Investigations of Physicochemical Properties of Size-Resolved, Subsaturated, Atmospheric Aerosol Particles: Instrument Development, Field Measurements, and Data Analysis

摘要

Aerosol particle properties and their impact on air quality, clouds, and the hydrologic cycle remain a critically important factor for the understanding of our atmosphere. Particle hygroscopic growth leads to impacts on direct and indirect radiative forcing properties, the likelihood for particles to act as cloud condensation nuclei, and aerosol-cloud interactions. Current instruments measuring hygroscopic growth have a number of limitations, lacking either the ability to measure size-resolved particles or process samples at a fast enough resolution to be suitable for airborne deployment. Advanced in-situ airborne particle retrieval and measurements of aerosol hygroscopic growth and scattering properties are analyzed and discussed.To improve the analysis of cloud nuclei particles, an updated counterflow virtual impact inlet was characterized and deployed during the 2011 E-PEACE field campaign. Theoretical and laboratory based cut size diameters were determined and validated against data collected from an airborne platform. In pursuit of higher quality aerosol particle hygroscopicity measurements, a newer instrument, the differential aerosol sizing and hygroscopicity probe (DASH-SP) has been developed in the recent past and only flown on a handful of campaigns. It has been proven to provide quality, rapid, size-resolved hygroscopic growth factor data, but was further improved into a smaller form factor making it easier for deployment on airborne platforms. It was flown during the 2013 SEAC4RS field campaign and the data was analyzed to composite air mass based hygroscopicity and refractive index (real portion only) statistics. Additionally, a comparison of bulk and size-resolved hygroscopic growth measurements was conducted. Significant findings include a potential particle size bias on bulk scattering measurements as well as a narrow range of ambient real portion of refractive index values. An investigation into the first reported ambient hygroscopicity measurements of particle shrinkage, or "sub-1" growth is conducted. Possible explanations, including particle restructuring, measurement sensitivity to refractive index, evaporative loss, and influence of ambient external mixtures on data processing are examined.