Enhanced formation of nitrogenous organic aerosols and brown carbon after aging in the planetary boundary layer

Abstract

Particulate organic nitrates (pON) significantly contribute to the mass of organic aerosol and influence the NOX cycle in the atmosphere, but their evolution and lifetime remain uncertain. This study performed simultaneous measurements on the anthropogenically affected surface site and the mountain site on top of the polluted planetary boundary layer (PBL). After aging in the PBL, organic nitrate was converted from primary sources (decreased from 8.7 % to 4.3 %) to secondary sources (increased from 6.3 % to 36.1 %), spanning from the surface to the mountain. The evaporation of more volatile inorganic nitrate and the production of secondary organic nitrate during aging in the PBL contributed to the enhanced pON fraction over the top of PBL. The contribution of light absorption by brown carbon increased by 43 % at the top of PBL compared to the surface, consistent with the higher fraction of nitrogenous organic aerosols over the mountain. The results provide field evidence that the nitrogenous OA may be preserved by adding into secondary OA and significantly contribute to the enhanced importance of brown carbon after aging the vertical transport in the PBL.