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Paulsen, ML, Andersson AJ, Aluwihare L, Cyronak T, D'Angelo S, Davidson C, Elwany H, Giddings SN, Page HN, Porrachia M, Schroeter S.  2018.  Temporal changes in seawater carbonate chemistry and carbon export from a Southern California estuary. Estuaries and Coasts. 41:1050-1068.   10.1007/s12237-017-0345-8   AbstractWebsite

Estuaries are important subcomponents of the coastal ocean, but knowledge about the temporal and spatial variability of their carbonate chemistry, as well as their contribution to coastal and global carbon fluxes, are limited. In the present study, we measured the temporal and spatial variability of biogeochemical parameters in a saltmarsh estuary in Southern California, the San Dieguito Lagoon (SDL). We also estimated the flux of dissolved inorganic carbon (DIC) and total organic carbon (TOC) to the adjacent coastal ocean over diel and seasonal timescales. The combined net flux of DIC and TOC (FDIC + TOC) to the ocean during outgoing tides ranged from - 1.8 +/- 0.5 x 10(3) to 9.5 +/- 0.7 x 10(3) mol C h(-1) during baseline conditions. Based on these fluxes, a rough estimate of the net annual export of DIC and TOC totaled 10 +/- 4 x 10(6) mol C year(-1). Following a major rain event (36 mm rain in 3 days), FDIC + TOC increased and reached values as high as 29.0 +/- 0.7 x 10(3) mol C h(-1). Assuming a hypothetical scenario of three similar storm events in a year, our annual net flux estimate more than doubled to 25 +/- 4 x 10(6) mol C year(-1). These findings highlight the importance of assessing coastal carbon fluxes on different timescales and incorporating event scale variations in these assessments. Furthermore, for most of the observations elevated levels of total alkalinity (TA) and pH were observed at the estuary mouth relative to the coastal ocean. This suggests that SDL partly buffers against acidification of adjacent coastal surface waters, although the spatial extent of this buffering is likely small.

Andersson, AJ, Krug LA, Bates NR, Doney SC.  2013.  Sea-air CO2 flux in the North Atlantic subtropical gyre: Role and influence of Sub-Tropical Mode Water formation. Deep-Sea Research Part Ii-Topical Studies in Oceanography. 91:57-70.   10.1016/j.dsr2.2013.02.022   AbstractWebsite

The uptake of atmospheric carbon dioxide (CO2) into the mid-latitudes of the North Atlantic Ocean through the production of wintertime Sub-Tropical Mode Water (STMW) also known as Eighteen Degree Water (EDW) is poorly quantified and constrained. Nonetheless, it has been proposed that the EDW could serve as an important short-term sink of anthropogenic CO2. The objective of the present investigation was to determine sea-air CO2 gas exchange rates and seawater CO2 dynamics during wintertime formation of EDW in the North Atlantic Ocean. During 2006 and 2007, several research cruises were undertaken as part of the CLIMODE project across the northwest Atlantic Ocean with the intent to study the pre-conditioning, formation, and the evolution of EDW. Sea-air CO2 exchange rates were calculated based on measurements of atmospheric pCO(2), surface seawater pCO(2) and wind speed with positive values denoting a net flux from the surface ocean to the atmosphere. Average sea-air CO2 flux calculated along cruise tracks in the formation region equaled -18 +/- 6 mmol CO2 m(-2) d(-1) and -14 +/- 9 mmol CO2 m(-2) d(-1) in January of 2006 and March of 2007, respectively. Average sea-air CO2 flux in newly formed outcropping EDW in February and March of 2007 equaled -28 +/- 10 mmol CO2 m(-2) d(-1). These estimates exceeded previous flux estimates in this region by 40-185%. The magnitude of CO2 flux was mainly controlled by the observed variability in wind speed and Delta pCO(2) with smaller changes owing to variability in sea surface temperature. Small but statistically significant difference (4.1 +/- 2.6 mu mol kg(-1)) in dissolved inorganic carbon (DIC) was observed in two occurrences of newly formed EDW in February and March of 2007. This difference was explained either by differences in the relative contribution from different water masses involved in the initial formation process of EDW or temporal changes owing to sea-air CO2 exchange (similar to 25%) and vertical and/or lateral mixing (similar to 75%) with water masses high in DIC from the cold side of the Gulf Stream and/or from below the permanent thermocline. Based on the present estimate of sea-air CO2 flux in newly formed EDW and a formation rate of 9.3 Sv y (Sverdrup year = 10(6) m(3) s(-1) flow sustained for 1 year), CO2 uptake by newly formed EDW may constitute 3-6% of the total North Atlantic CO2 sink. However, advection of surface waters that carry an elevated burden of anthropogenic CO2 that are transported to the formation region and transformed to mode water may contribute additional CO2 to the total net uptake and sequestration of anthropogenic CO2 to the ocean interior. (c) 2013 Elsevier Ltd. All rights reserved.

Lerman, A, Guidry M, Andersson AJ, Mackenzie FT.  2011.  Coastal Ocean Last Glacial Maximum to 2100 CO(2)-Carbonic Acid-Carbonate System: A Modeling Approach. Aquatic Geochemistry. 17:749-773.   10.1007/s10498-011-9146-z   AbstractWebsite

Using coupled terrestrial and coastal zone models, we investigated the impacts of deglaciation and anthropogenic inputs on the CO(2)-H(2)O-CaCO(3) system in global coastal ocean waters from the Last Glacial Maximum (LGM: 18,000 year BP) to the year 2100. With rising sea level and atmospheric CO(2), the carbonate system of coastal ocean water changed significantly. We find that 6 x 10(12) metric tons of carbon were emitted from the coastal ocean, growing due to the sea level rise, from the LGM to late preindustrial time (1700 AD) because of net heterotrophy and calcification processes. This carbon came to reside in the atmosphere and in the growing vegetation on land and in uptake of atmospheric CO(2) through the weathering of rocks on land. It appears that carbonate accumulation, mainly, but not exclusively, in coral reefs from the LGM to late preindustrial time could account for about 24 ppmv of the 100 ppmv rise in atmospheric CO(2), lending some support to the "coral reef hypothesis". In addition, the global coastal ocean is now, or soon will be, a sink of atmospheric CO(2). The temperature rise of 4-5A degrees C since the LGM led to increased weathering rates of inorganic and organic materials on land and enhanced riverine fluxes of total C, N, and P to the coastal ocean of 68%, 108%, and 97%, respectively, from the LGM to late preindustrial time. During the Anthropocene, these trends have been exacerbated owing to rising atmospheric CO(2), due to fossil fuel combustion and land-use practices, other human activities, and rising global temperatures. River fluxes of total reactive C, N, and P are projected to increase from late preindustrial time to the year 2100 by 150%, 380%, and 257%, respectively, modifying significantly the behavior of these element cycles in the coastal ocean, particularly in proximal environments. Despite the fact that the global shoal water carbonate mass has grown extensively since the LGM, the pH(T) (pH values on the total proton scale) of global coastal waters has decreased from similar to 8.35 to similar to 8.18 and the carbonate ion concentration declined by similar to 19% from the LGM to late preindustrial time. The latter represents a rate of decline of about 0.028 mu mol CO(3) (2-) per decade. In comparison, the decrease in coastal water pH(T) from the year 1900 to 2000 was about 8.18-8.08 and is projected to decrease further from about 8.08 to 7.85 between 2000 and 2100, according to the IS92a business-as-usual scenario of CO(2) emissions. Over these 200 years, the carbonate ion concentration will fall by similar to 120 mu mol kg(-1) or 6 mu mol kg(-1) per decade. This decadal rate of decline of the carbonate ion concentration in the Anthropocene is 214 times the average rate of decline for the entire Holocene. Hence, when viewed against the millennial to several millennial timescale of geologic change in the coastal ocean marine carbon system, one can easily appreciate why ocean acidification is the "other CO(2) problem".

Mackenzie, FT, Andersson AJ, Arvidson RS, Guidry MW, Lerman A.  2011.  Land-sea carbon and nutrient fluxes and coastal ocean CO(2) exchange and acidification: Past, present, and future. Applied Geochemistry. 26:S298-S302.   10.1016/j.apgeochem.2011.03.087   AbstractWebsite

Epochs of changing atmospheric CO(2) and seawater CO(2)-carbonic acid system chemistry and acidification have occurred during the Phanerozoic at various time scales. On the longer geologic time scale, as sea level rose and fell and continental free board decreased and increased, respectively, the riverine fluxes of Ca, Mg, DIC, and total alkalinity to the coastal ocean varied and helped regulate the C chemistry of seawater, but nevertheless there were major epochs of ocean acidification (OA). On the shorter glacial-interglacial time scale from the Last Glacial Maximum (LGM) to late preindustrial time, riverine fluxes of DIC, total alkalinity, and N and P nutrients increased and along with rising sea level, atmospheric PCO(2) and temperature led, among other changes, to a slightly deceasing pH of coastal and open ocean waters, and to increasing net ecosystem calcification and decreasing net heterotrophy in coastal ocean waters. From late preindustrial time to the present and projected into the 21st century, human activities, such as fossil fuel and land-use emissions of CO(2) to the atmosphere, increasing application of N and P nutrient subsidies and combustion N to the landscape, and sewage discharges of C, N, P have led, and will continue to lead, to significant modifications of coastal ocean waters. The changes include a rapid decline in pH and carbonate saturation state (modern problem of ocean acidification), a shift toward dissolution of carbonate substrates exceeding production, potentially leading to the "demise" of the coral reefs, reversal of the direction of the sea-to-air flux of CO(2) and enhanced biological production and burial of organic C, a small sink of anthropogenic CO(2), accompanied by a continuous trend toward increasing autotrophy in coastal waters. (C) 2011 Elsevier Ltd. All rights reserved.

Andersson, AJ, Mackenzie FT, Lerman A.  2006.  Coastal ocean CO(2)-carbonic acid-carbonate sediment system of the Anthropocene. Global Biogeochemical Cycles. 20   10.1029/2005gb002506   AbstractWebsite

[1] There is little doubt that human activities such as burning of fossil fuels and land use practices have changed and will continue to change the cycling of carbon in the global coastal ocean. In the present study, two biogeochemical box models were used to investigate the consequences of increasing atmospheric CO(2) and subsequent ocean acidification and increasing riverine transport of organic matter and nutrients arising from human activities on land on the global coastal ocean between the years 1700 and 2300. Numerical simulations show that the net flux of CO(2) between coastal ocean surface water and the atmosphere is likely to change during this time from net evasion to net invasion owing to increasing atmospheric CO(2), increasing net ecosystem production arising from increasing nutrient loading to this region, and decreasing net ecosystem calcification due to lower carbonate ion concentration and subsequent lower surface water saturation state with respect to carbonate minerals. Model calculations show that surface water saturation state with respect to calcite will decrease 73% by the year 2300 under a business-as-usual scenario, which in concert with increasing temperature will cause overall biogenic calcification rate to decrease by 90%. Dissolution of carbonate minerals increased by 267% throughout the model simulation. This increase was in part due to increased invasion of atmospheric CO(2), but mainly due to greater deposition and remineralization of land-derived and in situ produced organic matter in the sediments, producing CO(2) that caused pore water pH and carbonate saturation state to decrease. This decrease, in turn, drove selective dissolution of metastable carbonate minerals. As a consequence, the relative carbonate composition of the sediments changed in favor of carbonate phases with lower solubility than that of an average 15 mol% magnesian calcite phase. Model projected changes in surface water carbonate saturation state agree well with observations from the Hawaiian Ocean Time series and the calculated air-sea CO(2) exchanged agrees well with a recent independent estimate of this flux derived from measurements from diverse coastal ecosystems scaled up to the global coastal ocean area.

Andersson, AJ, Mackenzie FT, Lerman A.  2005.  Coastal ocean and carbonate systems in the high CO(2) world of the anthropocene. American Journal of Science. 305:875-918.   10.2475/ajs.305.9.875   AbstractWebsite

The behavior of the ocean carbon cycle has been, and will continue to be, modified by the increase in atmospheric CO(2) due to fossil fuel combustion and land-use emissions of this gas. The consequences of a high-CO(2) world and increasing riverine transport of organic matter and nutrients arising from human activities were investigated by means of two biogeochemical box models. Model numerical simulations ranging from the year 1700 to 2300 show that the global coastal ocean changes from a net source to a net sink of atmospheric CO(2) over time; in the 18th and 19th centuries, the direction of the CO(2) flux was from coastal surface waters to the atmosphere, whereas at present or in the near future the net CO(2) flux is into coastal surface waters. These results agree well with recent syntheses of measurements of air-sea CO(2) exchange fluxes from various coastal ocean environments. The model calculations also show that coastal ocean surface water carbonate saturation state would decrease 46 percent by the year 2100 and 73 percent by 2300. Observational evidence from the Pacific and Atlantic Oceans shows that die carbonate saturation state of surface ocean waters has already declined during recent decades. For atolls and other semi-enclosed carbonate systems, the rate of decline depends strongly on the residence time of the water in the system. Based on the experimentally observed positive relationship between saturation state and calcification rate for many calcifying organisms, biogenic production of CaCO(3) may decrease by 42 percent by the year 2100 and by 85 to 90 percent by 2300 relative to its value of about 24 x 10(12) moles C/yr in the year 2000. If the predicted change in carbonate production were to occur along with rising temperatures, it would make it difficult for coral reef and other carbonate systems, to exist as we know them now into future centuries. Because high-latitude, cold-water carbonates presently occur in waters closer to saturation with respect to carbonate minerals than the more strongly supersaturated waters of the lower latitudes, it might be anticipated that the cool-water carbonate systems might feel the effects of rising atmospheric CO(2) (and temperature) before those at lower latitudes. In addition, modeling results show that the carbonate saturation state of coastal sediment pore water will decrease in the future owing to a decreasing pore water pH and increasing CO(2) concentrations attributable to greater deposition and remineralization of land-derived and in situ produced organic matter in sediments. The lowered carbonate saturation state drives selective dissolution of metastable carbonate minerals while a metastable equilibrium is maintained between the pore water and the most soluble carbonate phase present in the sediments. In the future, the average composition of carbonate sediments and cements may change as the more soluble Mg-calcites and aragonite are preferentially dissolved and phases of lower solubility, such as calcites with lower magnesium content, increase in percentage abundance in the sediments.

Mackenzie, FT, Lerman A, Andersson AJ.  2004.  Past and present of sediment and carbon biogeochemical cycling models. Biogeosciences. 1:11-32. AbstractWebsite

The global carbon cycle is part of the much more extensive sedimentary cycle that involves large masses of carbon in the Earth's inner and outer spheres. Studies of the carbon cycle generally followed a progression in knowledge of the natural biological, then chemical, and finally geological processes involved, culminating in a more or less integrated picture of the biogeochemical carbon cycle by the 1920s. However, knowledge of the ocean's carbon cycle behavior has only within the last few decades progressed to a stage where meaningful discussion of carbon processes on an annual to millennial time scale can take place. In geologically older and pre-industrial time, the ocean was generally a net source of CO2 emissions to the atmosphere owing to the mineralization of land-derived organic matter in addition to that produced in situ and to the process of CaCO3 precipitation. Due to rising atmospheric CO2 concentrations because of fossil fuel combustion and land use changes, the direction of the air-sea CO2 flux has reversed, leading to the ocean as a whole being a net sink of anthropogenic CO2. The present thickness of the surface ocean layer, where part of the anthropogenic CO2 emissions are stored, is estimated as of the order of a few hundred meters. The oceanic coastal zone net air-sea CO2 exchange flux has also probably changed during industrial time. Model projections indicate that in preindustrial times, the coastal zone may have been net heterotrophic, releasing CO2 to the atmosphere from the imbalance between gross photosynthesis and total respiration. This, coupled with extensive CaCO3 precipitation in coastal zone environments, led to a net flux of CO2 out of the system. During industrial time the coastal zone ocean has tended to reverse its trophic status toward a non-steady state situation of net autotrophy, resulting in net uptake of anthropogenic CO2 and storage of carbon in the coastal ocean, despite the significant calcification that still occurs in this region. Furthermore, evidence from the inorganic carbon cycle indicates that deposition and net storage of CaCO3 in sediments exceed inflow of inorganic carbon from land and produce CO2 emissions to the atmosphere. In the shallow-water coastal zone, increase in atmospheric CO2 during the last 300 years of industrial time may have reduced the rate of calcification, and continuation of this trend is an issue of serious environmental concern in the global carbon balance.