Abstract

Atmospheric deposition of reactive nitrogen (N) species from large fires may contribute to enrichment of nutrients in aquatic ecosystems. Here we use an atmospheric chemistry transport model to investigate the supply of soluble organic nitrogen (ON) from open biomass burning to the ocean. The model results show that the annual deposition rate of soluble ON to the oceans (14 Tg N yr−1) is increased globally by 13% with the increase being particularly notable over the tropical oceans downwind from the source regions. The estimated deposition of soluble ON due to biomass burning from the secondary formation (1.0 Tg N yr−1) is close to that from the primary sources (1.2 Tg N yr−1). We examine the secondary formation of particulate C–N compounds (i.e., imidazole, methyl imidazole, and N-containing oligomers) from the reactions of glyoxal (CHOCHO) and methylglyoxal (CH3COCHO) with ammonium (NH4+) in wet aerosols and upon cloud evaporation. These ON sources result in a significant contribution to the open ocean (1.3 Tg N yr−1), suggesting that atmospheric processing in aqueous-phase may have a large effect. We compare the soluble ON concentration in aerosols with and without open biomass burning as a case study in Singapore. The model results demonstrate that the soluble ON concentration in aerosols is episodically enriched during the fire events, compared to the case without smoke simulations. At the same time, the model results show that the daily soluble ON concentration can be also enhanced in the case without smoke simulations, compared to the monthly averages. These results may suggest that both the primary source strength of ON and the secondary formation rates of ON should be taken into consideration when using in-situ observations to constrain the calculated soluble ON burden due to biomass burning. More accurate quantification of the soluble ON burdens both with and without smoke sources is therefore needed to assess the effect of biomass burning on bioavailable ON input to the oceans.

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