, R. M.; Riemer, N.; Wenger, J. C. Atmospheric Chemistry and Physics, Vol. 14, Issue 12 https://doi.org/10.5194/acp-14-6289-2014	journal	January 2014
Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES Setyan, A.; Song, C.; Merkel, M. Atmospheric Chemistry and Physics, Vol. 14, Issue 13 https://doi.org/10.5194/acp-14-6477-2014	journal	January 2014
Organic aerosol and global climate modelling: a review Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N. Atmospheric Chemistry and Physics, Vol. 5, Issue 4 https://doi.org/10.5194/acp-5-1053-2005	journal	January 2005
Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area Johnson, K. S.; Zuberi, B.; Molina, L. T. Atmospheric Chemistry and Physics, Vol. 5, Issue 11 https://doi.org/10.5194/acp-5-3033-2005	journal	January 2005
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity Petters, M. D.; Kreidenweis, S. M. Atmospheric Chemistry and Physics, Vol. 7, Issue 8 https://doi.org/10.5194/acp-7-1961-2007	journal	January 2007
Organic aerosol and global climate modelling: a review Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N. Atmospheric Chemistry and Physics Discussions, Vol. 4, Issue 5 https://doi.org/10.5194/acpd-4-5855-2004	journal	January 2004
Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area Johnson, K. S.; Zuberi, B.; Molina, L. T. Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acpd-5-5585-2005	journal	August 2005
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity Petters, M. D.; Kreidenweis, S. M. Atmospheric Chemistry and Physics Discussions, Vol. 6, Issue 5 https://doi.org/10.5194/acpd-6-8435-2006	journal	January 2006
Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces Bateman, Adam P.; Belassein, Helene; Martin, Scot T. Taylor & Francis https://doi.org/10.6084/m9.figshare.969666	text	January 2014
Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces Bateman, Adam P.; Belassein, Helene; Martin, Scot T. Taylor & Francis https://doi.org/10.6084/m9.figshare.969666.v1	text	January 2014

Cited By (11)

X-ray Microscopy Jacobsen, Chris Cambridge University Press https://doi.org/10.1017/9781139924542	book	January 2019
Aerosol Mixing State: Measurements, Modeling, and Impacts Riemer, N.; Ault, A. P.; West, M. Reviews of Geophysics, Vol. 57, Issue 2 https://doi.org/10.1029/2018rg000615	journal	May 2019
Methodology for quantifying the volatile mixing state of an aerosol Dickau, Matthew; Olfert, Jason; Stettler, Marc E. J. Aerosol Science and Technology, Vol. 50, Issue 8 https://doi.org/10.1080/02786826.2016.1185509	journal	May 2016
X-ray microscopy Cosslett, V. E. Reports on Progress in Physics, Vol. 28, Issue 1 https://doi.org/10.1088/0034-4885/28/1/311	journal	July 1965
X-ray microscopy Lider, V. V. Physics-Uspekhi, Vol. 60, Issue 2 https://doi.org/10.3367/ufne.2016.06.037830	journal	February 2017
A Review of the Representation of Aerosol Mixing State in Atmospheric Models Stevens, Robin; Dastoor, Ashu Atmosphere, Vol. 10, Issue 4 https://doi.org/10.3390/atmos10040168	journal	March 2019
Machine Learning to Predict the Global Distribution of Aerosol Mixing State Metrics Hughes, Michael; Kodros, John; Pierce, Jeffrey Atmosphere, Vol. 9, Issue 1 https://doi.org/10.3390/atmos9010015	journal	January 2018
Morphology and mixing of black carbon particles collected in central California during the CARES field study Moffet, Ryan C.; O'Brien, Rachel E.; Alpert, Peter A. Atmospheric Chemistry and Physics, Vol. 16, Issue 22 https://doi.org/10.5194/acp-16-14515-2016	journal	January 2016
Metrics to quantify the importance of mixing state for CCN activity Ching, Joseph; Fast, Jerome; West, Matthew Atmospheric Chemistry and Physics, Vol. 17, Issue 12 https://doi.org/10.5194/acp-17-7445-2017	journal	January 2017
The diverse chemical mixing state of aerosol particles in the southeastern United States Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C. Atmospheric Chemistry and Physics, Vol. 18, Issue 16 https://doi.org/10.5194/acp-18-12595-2018	journal	January 2018
Quantitative capabilities of STXM to measure spatially resolved organic volume fractions of mixed organic ∕ inorganic particles Fraund, Matthew; Park, Tim; Yao, Lin Atmospheric Measurement Techniques, Vol. 12, Issue 3 https://doi.org/10.5194/amt-12-1619-2019	journal	January 2019

Similar Records

Chemical Imaging of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

Journal Article · Mon Sep 28 00:00:00 EDT 2015 · Journal of Geophysical Research: Atmospheres (Online) · OSTI ID:1229980

Microscopic Characterization of Carbonaceous Aerosol Particle Aging in the Outflow from Mexico City

Journal Article · Sun Jan 31 23:00:00 EST 2010 · Atmospheric Chemistry and Physics, 10(3):961-976 · OSTI ID:974928

Microscopic Characterization of Carbonaceous Aerosol Particle Aging in the Outflow from Mexico City

Journal Article · Wed Sep 16 00:00:00 EDT 2009 · Atmospheric Chemistry and Physics · OSTI ID:973571

Related Subjects

54 ENVIRONMENTAL SCIENCES

Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

Citation Formats

References (44)

Cited By (11)

Similar Records

Related Subjects