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Observations of heterogeneous reactions between Asian pollution and mineral dust over the Eastern North Pacific during INTEX-B

McNaughton, C. S. and Clarke, A. D. and Kapustin, V. and Shinozuka, Y. and Howell, S. G. and Anderson, B. E. and Winstead, E. and Dibb, J. and Scheuer, E. and Cohen, R. C. and Wooldridge, P. and Perring, A. and Huey, L G. and Kim, S. and Jimenez, J. L. and Dunlea, E. J. and DeCarlo, P. F. and Wennberg, P. O. and Crounse, J. D. and Weinheimer, A. J. and Flocke, F. (2009) Observations of heterogeneous reactions between Asian pollution and mineral dust over the Eastern North Pacific during INTEX-B. Atmospheric Chemistry and Physics, 9 (21). pp. 8283-8308. ISSN 1680-7316. http://resolver.caltech.edu/CaltechAUTHORS:20091211-141548258

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Abstract

In-situ airborne measurements of trace gases, aerosol size distributions, chemistry and optical properties were conducted over Mexico and the Eastern North Pacific during MILAGRO and INTEX-B. Heterogeneous reactions between secondary aerosol precursor gases and mineral dust lead to sequestration of sulfur, nitrogen and chlorine in the supermicrometer particulate size range. Simultaneous measurements of aerosol size distributions and weak-acid soluble calcium result in an estimate of 11 wt% of CaCO_3 for Asian dust. During transport across the North Pacific, ~5–30% of the CaCO_3 is converted to CaSO_4 or Ca(NO_3)_2 with an additional ~4% consumed through reactions with HCl. The 1996 to 2008 record from the Mauna Loa Observatory confirm these findings, indicating that, on average, 19% of the CaCO_3 has reacted to form CaSO_4 and 7% has reacted to form Ca(NO_3)_2 and ~2% has reacted with HCl. In the nitrogen-oxide rich boundary layer near Mexico City up to 30% of the CaCO_3 has reacted to form Ca(NO_3)_2 while an additional 8% has reacted with HCl. These heterogeneous reactions can result in a ~3% increase in dust solubility which has an insignificant effect on their optical properties compared to their variability in-situ. However, competition between supermicrometer dust and submicrometer primary aerosol for condensing secondary aerosol species led to a 25% smaller number median diameter for the accumulation mode aerosol. A 10–25% reduction of accumulation mode number median diameter results in a 30–70% reduction in submicrometer light scattering at relative humidities in the 80–95% range. At 80% RH submicrometer light scattering is only reduced ~3% due to a higher mass fraction of hydrophobic refractory components in the dust-affected accumulation mode aerosol. Thus reducing the geometric mean diameter of the submicrometer aerosol has a much larger effect on aerosol optical properties than changes to the hygroscopic:hydrophobic mass fractions of the accumulation mode aerosol. In the presence of dust, nitric acid concentrations are reduced to <50% of total nitrate (nitric acid plus particulate nitrate). NO_y as a fraction of total nitrogen (NO_y plus particulate nitrate), is reduced from >85% to 60–80% in the presence of dust. These observations support previous model studies which predict irreversible sequestration of reactive nitrogen species through heterogeneous reactions with mineral dust during long-range transport.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://www.atmos-chem-phys.net/9/8283/2009/acp-9-8283-2009.htmlPublisherArticle
https://dx.doi.org/10.5194/acp-9-8283-2009DOIArticle
ORCID:
AuthorORCID
Wennberg, P. O.0000-0002-6126-3854
Crounse, J. D.0000-0001-5443-729X
Additional Information:© Author(s) 2009. This work is distributed under the Creative Commons Attribution 3.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 19 February 2009; Published in Atmos. Chem. Phys. Discuss.: 31 March 2009; revised: 11 September 2009; accepted: 15 September 2009; published: 3 November 2009. We gratefully acknowledge M. Avery for providing DC-8 measurements of O3. We appreciate the use of Barry Huebert’s MLO data, which was collected under NSF grants ATM01-04532 and ATM04-41274. This research was funded under NASA Grant: NNG06GA90G and NSF Grant: ATM05-11521. ED, PFD, and JLJ were supported by NASA grant NNG06GB03G and NSF grant ATM-0513116. We would also like to acknowledge J. Kelly, R. Sullivan and C. Zender for their constructive reviews of the original manuscript. This is SOEST publication number 7622. Edited by: H. Singh.
Funders:
Funding AgencyGrant Number
NSFATM01-04532
NSFATM04-41274
NASANNG06GA90G
NSFATM05-11521
NASANNG06GB03G
NSFATM-0513116
Record Number:CaltechAUTHORS:20091211-141548258
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20091211-141548258
Official Citation:McNaughton, C. S., Clarke, A. D., Kapustin, V., Shinozuka, Y., Howell, S. G., Anderson, B. E., Winstead, E., Dibb, J., Scheuer, E., Cohen, R. C., Wooldridge, P., Perring, A., Huey, L. G., Kim, S., Jimenez, J. L., Dunlea, E. J., DeCarlo, P. F., Wennberg, P. O., Crounse, J. D., Weinheimer, A. J., and Flocke, F.: Observations of heterogeneous reactions between Asian pollution and mineral dust over the Eastern North Pacific during INTEX-B, Atmos. Chem. Phys., 9, 8283-8308, 2009.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:16966
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:16 Dec 2009 22:26
Last Modified:07 Apr 2017 00:02

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