The analysis of in situ and retrieved aerosol properties measured during three airborne field campaigns

Aerosols can directly influence climate, visibility, and photochemistry by scattering and absorbing solar radiation. Aerosol chemical and physical properties determine how efficiently a particle scatters and/or absorbs incoming short-wave solar radiation. Because many types of aerosol can act as nuclei for cloud droplets (CCN) and a smaller population of airborne particles facilitate ice crystal formation (IN), aerosols can also alter cloud-radiation interactions which have subsequent impacts on climate. Thus aerosol properties determine the magnitude and sign of both the direct and indirect impacts of aerosols on radiation-dependent Earth System processes.;This dissertation will fill some gaps in our understanding of the role of aerosol properties on aerosol absorption and cloud formation. Specifically, the impact of aerosol oxidation on aerosol spectral (350nm < lambda< 500nm) absorption was examined for two biomass burning plumes intercepted by the NASA DC-S aircraft during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission in Spring and Summer 2008. Spectral aerosol single scattering albedo (SSA) retrieved using actinic flux measured aboard the NASA DC-8 was used to calculate the aerosol absorption Angstrom exponents (AAE) for a 6-day-old plume on April 17 th and a 3-hour old plume on June 29th. Higher AAE values for the April 17th plume (6.78+/-0.38) indicate absorption by aerosol was enhanced in the ultraviolet relative to the visible portion of the short-wave spectrum in the older plume compared to the fresher plume (AAE= 3.34 0.11). These differences were largely attributed to the greater oxidation of the organic aerosol in the April 17th plume which can arise either from the aging of primary organic aerosol or the formation of spectrally-absorbing secondary organic aerosol.;The validity of the actinic flux retrievals used above were also evaluated in this work by the comparison of SSA retrieved using actinic flux (AF SSA) to those retrieved using ratios of direct and diffuse irradiance (DDR SSA) at four wavelengths: 332, 368, 415, and 500 mn. Both actinic flux and irradiance were measured atop the University of Houston's Moody Tower in Houston, TX as part of the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission in September 2013. AF SSA values were consistently lower than DDR SSAs with largest offsets observed when aerosol optical depths was < ~0.2. AF SSA were also lower than those reported by the AErosol RObotic NETwork (AERONET) and column-averaged values calculated from aerosol scattering and absorption coefficients measured aboard the NASA P3-B aircraft at 450 and 550 nm. However, AAE values calculated from AF SSAs compared well to AERONET and column-averaged AAEs suggesting actinic flux retrievals can correctly resolve the spectral dependence of aerosol absorption.;Recent work has suggested that mineral dust is the most important IN found in both anvil and synoptically formed cirrus clouds over North America. The vertical transport processes sustaining significant mineral dust in the upper troposphere (> 9 km) where these clouds form are not well understood, but deep convective systems (thunder storms) likely play a role. Bulk aerosol Ca2+ concentrations and volume size distributions were measured aboard the NASA DC-8 during the NCAR Deep Convective Clouds and Chemistry Experiment (DC-3) conducted in May/June 2012 in both the inflow and outflow regions of twelve isolated, high cloud base storms over CO and OK. Outflow/inflow ratios of both Ca2+ and total coarse (limn < diameter ~0.9) suggesting a significant fraction of ingested coarse mode dust was transported through these systems. Elevated Ca2+ and Vc in the outflow were most likely not artifacts of ice shattering given the general absence of a relationship between these parameters and two ice concentration measurements (e.g., ice water content, 2D-S particle concentrations). Because mineral dust is an efficient IN, unactivated mineral dust particles are not expected in cold clouds. However, for these storms, inflow total coarse (0.5 microm < diameter < 5 microm) aerosol number (Nc)generally exceeded anvil cirrus ice particle concentrations, supporting the presence of interstitial dust in storm outflow. Thus efficient IN were likely made available in the upper troposphere by these twelve convective systems.