Timothy Logan

Date of Award

January 2014

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Atmospheric Sciences

First Advisor

Baike Xi

Second Advisor

Xiquan Dong

Abstract

Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations:

SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites?

SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport?

SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration?

This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angström exponent (AEAOD) and single scattering co-albedo (ωoabs) to denote aerosol size and absorptive properties. The aerosols events are

then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components.

There are strong regional and seasonal influences of the four aerosol types over the selected four Asian sites. A strongly absorbing mineral dust influence is seen at the Xianghe, Taihu, and SACOL sites during the spring months (MAM) as given by coarse mode dominance. There is a shift towards weakly absorbing pollution (sulfate) and biomass (OC) aerosol dominance in the summer (JJA) and autumn (SON) months as given by a strong fine mode influence. A winter season (DJF) shift toward strongly fine mode, absorbing particles (BC and OC) is observed at Xianghe and Taihu. At Mukdahan, a strong fine mode influence is evident year round with weakly and strongly absorbing biomass particles dominant in the autumn and winter months, respectively, while particles exhibit variable absorption during the spring season.

To address SQ2, four cases are selected in Asia to investigate how the optical properties of Asian aerosol plumes change during transport across the remote Pacific Ocean. In addition, six strong smoke events are selected to investigate how the physical and chemical properties of biomass smoke aerosols change during transport in North America. From four selected Asian cases, it was shown by DC-8 aircraft in situ measurements that the Asian plumes contained varying amounts of mineral dust and pollution aerosols during transport. In addition, backward trajectory analysis identified two main dust source regions (Gobi and Taklamakan deserts) and urban/industrial pollution regions in central and eastern China. During the anomalously active wildfire season of 2012 in North America, strong smoke events were observed over the Northern Great Plains region by the Grand Forks, North Dakota, AERONET site and selected as cases. The spectral dependences of absorption aerosol optical depth (AAOD) and ωoabs illustrated the varying absorption of the smoke plumes due to carbonaceous particle influences. The AAOD parameter was found to be primarily influenced by aerosol particle size while ωoabs was more sensitive to the carbonaceous content. The aerosols likely contain strongly absorbing carbonaceous particles generated from the flaming combustion mode. The cases represented complex mixtures of the flaming and smoldering combustion phases.

Lastly, SQ3 is addressed by using a multi-platform dataset from the Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) Graciosa, Azores, 2009-2010 field campaign. The seasonal aerosol particle volume and number size distributions, AOD, and AEAOD during the CAP-MBL campaign have shown that a low overall mean AOD440 of 0.12 denoted a clean environment over this region that typically contains MBL sea salt. In terms of aerosol volume, a bimodal signal was prominent where the coarse mode influence (r ≥ 1 μm) dominated that of the fine mode (r < 1 μm) throughout the year. However, there are considerable continental fine mode aerosols advected to the Azores region during summer months, including Saharan mineral dust, volcanic ash, biomass smoke, and pollution from North American as identified by HYSPLIT backward trajectories. These aerosol types have been shown to have impacts on MBL cloud condensation nuclei (CCN) that are likely different from coarse mode marine aerosols (e.g., sea salt) (Rémillard et al. 2014; Wood et al. 2014). The alternating presence of dominant clean air masses with periodic episodes of polluted air masses will provide a substantial variety in aerosol properties during the summer. This will provide a great opportunity to investigate the interactions between aerosol and cloud properties in terms of the aerosol indirect effect (AIE).

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