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Sanchez, KJ, Roberts GC, Calmer R, Nicoll K, Hashimshoni E, Rosenfeld D, Ovadnevaite J, Preissler J, Ceburnis D, O'Dowd C, Russell LM.  2017.  Top-down and bottom-up aerosol-cloud closure: towards understanding sources of uncertainty in deriving cloud shortwave radiative flux. Atmospheric Chemistry and Physics. 17:9797-9814.   10.5194/acp-17-9797-2017   AbstractWebsite

Top-down and bottom-up aerosol-cloud shortwave radiative flux closures were conducted at the Mace Head Atmospheric Research Station in Galway, Ireland, in August 2015. This study is part of the BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) European collaborative project, with the goal of understanding key processes affecting aerosol-cloud shortwave radiative flux closures to improve future climate predictions and develop sustainable policies for Europe. Instrument platforms include ground-based unmanned aerial vehicles (UAVs)(1) and satellite measurements of aerosols, clouds and meteorological variables. The ground-based and airborne measurements of aerosol size distributions and cloud condensation nuclei (CCN) concentration were used to initiate a 1-D microphysical aerosol-cloud parcel model (ACPM). UAVs were equipped for a specific science mission, with an optical particle counter for aerosol distribution profiles, a cloud sensor to measure cloud extinction or a five-hole probe for 3D wind vectors. UAV cloud measurements are rare and have only become possible in recent years through the miniaturization of instrumentation. These are the first UAV measurements at Mace Head. ACPM simulations are compared to in situ cloud extinction measurements from UAVs to quantify closure in terms of cloud shortwave radiative flux. Two out of seven cases exhibit sub-adiabatic vertical temperature profiles within the cloud, which suggests that entrainment processes affect cloud microphysical properties and lead to an overestimate of simulated cloud shortwave radiative flux. Including an entrainment parameterization and explicitly calculating the entrainment fraction in the ACPM simulations both improved cloud-top radiative closure. Entrainment reduced the difference between simulated and observation-derived cloud-top shortwave radiative flux (delta RF) by between 25 and 60Wm(-2). After accounting for entrainment, satellite-derived cloud droplet number concentrations (CDNCs) were within 30% of simulated CDNC. In cases with a well-mixed boundary layer, delta RF is no greater than 20Wm(-2) after accounting for cloud-top entrainment and up to 50Wm(-2) when entrainment is not taken into account. In cases with a decoupled boundary layer, cloud microphysical properties are inconsistent with ground-based aerosol measurements, as expected, and delta RF is as high as 88Wm(-2), even high (> 30Wm(-2)) after accounting for cloud-top entrainment. This work demonstrates the need to take in situ measurements of aerosol properties for cases where the boundary layer is decoupled as well as consider cloud-top entrainment to accurately model stratocumulus cloud radiative flux.

Ovadnevaite, J, Zuend A, Laaksonen A, Sanchez KJ, Roberts G, Ceburnis D, Decesari S, Rinaldi M, Hodas N, Facchini MC, Seinfeld JH, Dowd CO.  2017.  Surface tension prevails over solute effect in organic-influenced cloud droplet activation. Nature. 546:637-641.   10.1038/nature22806   AbstractWebsite

The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Kohler theory(1,2). This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants(1). Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet-vapour interface(3,4). Here we present observational and theoretical evidence illustrating that, in ambient air, surface tension lowering can prevail over the reduction in the Raoult effect, leading to substantial increases in cloud droplet concentrations. We suggest that consideration of liquid-liquid phase separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, can explain the lack of concomitant reduction of the Raoult effect, while maintaining substantial lowering of surface tension, even for partial surface coverage. Apart from the importance of particle size and composition in droplet activation, we show by observation and modelling that incorporation of phase-separation effects into activation thermodynamics can lead to a CCN number concentration that is up to ten times what is predicted by climate models, changing the properties of clouds. An adequate representation of the CCN activation process is essential to the prediction of clouds in climate models, and given the effect of clouds on the Earth's energy balance, improved prediction of aerosol-cloud-climate interactions is likely to result in improved assessments of future climate change.