Accurate representations of clouds are required in large-scale weather and climate models to make detailed and precise predictions of the Earth's weather and climate. Representations of clouds within these models are limited by the present understanding of the role of aerosols in the microphysical processes responsible for cloud formation and development. As part of a NERC funded CASE studentship with the Met Office, this thesis aims to test new aerosol-dependent mixed-phase cloud parametrizations by obtaining extensive cloud microphysical measurements in-situ and comparing and contrasting them with model simulations. Cloud particle concentrations were measured during the Ice NUcleation Process Investigation And Quantification (INUPIAQ) field campaign at Jungfraujoch in Switzerland. A new probe was used to separate droplet and small ice concentrations by using depolarisation ratio and size thresholds. Whilst the new small ice crystal and droplet number concentrations compared favourably with other instruments, the size and depolarisation ratio thresholds were found to be subjective, and suggested to vary from cloud to cloud. An upwind site was chosen to measure out-of-cloud aerosol particle concentrations during INUPIAQ. During periods where the site was out-of-cloud and upwind of Jungfraujoch, several large-scale model simulations were run using the aerosol concentrations in an aerosol-dependent ice nucleation parametrization. The inclusion of the parametrization failed to increase the simulated ice crystal number concentrations, which were several orders of magnitude below those observed in-situ at Jungfraujoch. Several possible explanations for the high observed ice crystal number concentrations at Jungfraujoch are tested using further model simulations. Further primary ice nucleation was ruled out, as the inclusion of additional ice nucleating particles in the model simulations suppressed the liquid water content, preventing the simulation of the mixed-phase clouds observed during INUPIAQ. The addition of ice crystals produced via the Hallett-Mossop process upwind of Jungfraujoch into the model only infrequently provided enough ice crystals to match the observed concentrations. The inclusion of a simple surface flux of hoar crystals into the model simulations was found to produce ice crystal number concentrations of a similar magnitude to those observed at Jungfraujoch, without depleting the simulated liquid water content. By confronting models with in-situ observations of cloud microphysical process, this thesis highlights interactions between surface ice crystals and mixed-phase clouds, and their potential impact on large-scale models.

Marine stratocumulus cloud regimes exert a strong climatic influence through their high solar reflectivity. Human-induced changes in stratocumulus clouds, attributed to an increase of the aerosol burden (indirect effects), can be significant given the cloud decks proximity to the continents; nevertheless, the magnitude and the final climatic consequences of these changes are uncertain. This thesis investigates further the interactions between aerosols, cloud microphysics, regional circulation, and radiative response in the Southeast Pacific stratocumulus cloud deck, one of the largest and most persistent cloud regimes in the planet. Specifically, three different aspects are addressed by this thesis: The importance of the synoptic atmospheric variability in controlling cloud microphysical and radiative changes, a validation analysis of satellite retrievals of cloud microphysics from MOderate Resolution Imaging Spectroradiometer (MODIS), and the quantitative assessments of cloud aerosol interactions along with their associated radiative forcing using primarily aircraft remote sensing data. Synoptic and satellite-derived cloud property variations for the Southeast Pacific region associated with changes in coastal satellite-derived cloud droplet number concentration (Nd) are analyzed through a composite technique. MAX and MIN Nd composites are defined by the top and bottom terciles of daily area-mean Nd values over the Arica Bight, the region with the largest mean oceanic Nd, for the five October months of 2001, 2005, 2006, 2007, and 2008. The MAX-Nd composite is characterized by a weaker subtropical anticyclone and weaker winds than the MIN-Nd composite. Additionally, the MAX-Nd composite clouds over the Arica Bight are thinner than the MIN-Nd composite clouds, have lower cloud tops, lower near-coastal cloud albedos, and occur below warmer and drier free tropospheres. At 85˚W, the top-of-atmosphere shortwave fluxes are significantly higher (50%) for the MAX-Nd, with thicker, lower clouds and higher cloud fractions than for the MIN-Nd. The change in Nd at this location is small, suggesting that the MAX-MIN Nd composite differences in radiative properties primarily reflects synoptic changes. The ability of MODIS level 2 retrievals to represent the cloud microphysics is assessed with in-situ measurements of droplet size distributions, collected during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The MODIS cloud optical thickness (t) correlates well with the in-situ values with a positive bias (1.42). In contrast, the standard 2.1 micron-derived MODIS cloud effective radius (r_e) is found to systematically exceed the in-situ cloud-top r_e, with a mean bias of 2.08 um. Three sources of errors that could contribute to the MODIS r_e positive bias are investigated further: the spread of the cloud droplet size distribution, the presence of a separate drizzle mode, and the sensor viewing angles. The sensor zenith viewing angles were found to have little impact, while the algorithm assumption about the cloud droplet spectra and presence of a precipitation mode could affect the retrievals but not by enough to fully explain the positive MODIS r_e bias. The droplet spectra effects account for r_e offsets smaller than 0.6 um, 0.9 um, and 1.6 um for non-drizzling, light-drizzling, and heavy-drizzling clouds respectively. An explanation for the observed MODIS bias is lacking although three-dimensional radiative effects were not considered. This investigation supports earlier studies documenting a similar bias, this time using data from newer probes. MODIS r_e and t were also combined to estimate a liquid water path (LWP) and Nd. A positive bias was also apparent in LWP, and attributed to r_e. However, when selected appropriate parameters a priori, the MODIS Nd estimate was found to agree the best with the insitu aircraft observations of the four MODIS variables. Lastly, the first aerosol indirect effect (Twomey effect) is explicitly investigated with VOCALS-REx observations, collected during three daytime research flights (Nov 9, 11, and 13), utilizing an aerosol-cloud interactions metric, and defined as ACI=dln(t)/dln(Na), with Na corresponding to the accumulation mode aerosol concentration, t derived from a broadband pyranometer, and ACI binned by cloud LWP derived from a millimeter-wavelength radiometer. Aircraft remote sensing estimates of the ACI, during sub-cloud transects, show that the cloud aerosol-interactions are strong and close to the maximum theoretical value for thin clouds, with a decrease of ACI with LWP. Although an explanation for the dependence of ACI on LWP is lacking, we found that a decrease in ACI with LWP is associated with decreases in both surface meridional winds and Nd. Similar to ACI, albedo fractional changes due to Nd fractional changes also tended to be smaller for higher LWPs, but with an overall radiative forcing larger than conservative global estimates obtained in global circulation models. The findings of this thesis emphasize the strong stratocumulus albedo response to an aerosol perturbation and its dependence on the regional scale atmospheric configuration. The results presented here can be used as a benchmark for testing regional and climate models, as well as helping to improve the current parameterizations of the first aerosol indirect effect.