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Many practical soot-emitting combustion systems such as diesel and jet engines rely on diffusion flames for efficient and reliable operation. Efforts to mitigate soot emissions from these systems are dependent on fundamental understanding of the physicochemical pathways leading from fuel to soot in laminar diffusion flames. Existing diffusion flame−based soot studies focused primarily on over-ventilated coflow flame where the fuel gas (or vapor) issues from a cylindrical tube into a co-flowing oxidizer, and counterflow flame, where a reacting zone is established between two opposing streams of fuel and oxidizer. As a canonical diffusion flame configuration, laminar counterflow diffusion flames have been widely used as a highly controllable environment for soot research, enabling significant progress in the understanding of soot formation for several decades. In view of the possibility of fuel/oxidizer premixing in …