Atmospheric P solubility affects the amount of P available for phytoplankton in the surface ocean, yet our understanding of the timing and extent of atmospheric P solubility is based on short-term leaching experiments where conditions may differ substantially from the surface ocean. We conducted longer- term dissolution experiments of atmospheric aerosols in filtered seawater, and found up to 9-fold greater dissolution of P after 72 h compared to instantaneous leaching. Samples rich in anthropogenic materials released dissolved inorganic P (DIP) faster than mineral dust. To gauge the effect of biota on the fate of atmospheric P, we conducted field incubations with aerosol samples collected in the Sargasso Sea and Red Sea. In the Sargasso Sea phytoplankton were not P limited, and biological activity enhanced DIP release from aerosols, and aerosols induced biological mineralization of dissolved organic P in seawater, leading to DIP accumulation. However, in the Red Sea where phytoplankton were colimited by P and N, soluble P was rapidly consumed by phytoplankton following aerosol enrichment. Our results suggest that atmospheric P dissolution could continue over multiple days once reaching the surface ocean, and that previous estimates of atmospheric P deposition may underestimate the contribution from this source.