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Coupling between dimethylsulfide emissions and the ocean–atmosphere exchange of ammonia

Coupling between dimethylsulfide emissions and the ocean–atmosphere exchange of ammonia Environmental context. Dimethylsulfide (DMS) is recognised as a potentially significant climate-forcing gas, owing to its role in particle and cloud formation in the marine atmosphere, where it is the dominant source of acidity. Ammonia, the dominant naturally occurring base in the atmosphere, plays an important role in neutralising particles formed from DMS oxidation products and may even enhance the formation rate of new particles. A biogeochemical coupling has previously been proposed between DMS and ammonia fluxes from the ocean to the atmosphere, in the form of coproduction of the two gases in seawater. We revise this suggestion by introducing the concept of ‘co-emission’ of the gases, where DMS emission controls the rate of emission of ammonia from the ocean by acidifying the atmosphere. Abstract. A strong correlation between aerosol ammonium and non-sea salt sulfate is commonly observed in the remote marine boundary layer. It has been suggested that this relationship implies a biogeochemical linkage between the nitrogen (N) and sulfur (S) cycles at the cellular biochemical level in phytoplankton in the ocean, or a linkage in the atmosphere (see P. S. Liss and J. N. Galloway, Interactions of C, N, P and S biogeochemical cycles and global change (Springer, 1993), and P. K. Quinn et al. in J. Geophys. Res. – Atmos. 1990 , 95 ). We argue that an oceanic linkage is unlikely and draw on mechanistic and observational evidence to make the argument that the atmospheric connection is based on simple physical chemistry. Drawing on an established analogous concept in terrestrial trace gas biogeochemistry, we propose that any emission of dimethylsulfide (DMS) from the ocean will indirectly influence the flux of NH 3 from the ocean, through the neutralisation of acidic DMS oxidation products and consequent lowering of the partial pressure of NH 3 in the atmosphere. We present a simple numerical model to investigate this hypothesised phenomenon, using a parameterisation of the rate and thermodynamics of gas-to-particle conversion of NH x and explicitly modelled ocean–atmosphere NH 3 exchange. The model indicates that emission of acidic sulfur to the atmosphere (e.g. as a product of DMS oxidation) may enhance the marine emission of NH 3 . It also suggests that the ratio of ammonium to non-sea salt sulfate in the aerosol phase is strongly dependent on seawater pH, temperature and wind speed – factors that control the ocean–atmosphere ammonia flux. Therefore, it is not necessary to invoke a stoichiometric link between production rates of DMS and ammonia in the ocean to explain a given ammonium to non-sea salt sulfate ratio in the aerosol. We speculate that this mechanism, which can provide a continuous resupply of ammonia to the atmosphere, may be involved in a series of biogeochemical-climate feedbacks. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Environmental Chemistry CSIRO Publishing

Coupling between dimethylsulfide emissions and the ocean–atmosphere exchange of ammonia

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References (58)

Publisher
CSIRO Publishing
Copyright
CSIRO
ISSN
1448-2517
eISSN
1449-8979
DOI
10.1071/EN08030
Publisher site
See Article on Publisher Site

Abstract

Environmental context. Dimethylsulfide (DMS) is recognised as a potentially significant climate-forcing gas, owing to its role in particle and cloud formation in the marine atmosphere, where it is the dominant source of acidity. Ammonia, the dominant naturally occurring base in the atmosphere, plays an important role in neutralising particles formed from DMS oxidation products and may even enhance the formation rate of new particles. A biogeochemical coupling has previously been proposed between DMS and ammonia fluxes from the ocean to the atmosphere, in the form of coproduction of the two gases in seawater. We revise this suggestion by introducing the concept of ‘co-emission’ of the gases, where DMS emission controls the rate of emission of ammonia from the ocean by acidifying the atmosphere. Abstract. A strong correlation between aerosol ammonium and non-sea salt sulfate is commonly observed in the remote marine boundary layer. It has been suggested that this relationship implies a biogeochemical linkage between the nitrogen (N) and sulfur (S) cycles at the cellular biochemical level in phytoplankton in the ocean, or a linkage in the atmosphere (see P. S. Liss and J. N. Galloway, Interactions of C, N, P and S biogeochemical cycles and global change (Springer, 1993), and P. K. Quinn et al. in J. Geophys. Res. – Atmos. 1990 , 95 ). We argue that an oceanic linkage is unlikely and draw on mechanistic and observational evidence to make the argument that the atmospheric connection is based on simple physical chemistry. Drawing on an established analogous concept in terrestrial trace gas biogeochemistry, we propose that any emission of dimethylsulfide (DMS) from the ocean will indirectly influence the flux of NH 3 from the ocean, through the neutralisation of acidic DMS oxidation products and consequent lowering of the partial pressure of NH 3 in the atmosphere. We present a simple numerical model to investigate this hypothesised phenomenon, using a parameterisation of the rate and thermodynamics of gas-to-particle conversion of NH x and explicitly modelled ocean–atmosphere NH 3 exchange. The model indicates that emission of acidic sulfur to the atmosphere (e.g. as a product of DMS oxidation) may enhance the marine emission of NH 3 . It also suggests that the ratio of ammonium to non-sea salt sulfate in the aerosol phase is strongly dependent on seawater pH, temperature and wind speed – factors that control the ocean–atmosphere ammonia flux. Therefore, it is not necessary to invoke a stoichiometric link between production rates of DMS and ammonia in the ocean to explain a given ammonium to non-sea salt sulfate ratio in the aerosol. We speculate that this mechanism, which can provide a continuous resupply of ammonia to the atmosphere, may be involved in a series of biogeochemical-climate feedbacks.

Journal

Environmental Chemistry – CSIRO Publishing

Published: Aug 19, 2008

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