Secondary organic aerosol (SOA) generated through the partitioning of gas phase volatile organic carbon compounds (VOCs) into the condensed phase has both epidemiological and climatic impacts through the growth of particulate matter into relevant sizes for respiratory interactions and cloud condensation nuclei activity. Considering the complex chemistry involved with VOC oxidation and subsequent formation of SOA, bulk properties like oxidation state, often represented by O:C ratio, and volatility are used to simplify the representation of SOA in chemical transport models (CTMs) and the like [e.g. Tsimpidi et al. 2010]. This preference for bulk properties is supported by the availability of ambient measurement techniques to constrain model parameters and scenarios. The volatility of SOA is often described by treating it as a mixture of components with differing partitioning coefficients through the volatility basis set (VBS) approach rather than explicitly resolving the complex chemistry [Donahue et al., 2006]. This study presents a method of determining the volatility of an aerosol sample through the use of an optimizing thermodenuder (TD) instrument model that is used to fit laboratory data. Data collected using a volatility tandem differential mobility analyzer (VTDMA) setup consist of inlet and outlet particle size and number concentrations for select dicarboxylic acids - compounds known to contribute to atmospheric SOA. These are interpreted by the model through an iterative optimization routine to obtain estimates of volatility parameters (e.g. saturation concentrations) which are compared to available literature data. The instrument model is currently divided into two decoupled modules. The first resolves the flow field characteristics, obtaining the temperature profile, pressure variations, and radial velocity distribution of the TD, and the second resolves the gas to particle partitioning of aerosol with a given condensed-phase volatility distribution in the TD using the VBS approach as described in the literature. Solving the full hydrodynamic equations for the flow characteristics provides a better numeric representation of entry length and radial velocity variations and is an improvement over similar TD modeling studies in the literature. However, results indicate that coupling the two modules is necessary to more accurately resolve the suppression of evaporation due to buildup of organic vapors in the TD, even at the low mass concentrations involved with the presented experiments.
| Identifer | oai:union.ndltd.org:GATECH/oai:smartech.gatech.edu:1853/45939 |
| Date | 14 November 2012 |
| Creators | Hite, James Ricky |
| Publisher | Georgia Institute of Technology |
| Source Sets | Georgia Tech Electronic Thesis and Dissertation Archive |
| Detected Language | English |
| Type | Thesis |
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