Shallow convective clouds are common, occurring over many areas of the world, and are an important component in the atmospheric radiation budget. In addition to synoptic and mesoscale meteorological conditions, land–atmosphere interactions and aerosol–radiation–cloud interactions can influence the formation of shallow clouds and their properties. These processes exhibit large spatial and temporal variability and occur at the subgrid scale for all current climate, operational forecast, and cloud-system-resolving models; therefore, they must be represented by parameterizations. Uncertainties in shallow cloud parameterization predictions arise from many sources, including insufficient coincident data needed to adequately represent the coupling of cloud macrophysical and microphysical properties with inhomogeneity in the surface-layer, boundary layer, and aerosol properties. Predictions of the transition of shallow to deep convection and the onset of precipitation are also affected by errors in simulated shallow clouds. Coincident data are a key factor needed to achieve a more complete understanding of the life cycle of shallow convective clouds and to develop improved model parameterizations. To address these issues, the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign was conducted near the Atmospheric Radiation Measurement (ARM) Southern Great Plains site in north-central Oklahoma during the spring and summer of 2016. We describe the scientific objectives of HI-SCALE as well as the experimental approach, overall weather conditions during the campaign, and preliminary findings from the measurements. Finally, we discuss scientific gaps in our understanding of shallow clouds that can be addressed by analysis and modeling studies that use HI-SCALE data.

Published by Copernicus Publications on behalf of the European Geosciences Union. E. Järvinen et al.: Observation of viscosity transition in α-pinene secondary organic aerosolAbstract. Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 • C and 80 % at −38 • C, confirming previous calculations of the viscositytransition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and icenucleation properties of SOA and SOA-coated particles in the atmosphere.

Abstract. Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the CLOUD experiment at CERN, we deployed a new in-situ optical method to detect the viscosity of α-pinene SOA particles and measured their transition from the amorphous viscous to liquid state. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical liquid particles during deliquescence. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.

Abstract. The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and − 10 • C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion -pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and −10 • C, indicating that, in contrast to some previous studies, the oxidation rates of SO 2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, supercooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 • C is correct.

Experimental investigations on the activation of NaCl and Ag aerosol particles by heterogeneous nucleation of n-propanol vapor at well-defined vapor saturation ratios are presented. Particular emphasis is placed on the temperature dependence of this process from -11 to +14 °C. Aerosols are generated in a tube furnace and electrostatically classified at mean geometric mobility equivalent diameters between 3.6 and 11 nm. Activation probabilities are measured by means of expansion chamber experiments, and onset n-propanol saturation ratios are subsequently determined. The experiments with Ag particles do not produce any unexpected results. The results for NaCl particles, however, show a temperature trend of the onset saturation ratios that is opposite to that predicted by classical nucleation theory. This stresses the important role that surface properties play in heterogeneous nucleation processes. By tentatively assuming a temperature-dependent contact angle, we are able to theoretically reproduce this reversed temperature trend. In addition, the shrinkage of NaCl condensation particles is investigated for varying amounts of n-propanol vapor, and contact angle measurements are performed at temperatures ranging from -7 to +30 °C.