A. J. Peters

Isotopic evidence for a marine ammonium source in rainwater at Bermuda

Emissions of anthropogenic nitrogen (N) to the atmosphere have increased tenfold since preindustrial times, resulting in increased N deposition to terrestrial and coastal ecosystems. The sources of N deposition to the ocean, however, are poorly understood. Two years of event-based rainwater samples were collected on the island of Bermuda in the western North Atlantic, which experiences both continent- and ocean-influenced air masses. The rainwater ammonium concentration ranged from 0.36 to 24.6 μM, and the ammonium δ15N from −12.5 to 0.7‰; and neither has a strong relationship with air mass history (6.0 ± 4.2 μM, −4.1 ± 2.6‰ in marine air masses and 5.9 ± 3.2 μM, −5.8 ± 2.5‰ in continental air masses; numerical average ± standard deviation). A simple box model suggests that the ocean can account for the concentration and isotopic composition of ammonium in marine rainwater, consistent with the lack of correlation between ammonium δ15N and air mass history. If so, ammonium deposition reflects the cycling of N between the ocean and the atmosphere, rather than representing a net input to the ocean. The δ15N data appear to require that most of the ammonium/a flux to the ocean is by dissolution in surface waters rather than atmospheric deposition. This suggests that the atmosphere and surface ocean are near equilibrium with respect to air/sea gas exchange, implying that anthropogenic ammonia will equilibrate near the coast and not reach the open marine atmosphere. Whereas ~90% of the ammonium deposition to the global ocean has previously been attributed to anthropogenic sources, the evidence at Bermuda suggests that the anthropogenic contribution could be much smaller.

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

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. 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.

Stable isotopes in the atmospheric marine boundary layer water vapour over the Atlantic Ocean, 2012–2015

The water vapour isotopic composition (1H216O, H218O and 1H2H16O) of the Atlantic marine boundary layer has been measured from 5 research vessels between 2012 and 2015. Using laser spectroscopy analysers, measurements have been carried out continuously on samples collected 10–20 meter above sea level. All the datasets have been carefully calibrated against the international VSMOW-SLAP scale following the same protocol to build a homogeneous dataset covering the Atlantic Ocean between 4°S to 63°N. In addition, standard meteorological variables have been measured continuously, including sea surface temperatures using calibrated Thermo-Salinograph for most cruises. All calibrated observations are provided with 15-minute resolution. We also provide 6-hourly data to allow easier comparisons with simulations from the isotope-enabled Global Circulation Models. In addition, backwards trajectories from the HYSPLIT model are supplied every 6-hours for the position of our measurements.