Extinction measurements for optical band gap determination of soot in a series of nitrogen-diluted ethylene/air non-premixed flames

摘要

Visible light extinction was measured in a series of nitrogen-diluted, ethylene/air, non-premixed flames and this data was used to determine the optical band gap, OBG, as a function of flame position. Collimated light from a supercontinuum source is telescopically expanded and refocused to match the f-number of a dispersing monochromator. The dispersed light is split into a power metering channel and a channel that is periscoped and focused into the flame. The transmitted light is then recollimated and focussed onto a silicon photodiode detector. After tomographic reconstruction of the radial extinction field, the OBG was derived from the near-edge absorption feature using Tauc/Davis-Mott analysis. A slight evolution in OBG was observed throughout all flame systems with a consistent range of OBG observed between approximately 1.85 eV and 2.35 eV. Averaging over all positions the mean OBG was approximately 2.09 eV for all flame systems. Comparing these results to previously published computational results relating calculated HOMO-LUMO gaps for a variety of D-2h PAH molecules to the number of aromatic rings in the structure, showed that the observed optical band gap is consistent with a PAH of about 14 rings or a conjugation length of 0.97 nm. This work provides experimental support to the model of soot formation where the transition from chemical to physical growth starts at a modest molecular size; about the size of circumpyrene.