Record of 3H and 36Cl from the Fukushima nuclear accident recovered from soil water in the unsaturated zone at Koriyama.

The opportunity to measure the concentrations of 3H and 36Cl released by the Fukushima nuclear accident in 2011 directly in rain was lost in the early stage of the accident. We have, however, been able to reconstruct the deposition record of atmospheric 3H and 36Cl following the accident using a bore hole that was drilled in 2014 at Koriyama at a distance of 60 km from the accident. The contributions of 3H and 36Cl from the accident are 1.4 × 1013 and 2.0 × 1012 atoms m-2 respectively at this site. Very high concentrations of both 3H (46 Bq L-1) and 36Cl (3.36 × 1011 atoms L-1) were found in the unsaturated soil at depths between 300 and 350 cm. From these, conservative estimates for the 3H and 36Cl concentrations in the precipitation in the ~ 6 weeks following the accident were 607 Bq L-1 and 4.74 × 1010 atoms L-1, respectively. A second hole drilled in 2016 showed that 3H concentrations in the unsaturated soil and shallow groundwater had returned to close to natural levels, although the 36Cl concentrations were still significantly elevated above natural levels.

Timing and dynamics of Late Wolstonian Substage 'Moreton Stadial' (MIS 6) glaciation in the English West Midlands, UK.

Glaciation during the late Middle Pleistocene is widely recognized across continental northwest Europe, but its extent and palaeoenvironmental significance in the British Isles are disputed. Although glaciogenic sediments at Wolston, Warwickshire, in the English West Midlands, have been used to define the stratotype of the Wolstonian Stage, their age has been variably assigned between marine isotope stages (MIS) 12 and 6. Here we present sedimentological and stratigraphical observations from five sites across the English West Midlands whose chronology is constrained by new luminescence ages from glaciofluvial sediments, supplemented by cosmogenic 36Cl exposure dating of erratic boulders. The ages suggest that between 199 ± 5 and 147 ± 2.5 ka the British Ice Sheet advanced into the English West Midlands as far south as Moreton-in-Marsh, Gloucestershire. This advance is assigned to the Moreton Stadial of the Late Wolstonian Substage. Dating of the glaciation to this substage allows correlation of the Moreton Stadial glacial deposits in the English West Midlands with those of the Drenthe Stadial during the Late Saalian Substage across continental northwest Europe.

Plutonium isotopes in the North Western Pacific sediments coupled with radiocarbon in corals recording precise timing of the Anthropocene.

Plutonium (Pu) has been used as a mid-twentieth century time-marker in various geological archives as a result of atmospheric nuclear tests mainly conducted in 1950s. Advancement of analytical techniques allows us to measure 239Pu and 240Pu more accurately and can thereby reconstruct the Pacific Pu signal that originated from the former Pacific Proving Grounds (PPG) in the Marshall Islands. Here, we propose a novel method that couples annual banded reef building corals and nearshore anoxic marine sediments to provide a marker to precisely determine the start of the nuclear era which is known as a part of the Anthropocene. We demonstrate the efficacy of the methods using sediment obtained from Beppu Bay, Japan, and a coral from Ishigaki Island, Japan. The sedimentary records show a clear Pu increase from 1950, peaking during the 1960s, and then showing a sharp decline during the 1970s. However, a constantly higher isotope ratio between 239Pu and 240Pu suggest an additional contribution other than global fallout via ocean currents. Furthermore, single elevations in 240Pu/239Pu provide supportive evidence of close-in-fallout similar to previous studies. Coral skeletal radiocarbon displays a clear timing with the signatures supporting the reliability of the Beppu Bay sediments as archives and demonstrates the strength of this method to capture potential Anthropocene signatures.

Phasing of millennial-scale climate variability in the Pacific and Atlantic Oceans.

New radiocarbon and sedimentological results from the Gulf of Alaska document recurrent millennial-scale episodes of reorganized Pacific Ocean ventilation synchronous with rapid Cordilleran Ice Sheet discharge, indicating close coupling of ice-ocean dynamics spanning the past 42,000 years. Ventilation of the intermediate-depth North Pacific tracks strength of the Asian monsoon, supporting a role for moisture and heat transport from low latitudes in North Pacific paleoclimate. Changes in carbon-14 age of intermediate waters are in phase with peaks in Cordilleran ice-rafted debris delivery, and both consistently precede ice discharge events from the Laurentide Ice Sheet, known as Heinrich events. This timing precludes an Atlantic trigger for Cordilleran Ice Sheet retreat and instead implicates the Pacific as an early part of a cascade of dynamic climate events with global impact.

The 240Pu/239Pu atom ratio in Chinese soils.

The 240Pu/239Pu atom ratio is a very effective tool for the identification of the origin of plutonium (Pu) in the soil environment. We examine a dataset of 240Pu/239Pu atom ratios determined from surface and core soils at 240 sites across China. The data were compiled from 18 separate literature sources from the last 20 years. For the first time the spatial distribution (3 latitude bands and 7 natural regions) of the weighted average 240Pu/239Pu atom ratios in Chinese soils is investigated. An area to the West of Xining City, shows a weighted average 240Pu/239Pu atom ratio of 0.167 ±â€¯0.002, lower than that of average global fallout, which likely arises from the addition of local fallout radionuclides from the Chinese nuclear weapon tests at Lop Nor between 1964 and 1980. The Yumen and Jiuquan areas of Northwest China in particular show evidence of very low ratio material from the Chinese nuclear weapon tests. Excluding the impacted area around the test site the weighted average 240Pu/239Pu ratio of 0.182 ±â€¯0.002 suggests that global fallout is the main source of Pu in most Chinese soils.

Limits on Supernova-Associated

We searched for the presence of ^{26}Al in deep-sea sediments as a signature of supernova influx. Our data show an exponential dependence of ^{26}Al with the sample age that is fully compatible with radioactive decay of terrigenic ^{26}Al. The same set of samples demonstrated a clear supernova ^{60}Fe signal between 1.7 and 3.2 Myr ago. Combining our ^{26}Al data with the recently reported ^{60}Fe data results in a lower limit of 0.18_{-0.08}^{+0.15} for the local interstellar ^{60}Fe/^{26}Al isotope ratio. It compares to most of the ratios deduced from nucleosynthesis models and is within the range of the observed average galactic ^{60}Fe/^{26}Al flux ratio of (0.15±0.05).

Deposition of artificial radionuclides in sediments of Loch Etive, Scotland.

The nuclear fuel reprocessing plants on the Sellafield site (UK) have released low-level effluents into the Irish Sea under authorisation since 1952. This has led to the labelling of nearby offshore sediments with a range of artificial radionuclides. In turn, these sediments act as a long-term secondary source of both soluble and particle-associated radionuclides to coastal areas. These radionuclides are of interest both in assessing possible environmental impacts and as tracers for marine processes. Here we present results from a study of the geochemistry of natural (234, 238U) and artificial (137Cs, 241Am, 238Pu, 239+240Pu, and 236U) radionuclides and their accumulation in sediments from Loch Etive, Scotland. The data are interpreted in the context of the historical radioactive discharges to the Irish Sea and biogeochemical processes in marine sediments. Loch Etive is divided into two basins; a lower, seaward basin where the sedimentation rate (∼0.6 cm/yr) is about twice that of the more isolated upper basin (∼0.3 cm/yr). These accumulation rates are consistent with the broad distribution of 137Cs in the sediment profiles which can be related to the maximum Sellafield discharges of 137Cs in the mid-1970s and suggest that 137Cs was mainly transported in solution to Loch Etive during that period. Enrichments of Mn, Fe, and Mo in sediment and porewater from both Loch Etive basins result from contemporary biogeochemical redox processes. Enrichments of 238U and 234U in the lower basin may be a result of the cycling of natural U. By contrast, the Sellafield-derived artificial isotope 236U does not seem to be affected by the redox-driven reactions in the lower basin. The 238Pu/239,240Pu ratios suggest contributions from both historical Sellafield discharges and global fallout Pu. The uniform sediment distributions of Pu and Am, which do not reflect Sellafield historical discharges, suggest the existence of a homogenous secondary source. This could be the offshore 'mud patch' in the vicinity of Sellafield from which the supply of radionuclides reflects time-integrated Sellafield discharges. This source could also account for the continuing supply of Cs to Loch Etive, even after substantial reductions in discharge from the Sellafield site.

Continuous transport of Pacific-derived anthropogenic radionuclides towards the Indian Ocean.

Unusually high concentrations of americium and plutonium have been observed in a sediment core collected from the eastern Lombok Basin between Sumba and Sumbawa Islands in the Indonesian Archipelago. Gamma spectrometry and accelerator mass spectrometry data together with radiometric dating of the core provide a high-resolution record of ongoing deposition of anthropogenic radionuclides. A plutonium signature characteristic of the Pacific Proving Grounds (PPG) dominates in the first two decades after the start of the high yield atmospheric tests in 1950's. Approximately 40-70% of plutonium at this site in the post 1970 period originates from the PPG. This sediment record of transuranic isotopes deposition over the last 55 years provides evidence for the continuous long-distance transport of particle-reactive radionuclides from the Pacific Ocean towards the Indian Ocean.

Origin of artificial radionuclides in soil and sediment from North Wales.

During the operations at the Sellafield nuclear fuel reprocessing complex, artificial radionuclides are discharged to the Irish Sea under authorisation, where they are dispersed. In this study, the southern distribution and transport of Sellafield derived radionuclides have been investigated. Both natural and artificial radionuclides have been studied in a soil core from the riverbank of the Afon Goch in Anglesey, North Wales. Particulate input is dominant for all artificial radionuclides (including the more soluble (137)Cs and (236)U) with an estimated lag time of about a decade. The preferential northward seawater movement in the NE Irish Sea limits solution input of (137)Cs and (236)U to the areas south of Sellafield. The relatively long lag time reflects both the water circulation pattern and distance between the study site in north Wales and the source point in Cumbria. Two redox active zones are observed in the top and the bottom of this core, although there is no evidence for any redistribution of Pu and natural uranium by these redox processes. However, (236)U, derived from irradiated uranium, showed variable distribution in the core. This could be a potential response to the geochemical conditions, showing that (236)U may be a promising tracer for the environmental processes and a signature of the Sellafield historical discharges of irradiated uranium.

Uranium from German Nuclear Power Projects of the 1940s--A Nuclear Forensic Investigation.

Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence.

High (36)Cl/Cl ratios in Chernobyl groundwater.

After the explosion of the Chernobyl Nuclear Power Plant in April 1986, contaminated material was buried in shallow trenches within the exclusion zone. A (90)Sr plume was evidenced downgradient of one of these trenches, trench T22. Due to its conservative properties, (36)Cl is investigated here as a potential tracer to determine the maximal extent of the contamination plume from the trench in groundwater. (36)Cl/Cl ratios measured in groundwater, trench soil water and leaf leachates are 1-5 orders of magnitude higher than the theoretical natural (36)Cl/Cl ratio. This contamination occurred after the Chernobyl explosion and currently persists. Trench T22 acts as an obvious modern point source of (36)Cl, however other sources have to be involved to explain such contamination. (36)Cl contamination of groundwater can be explained by dilution of trench soil water by uncontaminated water (rainwater or deep groundwater). With a plume extending further than that of (90)Sr, radionuclide which is impacted by retention and decay processes, (36)Cl can be considered as a suitable tracer of contamination from the trench in groundwater provided that modern release processes of (36)Cl from trench soil are better characterized.

Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway.

A combination of state-of-the-art isotopic fingerprinting techniques and atmospheric transport modelling using real-time historical meteorological data has been used to demonstrate direct tropospheric transport of radioactive debris from specific nuclear detonations at the Semipalatinsk test site in Kazakhstan to Norway via large areas of Europe. A selection of archived air filters collected at ground level at 9 stations in Norway during the most intensive atmospheric nuclear weapon testing periods (1957-1958 and 1961-1962) has been screened for radioactive particles and analysed with respect to the concentrations and atom ratios of plutonium (Pu) and uranium (U) using accelerator mass spectrometry (AMS). Digital autoradiography screening demonstrated the presence of radioactive particles in the filters. Concentrations of (236)U (0.17-23nBqm(-3)) and (239+240)Pu (1.3-782µBqm(-3)) as well as the atom ratios (240)Pu/(239)Pu (0.0517-0.237) and (236)U/(239)Pu (0.0188-0.7) varied widely indicating several different sources. Filter samples from autumn and winter tended to have lower atom ratios than those sampled in spring and summer, and this likely reflects a tropospheric influence in months with little stratospheric fallout. Very high (236)U, (239+240)Pu and gross beta activity concentrations as well as low (240)Pu/(239)Pu (0.0517-0.077), (241)Pu/(239)Pu (0.00025-0.00062) and (236)U/(239)Pu (0.0188-0.046) atom ratios, characteristic of close-in and tropospheric fallout, were observed in filters collected at all stations in Nov 1962, 7-12days after three low-yield detonations at Semipalatinsk (Kazakhstan). Atmospheric transport modelling (NOAA HYSPLIT_4) using real-time meteorological data confirmed that long range transport of radionuclides, and possibly radioactive particles, from Semipalatinsk to Norway during this period was plausible. The present work shows that direct tropospheric transport of fallout from atmospheric nuclear detonations periodically may have had much larger influence on radionuclide air concentrations and deposition than previously anticipated.

Concentration and characterization of plutonium in soils of Hubei in central China.

To study the Pu concentration and isotope ratio distributions present in China, the (239+240)Pu total activities and (240)Pu/(239)Pu atom ratios in core soil samples from Hubei Province in central China were investigated using Accelerator Mass Spectrometry (AMS). The activities ranged from 0.019 to 0.502 mBqg(-1) and the (239+240)Pu inventories of 45 and approximately 55 Bqm(-2) agree well with that expected from global fallout. The (240)Pu/(239)Pu atom ratios in the soil ranged from 0.172 to 0.220. The ratios are similar to typical global fallout values. Hence, any close-in fallout contribution from the Chinese nuclear weapons tests, mainly conducted in the 1970s, must have either been negligible or had a similar (240)Pu/(239)Pu ratio to that of global fallout. The top 10 cm layer of the soil contributes approximately 90% of the total inventory and the maximum concentrations appeared in the 2-4 cm or 4-6 cm layers. It is suggested that climatic conditions and organic content are the two main factors that affect the vertical migration of plutonium in soil.

Association of plutonium with sediments from the Ob and Yenisey Rivers and Estuaries.

The present study applied sequential extraction techniques to investigate the binding and mobility of plutonium (Pu) in sediments from the rivers and estuaries of the Ob and Yenisey. As a study site, the Ob and Yenisey are particularly interesting as both rivers have weapons-grade Pu sources in their catchment areas, including the Russian Pu production and reprocessing plants at Mayak, Tomsk-7 and Krashnoyarsk, and the Semipalantinsk nuclear weapons testing site in Kazakhstan. Plutonium activity and (240)Pu/(239)Pu ratios were determined using accelerator mass spectrometry (AMS). Sequential extractions showed that between 47 and 80% of the Pu in Yenisey River sediments and 35-53% of the Pu in soils around the Techa River are mobilized with weak oxidising agents, which can indicate that Pu is bound to organic material. In contrast, Pu in Ob and Yenisey Estuarine sediments was more strongly bound, with 60-100% being found in the HNO(3)-extractable fraction. This change in speciation could reflect either that Pu bound to organic material in the Techa and Yenisey River sediments becomes more fixed to the sediments with time, or that organic-bound Pu is mobilized and released to the water when the sediments encounter the more saline water of the Ob and Yenisey estuaries. In general, (240)Pu/(239)Pu ratios were relatively consistent between different extraction fractions, although, in whole sediments, an increase in ratio was observed with distance from the source. This reflects the increased influence of weapon fallout from catchment runoff within the river systems, as compared to the weapons-grade sources close to the production and reprocessing plants. Knowledge of Pu speciation in the Ob and Yenisey Rivers, and the processes controlling its behaviour in estuarine systems, can improve predictions of its transfer and subsequent environmental impact to Arctic Seas.

Late-surviving megafauna in Tasmania, Australia, implicate human involvement in their extinction.

Establishing the cause of past extinctions is critical if we are to understand better what might trigger future occurrences and how to prevent them. The mechanisms of continental late Pleistocene megafaunal extinction, however, are still fiercely contested. Potential factors contributing to their demise include climatic change, human impact, or some combination. On the Australian mainland, 90% of the megafauna became extinct by approximately 46 thousand years (ka) ago, soon after the first archaeological evidence for human colonization of the continent. Yet, on the neighboring island of Tasmania (which was connected to the mainland when sea levels were lower), megafaunal extinction appears to have taken place before the initial human arrival between 43 and 40 ka, which would seem to exonerate people as a contributing factor in the extirpation of the island megafauna. Age estimates for the last megafauna, however, are poorly constrained. Here, we show, by direct dating of fossil remains and their associated sediments, that some Tasmanian megafauna survived until at least 41 ka (i.e., after their extinction on the Australian mainland) and thus overlapped with humans. Furthermore, a vegetation record for Tasmania spanning the last 130 ka shows that no significant regional climatic or environmental change occurred between 43 and 37 ka, when a land bridge existed between Tasmania and the mainland. Our results are consistent with a model of human-induced extinction for the Tasmanian megafauna, most probably driven by hunting, and they reaffirm the value of islands adjacent to continental landmasses as tests of competing hypotheses for late Quaternary megafaunal extinctions.

Absence of cooling in New Zealand and the adjacent ocean during the Younger Dryas chronozone.

As the climate warmed at the end of the last glacial period, a rapid reversal in temperature, the Younger Dryas (YD) event, briefly returned much of the North Atlantic region to near full-glacial conditions. The event was associated with climate reversals in many other areas of the Northern Hemisphere and also with warming over and near Antarctica. However, the expression of the YD in the mid- to low latitudes of the Southern Hemisphere (and the southwest Pacific region in particular) is much more controversial. Here we show that the Waiho Loop advance of the Franz Josef Glacier in New Zealand was not a YD event, as previously thought, and that the adjacent ocean warmed throughout the YD.

Coral reef sedimentation on Rodrigues and the Western Indian Ocean and its impact on the carbon cycle.

Coral reefs in the southwest Indian Ocean cover an area of ca. 18,530 km2 compared with a global reef area of nearly 300,000 km2. These regions are important as fishing grounds, tourist attractions and as a significant component of the global carbon cycle. The mass of calcium carbonate stored within Holocene neritic sediments is a number that we are only now beginning to quantify with any confidence, in stark contrast to the mass and sedimentation rates associated with pelagic calcium carbonate, which have been relatively well defined for decades. We report new data that demonstrate that the reefs at Rodrigues, like those at Reunion and Mauritius, only reached a mature state (reached sea level) by 2-3 ka: thousands of years later than most of the reefs in the Australasian region. Yet field observations show that the large lagoon at Rodrigues is already completely full of carbonate detritus (typical lagoon depth less than 1 m at low spring tide). The presence of aeolian dunes at Rodrigues indicates periodic exposure of past lagoons throughout the Pleistocene. The absence of elevated Pleistocene reef deposits on the island indicates that the island has not been uplifted. Most Holocene reefs are between 15 and 20 m in thickness and those in the southwest Indian Ocean appear to be consistent with this observation. We support the view that the CO2 flux associated with coral-reef growth acts as a climate change amplifier during deglaciation, adding CO2 to a warming world. southwest Indian Ocean reefs could have added 7-10% to this global flux during the Holocene.

Accelerator mass spectrometry measurement of 240Pu/239Pu isotope ratios in Novaya Zemlya and Kara Sea sediments.

Generally low levels of plutonium in environmental samples, often combined with limited sample sizes, necessitate reliable low-level techniques for determination of Pu isotopes. Accelerator mass spectrometry (AMS) has proved to be a powerful method for measuring low-level Pu activity concentrations and Pu isotope ratios. Based on procedural blanks, detection limits for AMS were below 1 fg Pu (equivalent to ca. 2 microBq 139Pu), which can compete with both TIMS, high sensitivity ICP-MS, and certainly alpha-spectrometry, while showing less interference, memory and matrix effects as compared to routine ICP-MS techniques. In addition to low detection limits, the technique offers the advantage of giving information on Pu isotope ratios. Measurements of sediments collected from dumping sites at Novaya Zemlya showed deviation from global fallout 240Pu/239Pu ratios.

Millennial and orbital variations of El Niño/Southern Oscillation and high-latitude climate in the last glacial period.

The El Niño/Southern Oscillation (ENSO) phenomenon is believed to have operated continuously over the last glacial-interglacial cycle. ENSO variability has been suggested to be linked to millennial-scale oscillations in North Atlantic climate during that time, but the proposals disagree on whether increased frequency of El Niño events, the warm phase of ENSO, was linked to North Atlantic warm or cold periods. Here we present a high-resolution record of surface moisture, based on the degree of peat humification and the ratio of sedges to grass, from northern Queensland, Australia, covering the past 45,000 yr. We observe millennial-scale dry periods, indicating periods of frequent El Niño events (summer precipitation declines in El Niño years in northeastern Australia). We find that these dry periods are correlated to the Dansgaard-Oeschger events--millennial-scale warm events in the North Atlantic climate record--although no direct atmospheric connection from the North Atlantic to our site can be invoked. Additionally, we find climatic cycles at a semiprecessional timescale (approximately 11,900 yr). We suggest that climate variations in the tropical Pacific Ocean on millennial as well as orbital timescales, which determined precipitation in northeastern Australia, also exerted an influence on North Atlantic climate through atmospheric and oceanic teleconnections.

Plutonium from global fallout recorded in an ice core from the Belukha glacier, Siberian Altai.

Ice cores from glaciers situated near anthropogenic sources of air pollution provide important archives of the emissions of species with short atmospheric lifetimes. Here we present the history of atmospheric Pu fallout reconstructed from an ice core from the Belukha glacier in the Siberian Altai. Fourteen ice core samples covering the time period 1941-1986 were selected for Pu analysis, chemically processed, and measured using accelerator mass spectrometry. The Pu concentration peaks in 1963, coinciding with the maximum of the nuclear weapons tests and in concordance with the 3H activity concentration peak. The shapes of the 239Pu and 3H profiles reflect two main periods of atmospheric nuclear test activity: premoratorium testing before 1958 and postmoratorium testing in 1961 and 1962. Premoratorium tests contribute about 45% of the integrated Pu inventory. The average 240Pu/239Pu isotopic ratio is 0.18 +/- 0.05, indicating that a large majority of the Pu in the Belukha glacier originates from global stratospheric fallout rather than from direct tropospheric input.