Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; de Sá, S. S.; McKinney, K.; Martin, S. T.; Hu, M.; Budisulistiorini, S. H.; Riva, M.; Surratt, J. D.; St. Clair, J. M.; Isaacman-Van Wertz, G.; Yee, L. D.; Goldstein, A. H.; Carbone, S.; Brito, J.; Artaxo, P.; de Gouw, J. A.; Koss, A.; Wisthaler, A.; Mikoviny, T.; Karl, T.; Kaser, L.; Jud, W.; Hansel, A.; Docherty, K. S.; Alexander, M. L.; Robinson, N. H.; Coe, H.; Allan, J. D.; Canagaratna, M. R.; Paulot, F.; Jimenez, J. L.

doi:10.5194/acp-15-11807-2015

Title: Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

Journal Article · Fri Oct 23 00:00:00 EDT 2015 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-15-11807-2015· OSTI ID:1243128

Hu, W. W.;

;

; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; de Sá, S. S.;

; Martin, S. T.; Hu, M.;

; Riva, M.;

;

; Isaacman-Van Wertz, G.;

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C₅H₆O⁺ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine f_C₅_H₆O ( f_C₅_H₆O= C₅H₆O⁺/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher f_C₅_H₆O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies.f_C₅_H₆O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low f_C₅_H₆O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. f_C₅_H₆O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the f_C₅_H₆O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.

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

Grant/Contract Number:: SC0011105

OSTI ID:: 1243128

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 15 Journal Issue: 20; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 157 works

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Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies Cubison, M. J.; Ortega, A. M.; Hayes, P. L. Atmospheric Chemistry and Physics, Vol. 11, Issue 23 https://doi.org/10.5194/acp-11-12049-2011	journal	January 2011
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Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia Schneider, J.; Freutel, F.; Zorn, S. R. Atmospheric Chemistry and Physics, Vol. 11, Issue 22 https://doi.org/10.5194/acp-11-11415-2011	journal	January 2011
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Characterization of high-resolution aerosol mass spectra of primary organic aerosol emissions from Chinese cooking and biomass burning He, L. -Y.; Lin, Y.; Huang, X. -F. Atmospheric Chemistry and Physics, Vol. 10, Issue 23 https://doi.org/10.5194/acp-10-11535-2010	journal	January 2010
Kinetics and Products of the Acid-Catalyzed Ring-Opening of Atmospherically Relevant Butyl Epoxy Alcohols Eddingsaas, Nathan C.; VanderVelde, David G.; Wennberg, Paul O. The Journal of Physical Chemistry A, Vol. 114, Issue 31 https://doi.org/10.1021/jp103907c	journal	August 2010
Unexpected Epoxide Formation in the Gas-Phase Photooxidation of Isoprene Paulot, F.; Crounse, J. D.; Kjaergaard, H. G. Science, Vol. 325, Issue 5941 https://doi.org/10.1126/science.1172910	journal	August 2009

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