No long-term variation of 240Pu/239Pu atom ratio in liver of Japanese common squid (Todarodes pacificus) collected from seven sea areas around Japan during 2003-2018.

The 239+240Pu concentrations and 240Pu/239Pu atom ratios were determined to trace the temporal variability in concentration and atom ratio in liver of the Japanese common squid during 2003-2018. The differences in their concentrations and atom ratios and the dependency on the collection areas and migratory history were compared. The organ affinity of Pu in mantle, limb, liver, and internal organs except liver was also investigated. The average 239+240Pu concentrations were the highest in liver followed in order by internal organs except liver, limb, and mantle. The Pu accumulation in liver could be explained by a mechanism for foreign substance processing. A significant difference in the average 239+240Pu concentrations in liver was found among the sea areas for specimen collection during 2003-2018. In spite of a noticeable difference in the average 239+240Pu concentrations, the 240Pu/239Pu atom ratios showed no significant temporal variability around Japan; thus, they were continuously uniform during 2003-2018.

129I in the SE-Dome ice core, Greenland: A new candidate golden spike for the Anthropocene.

The Anthropocene is a proposed geological epoch that will mark the time when humans have irreversibly affected the Earth. One of the primary requirements to formally establish this is a Global Boundary Stratotype Section and Point or "golden spike" - a record of a planetary signal marking the new epoch's beginning. The leading candidates for the Anthropocene's golden spike are the fallout peaks of 14C (T1/2 = 5730 y) and 239Pu (T1/2 = 24,110 y) from nuclear weapons testing in the 1960s. However, these radionuclides' half-lives may not be long enough for their signals to be observable in the far future and are, thus, not durable. In this regard, here we show the 129I time series record (1957-2007) of the SE-Dome ice core, Greenland. We find that 129I in SE-Dome records almost the entire history of the nuclear age in excellent detail at a time resolution of about four months. More specifically, 129I in SE-Dome reflects signals from nuclear weapons testing in 1958, 1961, and 1962, the Chernobyl Accident in 1986, and various signals from nuclear fuel reprocessing within the same year or a year after. The quantitative relationships between 129I in SE-Dome and these human nuclear activities were established using a numerical model. Similar signals are observed in other records from various environments worldwide, such as sediments, tree rings, and corals. This global ubiquity and synchronicity are comparable to those of the 14C and 239Pu bomb signals, but the much longer half-life of 129I (T1/2 = 15.7 My) makes it a more durable golden spike. For these reasons, the 129I record of the SE-Dome ice core can be considered an excellent candidate for the Anthropocene golden spike.

Mathematical simulation of the Pacific Proving Grounds 129I/127I nuclear bomb peaks in coral cores from the Philippines.

One recent way of reconstructing the historical impact of aboveground nuclear weapons testing (ANWT) in places lacking historical data is by measuring 129I in natural archives such as coral cores. However, discussions arising from 129I in corals remain qualitative or semi-quantitative, which do not maximize the potential information derivable from the data. In this study, we construct a mathematical model that simulates the 129I bomb peaks from the Pacific Proving Grounds (PPG) tests, as observed in available coral core data from the east (Baler) and west (Parola) sides of the Philippines. Results show that the model can determine the expected increase in 129I/127I ratio in the Philippines per megaton of ANWT detonated in the PPG; confirm time lags for each major transport pathway from the PPG to the Philippines, indicating when to expect the radioactivity spike after detonation; and determine the most significant transport pathway from the PPG to each coral location. This work increases the application and significance of 129I/127I coral core data by deriving quantitative information about the magnitude, timing, and transport pathways of radioactivity from the ANWT site to the coral location. In the future, the model can be expanded to simulate other 129I sources besides ANWT.

Transuranic nuclides Pu, Am and Cm isotopes, and 90Sr in seafloor sediments off the Fukushima Daiichi Nuclear Power Plant during the period from 2012 to 2019.

The 238Pu, 239+240Pu, 241Am, 242Cm, 243+244Cm and 90Sr concentrations in seafloor surface sediments collected at three sampling stations off the Fukushima Daiichi Nuclear Power Plant (FDNPP) site during the period from 2012 to 2019 were determined to elucidate the impacts of the FDNPP accident onto their concentrations in coastal sediments and to discuss the sources of the measured radionuclides. The 239+240Pu, 241Pu and 241Am concentrations and 240Pu/239Pu atom ratios in a sediment core were also determined to allow comparison of their inventories between this study and previously reported values and to identify the Pu sources. The 238Pu, 239+240Pu, 241Am and 90Sr concentrations showed no remarkable temporal variations; no significant increases in concentrations after the FDNPP accident were observed; these concentrations were comfortably within the previously reported concentration range; and no detectable 242Cm and 243+244Cm amounts were observed in surface sediments. The observed 238Pu/239+240Pu activity ratios were approximately two orders of magnitudes lower than those for the damaged FDNPP reactor core inventories and the observed values in terrestrial samples after the accident. The 239+240Pu, 241Pu and 241Am inventories in the sediment core were 389 ± 5, 503 ± 33 and 214 ± 3 Bq m-2, respectively. The 239+240Pu inventory was about an order of magnitude greater than the expected cumulative deposition density of global fallout from atmospheric nuclear weapons testing due to an enhanced scavenging effect. The 240Pu/239Pu atom ratios in the sediment core ranged from 0.239 to 0.246 with a mean value of 0.242 ± 0.002; these ratios were clearly greater than the mean global fallout ratio of 0.18. The results for 238Pu/239+240Pu activity ratios and 240Pu/239Pu atom ratios reflected a mixture of global fallout and Pacific Proving Grounds (PPG) close-in fallout Pu rather than Fukushima accident-derived Pu. The sediment column inventory for 239+240Pu originating from the PPG close-in fallout was calculated as 166 Bq m-2, which corresponded to 43% of the total inventory. A significant amount of the PPG-derived Pu has been transported by ocean currents and then preferentially scavenged in the coastal waters of Japan.

Plutonium isotopes in Northern Xinjiang, China: Level, distribution, sources and their contributions.

Plutonium in the environment has drawn significant attentions due to its radiotoxicity in high concentration and source term linked with nuclear accidents and contaminations. The isotopic ratio of plutonium is source dependent and can be used as a fingerprint to discriminate the sources of radioactive contaminant. 239Pu, 240Pu and 137Cs in surface soil and soil cores collected from Northern Xinjiang were determined in this work. The concentrations of 239,240Pu and 137Cs are in the range of 0.06-1.20 Bq kg-1, and <1.0-31.4 Bq kg-1 (decay corrected to Sep. 2017), respectively, falling in the ranges of global fallout in this latitude zone. The 240Pu/239Pu atomic ratios of 0.118-0.209 and 239,240Pu/137Cs activity ratios of 0.039-0.215 were measured. Among the investigated sites, distinctly lower 240Pu/239Pu atomic ratios of 0.118-0.133 and higher 239,240Pu/137Cs activity ratios of 0.065-0.215 compared to the global fallout values were observed in the northwest part, indicating a significant contribution from other source besides the global fallout. This extra source is mainly attributed to the releases of atmospheric nuclear weapons testing at Semipalatinsk Nuclear Test Site, which was transported by the west and northwest wind through the river valley among mountains in this region. This contribution is estimated to account for 28-43% of the global fallout in the northwest part of Northern Xinjiang. The contribution from the Chinese atmospheric nuclear weapons testing to this region is negligible due to the lack of appropriate wind direction to transport the radioactive releases to this region.

Carbon-14 content in surface soils near atmospheric and below ground nuclear detonations.

Global and regional releases of 14C have resulted from nuclear weapons testing activities; assessment of the chemical behavior and mechanisms of environmental transport and deposition of this radionuclide can assist remediation strategy development efforts and provide insights into global carbon cycling processes. This work reports a systematic evaluation of 14C in surface soils taken from the Nevada National Security Site. Surface soil samples are derived from above- and underground test locations, with underground test sites representing a range from near complete containment to uncontrolled radioactive releases. Only one surface soil taken from a underground test location (i.e. the Baneberry shot) shows elevated 14C concentrations (319 ±â€¯9 pMC) in addition to elevated concentrations of 137Cs, 60Co and 152Eu above regional backgrounds. Surface soils from above-ground test locations show extremely high 14C content (~1000 to 10,000 pMC); elevated concentrations of 152Eu and 60Co for these soils are also observed, with 137Cs at or below background levels. Taken together, these data suggest that 14C in surface soils from above-ground tests is primarily derived from in-situ neutron activation of the native soil material, whereas 14C in surface soils from underground tests may be from either recondensed particulate material or soil activation.

Radioactive level of coral reefs in the South China Sea.

In this study, we examined radioactivity simultaneously in surface marine sediments and coral skeletons collected from 12 locations of the fringing and atoll reefs in the South China Sea. Radioactive level declined from the fringing reefs to atoll reefs because of input of terrigenous minerals in the fringing reefs. Radioactivity was higher in coral skeletons than in marine sediments because of the high 228Ra activity in coral skeletons. Additionally, an abnormally low 226Ra/238U activity ratio (<0.1) of marine sediments in coral reefs was attributed to the biological process of active uptake of 226Ra and 238U from seawater by coral polyps rather than the ingrowth process in the 238U-230Th-226Ra decay chain. Several radiological indices were evaluated in coral reefs and significantly lower than recommended values. Particularly, the average Raeq in the atoll reefs was <5% of the world's average of Raeq. Our results displayed typically radioactive status in coral reefs without close-in fallout of anthropogenic radionuclides.

High-resolution 129I bomb peak profile in an ice core from SE-Dome site, Greenland.

129I in natural archives, such as ice cores, can be used as a proxy for human nuclear activities, age marker, and environmental tracer. Currently, there is only one published record of 129I in ice core (i.e., from Fiescherhorn Glacier, Swiss Alps) and its limited time resolution (1-2 years) prevents the full use of 129I for the mentioned applications. Here we show 129I concentrations in an ice core from SE-Dome, Greenland, covering years 1956-1976 at a time resolution of ∼6 months, the most detailed record to date. Results revealed 129I bomb peaks in years 1959, 1962, and 1963, associated to tests performed by the former Soviet Union, one year prior, in its Novaya Zemlya test site. All 129I bomb peaks were observed in winter (1958.9, 1962.1, and 1963.0), while tritium bomb peaks, another prominent radionuclide associated with nuclear bomb testing, were observed in spring or summer (1959.3, and 1963.6; Iizuka et al., 2017). These results indicate that 129I bomb peaks can be used as annual and seasonal age markers for these years. Furthermore, we found that 129I recorded nuclear fuel reprocessing signals and that these can be potentially used to correct timing of estimated 129I releases during years 1964-1976. Comparisons with other published records of 129I in natural archives showed that 129I can be used as common age marker and tracer for different types of records. Most notably, the 1963 129I bomb peak can be used as common age marker for ice and coral cores, providing the means to reconcile age models and associated trends from the polar and tropical regions, respectively.

Impact of Fukushima-derived radiocesium in the western North Pacific Ocean about ten months after the Fukushima Dai-ichi nuclear power plant accident.

We measured vertical distributions of radiocesium ((134)Cs and (137)Cs) at stations along the 149°E meridian in the western North Pacific during winter 2012, about ten months after the Fukushima Dai-ichi Nuclear Power Plant (FNPP1) accident. The Fukushima-derived (134)Cs activity concentration and water-column inventory were largest in the transition region between 35 and 40°N approximately due to the directed discharge of the contaminated water from the FNPP1. The bomb-derived (137)Cs activity concentration just before the FNPP1 accident was derived from the excess (137)Cs activity concentration relative to the (134)Cs activity concentration. The water-column inventory of the bomb-derived (137)Cs was largest in the subtropical region south of 35°N, which implies that the Fukushima-derived (134)Cs will also be transported from the transition region to the subtropical region in the coming decades. Mean values of the water-column inventories decay-corrected for the Fukushima-derived (134)Cs and the bomb-derived (137)Cs were estimated to be 1020 ± 80 and 820 ± 120 Bq m(-2), respectively, suggesting that in winter 2012 the impact of the FNPP1 accident in the western North Pacific Ocean was nearly the same as that of nuclear weapons testing. Relationship between the water-column inventory and the activity concentration in surface water for the radiocesium is essential information for future evaluation of the total amount of Fukushima-derived radiocesium released into the North Pacific Ocean.