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Time-resolved molecular characterization of organic aerosols by PILS + UPLC/ESI-Q-TOFMS

Zhang, X. and Dalleska, N. F. and Huang, D. D. and Bates, K. H. and Sorooshian, A. and Flagan, R. C. and Seinfeld, J. H. (2016) Time-resolved molecular characterization of organic aerosols by PILS + UPLC/ESI-Q-TOFMS. Atmospheric Environment, 130 . pp. 180-189. ISSN 1352-2310. doi:10.1016/j.atmosenv.2015.08.049.

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Real-time and quantitative measurement of particulate matter chemical composition represents one of the most challenging problems in the field of atmospheric chemistry. In the present study, we integrate the Particle-into-Liquid Sampler (PILS) with Ultra Performance Liquid Chromatography/Electrospray ionization Quadrupole Time-of-Flight High-Resolution/Mass Spectrometry (UPLC/ESI-Q-TOFMS) for the time-resolved molecular speciation of chamber-derived secondary organic aerosol (SOA). The unique aspect of the combination of these two well-proven techniques is to provide quantifiable molecular-level information of particle-phase organic compounds on timescales of minutes. We demonstrate that the application of the PILS + UPLC/ESI-Q-TOFMS method is not limited to water-soluble inorganic ions and organic carbon, but is extended to slightly water-soluble species through collection efficiency calibration together with sensitivity and linearity tests. By correlating the water solubility of individual species with their O:C ratio, a parameter that is available for aerosol ensembles as well, we define an average aerosol O:C ratio threshold of 0.3, above which the PILS overall particulate mass collection efficiency approaches ∼0.7. The PILS + UPLC/ESI-Q-TOFMS method can be potentially applied to probe the formation and evolution mechanism of a variety of biogenic and anthropogenic SOA systems in laboratory chamber experiments. We illustrate the application of this method to the reactive uptake of isoprene epoxydiols (IEPOX) on hydrated and acidic ammonium sulfate aerosols.

Item Type:Article
Related URLs:
URLURL TypeDescription
Dalleska, N. F.0000-0002-2059-1587
Bates, K. H.0000-0001-7544-9580
Sorooshian, A.0000-0002-2243-2264
Flagan, R. C.0000-0001-5690-770X
Seinfeld, J. H.0000-0003-1344-4068
Additional Information:© 2015 Elsevier Ltd. Received 29 May 2015; Received in revised form 18 August 2015; Accepted 18 August 2015; Available online 28 August 2015. Chemical Characterization of Secondary Organic Aerosol - Dedication to Professor Claeys This study was supported by Office of Naval Research grant N00014-14-1-0097.
Funding AgencyGrant Number
Office of Naval Research (ONR)N00014-14-1-0097
Subject Keywords:Particle-into-Liquid Samplers (PILS); Ultra Performance Liquid Chromatography (UPLC); Electrospray ionization (ESI); Quadrupole Time-of-Flight High-Resolution Mass Spectrometry (Q-TOFMS); Secondary organic aerosol (SOA); Isoprene epoxydiols (IEPOX)
Record Number:CaltechAUTHORS:20150909-091738012
Persistent URL:
Official Citation:X. Zhang, N.F. Dalleska, D.D. Huang, K.H. Bates, A. Sorooshian, R.C. Flagan, J.H. Seinfeld, Time-resolved molecular characterization of organic aerosols by PILS + UPLC/ESI-Q-TOFMS, Atmospheric Environment, Volume 130, April 2016, Pages 180-189, ISSN 1352-2310, (
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:60114
Deposited By: Tony Diaz
Deposited On:09 Sep 2015 22:04
Last Modified:10 Nov 2021 22:29

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