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  • 1
    Publication Date: 2022-05-25
    Description: Author Posting. © Elsevier B.V., 2008. 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 Journal of Environmental Radioactivity 99 (2008): 1596-1610, doi:10.1016/j.jenvrad.2008.06.010.
    Description: Results of groundwater and seawater analyses for radioactive (3H, 222Rn, 223Ra, 224Ra, 226Ra, 228Ra) and stable (2H, 18O) isotopes are presented together with in situ spatial mapping and time-series 222Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d-1 to 360 cm d-1; the unit represents cm3/cm2/day), as well as during a few hours (from 0 cm d-1 to 110 cm d-1), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous 222Rn measurements is 17±10 cm d-1. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7x103 m3 d-1 per km of the coast. The isotopic composition (δ2H and δ18O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time-series measurements of 222Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1-2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.
    Description: This research was supported by IAEA and UNESCO (IOC and IHP) in the framework of the joint SGD project. Science support for some U.S. investigators was provided by grants from the National Science Foundation (OCE03-50514 to WCB and OCE02-33657 to WSM).
    Keywords: Submarine groundwater discharge ; Groundwater ; Seawater ; Stable isotopes ; δD ; δ18O ; Tritium ; Radium isotopes ; Radon ; Coastal zone ; Ubatuba ; Brazil
    Repository Name: Woods Hole Open Access Server
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  • 2
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2010. 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 74 (2010): 3768-3784, doi:10.1016/j.gca.2010.03.035.
    Description: Subsurface microbial oxidation of overridden soils and vegetation beneath glaciers and ice sheets may affect global carbon budgets on glacial-interglacial timescales. The likelihood and magnitude of this process depends on the chemical nature and reactivity of the subglacial organic carbon stores. We examined the composition of carbon pools associated with different regions of the Greenland ice sheet (subglacial, supraglacial, proglacial) in order to elucidate the type of dissolved organic matter (DOM) present in the subglacial discharge over a melt season. Electrospray ionization (ESI) Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry coupled to multivariate statistics permitted unprecedented molecular level characterization of this material and revealed that carbon pools associated with discrete glacial regions are comprised of different compound classes. Specifically, a larger proportion of protein-like compounds were observed in the supraglacial samples and in the early melt season (spring) subglacial discharge. In contrast, the late melt season (summer) subglacial discharge contained a greater fraction of lignin-like and other material presumably derived from underlying vegetation and soil. These results suggest (1) that the majority of supraglacial DOM originates from autochthonous microbial processes on the ice sheet surface, (2) that the subglacial DOM contains allochthonous carbon derived from overridden soils and vegetation as well as autochthonous carbon derived from in situ microbial metabolism, and (3) that the relative contribution of allochthonous and autochthonous material in subglacial discharge varies during the melt season. These conclusions are consistent with the hypothesis that, given sufficient time (e.g., overwinter storage), resident subglacial microbial communities may oxidize terrestrial material beneath the Greenland ice sheet.
    Description: This research was supported by: the National Science Foundation (CAREER-OCE- 0529101 (EBK), ARC-0520077 (SBD)), National Atmospheric and Space Administration (SBD), the WHOI Clark Arctic Research Initiative (EBK, SBD, MAC), the WHOI Ocean Ventures Fund (MPB), and the National and Science Engineering Research Council of Canada (MPB).
    Keywords: Glacier ; Ultrahigh resolution mass spectrometry ; FT-ICR ; Organic carbon ; DOM
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  • 3
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2013. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 40 (2013): 2701–2706, doi:10.1002/grl.50192.
    Description: To better understand the physical drivers of submarine groundwater discharge (SGD) in the coastal ocean, we conducted a detailed field and modeling study within an unconfined coastal aquifer system. We monitored the hydraulic gradient across the coastal aquifer and movement of the mixing zone over multiple years. At our study site, sea level dominated over groundwater head as the largest contributor to variability in the hydraulic gradient and therefore SGD. Model results indicate the seawater recirculation component of SGD was enhanced during summer while the terrestrial component dominated during winter due to seasonal changes in sea level driven by a combination of long period solar tides, temperature and winds. In one year, sea level remained elevated year round due to a combination of ENSO and NAO climate modes. Hence, predicted changes in regional climate variability driven sea level may impact future rates of SGD and biogeochemical cycling within coastal aquifers.
    Description: This work is a result of research sponsored by the NSF Chemical Oceanography program (OCE- 0425061 to M.C. and A.M. and OCE-0751525 to M.C.) and an NDSEG graduate fellowship (to M.G.).
    Description: 2013-12-03
    Keywords: Groundwater ; Sea level ; Climate ; Submarine groundwater discharge ; Coastal aquifer
    Repository Name: Woods Hole Open Access Server
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  • 4
    Publication Date: 2022-05-25
    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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  • 5
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2011. 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 Journal of Environmental Radioactivity 104 (2012): 24-45, doi:10.1016/j.jenvrad.2011.09.009.
    Description: Submarine groundwater discharge (SGD) into a shallow lagoon on the west coast of Mauritius Island (Flic-en-Flac) was investigated using radioactive (3H, 222Rn, 223Ra, 224Ra, 226Ra, 228Ra) and stable (2H, 18O) isotopes and nutrients. SGD intercomparison exercises were carried out to validate the various approaches used to measure SGD including radium and radon measurements, seepage-rate measurements using manual and automated meters, sediment bulk conductivity and salinity surveys. SGD measurements using benthic chambers placed on the floor of the Flic-en-Flac Lagoon showed discharge rates up to 500 cm/day. Large variability in SGD was observed over distances of a few meters, which were attributed to different geomorphological features. Deployments of automated seepage meters captured the spatial and temporal variability of SGD with a mean seepage rate of 10 cm/day. The stable isotopic composition of submarine waters was characterized by significant variability and heavy isotope enrichment and was used to predict the contribution of fresh terrestrially derived groundwater to SGD (range from a few % to almost 100 %). The integrated SGD flux, estimated from seepage meters placed parallel to the shoreline, was 35 m3/m day, which was in a reasonable agreement with results obtained from hydrologic water balance calculation (26 m3/m day). SGD calculated from the radon inventory method using in situ radon measurements were between 5 and 56 m3/m per day. Low concentrations of radium isotopes observed in the lagoon water reflected the low abundance of U and Th in the basalt that makes up the island. High SGD rates contribute to high nutrients loading to the lagoon, potentially leading to eutrophication. Each of the applied methods yielded unique information about the character and magnitude of SGD. The results of the intercomparison studies have resulted a better understanding of groundwater-seawater interactions in coastal regions. Such information is an important pre-requisite for the protection management of coastal freshwater resources.
    Description: The financial support provided by the IOC and IHP of UNESCO for travel arrangements, and by the IAEA’s Marine Environment Laboratories for logistics is highly acknowledged. MAC and MEG were supported in part by the US National Science Foundation (OCE-0425061 and OCE-0751525). PPP acknowledges a support provided by the EU Research & Development Operational Program funded by the ERDF (project No. 26240220004), and the Slovak Scientific Agency VEGA (grant No. 1/108/08). The International Atomic Energy Agency is grateful to the Government of the Principality of Monaco for support provided to its Marine Environment Laboratories.
    Keywords: Submarine groundwater discharge ; Groundwater ; Seawater ; Seepage meters ; Stable isotopes ; δD ; δ18O ; Tritium ; Radium isotopes ; Radon ; Nutrients ; Coastal zone ; Volcanic island ; Mauritius Island
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  • 6
    Publication Date: 2022-05-25
    Description: This paper is not subject to U.S. copyright. The definitive version was published in Earth and Planetary Science Letters 462 (2017): 180-188, doi:10.1016/j.epsl.2016.12.039.
    Description: Water flow beneath the Greenland Ice Sheet (GrIS) has been shown to include slow-inefficient (distributed) and fast-efficient (channelized) drainage systems, in response to meltwater delivery to the bed via both moulins and surface lake drainage. This partitioning between channelized and distributed drainage systems is difficult to quantify yet it plays an important role in bulk meltwater chemistry and glacial velocity, and thus subglacial erosion. Radon-222, which is continuously produced via the decay of 226Ra, accumulates in meltwater that has interacted with rock and sediment. Hence, elevated concentrations of 222Rn should be indicative of meltwater that has flowed through a distributed drainage system network. In the spring and summer of 2011 and 2012, we made hourly 222Rn measurements in the proglacial river of a large outlet glacier of the GrIS (Leverett Glacier, SW Greenland). Radon-222 activities were highest in the early melt season (10–15 dpm L−1), decreasing by a factor of 2–5 (3–5 dpm L−1) following the onset of widespread surface melt. Using a 222Rn mass balance model, we estimate that, on average, greater than 90% of the river 222Rn was sourced from distributed system meltwater. The distributed system 222Rn flux varied on diurnal, weekly, and seasonal time scales with highest fluxes generally occurring on the falling limb of the hydrograph and during expansion of the channelized drainage system. Using laboratory based estimates of distributed system 222Rn, the distributed system water flux generally ranged between 1–5% of the total proglacial river discharge for both seasons. This study provides a promising new method for hydrograph separation in glacial watersheds and for estimating the timing and magnitude of distributed system fluxes expelled at ice sheet margins.
    Description: U.S. National Science Foundation Arctic Natural Sciences Program (ANS-1256669); Woods Hole Oceanographic Institution Arctic Research Initiative, Ocean Ventures Fund, and Ocean Climate Change Institute; United Kingdom Natural Environment Research Council studentship (NE/152830X/1); the Carnegie Trust, Edinburgh University Development Trust.
    Keywords: Radon ; Greenland ; Glacier ; Proglacial river ; Meltwater
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  • 7
    Publication Date: 2022-10-26
    Description: Author Posting. © The Japan Society for Analytical Chemistry, 2020. This article is posted here by permission of The Japan Society for Analytical Chemistry for personal use, not for redistribution. The definitive version was published in Nagao, S., Terasaki, S., Ochiai, S., Fukushi, K., Tomihara, S., Charette, M. A., & Buesseler, K. O. Desorption behavior of Fukushima-derived radiocesium in sand collected from Yotsukura Beach in Fukushima prefecture. Analytical Sciences, 36(5), (2020): 569-575, doi:10.2116/analsci.19SBP08.
    Description: Beach sand samples were collected along a coastal area 32 km south of the Fukushima Daiichi Nuclear Power Plant (FDNPP) in Fukushima Prefecture, Japan, 5 years after the FDNPP accident. Desorption experiments were performed on the sand samples using seawater in a batch experimental system to understand the forms of existence of radiocesium in sand and their desorption behavior in a coastal environment. The percentage of radiocesium desorption decreased exponentially with an increase in the number of desorption experiments for the four sand samples, with 137Cs radioactivity from 16 to 1077 Bq kg−1 at surface and deeper layers from three sites. Total desorption percentage ranged from 19 to 58% in 12 desorption experiments. The results indicate that the weak adsorption varies with the sampling sites and their depth layer. To understand the desorption behavior of radiocesium in the sand samples, the desorption experiments were performed for a sand sample by using natural and artificial seawater, and NaCl solution in the presence and absence of KCl. The 137Cs desorption from the sand collected at a depth of 100 – 105 cm from the ground surface (137Cs radioactivity 1052 ± 25 Bq kg−1) was 0.1% by ultrapure water, 3.7% by 1/4 seawater and 7.1% by 1/2 seawater, 2.2% by 470 mM NaCl solution (corresponding to a similar concentration of seawater) and 10 – 12% by seawater, artificial seawater and 470 mM NaCl + 8 mM KCl solution. These results indicate that about 10% of radiocesium adsorbed on the sand is mainly desorbed by ion exchange of potassium ion in seawater, though the concentration of major cation, or sodium ion, in seawater makes a small contribution on 137Cs desorption from the sand samples.
    Description: This study was partly supported by a Grant-in-Aid for scientific research (2411008) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), and the Gordon and Betty Moore Foundation. We thank Kousuke Yoshida, Maxi Castrillejo and Nuria Casacuberta for the help with beach sampling.
    Keywords: Cs ; Beach sand ; Ion exchange ; Potassium ion ; Groundwater ; Fukushima Daiichi Nuclear Power Plant accident
    Repository Name: Woods Hole Open Access Server
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