Abstract. The VAMOS Ocean-Cloud-Atmosphere-Land Regional Experiment (VOCALS-REx) was conducted from 15 October to 15 November 2008 in the South East Pacific (SEP) region to investigate interactions between land, sea and atmosphere in this unique tropical eastern ocean environment and to improve the skill of global and regional models in representing the region. This study synthesises selected aircraft, ship and surface site observations from VOCALSREx to statistically summarise and characterise the atmospheric composition and variability of the Marine Boundary Layer (MBL) and Free Troposphere (FT) along the 20 • S parallel between 70 • W and 85 • W. Significant zonal gradients in mean MBL sub-micron aerosol particle size and composition, carbon monoxide, sulphur dioxide and ozone were seen over the campaign, with a generally more variable and polluted coastal environment and a less variable, more pristine remote maritime regime. Gradients in aerosol and trace gas concentrations were observed to be associated with strong gradients in cloud droplet number. The FT wasCorrespondence to: G. Allen (grant.allen@manchester.ac.uk) often more polluted in terms of trace gases than the MBL in the mean; however increased variability in the FT composition suggests an episodic nature to elevated concentrations. This is consistent with a complex vertical interleaving of airmasses with diverse sources and hence pollutant concentrations as seen by generalised back trajectory analysis, which suggests contributions from both local and longrange sources. Furthermore, back trajectory analysis demonstrates that the observed zonal gradients both in the boundary layer and the free troposphere are characteristic of marked changes in airmass history with distance offshore -coastal boundary layer airmasses having been in recent contact with the local land surface and remote maritime airmasses having resided over ocean for in excess of ten days. Boundary layer composition to the east of 75 • W was observed to be dominated by coastal emissions from sources to the west of the Andes, with evidence for diurnal pumping of the Andean boundary layer above the height of the marine capping inversion. Analysis of intra-campaign variability in atmospheric composition was not found to be significantly correlated with observed low-frequency variability in the large scale flow pattern; campaign-average interquartile ranges of Published by Copernicus Publications on behalf of the European Geosciences Union. 5238 G. Allen et al.: South East Pacific composition during VOCALS-REx CO, SO 2 and O 3 concentrations at all longitudes were observed to dominate over much smaller differences in median concentrations calculated between periods of different flow regimes. The campaign climatology presented here aims to provide a valuable dataset to inform model simulation and future process studies, particularly in the context of aerosolcloud interaction and further evaluation of dynamical processes in the SEP region for conditions analogous to those during VOCALS-REx....

Abstract. The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses.

Abstract. This paper presents a comparison of ice water content (q i ) data from a variety of measurement techniques on the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 research aircraft. Data are presented from a range of cloud types measured during the PIKNMIX field experiment that include mixed-phase stratocumulus, cumulus congestus and cirrus clouds. These measurements cover a broad range of conditions in which atmospheric ice particles are found in nature, such as the low-ice-water-content environments typically found in midlatitude cirrus and the environments with much higher ice water content often observed in cold convective clouds. The techniques include bulk measurements from (i) a Nevzorov hot-wire probe, (ii) the difference between the measured total water content (condensed plus vapour) and the water vapour content of the atmosphere and (iii) a counterflow virtual impactor (CVI) (only for cirrus measurements). We also estimate the q i from integration of the measured particle size distribution (PSD) with assumptions on how the density of ice particles varies as a function of size.The results show that the only bulk ice water content technique capable of measuring high q i values (several g m −3 ) was the method of total water content minus water vapour. For low ice water contents we develop a new parametrisation of the Nevzorov baseline drift that enables the probe to be sensitive to q i ± 0.002 g m −3 . In cirrus clouds the agreement between the Nevzorov and other bulk measurements was typically better than a factor of 2 for the CVI (q i > 0.008 g m −3 ) and the method of total water content minus water vapour (q i > 0.02 g m −3 ). Good agreement with the bulk measurements for all cases could be obtained with the estimate from the PSD provided that appropriate a priori assumptions on the mass-dimension relationship were made. This is problematic in the convective clouds sampled because pristine ice particles, heavily rimed particles and supercooled liquid drops were all present. In a cirrus case, we show that using a temperature-dependent mass-dimension relation was required to match the bulk measurement of q i .

Abstract. This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm−3) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ∼ 1000 cm−3. Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

Abstract. The science guiding the EUREC4A campaign and its measurements is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced ground-based cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement.

Abstract. Representing the number and mass of cloud and aerosol particles independently in a climate, weather prediction or air quality model is important in order to simulate aerosol direct and indirect effects on radiation balance. Here we introduce the first configuration of the UK Met Office Unified Model in which both cloud and aerosol particles have “double-moment” representations with prognostic number and mass. The GLObal Model of Aerosol Processes (GLOMAP) aerosol microphysics scheme, already used in the Hadley Centre Global Environmental Model version 3 (HadGEM3) climate configuration, is coupled to the Cloud AeroSol Interacting Microphysics (CASIM) cloud microphysics scheme. We demonstrate the performance of the new configuration in high-resolution simulations of a case study defined from the CLARIFY aircraft campaign in 2017 near Ascension Island in the tropical southern Atlantic. We improve the physical basis of the activation scheme by representing the effect of existing cloud droplets on the activation of new aerosol, and we also discuss the effect of unresolved vertical velocities. We show that neglect of these two competing effects in previous studies led to compensating errors but realistic droplet concentrations. While these changes lead only to a modest improvement in model performance, they reinforce our confidence in the ability of the model microphysics code to simulate the aerosol–cloud microphysical interactions it was designed to represent. Capturing these interactions accurately is critical to simulating aerosol effects on climate.

Abstract. The science guiding the EUREC4A campaign and its measurements are presented. EUREC4A comprised roughly five weeks of measurements in the downstream winter trades of the North Atlantic – eastward and south-eastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or, or the life-cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso (200 km) and larger (500 km) scales, roughly four hundred hours of flight time by four heavily instrumented research aircraft, four global-ocean class research vessels, an advanced ground-based cloud observatory, a flotilla of autonomous or tethered measurement devices operating in the upper ocean (nearly 10000 profiles), lower atmosphere (continuous profiling), and along the air-sea interface, a network of water stable isotopologue measurements, complemented by special programmes of satellite remote sensing and modeling with a new generation of weather/climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from Brazil Ring Current Eddies to turbulence induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice.

Abstract. Observations of vertically resolved turbulence and cloud microphysics in a mixed-phase altocumulus cloud are presented using in situ measurements from an instrumented aircraft. The turbulence spectrum is observed to have an increasingly negative skewness with distance below cloud top, suggesting that long-wave radiative cooling from the liquid cloud layer is an important source of turbulence kinetic energy. Turbulence measurements are presented from both the liquid cloud layer and ice virga below. Vertical profiles of both bulk and microphysical liquid and ice cloud properties indicate that ice is produced within the liquid layer cloud at a temperature of −30 ∘C. These high-resolution in situ measurements support previous remotely sensed observations from both ground-based and space-borne instruments and could be used to evaluate numerical model simulations of altocumulus clouds at spatial scales from eddy-resolving models to global numerical weather prediction models and climate simulations.