Direct observation of the chemical evolution of flame-generated soot was de
monstrated for the first time using real-time aerosol mass spectrometry. Th
e data presented unambiguously show the transformation of particle phase po
lycyclic aromatic hydrocarbons (PAHs) into carbonaceous soot containing ful
lerenes. The mechanism of fullerene formation in the particle phase that is
revealed is not consistent with conventional gas-phase formation mechanism
s. This mechanism suggests the possibility of a controlled condensed phase
synthesis of fullerenes.