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Interactions between Surface Chemistry and Gas-Phase Combustion: New Optical Tools for Probing Flame-Wall Interactions and the Heterogeneous Chemistry of Soot Growth and Oxidation in Flame. Final report

Kliewer, Christopher J.

Some of the most stubborn and technologically critical problems in combustion are dominated by heterogeneous processes. While purely gas-phase combustion systems have been the subject of intense theoretical and experimental study, combustion phenomena occurring at interfaces are far less understood. This is partly caused by the lack of experimental approaches capable of probing locations very close to an interface, especially in the hostile environment of combustion. For laser-based optical techniques, measurements taken near interfaces are often complicated by laser scattering from the surface interfering with relatively weak signals. Further, for measurements intended to probe molecular species adsorbed at the interface between a gas-phase combustion reaction and a condensed phase material, signals are generally overwhelmed by contributions from the bulk phases, causing the small contribution from the interfacial molecular species to be undetectable. Our goal in this project has been to develop new optical tools for imaging chemical species, temperature, and surface species at and near surfaces or interfaces of relevance to combustion. We have placed focus on the development and refinement of ultrafast techniques such as femtosecond coherent Raman imaging and femtosecond/picosecond sum-frequency generation (SFG) scattering, as well as the models used to simulate such spectra under differing conditions of pressure and chemical speciation. The two physical phenomena initially targeted for study in this project were flamewall interactions, and the growth of particulates in flames.