Marine biogenic source of atmospheric organic nitrogen in the subtropical North Atlantic

Katye E. Altieri; Sarah E. Fawcett; Andrew J. Peters; Daniel M. Sigman; Meredith G. Hastings

doi:10.1073/pnas.1516847113

Edited by John H. Seinfeld, California Institute of Technology, Pasadena, CA, and approved December 9, 2015 (received for review August 24, 2015)

Significance

Global models indicate that the human-derived nitrogen emissions that reach the ocean through atmospheric transport and deposition directly impact biology and the oceanic carbon dioxide (CO₂) sink. Here, we find that the organic nitrogen in marine aerosols derives predominantly from biological production in the surface ocean rather than from pollution on land. Our previous work has shown significant anthropogenic influence on North Atlantic nitrate deposition, whereas ammonium cycles dynamically between the upper ocean and lower atmosphere. Collectively, these findings indicate that the ocean is not a passive recipient of anthropogenic nitrogen deposition, as it has previously been considered. This implies that the contribution of atmospheric nitrogen deposition to ocean fertility, oceanic CO₂ removal, and nitrous oxide emissions has been overestimated.

Abstract

Global models estimate that the anthropogenic component of atmospheric nitrogen (N) deposition to the ocean accounts for up to a third of the ocean’s external N supply and 10% of anthropogenic CO₂ uptake. However, there are few observational constraints from the marine atmospheric environment to validate these findings. Due to the paucity of atmospheric organic N data, the largest uncertainties related to atmospheric N deposition are the sources and cycling of organic N, which is 20–80% of total N deposition. We studied the concentration and chemical composition of rainwater and aerosol organic N collected on the island of Bermuda in the western North Atlantic Ocean over 18 mo. Here, we show that the water-soluble organic N concentration ([WSON]) in marine aerosol is strongly correlated with surface ocean primary productivity and wind speed, suggesting a marine biogenic source for aerosol WSON. The chemical composition of high-[WSON] aerosols also indicates a primary marine source. We find that the WSON in marine rain is compositionally different from that in concurrently collected aerosols, suggesting that in-cloud scavenging (as opposed to below-cloud “washout”) is the main contributor to rain WSON. We conclude that anthropogenic activity is not a significant source of organic N to the marine atmosphere over the North Atlantic, despite downwind transport from large pollution sources in North America. This, in conjunction with previous work on ammonium and nitrate, leads to the conclusion that only 27% of total N deposition to the global ocean is anthropogenic, in contrast to the 80% estimated previously.

Footnotes

↵¹To whom correspondence should be addressed. Email: katye.altieri{at}uct.ac.za.

Author contributions: K.E.A., A.J.P., D.M.S., and M.G.H. designed research; K.E.A. and A.J.P. performed research; K.E.A., S.E.F., D.M.S., and M.G.H. analyzed data; and K.E.A., S.E.F., D.M.S., and M.G.H. wrote the paper.
The authors declare no conflict of interest.
This article is a PNAS Direct Submission.
This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1516847113/-/DCSupplemental.

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