Oxygen concentrations in the bottom waters of the Lower St. Lawrence estuary (LSLE) decreased from 125 mol L Ϫ1 (37.7% saturation) in the 1930s to an average of 65 mol L Ϫ1 (20.7% saturation) for the 1984-2003 period. A concurrent 1.65ЊC warming of the bottom water from the 1930s to the 1980s suggests that changes in the relative proportions of cold, fresh, oxygen-rich Labrador Current Water (LCW) and warm, salty, oxygen-poor North Atlantic Central Water (NACW) in the water mass entering the Laurentian Channel probably played a role in the oxygen depletion. We estimate that about one half to two thirds of the oxygen loss in the bottom waters of the LSLE can be attributed to a decreased proportion of LCW. This leaves between one third and one half of the oxygen decrease to be explained by causes other than changes in water mass composition. An increase in the along-channel oxygen gradient from Cabot Strait to the LSLE over the past decades, combined with data from sediment cores, suggests that increased sediment oxygen demand may be partly responsible for the remainder of the oxygen decline. In July 2003, approximately 1,300 km 2 of seafloor in the LSLE was bathed in hypoxic water (Ͻ62.5 mol L Ϫ1).Severe hypoxia is a condition that occurs in the water column when oxygen (O 2 ) falls below the 2 mg L

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Considerable discussion surrounds the potential role of anoxygenic phototrophic Fe(II)-oxidizing bacteria in both the genesis of Banded Iron Formations (BIFs) and early marine productivity. However, anoxygenic phototrophs have yet to be identified in modern environments with comparable chemistry and physical structure to the ancient Fe(II)-rich (ferruginous) oceans from which BIFs deposited. Lake Matano, Indonesia, the eighth deepest lake in the world, is such an environment. Here, sulfate is scarce (<20 mol⅐liter ؊1 ), and it is completely removed by sulfate reduction within the deep, Fe(II)-rich chemocline. The sulfide produced is efficiently scavenged by the formation and precipitation of FeS, thereby maintaining very low sulfide concentrations within the chemocline and the deep ferruginous bottom waters. Low productivity in the surface water allows sunlight to penetrate to the >100-m-deep chemocline. Within this sulfide-poor, Fe(II)-rich, illuminated chemocline, we find a populous assemblage of anoxygenic phototrophic green sulfur bacteria (GSB). These GSB represent a large component of the Lake Matano phototrophic community, and bacteriochlorophyll e, a pigment produced by low-light-adapted GSB, is nearly as abundant as chlorophyll a in the lake's euphotic surface waters. The dearth of sulfide in the chemocline requires that the GSB are sustained by phototrophic oxidation of Fe(II), which is in abundant supply. By analogy, we propose that similar microbial communities, including populations of sulfate reducers and photoferrotrophic GSB, likely populated the chemoclines of ancient ferruginous oceans, driving the genesis of BIFs and fueling early marine productivity.anoxygenic photosynthesis ͉ banded iron formation ͉ green sulfur bacteria ͉ iron oxidation ͉ Lake Matano

We examined the chemical composition of the water column of Lake Matano, Sulawesi Island, Indonesia, to document how the high abundances of Fe (hydr)oxides in tropical soils and minimal seasonal temperature variability affect biogeochemical cycling in lakes. Lake Matano exhibits weak thermal stratification, yet a persistent pycnocline separates an oxic epilimnion from anoxic meta-and hypolimnions. The concentration of soluble P in the epilimnetic waters is very low and can be attributed to scavenging by Fe (hydr)oxides. Chromium concentrations in the epilimnion are high (up to 180 nmol L 21 ), but below U.S. Environmental Protection Agency guidelines for aquatic ecosystems. The concentration of chromium decreases sharply across the oxic-anoxic boundary, revealing that the hypolimnion is a sink for Cr. Flux calculations using a one-dimensional transportreaction model for the water column fail to satisfy mass balance requirements and indicate that sediment transport and diagenesis play an important role in the exchange of Fe, Mn, P, and Cr between the epilimnion and hypolimnion. Exchange of water between the epilimnion and hypolimnion is slow and on a time scale similar to temperate meromictic lakes. This limits recycling of P and N to the epilimnion and removal of Cr to the hypolimnion, both of which likely restrict primary production in the epilimnion. Owing to the slow exchange, steep concentration gradients in Fe and Mn species develop in the metalimnion. These concentration gradients are AcknowledgmentsWe thank the International Nickel Company (INCO) Canada and PT INCO Tbk. for their financial and logistical support of both field and laboratory work. Support for Sean A. Crowe was partly provided by a Natural Sciences and Engineering Research Council (NSERC) Industrial Partnership Scholarship sponsored by INCO Canada. We are grateful to Bill Napier, Les Huelett, and Matt Orr for logistical support; Jim Gowans for the use of his patio boat, the

Soluble manganese(III) [Mn(III)] can potentially serve as both oxidant and reductant in one-electron-transfer reactions with other redox species. In near-surface sediment porewater, it is often overlooked as a major component of Mn cycling. Applying a spectrophotometric kinetic method to hemipelagic sediments from the Laurentian Trough (Quebec, Canada), we found that soluble Mn(III), likely stabilized by organic or inorganic ligands, accounts for up to 90% of the total dissolved Mn pool. Vertical profiles of dissolved oxygen and dissolved and solid Mn suggest that soluble Mn(III) is primarily produced via oxidation of Mn(II) diffusing upwards from anoxic sediments with lesser contributions from biotic and abiotic reductive dissolution of MnO2. The conceptual model of the sedimentary redox cycle should therefore explicitly include dissolved Mn(III).

In Lake Matano, Indonesia, the world's largest known ferruginous basin, more than 50% of authigenic organic matter is degraded through methanogenesis, despite high abundances of Fe (hydr)oxides in the lake sediments. Biogenic CH 4 accumulates to high concentrations (up to 1.4 mmol L ) and SO 4 2) in Lake Matano waters suggests that anaerobic methane oxidation may be coupled to the reduction of Fe (and ⁄ or Mn) (hydr)oxides. Thermodynamic considerations reveal that CH 4 oxidation coupled to Fe(III) or Mn(III ⁄ IV) reduction would yield sufficient free energy to support microbial growth at the substrate levels present in Lake Matano. Flux calculations imply that Fe and Mn must be recycled several times directly within the water column to balance the upward flux of CH 4 . 16S gene cloning identified methanogens in the anoxic water column, and these methanogens belong to groups capable of both acetoclastic and hydrogenotrophic methanogenesis. We find that methane is important in C cycling, even in this very Fe-rich environment. Such Fe-rich environments are rare on Earth today, but they are analogous to conditions in the ferruginous oceans thought to prevail during much of the Archean Eon. By analogy, methanogens and methanotrophs could have formed an important part of the Archean Ocean ecosystem.

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