Toward defining the Anthropocene onset using a rapid increase in anthropogenic fingerprints in global geological archives.

One of the remaining issues regarding the Anthropocene is the lack of stratigraphic evidence indicating when the cumulative human pressure from the early Holocene began to fundamentally change the Earth system. Herein, we compile anthropogenic fingerprints from various high-precision-dated proxy records for 137 global sites to determine the age of the unprecedented surge in these records over the last 7700 y. The cumulative number of fingerprints revealed an unprecedented surge in diverse anthropogenic fingerprints starting in 1952 ± 3 CE, corresponding to the onset of the Great Acceleration. Notably, the period from 1953 to 1958 CE saw a nearly simultaneous surge in fingerprints across all regions, including Antarctica, the Arctic, East Asia, Europe, North America, and Oceania. This synchronous upsurge reflects the moment when human impacts led to rapid transformations in various natural processes and cycles, with humans becoming a geological force capable of inscribing abundant and diverse anthropogenic fingerprints in global strata. Following this global fingerprint explosion, profound planetary-scale changes, including deviations from the established natural climatic conditions, begin. This unprecedented surge in anthropogenic signals worldwide suggests that human influences started to match many natural forces controlling the processes and cycles and overwhelm some of the functioning of the Earth system around 1952.

Radionuclide Solid:liquid partitioning in an aged, reducing-grout wasteform recovered from a disposal facility.

The Saltstone Disposal Facility on the Savannah River Site in South Carolina disposes of Low-Level Waste in a reducing-grout waste form. Reducing grout is presently being evaluated as a subsurface disposal waste form at several other locations in the United States, as well as in Europe and Asia. The objective of this study was to collect core samples directly from the Saltstone Disposal Facility and measure desorption distribution coefficients (Kd; radionuclide concentration ratio of saltstone:liquid; (Bq/kg)/Bq/L)) and desorption apparent solubility values (ksp; radionuclide aqueous concentration (moles/L)). An important attribute of this study was that these tests were conducted with actual aged, grout waste form materials, not small-volume simulants prepared in a laboratory. The reducing grout is comprised of blast furnace slag, Class F fly ash, ordinary portland cement, and a radioactive salt waste solution generated during nuclear processing. The grout sample used in this study underwent hydrolyzation in the disposal facility for 30 months prior to measuring radionuclide leaching. Leaching experiments were conducted either in an inert (no oxygen) atmosphere to simulate conditions within the saltstone monolith prior to aging (becoming oxidized) or they were exposed to atmosphere conditions to simulate conditions of an aged saltstone. Importantly, these experiments were designed not to be diffusion limited, that is, the saltstone was ground finely and the suspensions were under constant agitation during the equilibration period. Under oxidized conditions, measured Tc Kd values were 10 mL/g, which was appreciably greater than the historical best-estimate value of 0.8 mL/g. This difference is likely the result of a fraction of the Tc remaining in the less soluble Tc(IV) form, even after extensive oxidation during the experiment. Under oxidized and reducing conditions, the measured Ba and Sr (both divalent alkaline earth metals) Kd value were more than an order of magnitude greater than historical best-estimate values of 100 mL/g. The unexpectedly high Ba and Sr Kd values were attributed to these radionuclides having sufficient time to age (form strong bonds) in the sulfur-rich saltstone sample. Apparent ksp values under reducing conditions were 10-9 mol/L Tc and 10-13 mol/L Pu, consistent with values measured with surrogate materials. Measured apparent Ba, Sr, and Th ksp values were significantly greater than historical best-estimates. The implications of the generally greater Kd values and lower ksp values in these measurements is that these cementitious waste forms have greater radionuclide retention than was previously estimated based on laboratory studies using surrogate materials. This work represents the first leaching study performed with an actual aged, reducing-grout sample and as such provides an important comparison to studies conducted with surrogate materials, and provides high pedigree data for other programs around the world evaluating reducing grouts as a wasteform for subsurface nuclear waste disposal.

Plutonium in the coastal seawater around Chinese nuclear power plants: Sources, distribution, and environmental implications.

Coastal surface seawater samples within 30 km around ten Chinese nuclear power plants (NPPs) were systematically investigated. The 239+240Pu activity concentration in the samples varied from 0.226 mBq/m3 to 3.098 mBq/m3, meanwhile the 240Pu/239Pu atom ratios ranged from 0.151 to 0.353. Besides, the Pacific Proving Ground (PPG) close-in fallout and the global fallout were recognized as two primary sources of Pu in these samples. The 239+240Pu activity concentration as well as the PPG contribution showed similar trends as the Kuroshio intrusion path and the coastal currents in the China Seas, illustrating long-range transport and consuming of PPG derived Pu in the coastal China Seas. Moreover, accumulation of PPG sourced Pu in the Beibu Gulf were observed and was attributed to the continuous invasion of the high isotopic Pu that remobilized from the South China Sea (SCS).

Plutonium Speciation and Oxidation State Distributions in the Presence of Citrate.

We explored the speciation and kinetics of the Pu(VI)-citrate and Pu(III)-citrate systems (pHm = 2.5-11.0, I = 0.1 M NaCl, T = 23 °C, O2(g) < 2 ppm) using ultraviolet-visible-near-infrared (UV-vis-NIR) spectrophotometry, solvent extraction, and PHREEQC modeling. Formation constants were determined for PuO2(HcitH)(aq) (log K°1,1 = 1.09 ± 0.05) and PuO2(HcitH)(citH)3- (log K°1,2 = -0.20 ± 0.07), and evidence for (PuO2)m(citH-k)n(OH)x2m(3+k)n-x was identified under alkaline conditions. Pu(VI) species were found to be less stable in the presence of citrate than in the absence of citrate (t ≤ 168 days); the rate of reduction increased with increasing pH. The direct reduction of Pu(VI) to Pu(IV) was required to fit experimental data in the presence of citrate but did not improve the fit for Pu in the absence of citrate. We also observed increased Pu(III) stability in the presence of citrate (t ≤ 293 days), with higher concentrations of Pu(III) favored at lower pH. Finally, we provide evidence of a radiolysis-driven mechanism for the citrate-mediated reduction of plutonium that involves electron transfer from the oxidative breakdown of citrate. Our work highlights the need to investigate the redox effect of organic ligands on plutonium oxidation states under repository-relevant conditions.

Isotopic signature of plutonium accumulated in cryoconite on glaciers worldwide.

Glaciers are recognized as repositories for atmospheric pollutants, however, due to climate change and enhanced melting rates, they are rapidly transitioning from being repositories to secondary sources of such apollutants. Artificial radionuclides are one of the pollutants found on glaciers that efficiently accumulate onto glacier surfaces within cryoconite deposits; a dark, often biogenic sediment. This work provides information about the accumulation, distribution and sources of plutonium (Pu) isotopes in cryoconite samples from glaciers worldwide. Plutonium is an artificial radionuclide spread into the environment in the last decades as a consequence of nuclear test explosions, accidents and nuclear fuel re-processing. Samples collected from 49 glaciers across nine regions of Earth are considered. Activity concentrations of plutonium in cryoconite are orders of magnitude higher than in other environmental matrices typically used for environmental monitoring (e.g. lichens, mosses, soils and sediments), particularly in the Northern Hemisphere. Isotopic ratios indicate that plutonium contamination of cryoconite is dominated by the global signal of stratospheric fallout related to atmospheric nuclear tests. However, specific glaciers in Svalbard reveal a signature compatible with a contribution from the re-entry of the SNAP-9A satellite in 1964, which was equipped with a 238Pu radioisotope thermoelectric generator. Similarly, an excess of 238Pu is observed in cryoconite from the Exploradores Glacier (Chile). This could be associated with the November 1996 crash of the automatic Interplanetary Station "Mars '96" which was carrying a 238Pu thermoelectric generator. This is the first time ever that an isotopic evidence for this event is reported. These findings highlight the role that cryoconite can play in reconstructing the radioactive contamination history of different glaciated regions of the Earth.

Going deeper into plutonium sorption affected by redox.

Sorption of Pu(VI) onto synthesized goethite under oxidizing and normal conditions was investigated, which revealed its pH dependence on different solid/liquid ratios. Pu speciation upon sorption on the solid phase was characterized via extended X-ray absorption fine structure (EXAFS) spectroscopy, while that in solution was assessed using ultraviolet-visible (UV-Vis) spectroscopy and liquid-liquid extraction. The obtained results demonstrate differences in plutonium behavior in the studied systems. Pu(VI) remains hexavalent on the goethite surface and in solution under oxidizing conditions. While Pu(IV) is stabilized on the mineral and Pu(V) is found in solution under normal conditions. This study provides the thermodynamic descriptions of these reactions.

Electronic structure of the strongly correlated electron system plutonium hexaboride: A study from single-particle approximations and many-body calculations.

The electronic structure of the strongly correlated electron system plutonium hexaboride is studied by using single-particle approximations and a many-body approach. Imaginary components of impurity Green's functions show that 5fj=5/2 and 5fj=7/2 manifolds are in conducting and insulating regimes, respectively. Quasi-particle weights and their ratio suggest that the intermediate coupling mechanism is applicable for Pu 5f electrons, and PuB6 might be in the orbital-selective localized state. The weighted summation of occupation probabilities yields the interconfiguration fluctuation and average occupation number of 5f electrons n5f ~ 5.101. The interplay of 5f-5f correlation, spin-orbit coupling, Hund's exchange interaction, many-body transition of 5f configurations, and final state effects might be responsible for the quasiparticle multiplets in electronic spectrum functions. Prominent characters in the density of state, such as the coexistence of atomic multiplet peaks in the vicinity of the Fermi level and broad Hubbard bands in the high-lying regime, suggest that PuB6 could be identified as a Racah material. Finally, the quasiparticle band structure is also presented.

Wavelet transform of autoradiographs: Analysis of MOX fuel heterogeneity.

Radiation imaging is extensively applied in nuclear industry for various purposes including fuel characterization. Accurate quantitative evaluation of these radiographic images is difficult by the existing manual process and therefore image analytical methods have been attempted. The method of wavelet transform analysis has been applied on Gamma autoradiography (GAR) images of experimental (U, Pu)O2 mixed oxide (MOX) fuel pins with the objective to investigate the effectiveness of the method for fuel homogeneity characterization. The method was found effective to carry out quantified estimations of size and relative plutonium concentration of the heterogeneous portions in the fuel. The results were validated with theoretically simulated results as practical standards and calibrations are not possible in these samples. The results of wavelet transformation analysis were found to be more accurate with reference to the theoretically simulated values in comparison with conventional pixel analysis applied on the original GAR images.

Neutron spectroscopy of plutonium using a handheld detection system.

The ability to distinguish multiple forms of plutonium from one another, such as oxide and metal, is paramount in areas of nuclear nonproliferation and international safeguards. In its metal form, plutonium can be readily used in a nuclear weapon, while oxide forms are associated with nuclear reactor fuel. Oxide-based plutonium forms emit neutrons with an energy spectrum that is significantly different from the fission neutrons that are emitted from plutonium metal. Organic scintillation detectors output pulses that are proportional to the neutron energy deposited, and therefore present a means of distinguishing these plutonium forms based on their energy spectra. In this work, metal and oxide forms of plutonium were measured using a handheld detection system based on an organic glass scintillator. Monte Carlo modeling of these experiments was performed to provide insight into the origin of the features in the observed light output spectra. Through analysis of multiple regions of these spectra, in a matter of minutes we were able to unambiguously discriminate oxide and metal plutonium forms from one another and from a plutonium-beryllium neutron source, which was considered for comparison because these sources are commonly used in industrial applications. The ability to discriminate weapons-usable material from nuclear reactor fuel has applications in nuclear treaty verification and safeguards.

Review of the sources and behaviors of plutonium isotopes in the atmosphere and ocean.

Plutonium, as well as fission products such as 137Cs, had been released into the earth environment in 1945 after the first atmospheric nuclear explosion of plutonium bomb in the desert of New Mexico (USA, July 16) and later over Nagasaki (August 9), followed then by many other explosions. Thus, plutonium cycling in the atmosphere and ocean has become a major public concern as a result of the radiological and chemical toxicity of plutonium. However, plutonium isotopes and 137Cs are important transient tracers of biogeochemical and physical processes in the environment, respectively. In this review, we show that both physical and chemical approaches are needed to comprehensively understand the behaviors of plutonium in the atmosphere and ocean. In the atmosphere, plutonium and 137Cs attach with aerosols; thus, plutonium moves according to physical and chemical processes in connection with aerosols; however, since plutonium is a chemically reactive element, its behavior in an aqueous environment is more complicated, because biogeochemical regulatory factors, in addition to geophysical regulatory factors, must be considered. Meanwhile, 137Cs is chemically inert in aqueous environments. Therefore, the biogeochemical characteristics of plutonium can be elucidated through a comparison with those of 137Cs, which show conservative properties and moves according to physical processes. Finally, we suggest that monitoring of both plutonium and 137Cs can help elucidate geophysical and biogeochemical changes from climate changes.

Effects of liver's state of health on its iron and plutonium content.

PURPOSE: Plutonium and iron share a common metabolism in terms of their transportation and accumulation in the human body. This study examined their concentrations in livers with different states of health, and the effects of fatty degeneration and cirrhosis on their accumulation in the liver. MATERIALS AND METHODS: We determined the concentrations of plutonium and iron in autopsy liver samples from 1976-1979. Using statistical analysis, we investigated the relationships between the different variables. RESULTS AND CONCLUSIONS: The burdens of 239,240Pu and Fe correlated positively (Rs = 0.411) in the healthy livers, but not in the livers that had pathological findings. In contrast to the Fe content, the 239,240Pu content in the fatty degenerated or cirrhotic livers was significantly lower than that in normal livers. This difference may suggest that plutonium and iron do not accumulate or are not excreted in the same way in fatty degenerated and cirrhotic livers. The reaction mechanisms for the binding and excretion of plutonium, particularly in a fatty degenerated liver, are not yet fully known.

Subsurface Transport of Plutonium in Organic and Aqueous Acidic Processing Wastes at the Hanford Site, USA.

Over 4 million liters of mixed acidic (∼pH 2.5), high ionic strength (∼5 M nitrate) plutonium (Pu) processing waste were released into the 216-Z-9 (Z-9) trench at the Hanford Site, USA, and trace Pu has migrated 37 m below the trench. In this study, we used flowthrough columns to investigate Pu transport in simplified processing waste through uncontaminated Hanford sediments to determine the conditions that led to Pu migration. In low pH aqueous fluids, some Pu breakthrough is observed at pH < 4, and increased Pu transport (14% total Pu breakthrough) is observed at pH < 2. However, Pu migrates in organic processing solvents through low pH sediments virtually uninhibited with approximately 94 and 86% total Pu breakthrough observed at pH 1 and pH 3, respectively. This study demonstrates that Pu migration can occur both with and without organic solvents at pH < 4, but significantly more Pu can be transported when partitioned into organic processing solvents. Our data suggest that under acidic conditions (pH < 4) in the vadose zone beneath the Z-9 trench, Pu present in organic processing solvents moved relatively unhindered and may explain the historical downward migration of Pu tens of meters below the Z-9 trench.

System optimization study of hybrid K-edge/XRF densitometer for uranium-plutonium solution measurement.

In this paper, a comprehensive hybrid K-edge/XRF densitometer (HKED) device model is constructed using MCNP simulation. After the modeling process, a systematic simulation study is conducted to analyze the physical parameters and material selection of KED and XRF. The simulation results reveal that the optimal parameters for the X-ray tube are an X-ray source voltage of 160 kV and a 1 mm Fe filter. The sample should be placed in a vial with an inner diameter of 1.4 cm and an outer diameter of 2 cm. For the KED technique, the determined main parameters are a 1.9 cm Fe filter rod and an inner diameter of 0.08 cm for the collimator. For the XRF technique, the determined main parameters are a 0.01 cm Gd filter and an inner diameter of 0.3 cm for the collimator, with a detector angle of 150°. After selecting appropriate parameters, the average calibration factor Δµ of the KED technique was found to be 3.301 cm2 g-1, with a relative standard deviation (RSD) of 3.36%. Additionally, the comparison between the simulated and calculated values of uranium concentration revealed a minimum measurement error of 0.4%. The minimum detection concentration of KED for uranium solutions is approximately 1 g/L. For plutonium solutions ranging from 0.5 to 20 g/L, linear fitting of the Ka1 net peak area and plutonium concentration showed a coefficient of determination (R2) of 0.999. The detection limit of XRF for plutonium measurement was 2.33✕10-4 g/L. The linear fitting coefficients (R2) of uranium concentration versus K-edge transmission rate and plutonium concentration versus Ka1 net peak area for the hybrid technique in measuring uranium-plutonium mixed solutions are determined as 0.999 and 0.996, respectively, demonstrating the response relationship of the HKED device to uranium and plutonium under different concentrations.

Quantitative estimation of dust transport in the desert region of northwest China by plutonium isotopes.

Dust is an important source of atmospheric pollution, and quantitative estimation of desert dust transport is crucial for air pollution control. In this study, five typical sandy soil profiles in the Tengger Desert were collected and analyzed for 239,240Pu concentration and 240Pu/239Pu atomic ratios in order to identify the source of 239,240Pu in this area and explore the sedimentary characteristics of dust in different profiles. The results revealed that the concentrations of 239,240Pu in the soil profiles were between 0.002 and 0.443 mBq/g with an exception of the deep layer soil at one site. The measured atomic ratios of 240Pu/239Pu are at the global atmospheric fallout level with a mean of 0.184 ± 0.020, indicating that global fallout is the dominant source of plutonium in this region. The total inventories of 239,240Pu in the reference sites in this area were estimated to be 39.2-44.6 Bq/m2, this is in agreement with the value from the global fallout of atmospheric nuclear weapon tests at the similar latitude (30-40 °N: 42 Bq/m2). The estimated erosion rate in the erosion profile utilizing soil erosion intensity mode is 2491 t/km2/yr and the soil erosion depth is 9.86 cm, While, the stacking rate of the accumulation profile is 1383 t/km2/yr, and the depth of accumulation is estimated to be 5.48 cm. The difference between the erosion and accumulation profiles indicated that approximately 1107 t/km2/yr of dust was exported from the Gobi landform area of the Tengger Desert, which might be transported long distance in the downwind direction.

Laser-Induced Plasmas of Plutonium Dioxide in a Double-Walled Cell.

Plutonium research has been stifled by the significant number of administrative controls and safety procedures, space and instrumentation limitations in radiological gloveboxes, and the potential for personnel and equipment contamination. To address the limited number of spectroscopic studies in Pu-bearing compounds in the current scientific literature, this work presents the use of double-walled cells (DWCs) in "clean" buildings/laboratories as an alternative to research in radiological gloveboxes. This study reports the first laser-induced breakdown spectroscopy (LIBS) experiments of a PuO2 pellet contained within a DWC, where the formation of elemental (atomic and ionic) species as well as the evolution from elemental to molecular products (PuxOy) was measured. Raman spectroscopy was also used to characterize the surface of the ablated pellet and the particulates deposited on the window of the inner cell. The full width half-maximum of the T2g band enabled us to obtain an estimate of the temperature at the pellet surface after the ablation pulse and the particulates based on the crystal lattice disorder. Particulates deposited on the window of the DWC during laser ablation were characterized using scanning electron microscopy, where molten irregular particulates and spheroids were observed. This exciting research conducted in a DWC describes our initial attempts to incorporate LIBS in the arsenal of spectroscopic tools for nuclear forensics applications.

Indications of flat bands driving the δ to α volume collapse of plutonium.

On cooling from the melt, plutonium (Pu) undergoes a series of structural transformations accompanied by a ≈ 28% reduction in volume from its δ phase to its α phase at low temperatures. While Pu's partially filled 5f-electron shells are known to be involved, their precise role in the transformations has remained unclear. By using calorimetry measurements on α-Pu and gallium-stabilized δ-Pu combined with resonant ultrasound and X-ray scattering data to account for the anomalously large softening of the lattice with temperature, we show here that the difference in electronic entropy between the α and δ phases dominates over the difference in phonon entropy. Rather than finding an electronic specific heat characteristic of broad f-electron bands in α-Pu, as might be expected to occur within a Kondo collapsed phase in analogy with cerium, we find it to be indicative of flatter subbands. An important role played by Pu's 5f electrons in the formation of its larger unit cell α phase comprising inequivalent lattice sites and varying bond lengths is therefore suggested.

Transport and deposition of radionuclides from northern Africa to the southern Iberian Peninsula and the Canary Islands during the intense dust intrusions of March 2022.

The present study focuses on the two consecutive and markedly intense Saharan dust intrusion episodes that greatly affected southern Spain (Málaga) and, to a lesser extent, the Canary Islands (Tenerife), in March 2022. These two episodes were the result of atypical meteorological conditions in the region and resulted in record levels of aerosols in the air at the Málaga location. The activity levels of various natural and artificial radionuclides (7Be, 210Pb, 40K, 137Cs, 239Pu, 240Pu, 239+240Pu) and radioactive indicators (gross alpha and gross beta) were impacted by these events and the results are described herein. These episodes caused, for example, the activities of 137Cs in aerosol samples at the Málaga monitoring station to reach the highest concentrations ever recorded since high-volume aerosol monitoring started at this site in 2009. A link between the activity levels of 137Cs, 40K and gross alpha in the atmospheric aerosols and daily PM10 concentrations during the episodes is also reported. In addition, isotopic ratios are discussed in the context of the source and destination of the various anthropogenic radionuclides measured. The atmospheric residence time of aerosols during these episodes is also evaluated because it concerns how intrusions to the Canary Islands should be analysed. Finally, for the first time, the concentrations of 137Cs deposition by rainwater during a Saharan dust intrusion are reported and the deposition rate of these radionuclides during these episodes is discussed.

The bioreduction of U(VI) and Pu(IV): Experimental and thermodynamic studies.

The experimental and thermodynamic bioreduction of U(VI)aq and Pu(IV)am was studied in order to more accurately predict their transport velocities in groundwater and assess the contamination risks to the associated environments. The results obtained in this study emphasize the impact of carbonate-calcium and humic acids at 7.1 and anoxic solutions on the rate and extent of U(VI)aq and Pu(IV)am bioreduction by Shewanella putrefaciens. We found that the bioreduction rate of U(VI)aq became slow in the presence of NaHCO3/CaCl2. The more negative standard redox potentials of the ternary complexes of U(VI)-Ca2+-CO32- accounted for the decreased rate of bioreduction, e.g., [Formula: see text]  = -0.6797 V ≪ [Formula: see text]  = 0.3862 V. The bioreduction of Pu(IV)am seemed feasible, while humic acids accepted the adequate extracellular electrons secreted by S. putrefaciens, and the redox potential of Eh(HAox/HAred) was lower than Eh(PuO2(am)/Pu3+), e.g., Eh(HAox/HAred) ≦ Eh(PuO2(am)/Pu3+) if humic acids accepted ≧ 7.952 × 10-7 mol of electrons. The standard redox potentials, Eho(PuO2(am)/Pu3+) = 0.9295 V ≫ [Formula: see text]  = -0.6797 V, cannot explain the reduction extent of Pu(IV)am (8.9%), which is notably smaller than that of U(VI)aq (74.9%). In fact, the redox potential of Pu(IV)am was distinctly negative under the experimental conditions of trace-level Pu(IV)am (∼2.8 × 10-9 mol/L Pu(IV) if Pu(IV)am was completely dissolved), e.g., Eh(PuO2(am)/Pu3+) = -0.1590 V (α(Pu3+) = 10-10 mol/L, pH = 7.1). Therefore, the chemical factor of Pu3+ activity, leading to a rapid drop in Eh(PuO2(am)/Pu3+) at trace-level Pu(IV)am, was responsible for the relatively small reduction extent of Pu(IV)am.

New data on mobility of transuranium elements in sediments of the Yenisei River.

The inflow of transuranium elements to the Yenisei River was previously associated with the production of weapons-grade plutonium at the Mining-and-Chemical Combine (MCC, Zheleznogorsk, Russia), but the source of transuranium elements in the River today is fabrication of MOX fuel that started recently at the MCC. The current study presents results of sequential chemical extraction of radionuclides from sediment samples collected in 2014 and 2020 in two areas near the MCC discharge site and compares these results with the data obtained previously by sequential extraction of sediments collected during 1999-2007. Over the study period, the strength of binding of 137Cs and 60Co in the Yenisei River sediments was high (up to 100%) and remained so, while the percentages of 241Am and 152Eu in residual solids after sequential extraction increased considerably and the percentage of 239,240Pu in residual solids decreased in samples from all study areas. In samples collected at the position located close to the MCC discharge site, the percentages of the strongly bound 241Am and 152Eu as well as 239,240Pu were lower than in the samples from the other positions. The study demonstrated an enormous increase in 239,240Pu activity concentration in the top sediment layers collected at all positions in 2020 relative to 2014. In the same period, as literature data suggest, 239,240Pu activity concentrations also increased in aquatic organisms of the Yenisei River, which can be indicative of the growing potential bioavailability of plutonium in the aquatic ecosystem, which could be caused by the presence of the mobile form of plutonium in the routine discharges from the MCC.

Anthropogenic uranium signatures in turtles, tortoises, and sea turtles from nuclear sites.

Chelonians (turtles, tortoises, and sea turtles) grow scute keratin in sequential layers over time. Once formed, scute keratin acts as an inert reservoir of environmental information. For chelonians inhabiting areas with legacy or modern nuclear activities, their scute has the potential to act as a time-stamped record of radionuclide contamination in the environment. Here, we measure bulk (i.e. homogenized scute) and sequential samples of chelonian scute from the Republic of the Marshall Islands and throughout the United States of America, including at the Barry M. Goldwater Air Force Range, southwestern Utah, the Savannah River Site, and the Oak Ridge Reservation. We identify legacy uranium (235U and 236U) contamination in bulk and sequential chelonian scute that matches known nuclear histories at these locations during the 20th century. Our results confirm that chelonians bioaccumulate uranium radionuclides and do so sequentially over time. This technique provides both a time series approach for reconstructing nuclear histories from significant past and present contexts throughout the world and the ability to use chelonians for long-term environmental monitoring programs (e.g. sea turtles at Enewetok and Bikini Atolls in the Republic of the Marshall Islands and in Japan near the Fukushima Daiichi reactors).