We performed a study of the evolution of soot composition and fine structure, i.e., maturity level, in an atmospheric ethylene-air diffusion flame. We used laser-induced incandescence (LII) to provide information about maturity level of the bulk primary particle and X-ray photoelectron spectroscopy (XPS) to provide complementary information about particle-surface-maturity level. The results demonstrate that the bulk material and the particle surface evolve separately in the flame. Increased soot-maturity level is associated with increased long-range order of the particle fine structure. This increased order leads to an increase in the absorption cross-section in the visible and near-infrared and a shift of the absorption to longer wavelengths with increasing maturity level of the bulk particle. These trends result in a decrease in the dispersion exponent (xi) and increase in the absorption cross-section scaling factor (beta), as inferred from LII measurements. LII measurements demonstrate that bulk-maturity level increases with height-above-the-burner (HAB) until it reaches a plateau in the center of the flame at the maximum in the soot volume fraction. Bulk-maturity level only slightly decreases as soot is oxidized at larger HABs. Increased maturity level also leads to an increase in long-range sp(2) hybridization. XPS measurements of the sp(2)/defect ratio demonstrate an increase in soot surface-maturity level with increasing HAB, but the surface-maturity level increases more gradually with HAB than the bulk-maturity level. Whereas the bulk-fine-structure order decreases slightly in the oxidation region, the surface order decreases dramatically, indicating that oxidation occurs preferentially at the surface under these conditions.
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