Publications

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2009
Sullivan, RC, Moore MJK, Petters MD, Kreidenweis SM, Roberts GC, Prather KA.  2009.  Timescale for hygroscopic conversion of calcite mineral particles through heterogeneous reaction with nitric acid. Physical Chemistry Chemical Physics. 11:7826-7837.   10.1039/b904217b   AbstractWebsite

Atmospheric heterogeneous reactions can potentially change the hygroscopicity of atmospheric aerosols as they undergo chemical aging processes in the atmosphere. A particle's hygroscopicity influences its cloud condensation nuclei (CCN) properties with potential impacts on cloud formation and climate. In this study, size-selected calcite mineral particles were reacted with controlled amounts of nitric acid vapour over a wide range of relative humidities in an aerosol flow tube to study the conversion of insoluble and thus apparently non-hygroscopic calcium carbonate into soluble and hygroscopic calcium nitrate. The rate of hygroscopic change particles undergo during a heterogeneous reaction is derived from experimental measurements for the first time. The chemistry of the reacted particles was determined using an ultra. ne aerosol time-of-flight mass spectrometer (UF-ATOFMS) while the particles' hygroscopicity was determined through measuring CCN activation curves fit to a single parameter of hygroscopicity, kappa. The reaction is rapid, corresponding to atmospheric timescales of hours. At low to moderate HNO(3) exposures, the increase in the hygroscopicity of the particles is a linear function of the HNO(3)(g) exposure. The experimentally observed conversion rate was used to constrain a simple but accurate kinetic model. This model predicts that calcite particles will be rapidly converted into hygroscopic particles (kappa > 0.1) within 4 h for low HNO(3) mixing ratios (10 pptv) and in less than 3 min for 1000 pptv HNO(3). This suggests that the hygroscopic conversion of the calcite component of atmospheric mineral dust aerosol will be controlled by the availability of nitric acid and similar reactants, and not by the atmospheric residence time.

2008
Roberts, GC, Ramana MV, Corrigan C, Kim D, Ramanathan V.  2008.  Simultaneous observations of aerosol-cloud-albedo interactions with three stacked unmanned aerial vehicles. Proceedings of the National Academy of Sciences of the United States of America. 105:7370-7375.   10.1073/pnas.0710308105   AbstractWebsite

Aerosol impacts on climate change are still poorly understood, in part, because the few observations and methods for detecting their effects are not well established. For the first time, the enhancement in cloud albedo is directly measured on a cloud-by-cloud basis and linked to increasing aerosol concentrations by using multiple autonomous unmanned aerial vehicles to simultaneously observe the cloud microphysics, vertical aerosol distribution, and associated solar radiative fluxes. In the presence of long-range transport of dust and anthropogenic pollution, the trade cumuli have higher droplet concentrations and are on average brighter. Our observations suggest a higher sensitivity of radiative forcing by trade cumuli to increases in cloud droplet concentrations. than previously reported owing to a constrained droplet radius such that increases in droplet concentrations also increase cloud liquid water content. This aerosol-cloud forcing efficiency is as much as -60 W m(-2) per 100% percent cloud fraction for a doubling of droplet concentrations and associated increase of liquid water content. Finally, we develop a strategy for detecting aerosol-cloud interactions based on a nondimensional scaling analysis that relates the contribution of single clouds to albedo measurements and illustrates the significance of characterizing cloud morphology in resolving radiometric measurements. This study demonstrates that aerosol-cloud-albedo interactions can be directly observed by simultaneous observations below, in, and above the clouds.