Atmospheric inputs of iron to the open ocean are hypothesized to modulate ocean biogeochemistry. This review presents an integration of available observations of atmospheric iron and iron deposition, and also covers bioavailable iron distributions. Methods for estimating temporal variability in ocean deposition over the recent past are reviewed. Desert dust iron is estimated to represent 95% of the global atmospheric iron cycle, and combustion sources of iron are responsible for the remaining 5%. Humans may be significantly perturbing desert dust (up to 50%). The sources of bioavailable iron are less well understood than those of iron, partly because we do not know what speciation of the iron is bioavailable. Bioavailable iron can derive from atmospheric processing of relatively insoluble desert dust iron or from direct emissions of soluble iron from combustion sources. These results imply that humans could be substantially impacting iron and bioavailable iron deposition to ocean regions, but there are large uncertainties in our understanding.

[1] Iron is hypothesized to be an important micronutrient for ocean biota, thus modulating carbon dioxide uptake by the ocean biological pump. Studies have assumed that atmospheric deposition of iron to the open ocean is predominantly from mineral aerosols. For the first time we model the source, transport, and deposition of iron from combustion sources. Iron is produced in small quantities during fossil fuel burning, incinerator use, and biomass burning. The sources of combustion iron are concentrated in the industrialized regions and biomass burning regions, largely in the tropics. Model results suggest that combustion iron can represent up to 50% of the total iron deposited, but over open ocean regions it is usually less than 5% of the total iron, with the highest values (<30%) close to the East Asian continent in the North Pacific. For ocean biogeochemistry the bioavailability of the iron is important, and this is often estimated by the fraction which is soluble (Fe(II)). Previous studies have argued that atmospheric processing of the relatively insoluble Fe(III) occurs to make it more soluble (Fe(II)). Modeled estimates of soluble iron amounts based solely on atmospheric processing as simulated here cannot match the variability in daily averaged in situ concentration measurements in Korea, which is located close to both combustion and dust sources. The best match to the observations is that there are substantial direct emissions of soluble iron from combustion processes. If we assume observed soluble Fe/black carbon ratios in Korea are representative of the whole globe, we obtain the result that deposition of soluble iron from combustion contributes 20-100% of the soluble iron deposition over many ocean regions. This implies that more work should be done refining the emissions and deposition of combustion sources of soluble iron globally.

Shallow, maritime cumuli are ubiquitous over much of the tropical oceans, and characterizing their properties is important to understanding weather and climate. The Rain in Cumulus over the Ocean (RICO) field campaign, which took place during November 2004–January 2005 in the trades over the western Atlantic, emphasized measurements of processes related to the formation of rain in shallow cumuli, and how rain subsequently modifies the structure and ensemble statistics of trade wind clouds. Eight weeks of nearly continuous S-band polarimetric radar sampling, 57 flights from three heavily instrumented research aircraft, and a suite of ground- and ship-based instrumentation provided data on trade wind clouds with unprecedented resolution. Observational strategies employed during RICO capitalized on the advances in remote sensing and other instrumentation to provide insight into processes that span a range of scales and that lie at the heart of questions relating to the cause and effects of rain from shallow maritime cumuli.

[1] Cloud responses to changes in aerosol remain a dominant uncertainty in the radiative forcing of climate. Two main constructs related to aerosol effects on clouds have been postulated: (i) the ''albedo effect'' whereby anthropogenic aerosol results in increased droplet concentrations that generate increases in cloud albedo, all else (particularly cloud water) being equal; (ii) the ''lifetime effect'' whereby anthropogenic aerosol suppresses precipitation and results in clouds with more liquid water, higher fractional cloudiness, and longer lifetimes. Based on new observations presented here, and supported by previous fine-scale modeling studies, we suggest that the balance of evidence shows that non-precipitating cumulus clouds can experience an evaporation-entrainment feedback, and respond to aerosol perturbations in a manner inconsistent with the traditional ''lifetime effect.'' Because most cumulus clouds evaporate without producing significant precipitation, this is particularly relevant to estimates of aerosol indirect effects on climate.

Under certain conditions mass transfer limitations on the growth of cloud condensation nuclei (CCN) may have a significant impact on the number of droplets that can form in a cloud. The assumption that particles remain in equilibrium until activated may therefore not always be appropriate for aerosol populations existing in the atmosphere. This work identifies three mechanisms that lead to kinetic limitations, the effect of which on activated cloud droplet number and cloud albedo is assessed using a one-dimensional cloud parcel model with detailed microphysics for a variety of aerosol size distributions and updraft velocities. In assessing the effect of kinetic limitations, we have assumed as cloud droplets not only those that are strictly activated (as dictated by classical Kö hler theory), but also unactivated drops large enough to have an impact on cloud optical properties. Aerosol number concentration is found to be the key parameter that controls the significance of kinetic effects. Simulations indicate that the equilibrium assumption leads to an overprediction of droplet number by less than 10% for marine aerosol; this overprediction can exceed 40% for urban type aerosol. Overall, the effect of kinetic limitations on cloud albedo can be considered important when equilibrium activation theory consistently overpredicts droplet number by more than 10%. The maximum change in cloud albedo as a result of kinetic limitations is less than 0.005 for cases such as marine aerosol; however albedo differences can exceed 0.1 under more polluted conditions. Kinetic limitations are thus not expected to be climatically significant on a global scale, but can regionally have a large impact on cloud albedo.