Aerosol‐cloud interactions (ACI) represent a significant source of forcing uncertainty in global climate models (GCMs). Estimates of radiative forcing due to ACI in Fifth Assessment Report range from −0.5 to −2.5 W m−2. A portion of this uncertainty is related to the first indirect, or Twomey, effect whereby aerosols act as nuclei for cloud droplets to condense upon. At constant liquid water content this increases the number of cloud droplets (Nd) and thus increases the cloud albedo. In this study we use remote‐sensing estimates of Nd within stratocumulus regions in combination with state‐of‐the‐art aerosol reanalysis from Modern‐Era Retrospective Analysis for Research and Applications version 2 (MERRA2) to diagnose how aerosols affect Nd. As in previous studies, Nd is related to sulfate mass through a power law relationship. The slope of the log‐log relationship between Nd and SO4 in maritime stratocumulus is found to be 0.31, which is similar to the range of 0.2–0.8 from previous in situ studies and remote‐sensing studies in the pristine Southern Ocean. Using preindustrial emissions models, the change in Nd between preindustrial and present day is estimated. Nd is inferred to have more than tripled in some regions. Cloud properties from Moderate Resolution Imaging Spectroradiometer (MODIS) are used to estimate the radiative forcing due to this change in Nd. The Twomey effect operating in isolation is estimated to create a radiative forcing of −0.97 ± 0.23 W m−2 relative to the preindustrial era.

A common feature of the stratocumulus-to-cumulus transition (SCT) is the presence of layers in which the concentration of particles larger than 0.1 μm is below 10 cm−3. These ultraclean layers (UCLs) are explored using aircraft observations from 14 flights of the NSF–NCAR Gulfstream V (G-V) aircraft between California and Hawaii. UCLs are commonly located in the upper part of decoupled boundary layers, with coverage increasing from less than 5% within 500 km of the California coast to ~30%–60% west of 130°W. Most clouds in UCLs are thin, horizontally extensive layers containing drops with median volume radii ranging from 15 to 30 μm. Many UCL clouds are optically thin and do not fully attenuate the G-V lidar and yet are frequently detected with a 94-GHz radar with a sensitivity of around −30 dB Z. Satellite data indicate that UCL clouds have visible reflectances of ~0.1–0.2 and are often quasi laminar, giving them a veil-like appearance. These optically thin veil clouds exist for 1–3 h or more, are associated with mesoscale cumulus clusters, and likely grow by spreading under strong inversions. Active updrafts in cumulus (Cu) clouds have droplet concentrations of ~25–50 cm−3. Collision–coalescence in the Cu and later sedimentation in the thinner UCL clouds are likely the key processes that remove droplets in UCL clouds. UCLs are relatively quiescent, and a lack of mixing with dry air above and below the cloud may help to explain their longevity. The very low and highly variable droplet concentrations in UCL clouds, together with their low geometrical and optical thickness, make these clouds particularly challenging to represent in large-scale models.

Abstract. Cloud droplet number concentration (CDNC) is the key state variable that moderates the relationship between aerosol and the radiative forcing arising from aerosolcloud interactions. Uncertainty related to the effect of anthropogenic aerosol on cloud properties represents the largest uncertainty in total anthropogenic radiative forcing. Here we show that regionally averaged time series of the ModerateResolution Imaging Spectroradiometer (MODIS) observed CDNC of low, liquid-topped clouds is well predicted by the MERRA2 reanalysis near-surface sulfate mass concentration over decadal timescales. A multiple linear regression between MERRA2 reanalyses masses of sulfate (SO 4 ), black carbon (BC), organic carbon (OC), sea salt (SS), and dust (DU) shows that CDNC across many different regimes can be reproduced by a simple power-law fit to near-surface SO 4 , with smaller contributions from BC, OC, SS, and DU. This confirms previous work using a less sophisticated retrieval of CDNC on monthly timescales. The analysis is supported by an examination of remotely sensed sulfur dioxide (SO 2 ) over maritime volcanoes and the east coasts of North America and Asia, revealing that maritime CDNC responds to changes in SO 2 as observed by the ozone monitoring instrument (OMI). This investigation of aerosol reanalysis and top-down remote-sensing observations reveals that emission controls in Asia and North America have decreased CDNC in their maritime outflow on a decadal timescale.

The Cloud System Evolution in the Trades (CSET) study was designed to describe and explain the evolution of the boundary layer aerosol, cloud, and thermodynamic structures along trajectories within the North Pacific trade winds. The study centered on seven round trips of the National Science Foundation–National Center for Atmospheric Research (NSF–NCAR) Gulfstream V (GV) between Sacramento, California, and Kona, Hawaii, between 7 July and 9 August 2015. The CSET observing strategy was to sample aerosol, cloud, and boundary layer properties upwind from the transition zone over the North Pacific and to resample these areas two days later. Global Forecast System forecast trajectories were used to plan the outbound flight to Hawaii with updated forecast trajectories setting the return flight plan two days later. Two key elements of the CSET observing system were the newly developed High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Cloud Radar (HCR) and the high-spectral-resolution lidar (HSRL). Together they provided unprecedented characterizations of aerosol, cloud, and precipitation structures that were combined with in situ measurements of aerosol, cloud, precipitation, and turbulence properties. The cloud systems sampled included solid stratocumulus infused with smoke from Canadian wildfires, mesoscale cloud–precipitation complexes, and patches of shallow cumuli in very clean environments. Ultraclean layers observed frequently near the top of the boundary layer were often associated with shallow, optically thin, layered veil clouds. The extensive aerosol, cloud, drizzle, and boundary layer sampling made over open areas of the northeast Pacific along 2-day trajectories during CSET will be an invaluable resource for modeling studies of boundary layer cloud system evolution and its governing physical processes.