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 alone is unlikely to be an important factor in the observed inverse relationship between the FS-Fe and FS-Al and the atmospheric mineral dust mass concentrations. The results suggest that processes such as chemical reactions and/or mixing with combustion particles are the main mechanisms to cause the increased FS-Fe in long-range transported dust aerosols.