The challenge of simulating the sensitivity of the Amazonian cloud microstructure to cloud condensation nuclei number concentrations

The realistic representation of aerosol-cloud interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon region has been one of the motivations for several field campaigns, including the airborne "Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems-Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA)" campaign based in Manaus, Brazil, in September 2014. In this work we combine in situ and remotely sensed aerosol, cloud, and atmospheric radiation data collected during ACRIDICON-CHUVA with regional, online-coupled chemistry-transport simulations to evaluate the model's ability to represent the indirect effects of biomass burning aerosol on cloud microphysical and optical properties (droplet number concentration and effective radius). We found agreement between the modeled and observed median cloud droplet number concentration (CDNC) for low values of CDNC, i.e., low levels of pollution. In general, a linear relationship between modeled and observed CDNC with a slope of 0.3 was found, which implies a systematic underestimation of modeled CDNC when compared to measurements. Variability in cloud condensation nuclei (CCN) number concentrations was also underestimated, and cloud droplet effective radii (reff) were overestimated by the model. Modeled effective radius profiles began to saturate around 500 CCN cm(-3) at cloud base, indicating an upper limit for the model sensitivity well below CCN concentrations reached during the burning season in the Amazon Basin. Additional CCN emitted from local fires did not cause a notable change in modeled cloud droplet effective radii. Finally, we also evaluate a parameterization of CDNC at cloud base using more readily available cloud microphysical properties, showing that we are able to derive CDNC at cloud base from cloud-side remote-sensing observations