Understanding the nature of atmospheric acid processing of mineral dusts in supplying bioavailable phosphorus to the oceans.

Acidification of airborne dust particles can dramatically increase the amount of bioavailable phosphorus (P) deposited on the surface ocean. Experiments were conducted to simulate atmospheric processes and determine the dissolution behavior of P compounds in dust and dust precursor soils. Acid dissolution occurs rapidly (seconds to minutes) and is controlled by the amount of H+ ions present. For H+ < 10-4 mol/g of dust, 1-10% of the total P is dissolved, largely as a result of dissolution of surface-bound forms. At H+ > 10-4 mol/g of dust, the amount of P (and calcium) released has a direct proportionality to the amount of H+ consumed until all inorganic P minerals are exhausted and the final pH remains acidic. Once dissolved, P will stay in solution due to slow precipitation kinetics. Dissolution of apatite-P (Ap-P), the major mineral phase in dust (79-96%), occurs whether calcium carbonate (calcite) is present or not, although the increase in dissolved P is greater if calcite is absent or if the particles are externally mixed. The system was modeled adequately as a simple mixture of Ap-P and calcite. P dissolves readily by acid processes in the atmosphere in contrast to iron, which dissolves more slowly and is subject to reprecipitation at cloud water pH. We show that acidification can increase bioavailable P deposition over large areas of the globe, and may explain much of the previously observed patterns of variability in leachable P in oceanic areas where primary productivity is limited by this nutrient (e.g., Mediterranean).

Sensitivity of liquid clouds to homogenous freezing parameterizations.

Water droplets in some clouds can supercool to temperatures where homogeneous ice nucleation becomes the dominant freezing mechanism. In many cloud resolving and mesoscale models, it is assumed that homogeneous ice nucleation in water droplets only occurs below some threshold temperature typically set at -40°C. However, laboratory measurements show that there is a finite rate of nucleation at warmer temperatures. In this study we use a parcel model with detailed microphysics to show that cloud properties can be sensitive to homogeneous ice nucleation as warm as -30°C. Thus, homogeneous ice nucleation may be more important for cloud development, precipitation rates, and key cloud radiative parameters than is often assumed. Furthermore, we show that cloud development is particularly sensitive to the temperature dependence of the nucleation rate. In order to better constrain the parameterization of homogeneous ice nucleation laboratory measurements are needed at both high (>-35°C) and low (<-38°C) temperatures. KEY POINTS: Homogeneous freezing may be significant as warm as -30°CHomogeneous freezing should not be represented by a threshold approximationThere is a need for an improved parameterization of homogeneous ice nucleation.