1NASA Langley Research Center, Hampton, VA 23681-0001, USA
2Dept. Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, USA
3Division of Engineering and Applied Science, Harvard University, Cambridge, MA 02138 USA
4Climate Change Research Center, University of New Hampshire, Durham, NH 03824, USA
5Dept. Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
6Dept. Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, B3H 4R2, Canada
Received: 18 Oct 2009 – Published in Atmos. Chem. Phys. Discuss.: 17 Nov 2009
Abstract. We use a 3-D global chemical transport model (GEOS-Chem) to interpret aircraft observations of nitrate and sulfate partitioning in transpacific dust plumes during the INTEX-B campaign of April–May 2006. The model includes explicit transport of size-resolved mineral dust and its alkalinity, nitrate, and sulfate content. The observations show that particulate nitrate is primarily associated with dust, sulfate is primarily associated with ammonium, and Asian dust remains alkaline across the Pacific. This can be reproduced in the model by using a reactive uptake coefficient for HNO3 on dust (γ(HNO3) ~10−3) much lower than commonly assumed in models and possibly reflecting limitation of uptake by dust dissolution. The model overestimates gas-phase HNO3 by a factor of 2–3, typical of previous model studies; we show that this cannot be corrected by uptake on dust. We find that the fraction of aerosol nitrate on dust in the model increases from ~30% in fresh Asian outflow to 80–90% over the Northeast Pacific, reflecting in part the volatilization of ammonium nitrate and the resulting transfer of nitrate to the dust. Consumption of dust alkalinity by uptake of acid gases in the model is slow relative to the lifetime of dust against deposition, so that dust does not acidify (at least not in the bulk). This limits the potential for dust iron released by acidification to become bio-available upon dust deposition. Observations in INTEX-B show no detectable ozone depletion in Asian dust plumes, consistent with the model. Uptake of HNO3 by dust, suppressing its recycling to NOx, reduces Asian pollution influence on US surface ozone in the model by 10–15% or up to 1 ppb.
Revised: 22 Mar 2010 – Accepted: 31 Mar 2010 – Published: 29 Apr 2010
Fairlie, T. D., Jacob, D. J., Dibb, J. E., Alexander, B., Avery, M. A., van Donkelaar, A., and Zhang, L.: Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes, Atmos. Chem. Phys., 10, 3999-4012, doi:10.5194/acp-10-3999-2010, 2010.