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Response of the Aerodyne Aerosol Mass Spectrometer to Inorganic Sulfates and Organosulfur Compounds: Applications in Field and Laboratory Measurements

Chen, Yunle and Xu, Lu and Humphry, Tim and Hettiyadura, Anusha P. S. and Ovadnevaite, Jurgita and Huang, Shan and Poulain, Laurent and Schroder, Jason C. and Campuzano-Jost, Pedro and Jimenez, Jose L. and Herrmann, Hartmut and O’Dowd, Colin D. and Stone, Elizabeth A. and Ng, Nga Lee (2019) Response of the Aerodyne Aerosol Mass Spectrometer to Inorganic Sulfates and Organosulfur Compounds: Applications in Field and Laboratory Measurements. Environmental Science and Technology, 53 (9). pp. 5176-5186. ISSN 0013-936X.

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Organosulfur compounds are important components of secondary organic aerosols (SOA). While the Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS) has been extensively used in aerosol studies, the response of the AMS to organosulfur compounds is not well-understood. Here, we investigated the fragmentation patterns of organosulfurs and inorganic sulfates in the AMS, developed a method to deconvolve total sulfate into components of inorganic and organic origins, and applied this method in both laboratory and field measurements. Apportionment results from laboratory isoprene photooxidation experiment showed that with inorganic sulfate seed, sulfate functionality of organic origins can contribute ∼7% of SOA mass at peak growth. Results from measurements in the Southeastern U.S. showed that 4% of measured sulfate is from organosulfur compounds. Methanesulfonic acid was estimated for measurements in the coastal and remote marine boundary layer. We explored the application of this method to unit mass-resolution data, where it performed less well due to interferences. Our apportionment results demonstrate that organosulfur compounds could be a non-negligible source of sulfate fragments in AMS laboratory and field data sets. A reevaluation of previous AMS measurements over the full range of atmospheric conditions using this method could provide a global estimate/constraint on the contribution of organosulfur compounds.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Chen, Yunle0000-0001-9904-2638
Xu, Lu0000-0002-0021-9876
Huang, Shan0000-0001-5575-4510
Campuzano-Jost, Pedro0000-0003-3930-010X
Jimenez, Jose L.0000-0001-6203-1847
Herrmann, Hartmut0000-0001-7044-2101
Ng, Nga Lee0000-0001-8460-4765
Additional Information:© 2019 American Chemical Society. Received: February 11, 2019; Accepted: April 2, 2019; Published: April 2, 2019. This research was supported by NSF AGS-1455588 and U.S. Environmental Protection Agency STAR grant RD-83540301. We thank Dan Dan Huang and Chak K. Chan for helpful discussions. E.A.S., A.P.S.H., and T. H. were supported by EPA STAR grant 83540101. The measurements and data analysis at Centreville were supported by NSF AGS-1242258 and EPA RD-83540301. The measurements and data analysis at Mace Head were supported by the Horizon 2020 research and innovation programme ACTRIS-2 Integrating Activities (grant agreement No. 654109) and EPA-Ireland (AEROSOURCE, 2016-CCRP-MS-31). The measurements on board R/V Polarstern were supported by Polarstern expedition AWI_ANT XXVII/4, and the data analysis was supported by Gottfried Wilhelm Leibniz Association (OCEANET project in the framework of PAKT). J.C.S., P.C.J., and J.L.J. acknowledge funding from NSF AGS-1822664 and NASA NNX15AT96G. This publication’s contents are solely the responsibility of the grantee and do not necessarily represent the official views of the US EPA. Further, U.S. EPA does not endorse the purchase of any commercial products or services mentioned in the publication. The authors declare no competing financial interest.
Funding AgencyGrant Number
Environmental Protection Agency (EPA)RD-83540301
Environmental Protection Agency (EPA)RD-83540101
European Research Council (ERC)654109
Environmental Protection Agency-IrelandAEROSOURCE, 2016-CCRP-MS-31
Polarstern ExpeditionAWI_ANT XXVII/4
Gottfried Wilhelm Leibniz AssociationUNSPECIFIED
Issue or Number:9
Record Number:CaltechAUTHORS:20190402-135702303
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Official Citation:Response of the Aerodyne Aerosol Mass Spectrometer to Inorganic Sulfates and Organosulfur Compounds: Applications in Field and Laboratory Measurements. Yunle Chen, Lu Xu, Tim Humphry, Anusha P. S. Hettiyadura, Jurgita Ovadnevaite, Shan Huang, Laurent Poulain, Jason C. Schroder, Pedro Campuzano-Jost, Jose L. Jimenez, Hartmut Herrmann, Colin O’Dowd, Elizabeth A. Stone, and Nga Lee Ng. Environmental Science & Technology 2019 53 (9), 5176-5186 DOI: 10.1021/acs.est.9b00884
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:94374
Deposited By: Tony Diaz
Deposited On:02 Apr 2019 21:39
Last Modified:03 Oct 2019 21:03

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