Arrival of the Fukushima radioactivity plume in North American continental waters.

The large discharge of radioactivity into the northwest Pacific Ocean from the 2011 Fukushima Dai-ichi nuclear reactor accident has generated considerable concern about the spread of this material across the ocean to North America. We report here the first systematic study to our knowledge of the transport of the Fukushima marine radioactivity signal to the eastern North Pacific. Time series measurements of (134)Cs and (137)Cs in seawater revealed the initial arrival of the Fukushima signal by ocean current transport at a location 1,500 km west of British Columbia, Canada, in June 2012, about 1.3 y after the accident. By June 2013, the Fukushima signal had spread onto the Canadian continental shelf, and by February 2014, it had increased to a value of 2 Bq/m(3) throughout the upper 150 m of the water column, resulting in an overall doubling of the fallout background from atmospheric nuclear weapons tests. Ocean circulation model estimates that are in reasonable agreement with our measured values indicate that future total levels of (137)Cs (Fukushima-derived plus fallout (137)Cs) off the North American coast will likely attain maximum values in the 3-5 Bq/m(3) range by 2015-2016 before declining to levels closer to the fallout background of about 1 Bq/m(3) by 2021. The increase in (137)Cs levels in the eastern North Pacific from Fukushima inputs will probably return eastern North Pacific concentrations to the fallout levels that prevailed during the 1980s but does not represent a threat to human health or the environment.

Below the disappearing marshes of an urban estuary: historic nitrogen trends and soil structure.

Marshes in the urban Jamaica Bay Estuary, New York, USA are disappearing at an average rate of 13 ha/yr, and multiple stressors (e.g., wastewater inputs, dredging activities, groundwater removal, and global warming) may be contributing to marsh losses. Among these stressors, wastewater nutrients are suspected to be an important contributing cause of marsh deterioration. We used census data, radiometric dating, stable nitrogen isotopes, and soil surveys to examine the temporal relationships between human population growth and soil nitrogen; and we evaluated soil structure with computer-aided tomography, surface elevation and sediment accretion trends, carbon dioxide emissions, and soil shear strength to examine differences among disappearing (Black Bank and Big Egg) and stable marshes (JoCo). Radiometric dating and nitrogen isotope analyses suggested a rapid increase in human wastewater nutrients beginning in the late 1840s, and a tapering off beginning in the 1930s when wastewater treatment plants (WWTPs) were first installed. Current WWTPs nutrient loads to Jamaica Bay are approximately 13 995 kg N/d and 2767 kg P/d. At Black Bank, the biomass and abundance of roots and rhizomes and percentage of organic matter on soil were significantly lower, rhizomes larger in diameter, carbon dioxide emission rates and peat particle density significantly greater, and soil strength significantly lower compared to the stable JoCo Marsh, suggesting Black Bank has elevated decomposition rates, more decomposed peat, and highly waterlogged peat. Despite these differences, the rates of accretion and surface elevation change were similar for both marshes, and the rates of elevation change approximated the long-term relative rate of sea level rise estimated from tide gauge data at nearby Sandy Hook, New Jersey. We hypothesize that Black Bank marsh kept pace with sea level rise by the accretion of material on the marsh surface, and the maintenance of soil volume through production of larger diameter rhizomes and swelling (dilation) of waterlogged peat. JoCo Marsh kept pace with sea-level rise through surface accretion and soil organic matter accumulation. Understanding the effects of multiple stressors, including nutrient enrichment, on soil structure, organic matter accumulation, and elevation change will better inform management decisions aimed at maintaining and restoring coastal marshes.

Molybdenum accumulation in sediments: a quantitative indicator of hypoxic water conditions in Narragansett Bay, RI.

Authigenic molybdenum (Mo) accumulation in marine sediments has often been used as a qualitative indicator of hypoxic bottom water. To investigate its use as a quantitative indicator of hypoxic exposure, sediment cores were collected from water quality monitoring sites in Narragansett Bay (RI, USA) that experience varying periods of hypoxia. Total Mo concentrations in surficial (0-1 cm) sediments were determined by total digestion and ICP-MS analysis. Lithogenic contributions to total Mo concentrations were estimated by multiplying measured concentrations of aluminum (Al) by the mean crustal Mo:Al ratio and subtracting them from the total concentrations to yield the authigenic fraction. 210Pb dating was used to determine sediment accumulation rates at each site. Mean annual periods of hypoxia in bottom waters were determined from continuous monitoring data for the years coinciding with the top 1 cm of sediment. Results indicated a linear relationship between authigenic Mo concentrations and frequency of hypoxia, although the relationships differed between different sampling periods. These results demonstrate the potential of sedimentary Mo as a tool for assessing the spatial and temporal extent of hypoxia in coastal waters.

Changes in Circulation and Particle Scavenging in the Amerasian Basin of the Arctic Ocean over the Last Three Decades Inferred from the Water Column Distribution of Geochemical Tracers.

Since the 1980-1990s, international research efforts have augmented our knowledge of the physical and chemical properties of the Arctic Ocean water masses, and recent studies have documented changes. Understanding the processes responsible for these changes is necessary to be able to forecast the local and global consequences of these property evolutions on climate. The present work investigates the distributions of geochemical tracers of particle fluxes and circulation in the Amerasian Basin and their temporal evolution over the last three decades (from stations visited between 1983 and 2015). Profiles of 230-thorium (230Th) and 231-protactinium (231Pa) concentrations and neodymium isotopes (expressed as εNd) measured in the Amerasian Basin prior to 2000 are compared to a new, post-2000s data set. The comparison shows a large scale decrease in dissolved 230Th and 231Pa concentrations, suggesting intensification of scavenging by particle flux, especially in coastal areas. Higher productivity and sediment resuspension from the shelves appear responsible for the concentration decrease along the margins. In the basin interior, increased lateral exchanges with the boundary circulation also contribute to the decrease in concentration. This study illustrates how dissolved 230Th and 231Pa, with εNd support, can provide unique insights not only into changes in particle flux but also into the evolution of ocean circulation and mixing.

Linking the distribution of (210)Po and (210)Pb with plankton community along Line P, Northeast Subarctic Pacific.

Depth profiles of (210)Po and (210)Pb activity and phytoplankton and zooplankton abundance were collected during two cruises along the Canadian time-series Line P in the Northeast Subarctic Pacific (ranging from 48o39 N to 50o00 N and 126o40 W to 145o00 W) in August 2010 and February 2011 to evaluate connections between the planktonic community and distributions of these radionuclides in the upper 500 m of the water column. Statistical analysis indicates that (210)Po is more effectively removed from the surface ocean when large (>0.1 mg ind(-1) dry wt) zooplankton dominate, and is less effectively scavenged when the picoplankton Synechococcus is present at high concentrations (>1 × 10(5) cells ml(-1)). While the zooplankton field data are consistent with previous lab studies and field observations, the phytoplankton results seem to conflict with recent evidence that small cells may contribute significantly to export in other oligotrophic regions. Differences in ecosystem mechanisms between the Subarctic Pacific and other oligotrophic systems that limit the contribution of small cells to sinking flux remain to be identified.

Direct comparison of 210Po, 234Th and POC particle-size distributions and export fluxes at the Bermuda Atlantic Time-series Study (BATS) site.

Particle-reactive, naturally occurring radionuclides are useful tracers of the sinking flux of organic matter from the surface to the deep ocean. Since the Joint Global Ocean Flux Study (JGOFS) began in 1987, the disequilibrium between (234)Th and its parent (238)U has become widely used as a technique to measure particle export fluxes from surface ocean waters. Another radionuclide pair, (210)Po and (210)Pb, can be used for the same purpose but has not been as widely adopted due to difficulty with accurately constraining the (210)Po/(210)Pb radiochemical balance in the ocean and because of the more time-consuming radiochemical procedures. Direct comparison of particle flux estimated in different ocean regions using these short-lived radionuclides is important in evaluating their utility and accuracy as tracers of particle flux. In this paper, we present paired (234)Th/(238)U and (210)Po/(210)Pb data from oligotrophic surface waters of the subtropical Northwest Atlantic and discuss their advantages and limitations. Vertical profiles of total and particle size-fractionated (210)Po and (234)Th activities, together with particulate organic carbon (POC) concentrations, were measured during three seasons at the Bermuda Atlantic Time-series Study (BATS) site. Both (210)Po and (234)Th reasonably predict sinking POC flux caught in sediment traps, and each tracer provides unique information about the magnitude and efficiency of the ocean's biological pump.

Stable Pb isotope ratios in aerosols, precipitation, and size-fractionated particulate matter in the Gulf of Maine, Scotian Shelf, and Labrador Sea.

Measurements of Pb isotopes in aerosols, precipitation, and size-fractionated particulate matter from the Gulf of Maine, Scotian Shelf and Labrador Sea are used to investigate the source of Pb. The (206)Pb/(207)Pb ratio in aerosols and precipitation collected at New Castle, NH suggests that anthropogenic Pb is a mixture of US and Canadian sources. (206)Pb/(207)Pb ratios in >53 microm particulate matter from the Gulf of Maine and Scotian Shelf slope waters are consistent with contaminant Pb inputs predominantly from US and Canadian sources, while in shelf waters (206)Pb/(207)Pb ratios in >0.4 microm and >53 microm particles are consistent with a mixture of US and Canadian sources, as well as Pb associated with resuspended surface sediment. (206)Pb/(207)Pb ratios in particulate matter (>0.4 microm, 10-53 microm, and >53 microm) from Labrador Sea surface waters range from 1.165 to 1.211 and are a mixture of Pb derived from ore compositions consistent with Broken Hill, Australia and southeast Missouri, US sources.

Measurement of attogram quantities of 231Pa in dissolved and particulate fractions of seawater by isotope dilution thermal ionization mass spectroscopy.

A technique has been developed to quantify ultratrace 231Pa (50-2000 ag; 1 ag = 10(-18) g) concentrations in seawater using isotope-dilution thermal ionization mass spectrometry (TIMS). The method is a modification of a process developed by Pickett et al. (Pickett, D. A.; Murrell, M. T.; Williams, R. W. Anal. Chem. 1994, 66, 1044-1049) and extends the technique to very low levels of protactinium. The procedural blank is 16 +/- 15 ag (2sigma), and the ionization efficiency (ions generated/atom loaded) approaches 0.5%. Measurement time is <1 h. The amount of 231Pa needed to produce 231Pa data with an uncertainty of +/-4-12% is 100-1000 ag (approximately 3 x 10(5) to 3 x 10(6) atoms). Replicate measurements made on known standards and seawater samples demonstrate that the analytical precision approximates that expected from counting statistics and that, based on detection limits of 38 and 49 ag, protactinium can be detected in a minimum sample size of surface seawater of approximately 2 L for suspended particulate matter and <0.1 L for filtered (<0.4 microm) seawater, respectively. The concentration of 231Pa (tens of attograms per liter) can be determined with an uncertainty of +/-5-10% (2sigma) for suspended particulate matter filtered from 5 to 10 L of seawater. For the dissolved fraction, 0.5-1 L of seawater yields 231Pa measurements with a precision of 1-10%. Sample size requirements are orders of magnitude less than traditional decay-counting techniques and significantly less than previously reported ICP-MS techniques. Our technique can also be applied to other environmental samples, including cave waters, rivers, and igneous rocks.