Brown carbon in aerosol remains a significant source of error in global climate modeling due to its complex nature and limited product characterization. Though significant efforts have been made in the previous decade to identify the major lightabsorbing brown carbon chromophores formed through the reactions of carbonylcontaining compounds with ammonium, substantial work is still required to identify the main absorbing species resulting from reactions of glyoxal, glycolaldehyde, and hydroxyacetone with ammonium sulfate (AS). Using tandem mass spectrometry and 15 N experiments to confirm proposed structures and support their mechanistic pathways, compelling evidence is provided for the formation of pyrazines and imidazoles in the glyoxal + AS, glycolaldehyde + AS, and hydroxyacetone + AS systems. Through density functional theory calculations, the N-containing oligomers and aromatic heterocycles formed within these reaction systems are shown to contribute to brown carbon light absorption, thus holding significant relevance toward accurately predicting their effects on global climate.