Response to Comment on "Dissolved organic sulfur in the ocean: Biogeochemistry of a petagram inventory".

Dittmar et al proposed that mixing alone can explain our observed decrease in marine dissolved organic sulfur with age. However, their simple model lacks an explanation for the origin of sulfur-depleted organic matter in the deep ocean and cannot adequately reproduce our observed stoichiometric changes. Using radiocarbon age also implicitly models the preferential cycling of sulfur that they are disputing.

Dissolved organic sulfur in the ocean: Biogeochemistry of a petagram inventory.

Although sulfur is an essential element for marine primary production and critical for climate processes, little is known about the oceanic pool of nonvolatile dissolved organic sulfur (DOS). We present a basin-scale distribution of solid-phase extractable DOS in the East Atlantic Ocean and the Atlantic sector of the Southern Ocean. Although molar DOS versus dissolved organic nitrogen (DON) ratios of 0.11 ± 0.024 in Atlantic surface water resembled phytoplankton stoichiometry (sulfur/nitrogen ~ 0.08), increasing dissolved organic carbon (DOC) versus DOS ratios and decreasing methionine-S yield demonstrated selective DOS removal and active involvement in marine biogeochemical cycles. Based on stoichiometric estimates, the minimum global inventory of marine DOS is 6.7 petagrams of sulfur, exceeding all other marine organic sulfur reservoirs by an order of magnitude.

Evidence for the respiration of ancient terrestrial organic C in northern temperate lakes and streams.

Northern rivers and lakes process large quantities of organic and inorganic carbon from the surrounding terrestrial ecosystems. These external carbon inputs fuel widespread CO(2) supersaturation in continental waters, and the resulting CO(2) emissions from lakes and rivers are now recognized as a globally significant loss of terrestrial production to the atmosphere. Whereas the magnitude of emissions has received much attention, the pathways of C delivery and processing that generate these emissions are still not well-understood. CO(2) outgassing in aquatic systems has been unequivocally linked to microbial degradation and respiration of terrestrial organic carbon (OC), but the nature (i.e., age and source) of this OC respired in surface waters is largely unknown. We present direct radiocarbon measurements of OC respired by bacteria in freshwater aquatic systems, specifically temperate lakes and streams in Québec. Terrestrial OC fuels much of the respiration in these systems, and our results show that a significant fraction of the respired terrestrial OC is old (in the range of 1,000-3,000 y B.P.). Because the bulk OC pools in these lakes is relatively young, our results also suggest selective removal of an old but highly bioreactive terrestrial OC pool and its conversion to CO(2) by bacteria. The respiration of ancient (14)C-depleted terrestrial C in northern lakes and rivers provides a biological link between contemporary aquatic carbon biogeochemistry and paleo-conditions in the watershed, and it implies the aquatic-mediated return to the atmosphere of C putatively considered permanently stored, thus challenging current models of long-term C storage in terrestrial reservoirs.