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  • 1
    Publication Date: 2017-01-05
    Description: Author Posting. © Elsevier B.V., 2007. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Marine Chemistry 110 (2008): 120-127, doi:10.1016/j.marchem.2008.02.011.
    Description: Submarine groundwater discharge (SGD), in form of springs and diffuse seepage, has long been recognized as a source of chemical constituents to the coastal ocean. Because groundwater is two to four orders of magnitude richer in radon than surface water, it has been used as both a qualitative and a quantitative tracer of groundwater discharge. Besides this large activity gradient, the other perceived advantage of radon stems from its classification as noble gas; that is, its chemical behavior is expected not to be influenced by salinity, redox, and diagenetic conditions present in aquatic environments. During our three-year monthly sampling of the subterranean estuary (STE) in Waquoit Bay, MA, we found highly variable radon activities (50-1600 dpm L-1) across the fresh-saline interface of the aquifer. We monitored pore water chemistry and radon activity at 8 fixed depths spanning from 2 to 5.6 m across the STE, and found seasonal fluctuations in activity at depths where elevated radon was observed. We postulate that most of pore water 222Rn is produced from particle-surface bound 226Ra, and that the accumulation of this radium is likely regulated by the presence of manganese (hydr)oxides. Layers of manganese (hydr)oxides form at the salinity transition zone (STZ), where water with high salinity, high manganese, and low redox potential mixes with fresh water. Responding to the seasonality of aquifer recharge, the location of the STZ and the layers with radium enriched manganese (hydr)oxide follows the seasonal land- or bay-ward movement of the freshwater lens. This results in seasonal changes in the depth where elevated radon activities are observed. The conclusion of our study is that the freshwater part of the STE has a radon signature that is completely different from the STZ or recirculated sea water. Therefore, the radon activity in SGD will depend on the ratio of fresh and recirculated seawater in the discharging groundwater.
    Description: This work is a result of research sponsored by NSF (OCE- 0425061 to M.A.C.) and the WHOI Postdoctoral Scholar program (to H.D.).
    Keywords: Subterranean estuary ; Geochemical tracers ; Radon ; Radium ; Manganese ; Groundwater ; Submarine groundwater discharge ; Geochemical transformations
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  • 2
    Publication Date: 2016-04-26
    Description: Author Posting. © The Author(s), 2013. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 117 (2013): 33-52, doi:10.1016/j.gca.2013.03.021.
    Description: Submarine groundwater discharge (SGD) to the ocean supplies Sr with less radiogenic 87Sr/86Sr than seawater, and thus constitutes an important term in the Sr isotope budget in the modern ocean. However, few data exist for Sr in coastal groundwater or in the geochemically dynamic subterranean estuary (STE). We examined Sr concentrations and isotope ratios from nine globally-distributed coastal sites and characterized the behavior of Sr in the STE. Dissolved Sr generally mixed conservatively in the STE, although large differences were observed in the meteoric groundwater end-member Sr concentrations among sites (0.1 – 24 μM Sr). Strontium isotope exchange was observed in the STE at five of the sites studied, and invariably favored the meteoric groundwater end-member signature. Most of the observed isotope exchange occurred in the salinity range 5-15, and reached up to 40% exchange at salinity 10. Differences in fresh groundwater Sr concentrations and isotope ratios (87Sr/86Sr = 0.707-0.710) reflected aquifer lithology. The SGD end-member 87Sr/86Sr must be lower than modern seawater (i.e., less than 0.70916) in part because groundwater Sr concentrations are orders of magnitude higher in less-carbonate and volcanic island aquifers. A simple lithological model and groundwater Sr data compiled from the literature were used to estimate a global average groundwater end-member of 2.9 μM Sr with 87Sr/86Sr = 0.7089. This represents a meteoric-SGD-driven Sr input to the ocean of 0.7-2.8 × 1010 mol Sr y-1. Meteoric SGD therefore accounts for 2-8% of the oceanic Sr isotope budget, comparable to other known source terms, but is insufficient to balance the remainder of the budget. Using reported estimates for brackish SGD, the estimated volume discharge at salinity 10 (7-11 × 1015 L y-1) was used to evaluate the impact of isotope exchange in the STE on the brackish SGD Sr flux. A moderate estimate of 25% isotope exchange in the STE gives an SGD Sr end-member 87Sr/86Sr of 0.7091. The brackish SGD Sr flux thus accounts for 11-23% of the marine Sr isotope budget, but does not appear sufficient to balance the ~40% remaining after other known sources are included. Substantial uncertainties remain for estimating the SGD source of Sr to the global ocean, especially in the determination of the volume flux of meteoric SGD, and in the paucity of measurements of groundwater Sr isotope composition in major SGD regions such as Papua New Guinea, the South America west coast, and West Africa. Consequently, our global estimate should be viewed with some caution. Nevertheless, we show that the combined sources of meteoric SGD and brackish SGD coupled with isotope exchange in the STE may constitute a substantial component (~13-30%) of the modern oceanic 87Sr/86Sr budget, likely exceeding less radiogenic Sr inputs by sedimentary diagenesis and hydrothermal circulation through the mid-ocean ridge system. Temporal variation in SGD Sr fluxes and isotope composition may have contributed to fluctuations in the oceanic 87Sr/86Sr ratio over geologic time.
    Description: This project was supported by funding from the WHOI Coastal Ocean 670 Institute and the Tropical Research Initiative, and NSF OCE-0751525 to MAC. BPE acknowledges financial support from NSF ETBC-85101500 and a WHOI Coastal Ocean Institute Fellowship.
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  • 3
    Publication Date: 2017-01-04
    Description: Author Posting. © Association for the Sciences of Limnology and Oceanography, 2012. This article is posted here by permission of Association for the Sciences of Limnology and Oceanography for personal use, not for redistribution. The definitive version was published in Limnology and Oceanography: Methods 10 (2012): 451-463, doi:10.4319/lom.2012.10.451.
    Description: In anticipation of the international GEOTRACES program, which will study the global marine biogeochemistry of trace elements and isotopes, we conducted a multi-lab intercomparison for radium isotopes. The intercomparison was in two parts involving the distribution of: (1) samples collected from four marine environments (open ocean, continental slope, shelf, and estuary) and (2) a suite of four reference materials prepared with isotopic standards (circulated to participants as 'unknowns'). Most labs performed well with 228Ra and 224Ra determination, however, there were a number of participants that reported 226Ra, 223Ra, and 228Th (supported 224Ra) well outside the 95% confidence interval. Many outliers were suspected to be a result of poorly calibrated detectors, though other method specific factors likely played a role (e.g., detector leakage, insufficient equilibration). Most methods for radium analysis in seawater involve a MnO2 fiber column preconcentration step; as such, we evaluated the extraction efficiency of this procedure and found that it ranged from an average of 87% to 94% for the four stations. Hence, nonquantitative radium recovery from seawater samples may also have played a role in lab-to-lab variability.
    Description: This work was funded by grants from the National Science Foundation (OCE- 0751461to M.A.C and H.D. and OCE- 0751867 to W.S.M.).
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  • 4
    Publication Date: 2017-01-04
    Description: Author Posting. © Association for the Sciences of Limnology and Oceanography, 2012. This article is posted here by permission of Association for the Sciences of Limnology and Oceanography for personal use, not for redistribution. The definitive version was published in Limnology and Oceanography: Methods 10 (2012): 617, doi:10.4319/lom.2012.10.617.
    Description: In our original paper, Charette, M. A., H. Dulaiova, M. E. Gonneea, P. B. Henderson, W. S. Moore, J. C. Scholten, and M. K. Pham. 2012. GEOTRACES radium isotopes interlaboratory comparison experiment. Limonol. Oceanogr.: Methods 10:451, the incorrect headers were used for Table 9.
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  • 5
    Publication Date: 2017-08-16
    Description: Author Posting. © American Geophysical Union, 2017. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Paleoceanography 32 (2017): 146–160, doi:10.1002/2016PA002976.
    Description: Coral skeletons are valuable archives of past ocean conditions. However, interpretation of coral paleotemperature records is confounded by uncertainties associated with single-element ratio thermometers, including Sr/Ca. A new approach, Sr-U, uses U/Ca to constrain the influence of Rayleigh fractionation on Sr/Ca. Here we build on the initial Pacific Porites Sr-U calibration to include multiple Atlantic and Pacific coral genera from multiple coral reef locations spanning a temperature range of 23.15–30.12°C. Accounting for the wintertime growth cessation of one Bermuda coral, we show that Sr-U is strongly correlated with the average water temperature at each location (r2 = 0.91, P 〈 0.001, n = 19). We applied the multispecies spatial calibration between Sr-U and temperature to reconstruct a 96 year long temperature record at Mona Island, Puerto Rico, using a coral not included in the calibration. Average Sr-U derived temperature for the period 1900–1996 is within 0.12°C of the average instrumental temperature at this site and captures the twentieth century warming trend of 0.06°C per decade. Sr-U also captures the timing of multiyear variability but with higher amplitude than implied by the instrumental data. Mean Sr-U temperatures and patterns of multiyear variability were replicated in a second coral in the same grid box. Conversely, Sr/Ca records from the same two corals were inconsistent with each other and failed to capture absolute sea temperatures, timing of multiyear variability, or the twentieth century warming trend. Our results suggest that coral Sr-U paleothermometry is a promising new tool for reconstruction of past ocean temperatures.
    Description: NSF Graduate Research Fellowships Grant Numbers: NSF-OCE-1338320, NSF-OCE-1031971, NSF-OCE-0926986; WHOI Access to the Sea Grant Numbers: 27500056, 0734826; NSF HRD; UPR Central Administration to EAHD through the Center for Applied Tropical Ecology and Conservation of UPR
    Description: 2017-08-16
    Keywords: Coral ; Temperature ; Paleoceangraphy ; Paleothermometry ; Global warming ; Biomineralization
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  • 6
    Publication Date: 2017-01-04
    Description: Author Posting. © Elsevier B.V., 2007. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Deep Sea Research Part II: Topical Studies in Oceanography 54 (2007): 1989-1998, doi:10.1016/j.dsr2.2007.06.003.
    Description: Elevated levels of productivity in the wake of Southern Ocean island systems are common despite the fact that they are encircled by high nutrient low chlorophyll (HNLC) waters. In the Crozet Plateau region, it has been hypothesized that iron from island runoff or sediments of the plateau could be fueling the austral summer phytoplankton bloom. Here, we use radium isotopes to quantify the rates of surface ocean iron supply fueling the bloom in the Crozet Plateau region. A 1-D eddy-diffusion-mixing model applied to a 228Ra profile (t1/2 = 5.75 yr) at a station north of the islands suggested fast vertical mixing in the upper 300 m (Kz = 11-100 cm2 s- 1) with slower mixing between 300 and 1000 m (Kz = 1.5 cm2 s-1). This estimate is discussed in the context of Kz derived from the CTD/LADCP data. In combination with the dissolved Fe profile at this location, we estimated a vertical flux of between 5.6 and 31 nmol Fe m-2 d-1. The cross-plateau gradients in the short-lived radium isotopes, 224Ra (t1/2 = 3.66 d) and 223Ra (t1/2 = 11.4 d), yielded horizontal eddy diffusivities (Kh) of 39 m2 s-1 and 6.6 m2 s-1, respectively. If we assume that the islands (surface runoff) alone were supplying dissolved Fe to the bloom region, then the flux estimates range from 2.3 to 14 nmol Fe m-2 d-1. If the plateau sediments are considered a source of Fe, and conveyed to the bloom region through deep winter mixing combined with horizontal transport, then this flux may be as high as 64 to 390 nmol Fe m-2 d-1. Combined, these Fe sources are sufficient to initiate and maintain the annual phytoplankton bloom.
    Description: This work was funded by grants from the Natural Environment Research Council [NE/B502844/1] and the National Science Foundation (ANT-0443869 to M.A.C).
    Keywords: Radium isotopes ; Iron ; Productivity ; Ocean mixing ; Southern Ocean
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  • 7
    Publication Date: 2017-08-16
    Description: This paper is not subject to U.S. copyright. The definitive version was published in Geochimica et Cosmochimica Acta 209 (2017): 123-134, doi:10.1016/j.gca.2017.04.006.
    Description: Coral barium to calcium (Ba/Ca) ratios have been used to reconstruct records of upwelling, river and groundwater discharge, and sediment and dust input to the coastal ocean. However, this proxy has not yet been explicitly tested to determine if Ba inclusion in the coral skeleton is directly proportional to seawater Ba concentration and to further determine how additional factors such as temperature and calcification rate control coral Ba/Ca ratios. We measured the inclusion of Ba within aquaria reared juvenile corals (Favia fragum) at three temperatures (∼27.7, 24.6 and 22.5 °C) and three seawater Ba concentrations (73, 230 and 450 nmol kg−1). Coral polyps were settled on tiles conditioned with encrusting coralline algae, which complicated chemical analysis of the coral skeletal material grown during the aquaria experiments. We utilized Sr/Ca ratios of encrusting coralline algae (as low as 3.4 mmol mol−1) to correct coral Ba/Ca for this contamination, which was determined to be 26 ± 11% using a two end member mixing model. Notably, there was a large range in Ba/Ca across all treatments, however, we found that Ba inclusion was linear across the full concentration range. The temperature sensitivity of the distribution coefficient is within the range of previously reported values. Finally, calcification rate, which displayed large variability, was not correlated to the distribution coefficient. The observed temperature dependence predicts a change in coral Ba/Ca ratios of 1.1 μmol mol−1 from 20 to 28 °C for typical coastal ocean Ba concentrations of 50 nmol kg−1. Given the linear uptake of Ba by corals observed in this study, coral proxy records that demonstrate peaks of 10–25 μmol mol−1 would require coastal seawater Ba of between 60 and 145 nmol kg−1. Further validation of the coral Ba/Ca proxy requires evaluation of changes in seawater chemistry associated with the environmental perturbation recorded by the coral as well as verification of these results for Porites species, which are widely used in paleo reconstructions.
    Description: M.E.G. was supported by a NDSEG graduate fellowship. Funding for this research came from the NSF Chemical Oceanography program (OCE-0751525) and the Coastal Ocean Institute, the Ocean and Climate Change Institute and the Ocean Ventures Fund at Woods Hole Oceanographic Institution.
    Keywords: Coral Ba/Ca ; Barium ; Aragonite ; Distribution coefficient ; Favia fragum
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  • 8
    Publication Date: 2019-01-28
    Description: Author Posting. © American Geophysical Union, 2018. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research: Biogeosciences 123 (2018): 2234-2256, doi:10.1029/2018JG004556.
    Description: Coastal salt marshes play an important role in mitigating global warming by removing atmospheric carbon at a high rate. We investigated the environmental controls and emergent scaling of major greenhouse gas (GHG) fluxes such as carbon dioxide (CO2) and methane (CH4) in coastal salt marshes by conducting data analytics and empirical modeling. The underlying hypothesis is that the salt marsh GHG fluxes follow emergent scaling relationships with their environmental drivers, leading to parsimonious predictive models. CO2 and CH4 fluxes, photosynthetically active radiation (PAR), air and soil temperatures, well water level, soil moisture, and porewater pH and salinity were measured during May–October 2013 from four marshes in Waquoit Bay and adjacent estuaries, MA, USA. The salt marshes exhibited high CO2 uptake and low CH4 emission, which did not significantly vary with the nitrogen loading gradient (5–126 kg · ha−1 · year−1) among the salt marshes. Soil temperature was the strongest driver of both fluxes, representing 2 and 4–5 times higher influence than PAR and salinity, respectively. Well water level, soil moisture, and pH did not have a predictive control on the GHG fluxes, although both fluxes were significantly higher during high tides than low tides. The results were leveraged to develop emergent power law‐based parsimonious scaling models to accurately predict the salt marsh GHG fluxes from PAR, soil temperature, and salinity (Nash‐Sutcliffe Efficiency = 0.80–0.91). The scaling models are available as a user‐friendly Excel spreadsheet named Coastal Wetland GHG Model to explore scenarios of GHG fluxes in tidal marshes under a changing climate and environment.
    Description: National Oceanic and Atmospheric Administration Grant Numbers: NA09NOS4190153, NA14NOS4190145; National Science Foundation (NSF) Grant Numbers: 1705941, 1561941/1336911; USGS LandCarbon Program; NOAA National Estuarine Research Reserve Science Collaborative Grant Number: NA09NOS4190153 and NA14NOS4190145
    Description: 2019-01-28
    Keywords: Coastal salt marshes ; GHG fluxes ; Environmental controls ; Emergent scaling ; Modeling and predictions
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  • 9
    Publication Date: 2018-11-29
    Description: © The Author(s), 2018. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Marine Chemistry 206 (2018): 7-18, doi:10.1016/j.marchem.2018.08.005.
    Description: The lateral export of carbon from coastal marshes via tidal exchange is a key component of the marsh carbon budget and coastal carbon cycles. However, the magnitude of this export has been difficult to accurately quantify due to complex tidal dynamics and seasonal cycling of carbon. In this study, we use in situ, high-frequency measurements of dissolved inorganic carbon (DIC) and water fluxes to estimate lateral DIC fluxes from a U.S. northeastern salt marsh. DIC was measured by a CHANnelized Optical Sensor (CHANOS) that provided an in situ concentration measurement at 15-min intervals, during periods in summer (July – August) and late fall (December). Seasonal changes in the marsh had strong effects on DIC concentrations, while tidally-driven water fluxes were the fundamental vehicle of marsh carbon export. Episodic events, such as groundwater discharge and mean sea water level changes, can impact DIC flux through altered DIC concentrations and water flow. Variability between individual tides within each season was comparable to mean variability between the two seasons. Estimated mean DIC fluxes based on a multiple linear regression (MLR) model of DIC concentrations and high-frequency water fluxes agreed reasonably well with those derived from CHANOS DIC measurements for both study periods, indicating that high-frequency, modeled DIC concentrations, coupled with continuous water flux measurements and a hydrodynamic model, provide a robust estimate of DIC flux. Additionally, an analysis of sampling strategies revealed that DIC fluxes calculated using conventional sampling frequencies (hourly to two-hourly) of a single tidal cycle are unlikely to capture a representative mean DIC flux compared to longer-term measurements across multiple tidal cycles with sampling frequency on the order of tens of minutes. This results from a disproportionately large amount of the net DIC flux occurring over a small number of tidal cycles, while most tides have a near-zero DIC export. Thus, high-frequency measurements (on the order of tens of minutes or better) over the time period of interest are necessary to accurately quantify tidal exports of carbon species from salt marshes.
    Description: This work was funded by NSF Graduate Research Fellowship Program, NSF Ocean Sciences Postdoctoral Fellowship (OCE-1323728), Link FoundationOcean Engineering and Instrumentation Fellowship, National Institute of Science and Technology (NIST no. 60NANB10D024), the USGS LandCarbon and Coastal & Marine Geology Programs, NSF Chemical Oceanography Program (OCE-1459521), NSF Ocean Technology and Interdisciplinary Coordination program (OCE-1233654) and NOAA Science Collaborative (NA09NOS4190153).
    Keywords: Dissolved inorganic carbon ; Carbon export ; Salt marshes ; Wetlands
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  • 10
    Publication Date: 2019-04-10
    Description: © The Author(s), 2019. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Wang, F., Kroeger, K. D., Gonneea, M. E., Pohlman, J. W., & Tang, J. Water salinity and inundation control soil carbon decomposition during salt marsh restoration: An incubation experiment. Ecology and Evolution, 9(4), (2019):1911-1921, doi:10.1002/ece3.4884.
    Description: Coastal wetlands are a significant carbon (C) sink since they store carbon in anoxic soils. This ecosystem service is impacted by hydrologic alteration and management of these coastal habitats. Efforts to restore tidal flow to former salt marshes have increased in recent decades and are generally associated with alteration of water inundation levels and salinity. This study examined the effect of water level and salinity changes on soil organic matter decomposition during a 60‐day incubation period. Intact soil cores from impounded fresh water marsh and salt marsh were incubated after addition of either sea water or fresh water under flooded and drained water levels. Elevating fresh water marsh salinity to 6 to 9 ppt enhanced CO2 emission by 50%−80% and most typically decreased CH4 emissions, whereas, decreasing the salinity from 26 ppt to 19 ppt in salt marsh soils had no effect on CO2 or CH4 fluxes. The effect from altering water levels was more pronounced with drained soil cores emitting ~10‐fold more CO2 than the flooded treatment in both marsh sediments. Draining soil cores also increased dissolved organic carbon (DOC) concentrations. Stable carbon isotope analysis of CO2 generated during the incubations of fresh water marsh cores in drained soils demonstrates that relict peat OC that accumulated when the marsh was saline was preferentially oxidized when sea water was introduced. This study suggests that restoration of tidal flow that raises the water level from drained conditions would decrease aerobic decomposition and enhance C sequestration. It is also possible that the restoration would increase soil C decomposition of deeper deposits by anaerobic oxidation, however this impact would be minimal compared to lower emissions expected due to the return of flooding conditions.
    Description: We acknowledge collaboration and support from Tim Smith of the Cape Cod National Seashore, James Rassman and Tonna‐Marie Surgeon‐Rogers of the Waquoit Bay National Estuarine Research Reserve, Margot McKlveen of the Marine Biological Laboratory, Jennifer O'keefe Suttles, Wally Brooks and Michael Casso of the USGS, and Amanda Spivak of the Woods Hole Oceanographic Institution. This study was funded by the NOAA National Estuarine Research Reserve Science Collaborative (NA09NOS4190153 and NA14NOS4190145) awarded to JT and KK, MIT Sea Grant (2015‐R/RC‐141), and USGS‐Land Carbon and Coastal & Marine Geology projects. F.W. was also supported by funding from Natural Science Foundation of China (31300419, 31670621, 31870463). Any use of trade names is for descriptive purposes and does not imply endorsement by the U.S. government.
    Keywords: carbon dioxide ; greenhouse gas ; methane ; restoration ; salt marsh
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