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  • 1
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    Global estimate of submarine groundwater discharge based on an observationally constrained radium isotope model (2015)
    John Wiley & Sons
    Details
    Publication Date: 2022-05-25
    Description: © The Author(s), 2014. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Geophysical Research Letters 41 (2014): 8438–8444, doi:10.1002/2014GL061574.
    Description: Along the continental margins, rivers and submarine groundwater supply nutrients, trace elements, and radionuclides to the coastal ocean, supporting coastal ecosystems and, increasingly, causing harmful algal blooms and eutrophication. While the global magnitude of gauged riverine water discharge is well known, the magnitude of submarine groundwater discharge (SGD) is poorly constrained. Using an inverse model combined with a global compilation of 228Ra observations, we show that the SGD integrated over the Atlantic and Indo-Pacific Oceans between 60°S and 70°N is (12 ± 3) × 1013 m3 yr−1, which is 3 to 4 times greater than the freshwater fluxes into the oceans by rivers. Unlike the rivers, where more than half of the total flux is discharged into the Atlantic, about 70% of SGD flows into the Indo-Pacific Oceans. We suggest that SGD is the dominant pathway for dissolved terrestrial materials to the global ocean, and this necessitates revisions for the budgets of chemical elements including carbon.
    Description: This work was supported by the Ministry of Oceans and Fisheries, Korea, through the Korea Institute of Marine Science and Technology (KIMST) (20120176) and National Research Foundation (NRF) of Korea (2013R1A2A1A05004343 and 2013R1A1A1058203). Charette and Moore's contributions were supported by the US National Science Foundation through the GEOTRACES project.
    Keywords: Submarine groundwater discharge ; Radium ; Inverse modeling ; Land-ocean interaction ; Brackish groundwater ; Coastal flux
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  • 2
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    Molecular characterization of dissolved organic matter associated with the Greenland ice sheet (2010)
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    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
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    Assessment of groundwater discharges into West Neck Bay, New York, via natural tracers (2006)
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    Publication Date: 2022-05-25
    Description: Author Posting. © Elsevier B.V., 2006. 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 Continental Shelf Research 29 (2006): 1971-1983, doi:10.1016/j.csr.2006.07.011.
    Description: A field experiment to compare methods of assessing submarine groundwater discharge (SGD) was held on Shelter Island, NY, in May 2002. We evaluated the use of radon, radium isotopes, and methane to assess SGD rates and dynamics from a glacial aquifer in the coastal zone. Fluxes of radon across the sediment-water interface were calculated from changes in measured surface water inventories following evaluation and correction for tidal effects, atmospheric evasion, and mixing with offshore waters. These fluxes were then converted to SGD rates using the measured radon concentration in the groundwater. We used the short-lived radium isotopes to calculate a horizontal mixing coefficient to assess radon loss by mixing between nearshore and offshore waters. We also made an independent calculation of SGD using the Ra-derived mixing coefficient and the long-lived 226Ra concentration gradient in the bay. Seepage rates were calculated to range between 0 and 34 cm.day-1 using the radon measurements and 15 cm.day-1 as indicated by the radium isotopes. The radiotracer results were consistent and comparable to SGD rates measured directly with vented benthic chambers (seepage meters) deployed during this experiment. These meters indicated rates between 2 and 200 cm.day-1 depending on their location. Both the calculated radon fluxes and rates measured directly by the automated seepage meters revealed a clear reproducible pattern of higher fluxes during low tides. Considering that the two techniques are completely independent, the agreement in the SGD dynamics is significant. Methane concentration in groundwater was very low (~30 nM) and not suitable as SGD tracer at this study site.
    Description: The SGD intercomparison experiment was partially funded by SCOR, LOICZ, and UNESCO (IOC and IHP). W. C. Burnett acknowledges support from CICEET (Grant# 1368-810-41) and ONR (Grant# 1368-769-27). J. P. Chanton acknowledges support from Seagrant (R\C-E-44). The WHOI researchers acknowledge funding from CICEET (#NA07OR0351, NA17OZ2507).
    Keywords: Submarine groundwater discharge ; Radiotracers ; Radon ; Radium ; Methane ; Shelter Island, NY
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  • 4
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    Geochemical and physical sources of radon variation in a subterranean estuary — implications for groundwater radon activities in submarine groundwater discharge studies (2008)
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    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
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    Utility of Rn-222 as a passive tracer of subglacial distributed system drainage (2017)
    Elsevier
    Details
    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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  • 6
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    A new perspective for assessing water transport and associated retention effects in a large reservoir (2018)
    John Wiley & Sons
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    Publication Date: 2022-05-25
    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 Geophysical Research Letters 45 (2018): 9642-9650, doi:10.1029/2018GL079687.
    Description: Radioactive tracer techniques may be useful for assessing water transport and the overall effects of concurrent biogeochemical processes in river‐reservoir systems. In this study, we show that radium isotopes can assess the hydrodynamics and sediment/nutrient retention in the Xiaolangdi Reservoir, the largest impoundment along the Yellow River, China. Activity ratios of 224Ra/226Ra and 223Ra/226Ra were used for water mass age calculations in the riverine, transition, and lentic reaches of the reservoir. Water ages were combined with the length scale of three river‐reservoir zones to determine water transport rates of 3.6 ± 1.2, 1.3 ± 0.3, and 0.16 ± 0.14 km/day, respectively. Radium ages were also used to quantify the net retention of sediment and nutrients in different parts of the river‐reservoir system. Suspended sediment was removed at a rate of 1.4 ± 0.6 g/m3/day, mainly in the riverine zone. Nutrient dynamics were more complicated, with addition or removal at different rates within the three zones.
    Description: Ministry of Education of the People's Republic of China Grant Number: MS2014ZGHY028; Qingdao National Laboratory for Marine Science and Technology Grant Number: 2016ASKJ02; National Science Foundation of China Grant Numbers: 41521064, 41876075, 41576075; Ministry of Science and Technology of the People's Republic of China Grant Number: 2016YFA0600902
    Description: 2019-03-23
    Keywords: Radium ; Reservoir ; Water age ; Retention effects ; Nutrients
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  • 7
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    Shelf-basin interactions and water mass residence times in the western Arctic Ocean: Insights provided by radium isotopes (2019)
    American Geophysical Union
    Details
    Publication Date: 2022-10-26
    Description: Author Posting. © American Geophysical Union, 2019. 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-Oceans 124(5), (2019): 3279-3297, doi: 10.1029/2019JC014988.
    Description: Radium isotopes are produced through the decay of thorium in sediments and are soluble in seawater; thus, they are useful for tracing ocean boundary‐derived inputs to the ocean. Here we apply radium isotopes to study continental inputs and water residence times in the Arctic Ocean, where land‐ocean interactions are currently changing in response to rising air and sea temperatures. We present the distributions of radium isotopes measured on the 2015 U.S. GEOTRACES transect in the Western Arctic Ocean and combine this data set with historical radium observations in the Chukchi Sea and Canada Basin. The highest activities of radium‐228 were observed in the Transpolar Drift and the Chukchi shelfbreak jet, signaling that these currents are heavily influenced by interactions with shelf sediments. The ventilation of the halocline with respect to inputs from the Chukchi shelf occurs on time scales of ≤19–23 years. Intermediate water ventilation time scales for the Makarov and Canada Basins were determined to be ~20 and 〉30 years, respectively, while deep water residence times in these basins were on the order of centuries. The radium distributions and residence times described in this study serve as a baseline for future studies investigating the impacts of climate change on the Arctic Ocean.
    Description: We thank the captain and crew of the USCGC Healy (HLY1502) and the chief scientists D. Kadko and W. Landing for coordinating a safe and successful expedition. We thank the members of the pump team, P. Lam, E. Black, S. Pike, X. Yang, and M. Heller for their assistance with sample collection and for their unfailingly positive attitudes during this 65‐day expedition. We also appreciate sampling assistance from P. Aguilar and M. Stephens, and MATLAB assistance from B. Corlett, A. Pacini, P. Lin, and M. Li. The radium data from the HLY1502 expedition are available through the Biological & Chemical Oceanography Data Management Office (https://www.bco‐dmo.org/dataset/718440) and the radium measurements from the SHEBA, AWS‐2000, and SBI expeditions can be found in the supporting information. This work was funded by NSF awards OCE‐1458305 to M.A.C., OCE‐1458424 to W.S.M., and PLR‐1504333 to R.S.P. This research was conducted with Government support under and awarded by a DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship awarded to L.E.K., 32 CFR 168a.
    Description: 2019-10-26
    Keywords: Radium ; Arctic Ocean ; GEOTRACES ; Chukchi shelf
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  • 8
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    Lingering radioactivity at the Bikini and Enewetak Atolls (2018)
    Elsevier
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    Publication Date: 2022-05-26
    Description: © The Author(s), 2017. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Science of The Total Environment 621 (2018): 1185-1198, doi:10.1016/j.scitotenv.2017.10.109.
    Description: We made an assessment of the levels of radionuclides in the ocean waters, seafloor and groundwater at Bikini and Enewetak Atolls where the US conducted nuclear weapons tests in the 1940's and 50's. This included the first estimates of submarine groundwater discharge (SGD) derived from radium isotopes that can be used here to calculate radionuclide fluxes in to the lagoon waters. While there is significant variability between sites and sample types, levels of plutonium (239,240Pu) remain several orders of magnitude higher in lagoon seawater and sediments than what is found in rest of the world's oceans. In contrast, levels of cesium-137 (137Cs) while relatively elevated in brackish groundwater are only slightly higher in the lagoon water relative to North Pacific surface waters. Of special interest was the Runit dome, a nuclear waste repository created in the 1970's within the Enewetak Atoll. Low seawater ratios of 240Pu/239Pu suggest that this area is the source of about half of the Pu in the Enewetak lagoon water column, yet radium isotopes suggest that SGD from below the dome is not a significant Pu source. SGD fluxes of Pu and Cs at Bikini were also relatively low. Thus radioactivity associated with seafloor sediments remains the largest source and long term repository for radioactive contamination. Overall, Bikini and Enewetak Atolls are an ongoing source of Pu and Cs to the North Pacific, but at annual rates that are orders of magnitude smaller than delivered via close-in fallout to the same area.
    Description: Finally, none of this would have been possible without the generous financial support from the Dalio Explore Fund (WHOI #25531513) for the vessel and our post cruise analyses that together resulted in this unique and successful research program.
    Keywords: Marshall Islands ; Runit dome ; Plutonium ; Cesium ; Radium ; Nuclear weapons tests
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  • 9
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    New perspectives on radium behavior within a subterranean estuary (2008)
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    Publication Date: 2022-05-26
    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 109 (2008): 250-267, doi:10.1016/j.marchem.2007.12.002.
    Description: Over the past decade, radium isotopes have been frequently applied as tracers of submarine groundwater discharge (SGD). The unique radium signature of SGD is acquired within the subterranean estuary, a mixing zone between fresh groundwater and seawater in coastal aquifers, yet little is known about what controls Ra cycling in this system. The focus of this study was to examine controls on sediment and groundwater radium activities within permeable aquifer sands (Waquoit Bay, MA, USA) through a combination of field and laboratory studies. In the field, a series of sediment cores and corresponding groundwater profiles were collected for analysis of the four radium isotopes, as well as dissolved and sediment associated manganese, iron, and barium. We found that in addition to greater desorption at increasing salinity, radium was also closely tied to manganese and iron redox cycling within these sediments. A series of laboratory adsorption/desorption experiments helped elucidate the importance of 1) contact time between sediment and water, 2) salinity of water in contact with sediment, 3) redox conditions of water in contact with sediment, and 4) the chemical characteristics of sediment on radium adsorption/desorption. We found that these reactions are rapid (on the order of hours), desorption increases with increasing salinity and decreasing pH, and the presence of Fe and Mn (hydr)oxides on the sediment inhibit the release of radium. These sediments have a large capacity to sorb radium from fresh water. Combined with these experimental results, we present evidence from time series groundwater sampling that within this subterranean estuary there are cyclic periods of Ra accumulation and release controlled by changing salinity and redox conditions.
    Description: This work is a result of research sponsored by NSF (OCE- 0425061 to M.A.C.), the WHOI-NOC Student Exchange program (to P.J.M), and the WHOI Postdoctoral Scholar program (to H.D.).
    Keywords: Radium ; Sediments ; Desorption ; Adsorption ; Barium ; Submarine groundwater ; Subterranean estuary ; Redox reactions ; Ion exchange ; Distribution coefficient
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  • 10
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    The release of dissolved actinium to the ocean : A global comparison of different end-members (2008)
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    Publication Date: 2022-05-26
    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 109 (2008): 409-420, doi:10.1016/j.marchem.2007.07.005.
    Description: The measurement of short-lived 223Ra often involves a second measurement for supported activities, which represents 227Ac in the sample. Here we exploit this fact, presenting a set of 284 values on the oceanic distribution of 227Ac, which was collected when analyzing water samples for short-lived radium isotopes by the radium delayed coincidence counting system. The present work compiles 227Ac data from coastal regions all over the northern hemisphere, including values from ground water, from estuaries and lagoons, and from marine endmembers. Deep-sea samples from a continental slope off Puerto Rico and from an active vent site near Hawaii complete the overview of 227Ac near its potential sources. The average 227Ac activities of nearshore marine end-members range from 0.4 dpm * m-3 at the Gulf of Mexico to 3.0 dpm *m-3 in the coastal waters of the Korean Strait. In analogy to 228Ra, we find the extension of adjacent shelf regions to play a substantial role for 227Ac activities, although less pronounced than for radium, due to its weaker shelf source. Based on previously published values, we calculate an open ocean 227Ac inventory of 1.35 * 1018 dpm 227Acex in the ocean, which corresponds to 37 moles, or 8.4 kg. This implies a flux of 127 dpm*m-2*y-1 from the deep-sea floor. For the shelf regions, we obtain a global inventory of 227Ac of 4.5 * 1015 dpm, which cannot be converted directly into a flux value, as the regional loss term of 227Ac to the open ocean would have to be included. Ac has so far been considered to behave similarly to Ra in the marine environment, with the exception of a strong Ac source in the deep-sea due to 231Paex. Here, we present evidence of geochemical differences between Ac, which is retained in a warm vent system, and Ra, which is readily released (Moore et al., submitted). Another potential mechanism of producing deviations in 227Ac/228Ra and daughter isotope ratios from the expected production value of lithogenic material is observed at reducing environments, where enrichment in uranium may occur. The presented data here may serve as a reference for including 227Ac in circulation models, and the overview provides values for some end-members that contribute to the global Ac distribution.
    Keywords: Actinium ; Radium ; Submarine groundwater discharge ; Ocean mixing ; Continental shelf ; Global circulation models
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