1School of Ocean and Earth Science and Technology, University of Hawaii, Honolulu, HI, 96822, USA
2NASA Langley Research Center, Hampton, VA, 23665, USA
3University of New Hampshire, Durham, NH, 03824, USA
4University of California Berkeley, Berkeley, CA, 94720, USA
5Georgia Institute of Technology, Atlanta, GA, 30332, USA
6Cooperative Institute for Research in Environmental Sciences (CIRES) and University of Colorado, Boulder, CO, 80309, USA
7California Institute of Technology, Pasadena, CA, 91125, USA
8National Center for Atmospheric Research, Boulder CO, 80307, USA
*now at: NASA Ames Research Center, Moffett Field, CA, 94035, USA
**now at: Paul Scherrer Institute, Switzerland
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 during long-range transport lead to irreversible sequestration of sulfur and nitrogen compounds 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 CaCO3 for Asian dust. During transport across the North Pacific, 10–30% of the CaCO3 is converted to CaSO4 or Ca(NO3)2 through reactions with trace gases. The 11-year record from the Mauna Loa Observatory confirm these findings, indicating that, on average, 16% of the CaCO3 has reacted to form CaSO4 and 14% has reacted to form Ca(NO3)2. Heterogeneous reactions resulting in ~3% increase in dust solubility is shown to have 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 optics than changes to the hygroscopic:hydrophobic mass fractions of the aerosol.
In the presence of dust, nitric acid concentrations are reduced to <50% of total nitrate (nitric acid plus particulate nitrate). NOy as a fraction of total nitrogen (NOy 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.