Showing papers by "Karl D. Froyd published in 2011"

Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project

Abstract: . We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion. Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day −1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were emitted and the time they were observed in dense layers above the sea-ice inversion layer.

Hygroscopicity and composition of Alaskan Arctic CCN during April 2008

Abstract: . We present a comprehensive characterization of cloud condensation nuclei (CCN) sampled in the Alaskan Arctic during the 2008 Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project, a component of the POLARCAT and International Polar Year (IPY) initiatives. Four distinct air mass types were sampled including a cleaner Arctic background and a relatively pristine sea ice boundary layer as well as biomass burning and anthropogenic pollution plumes. Despite differences in chemical composition, inferred aerosol hygroscopicities were fairly invariant and ranged from κ = 0.1–0.3 over the atmospherically-relevant range of water vapor supersaturations studied. Organic aerosols sampled were found to be well-oxygenated, consistent with long-range transport and aerosol aging processes. However, inferred hygroscopicities are less than would be predicted based on previous parameterizations of biogenic oxygenated organic aerosol, suggesting an upper limit on organic aerosol hygroscopicity above which κ is less sensitive to the O:C ratio. Most Arctic aerosols act as CCN above 0.1 % supersaturation, although the data suggest the presence of an externally-mixed, non-CCN-active mode comprising approximately 0–20% of the aerosol number. CCN closure was assessed using measured size distributions, bulk chemical composition, and assumed aerosol mixing states; CCN predictions tended toward overprediction, with the best agreement (±0–20 %) obtained by assuming the aerosol to be externally-mixed with soluble organics. Closure also varied with CCN concentration, and the best agreement was found for CCN concentrations above 100 cm −3 with a 1.5- to 3-fold overprediction at lower concentrations.

Cloud condensation nuclei as a modulator of ice processes in Arctic mixed-phase clouds

Abstract: We propose that cloud condensation nuclei (CCN) concentrations are important for modulating ice formation of Arctic mixed-phase clouds, through modification of the droplet size distribution. Aircraft observations from the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) study in northern Alaska in April 2008 allow for identification and characterization of both aerosol and trace gas pollutants, which are then compared with cloud microphysical properties. Consistent with previous studies, we find that the concentration of precipitating ice particles ( > 400 µm) is correlated with the concentration of large droplets (> 30 µm). We are further able to link the observed micro- physical conditions to aerosol pollution, originating mainly from long range transport of biomass burning emissions. The case studies demonstrate that polluted mixed-phase clouds have narrower droplet size distributions and contain 1-2 or- ders of magnitude fewer precipitating ice particles than clean clouds at the same temperature. This suggests an aerosol in- direct effect leading to greater cloud lifetime, greater cloud emissivity, and reduced precipitation. This result is opposite to the glaciation indirect effect, whereby polluted clouds are expected to precipitate more readily due to an increase in the concentration of particles acting as ice nuclei.

In situ measurements of tropospheric volcanic plumes in Ecuador and Colombia during TC4

Abstract: A NASA DC-8 research aircraft penetrated tropospheric gas and aerosol plumes sourced from active volcanoes in Ecuador and Colombia during the Tropical Composition, Cloud and Climate Coupling (TC^4) mission in July–August 2007. The likely source volcanoes were Tungurahua (Ecuador) and Nevado del Huila (Colombia). The TC^4 data provide rare insight into the chemistry of volcanic plumes in the tropical troposphere and permit a comparison of SO_2 column amounts measured by the Ozone Monitoring Instrument (OMI) on the Aura satellite with in situ SO_2 measurements. Elevated concentrations of SO_2, sulfate aerosol, and particles were measured by DC-8 instrumentation in volcanic outflow at altitudes of 3–6 km. Estimated plume ages range from ~2 h at Huila to ~22–48 h downwind of Ecuador. The plumes contained sulfate-rich accumulation mode particles that were variably neutralized and often highly acidic. A significant fraction of supermicron volcanic ash was evident in one plume. In-plume O_3 concentrations were ~70%–80% of ambient levels downwind of Ecuador, but data are insufficient to ascribe this to O_3 depletion via reactive halogen chemistry. The TC^4 data record rapid cloud processing of the Huila volcanic plume involving aqueous-phase oxidation of SO_2 by H_2O_2, but overall the data suggest average in-plume SO_2 to sulfate conversion rates of ~1%–2% h^(−1). SO_2 column amounts measured in the Tungurahua plume (~0.1–0.2 Dobson units) are commensurate with average SO_2 columns retrieved from OMI measurements in the volcanic outflow region in July 2007. The TC^4 data set provides further evidence of the impact of volcanic emissions on tropospheric acidity and oxidizing capacity.