Marine boundary layer clouds tend to organize into closed or open mesoscale cellular convection (MCC). Here, two-dimensional wavelet analysis is applied for the first time to passive microwave retrievals of cloud water path (CWP), water vapor path (WVP), and rain rate from AMSR-E in 2008 over the Northeast and Southeast Pacific, and the Southeast Atlantic subtropical stratocumulus to cumulus transition regions. The (co-)variability between CWP, WVP, and rain rate in 160x160 km2 analysis boxes is partitioned between four mesoscale wavelength octaves (20, 40, 80, and 160 km). The cell scale is identified as the wavelength of the peak CWP variance. Together with a machine-learning classification of cell type, this allows the statistical characteristics of open and closed MCC of various scales, and its relation to WVP, rain rate and potential environmental controlling factors to be analyzed across a very large set of cases. The results show that the cell wavelength is most commonly 40-80 km. Cell-scale CWP perturbations are good predictors of the WVP and rain rate perturbations. A universal cubic dependence of rain rate on CWP is found in closed and open cells of all scales. This suggests that aerosol control on precipitation susceptibility is not as important for open cell formation as are processes that cause increases in cloud water. For cells larger than 20 km, there is no obvious dependence of cell scale on the environmental controlling factors tested, suggesting that the cell scale may depend more on its historical evolution than the current environmental conditions.

Biomass-burning emissions impact almost all of the radiative forcing terms considered by the IPCC, yet little is known about smoke aerosol aging in nature beyond a few days. The marine southeast Atlantic free-troposphere is a natural testbed for examining aging through photolysis/oxidation of African continental fire emissions advected westward. In-situ measurements primarily from September, 2016 indicate highly-oxidized aerosol with minimal primary source signatures after 4-9 model-predicted days since emission. Aerosol loses approximately one-half of its organic aerosol over the ocean. The organic aerosol to black carbon mass ratios decrease from 14 to 10, significantly lower than many model predictions. This mass loss, combined with stability in black carbon, supports an observed 20% increase in solar absorptivity. The decreased single scattering albedos, reaching 0.83 at 9 days, arguably represent the lowest values measured globally. The relationship of the aerosol properties to model-derived time since emission suggests a useful new modeling constraint.

The influence of aerosol particles on cloud reflectivity remains one of the largest sources of uncertainty in our understanding anthropogenic climate change. Commercial shipping constitutes a large and concentrated aerosol perturbation in a meteorological regime where clouds have a disproportionally large effect on climate. Yet, to date, studies have been unable to detect climatologically-relevant cloud radiative effects from shipping, despite models indicating that the cloud response should produce a sizable negative radiative forcing (perturbation to Earth’s energy balance). We attribute a significant increase in cloud reflectivity to enhanced cloud droplet number concentrations within a major shipping corridor in the southeast Atlantic. Prevailing winds constrain emissions around the corridor, which cuts through a climatically-important region of expansive low-cloud cover. We use universal kriging, a classic geostatistical method, to estimate what cloud properties would have been in the absence of shipping. In the morning, cloud brightening is consistent with changes in microphysics alone, whereas in the afternoon, increases in cloud brightness from microphysical changes are offset by decreases in the total amount of cloud water. We find a radiative forcing in the southeast Atlantic shipping corridor two orders of magnitude greater than previous observational estimates. Approximately five years of data are required to identify a clear signal. Extrapolating our results globally, we calculate an effective radiative forcing due to aerosol-cloud interactions in low clouds of -0.62 W/m2 (-1.23 to -0.08 W/m2). The unique setup in the southeast Atlantic could be an ideal test for the representation of aerosol-cloud interactions in climate models.

Cloud droplet number concentration (Nd) is a key microphysical property that is largely controlled by the balance between sources and sinks of aerosols that serve as cloud condensation nuclei (CCN). Despite being a key sink of CCN, the impact of coalescence scavenging on Southern Ocean (SO) cloud is poorly known. We apply a simple source-and-sink budget model based on parameterizations to austral summer aircraft observations to test model behavior and examine the relative influence of processes that determine Nd in SO stratocumulus clouds. The model predicts Nd with little bias and a correlation coefficient of ~0.7 compared with observations. Coalescence scavenging is found to be an important sink of CCN in both liquid and mixed-phase precipitating stratocumulus and reduces the predicted Nd by as much as 90% depending on the precipitation rate. The free tropospheric aerosol source controls Nd more strongly than the surface aerosol source during austral summer.