ALBERT

Description: We present a case study (20 September to 13 October 2015) of synergistic, multi-instrument observations of aerosols, clouds, and the marine boundary layer (MBL) at the Eastern North Atlantic (ENA) Atmospheric Radiation Measurement site centered on a period of exceptionally low (20–50 cm−3) surface accumulation mode (0.1–1 μm) aerosol particle number concentrations. We divide the case study into three regimes (high, clean, and ultraclean) based on daily median number concentrations and compare finer resolution (hourly or less) observations between these regimes. The analysis focuses on the possibility of using these ultraclean events to study pristine conditions in the remote MBL, as well as examining evidence for a recently proposed conceptual model for the large-scale depletion of cloud condensation nuclei-sized particles in postfrontal air masses. Relative to the high and clean regimes, the ultraclean regime tends to exhibit significantly fewer particles between 0.1 and 0.4 μm in diameter and a relatively increased prevalence of larger accumulation mode particles. In addition, supermicron particles tend to dominate total scattering in the ultraclean regime, and there is little evidence for absorbing aerosol. These observations are more in-line with a heavily scavenged but natural marine aerosol population and minimal contribution from continental sources such as anthropogenic pollution, biomass burning, or dust. The air masses with the consistently lowest accumulation mode aerosol number concentrations are largely dominated by heavily drizzling clouds with high liquid water path cores, deep decoupled boundary layers, open cellular organization, and notable surface forcing of subcloud turbulence, even at night. ©2017. American Geophysical Union. All Rights Reserved.

Description: We study forty-one days with daily median surface accumulation mode aerosol particle concentrations below 50 cm−3 (ultra-clean conditions) observed at Ascension Island (7.9° S, 14.4° W) between June 2016 and October 2017 as part of the Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign. Interestingly, these days occur during a period of great relevance for aerosol-cloud-radiation interactions, the southeast Atlantic (SEATL) biomass-burning season (approximately June–October). That means that these critical months can feature both the highest surface aerosol numbers, from smoke intrusion into the marine boundary layer, as well as the lowest. While carbon monoxide and refractory black carbon concentrations on ultra-clean days do not approach those on days with heavy smoke, they also frequently exceed background concentrations calculated in the non-burning season from December 2016–April 2017. This is evidence that even what become ultra-clean boundary layers can make contact with and entrain from an overlying SEATL smoke layer before undergoing a process of rapid aerosol removal. Because many ultra-clean and polluted boundary layers observed at Ascension Island follow similar isobaric back-trajectories, the variability in this entrainment is likely closely tied to the variability in the overlying smoke rather than large-scale horizontal circulation through the boundary layer. Finally, surface drizzle rates, frequencies and accumulation – as well as retrievals of liquid water path – all consistently tend toward higher values on ultra-clean days. This implicates enhanced coalescence scavenging in low clouds as the key driver of ultra-clean events in the southeast Atlantic marine boundary layer. These enhancements occur against and are likely mediated by the backdrop of a seasonal increase in daily mean cloud fraction and daily median liquid water path over ASI, peaking in September and October in both LASIC years. Therefore the seasonality in ultra-clean day occurrence seems directly linked to the seasonality in SEATL cloud properties. These results highlight the importance of two-way aerosol-cloud interactions in the region.

Description: The aerosol first indirect effect (FIE) is typically characterized by a reduction in cloud droplet size and an increase in cloud optical thickness in the presence of high concentrations of condensation nuclei. Past studies have derived observational evidence of the FIE in specific locations and conditions, yet critical uncertainties in the validity of this conceptual model as it applies to a range of cloud types and meteorological settings remain unaddressed. We utilize five years of surface aerosol measurements and Moderate Resolution Imaging Spectroradiometer (MODIS) observations of cloud properties to discern the FIE in springtime cloud statistics over the Southern Great Plains region of the United States. We extend this analysis to explore the role of three confounding factors: cloud phase, observational uncertainty and the role of regional meridional flow. While high aerosol days are dominated by smaller average droplet size in liquid clouds, the response of cloud optical thickness is variable and is dominantly a function of cloud water path. Ice clouds experience more variability in their response to high aerosol loading and satellite retrieval uncertainty thresholds. Finally, the direction of meridional flow does not play a large role in stratifying the cloud response to different aerosol loading. Overall, these observations show that much of the classical theory for liquid clouds is supported. Higher aerosol loadings are correlated with a reduction in effective radius and generally higher cloud optical thickness, and this relationship dominates over any driving influence from the low-level jet. However, for ice clouds we see a variable response that may be driven by aerosol composition and cold cloud microphysics. These observations provide further insight into the importance of considering deviations from the classic FIE in understanding regional variability in aerosol-cloud interactions in a continental setting.

Description: We study 41 d with daily median surface accumulation mode aerosol particle concentrations below 50 cm−3 (ultra-clean conditions) observed at Ascension Island (ASI; 7.9∘ S, 14.4∘ W) between June 2016 and October 2017 as part of the Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign. Interestingly, these days occur during a period of great relevance for aerosol–cloud–radiation interactions, the southeast Atlantic (SEATL) biomass-burning season (approximately June–October). That means that these critical months can feature both the highest surface aerosol numbers, from smoke intrusion into the marine boundary layer, as well as the lowest. While carbon monoxide and refractory black carbon concentrations on ultra-clean days do not approach those on days with heavy smoke, they also frequently exceed background concentrations calculated in the non-burning season from December 2016 to April 2017. This is evidence that even what become ultra-clean boundary layers can make contact with and entrain from an overlying SEATL smoke layer before undergoing a process of rapid aerosol removal. Because many ultra-clean and polluted boundary layers observed at Ascension Island during the biomass burning season follow similar isobaric back trajectories, the variability in this entrainment is likely more closely tied to the variability in the overlying smoke rather than large-scale horizontal circulation through the boundary layer. Since exceptionally low accumulation mode aerosol numbers at ASI do not necessarily indicate the relative lack of other trace pollutants, this suggests the importance of regional variations in what constitutes an “ultra-clean” marine boundary layer. Finally, surface drizzle rates, frequencies and accumulation – as well as retrievals of liquid water path – all consistently tend toward higher values on ultra-clean days. This implicates enhanced coalescence scavenging in low clouds as the key driver of ultra-clean events in the southeast Atlantic marine boundary layer. These enhancements occur against and are likely mediated by the backdrop of a seasonal increase in daily mean cloud fraction and daily median liquid water path over ASI, peaking in September and October in both LASIC years. Therefore the seasonality in ultra-clean day occurrence seems directly linked to the seasonality in SEATL cloud properties. These results highlight the importance of two-way aerosol–cloud interactions in the region.