| Summary: | Observations show that the fractional solubility of Fe (FS-Fe, percentage of dissolved to total Fe) in dust aerosol increases considerably from 0.1% in regions of high dust mass concentration to 80% in remote regions where concentrations are low. Here, we combined laboratory geochemical measurements with global aerosol model simulations to test the hypothesis that the increase in FS-Fe is due to physical size sorting during transport. We determined the FS-Fe and fractional solubility of Al (FS-Al) in size-fractionated dust generated from two representative soil samples collected from known Saharan dust source regions using a customized dust re-suspension and collection system. The results show that the FS-Fe is size-dependent and ranges from 0.1-0.3% in the coarse size fractions (> 1 mu m) to similar to 0.2-0.8% in the fine size fractions (< 1 mu m). The FS-Al shows a similar size distribution to that of the FS-Fe. The size-resolved FS-Fe data were then combined with simulated dust mass concentration and size distribution data from a global aerosol model, GLOMAP, to calculate the FS-Fe of dust aerosol over the tropical and subtropical North Atlantic Ocean. We find that the calculated FS-Fe in the dust aerosol increases systematically from similar to 0.1% at high dust mass concentrations (e. g., > 100 mu gm(-3)) to similar to 0.2% at low concentrations (< 100 mu gm(-3)) due to physical size sorting (i.e., particle gravitational settling). These values are one to two orders of magnitude smaller than those observed on cruises across the tropical and sub-tropical North Atlantic Ocean under an important pathway of Saharan dust plumes for similar dust mass concentrations. Even when the FS-Fe of sub-micrometer size fractions (0.18-0.32 mu m, 0.32-0.56 mu m, and 0.56-1.0 mu m) in the model is increased by a factor of 10 over the measured values, the calculated FS-Fe of the dust is still more than an order of magnitude lower than that measured in the field. Therefore, the physical sorting of dust particles ...
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