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Optical measurements of the microphysical properties of aerosol and small cloud particles in the CLOUD project
[Thesis]. Manchester, UK: The University of Manchester; 2017.
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Abstract
Clouds play an important role in precipitation, solar radiation budget and electrification of Earth’s atmosphere. The presence of small ice crystals in clouds and their morphology can complicate parametrisation and climate modelling, consequently leading to a net cooling feedback on climate. In situ airborne measurements provide single particle characterisation with high temporal and spatial resolution allowing better understanding of atmosphericprocesses of ice nucleation and growth. Simulations of the preindustrial clouds and accurate characterisation and comparison of the instruments require a well-controlled and often pristine environment. The experimental chamber setup allows simulations of these and other conditions.The microphysical features of the micrometric ice particles in clouds were examined in a laboratory setup, at numerous sub-zero temperatures [-10 to -50 ⁰C]. The following instruments were sampling the content of the CLOUD chamber air volume: Cloud and Aerosol Spectrometer with Polarisation (CASPOL), Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition), 3-View Cloud Particle Imager (3V-CPI), and the Scattering-Intensity-Measurements-for-the-Optical-detectioN-of-icE (SIMONE-Junior). Cluster analysis was applied to the data collected with CASPOL and compared with results from the other probes. We were able to discriminate and map the aerosol and cloud particles in the pristine chamber environment using polarisation ratios (Dpol/Backscatter and Dpol/Forwardscatter) of the scattered light. We demonstrate the sensitivity of the instruments in detecting secondary organic aerosol (SOA) phase transitions. Then, we show the ability of the viscous SOA to nucleate ice in a series of SPectrometer for Ice Nuclei (SPIN) measurements. The detected viscous SOA ice nucleation efficiency may affect global modelling and estimations of ice water content in the atmosphere.Subsequently, the analysis and discrimination technique used in the CLOUD chamber was applied to airborne measurements to test its efficiency and to retrieve the composition of clouds. Data from four flight campaigns on board of the FAAM BAe-146 were analysed: Aerosol-Cloud Coupling and Climate Interactions in the Arctic (ACCACIA), COnvective-Precipitation-Experiment (COPE) in south England, CIRrus Coupled Cloud-Radiation EXperiment (CIRCCREX), and PIKNMIX in Scotland. In these and other flights, we were able to identify unique clusters such as salts, minerals, organics, volcanic ash, water and ice, confirming some of the offline laboratory elemental analysis results, and providing complementary information.Single particle polarisation measurements were compared with bulk depolarisation, diffraction patterns, and imaging. Most of the optical instruments still suffer from ambiguity in phase derivation (i.e. water/ice) of optically spherical small shapes. We discuss some of the limitations of optical cloud particle discrimination in different ambient conditions and offer possible solutions to reduce the uncertainty, e.g., surface complexity derivation from scatteringpatterns. Our findings will help to develop better instruments and improve the models which are used for weather forecasts and climate change predictions.