Observations from June to October 2016, from a surface‐based ARM Mobile Facility deployment on Ascension Island (8°S, 14.5°W) indicate that refractory black carbon (rBC) is almost always present within the boundary layer. The rBC mass concentrations, light absorption coefficients, and cloud condensation nuclei concentrations vary in concert and synoptically, peaking in August. Light absorption coefficients at three visible wavelengths as a function of rBC mass are approximately double that calculated from black carbon in lab studies. A spectrally‐flat absorption angstrom exponent suggests most of the light absorption is from lens‐coated black carbon. The single‐scattering‐albedo increases systematically from August to October in both 2016 and 2017, with monthly means of 0.78 ± 0.02 (August), 0.81 ± 0.03 (September), and 0.83 ± 0.03 (October) at the green wavelength. Boundary layer aerosol loadings are only loosely correlated with total aerosol optical depth, with smoke more likely to be present in the boundary layer earlier in the biomass burning season, evolving to smoke predominantly present above the cloud layers in September–October, typically resting upon the cloud top inversion. The time period with the campaign‐maximum near‐surface light absorption and column aerosol optical depth, on 13–16 August 2016, is investigated further. Backtrajectories that indicate more direct boundary layer transport westward from the African continent is central to explaining the elevated surface aerosol loadings.

Marine cloud brightening (MCB) is the deliberate injection of aerosol particles into shallow marine clouds to increase their reflection of solar radiation and reduce the amount of energy absorbed by the climate system. From the physical science perspective, the consensus of a broad international group of scientists is that the viability of MCB will ultimately depend on whether observations and models can robustly assess the scale-up of local-to-global brightening in today’s climate and identify strategies that will ensure an equitable geographical distribution of the benefits and risks associated with projected regional changes in temperature and precipitation. To address the physical science knowledge gaps required to assess the societal implications of MCB, we propose a substantial and targeted program of research—field and laboratory experiments, monitoring, and numerical modeling across a range of scales.

Quantification of the radiative adjustment of marine low clouds to aerosol perturbations, regionally and globally, remains the largest source of uncertainty in assessing current and future climate. One of the important steps towards quantifying the role of aerosol in modifying cloud radiative properties is to quantify the susceptibility of cloud albedo and liquid water path (LWP) to perturbations in cloud droplet number concentration (N_d). We use 10 years of spaceborne observations from the polar-orbiting Aqua satellite to quantify the albedo susceptibility of marine low clouds to N_d perturbations over the northeast (NE) Pacific stratocumulus (Sc) region. Mutual information analysis reveals a dominating control of cloud state (e.g., LWP and N_d) on low-cloud albedo susceptibility, relative to the meteorological states that drive these cloud states. Through a LWP–N_d space decomposition of albedo susceptibilities, we show clear separation among susceptibility regimes (brightening or darkening), consistent with previously established mechanisms through which aerosol modulates cloud properties. These regimes include (i) thin non-precipitating clouds (LWP < 55 g m⁻²) that exhibit brightening (occurring 37 % of the time), corresponding to the Twomey effect; (ii) thicker non-precipitating clouds, corresponding to entrainment-driven negative LWP adjustments that manifest as a darkening regime (36 % of the time); and (iii) another brightening regime (22 % of the time) consisting of mostly precipitating clouds, corresponding to precipitation-suppression LWP positive adjustments. Overall, we find an annual-mean regional low-cloud brightening potential of 20.8±2.68 W m⁻² ln(N_d)⁻¹, despite an overall negative LWP adjustment for non-precipitating marine stratocumulus, owing to the high occurrence of the Twomey–brightening regime. Over the NE Pacific, clear seasonal covariabilities among meteorological factors related to the large-scale circulation are found to play an important role in grouping conditions favorable for each susceptibility regime. When considering the covarying meteorological conditions, our results indicate that for the northeastern Pacific stratocumulus, clouds that exhibit the strongest brightening potential occur most frequently within shallow marine boundary layers over a cool ocean surface with a stable atmosphere and a dry free troposphere above. Clouds that exhibit a darkening potential associated with negative LWP adjustments occur most frequently within deep marine boundary layers in which the atmospheric instability and the ocean surface are not strong and warm enough to produce frequent precipitation. Cloud brightening associated with warm-rain suppression is found to preferably occur either under unstable atmospheric conditions or humid free-tropospheric conditions that co-occur with a warm ocean surface.

Ascension Island (8^∘ S, 14.5^∘ W) is located at the northwestern edge of the south Atlantic stratocumulus deck, with most clouds in August characterized by surface observers as “stratocumulus and cumulus with bases at different levels”, and secondarily as “cumulus of limited vertical extent” and occurring within a typically decoupled boundary layer. Field measurements have previously shown that the highest amounts of sunlight-absorbing smoke occur annually within the marine boundary layer during August. On more smoke-free days, the diurnal cycle in cloudiness includes a nighttime maximum in cloud liquid water path and rain, an afternoon cloud minimum, and a secondary late-afternoon increase in cumulus and rain. The afternoon low-cloud minimum is more pronounced on days with a smokier boundary layer. The cloud liquid water paths are also reduced throughout most of the diurnal cycle when more smoke is present, with the difference from cleaner conditions most pronounced at night. Precipitation is infrequent. An exception is the mid-morning, when the boundary layer deepens and liquid water paths increase. The data support a view that a radiatively enhanced decoupling persisting throughout the night is key to understanding the changes in the cloud diurnal cycle when the boundary layer is smokier. Under these conditions, the nighttime stratiform cloud layer does not always recouple to the sub-cloud layer, and the decoupling maintains more moisture within the sub-cloud layer. After the sun rises, enhanced shortwave absorption in a smokier boundary layer can drive a vertical ascent that momentarily couples the sub-cloud layer to the cloud layer, deepening the boundary layer and ventilating moisture throughout, a process that may also be aided by a shift to smaller droplets. After noon, shortwave absorption within smokier boundary layers again reduces the upper-level stratiform cloud and the sub-cloud relative humidity, discouraging further cumulus development and again strengthening a decoupling that lasts longer into the night. The novel diurnal mechanism provides a new challenge for cloud models to emulate. The lower free troposphere above cloud is more likely to be cooler, when boundary layer smoke is present, and lower free-tropospheric winds are stronger and more northeasterly, with both (meteorological) influences supporting further smoke entrainment into the boundary layer from above.

Marine stratocumuli cool the Earth effectively due to their high reflectance of incoming solar radiation and persistent occurrence. The susceptibility of cloud albedo to droplet number concentration perturbations depends strongly on large-scale meteorological conditions. Studies focused on the meteorological dependence of cloud adjustments often overlook the covariability among meteorological factors and their geographical and temporal variability. We use 8 years of satellite observations sorted by day and geographical location to show the global distribution of marine low-cloud albedo susceptibility. We find an overall cloud brightening potential for most marine warm clouds, which is more pronounced over subtropical coastal regions. A weak cloud darkening potential in the annual mean is evident over the remote SE Pacific and SE Atlantic. We show that large-scale meteorological fields from the ERA5 reanalysis data, including lower-tropospheric stability, free-tropospheric relative humidity, sea surface temperature, and boundary layer depth, have distinct covariabilities over each of the eastern subtropical ocean basins where marine stratocumuli prevail. This leads to a markedly different annual cycle in albedo susceptibility over each basin. Moreover, we find that basin-specific regional relationships between key meteorological factors and albedo susceptibilities are absent in a global analysis. Our results stress the importance of considering the geographical distinctiveness of temporal meteorological covariability when scaling up the local-to-global response of cloud albedo to aerosol perturbations.

Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (∼1–2 K) and greatly enhanced moisture (>2 g kg⁻¹) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.