Mineral aerosol deposition is the dominant source of iron to the open ocean. Soil iron is typically insoluble and understanding the atmospheric processes that convert insoluble iron to the more soluble forms observed over the oceans is crucial. In this paper, we model several proposed processes for the conversion of Fe(III) to Fe(II), and compare with cruise observations. The comparisons show that the model results in similar averaged magnitudes of iron solubility as measured during 8 cruises in 2001–2003. Comparisons show that results of cases including cloud, SO₂ and hematite processing are better than the other approaches used using the reaction rates we assume in this paper; unfortunately the reaction rates are not well known, and this hampers our ability to conclusive show one process is more likely than another. The total soluble iron deposited to the global ocean is estimated by the model to range from 0.36 to 1.6 Tg y⁻¹, with 0.88 Tg y⁻¹ being the mean estimate; however there are large uncertainties in these estimates. Comparison shows that the regions with largest differences between the model simulations and observations of iron solubility are in the Southern Atlantic near South America coast and North Atlantic near Spain coast. More observations in these areas or in the South Pacific will help us identify the most important processes. Additionally, laboratory experiments that constrain the reaction rates of different compounds that will result in a net solubilization of iron in aerosols are required to better constrain iron processing in the atmosphere. Additionally, knowing what forms of iron are most bioavailable will assist atmospheric scientists in providing better budgets of iron deposited to the ocean surfaces.