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Particulate matter emissions are becoming a big issue for GDI engines as the emission regulations being more stringent. Methanol has been considered to be an important alternative fuel to reduce soot emissions. To understand the effect of methanol addition on soot and polycyclic aromatic hydrocarbons (PAHs) formation, the 2-D distributions of soot volume fraction and different size PAHs relative concentrations in methanol/gasoline laminar diffusion flames were measured by TC-LII and PLIF techniques. The effect of methanol was investigated under the conditions of the same carbon flow and the same flame height. The methanol volume fraction was set as M0/20/40/60/80. The results showed that the natural luminescent flame lift-off height and soot lift-off height increases consistently with the increasing methanol content due to the increase of outlet velocity of fuel vapor.