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).

Recent insights into trends of thyroid cancer incidence in Lithuanian population exposed to Chernobyl fallout early in life.

In the last three decades, an increase in thyroid cancer incidence has been observed worldwide, as well as in Lithuania. Although the rise was linked to overdiagnosis, the role of lifestyle and environmental factors, including exposure to ionizing radiation, cannot be excluded. In our retrospective study, we aimed to assess the association between the average age-specific thyroid dose due to the radioactive iodine uptake during childhood and adolescence from the Chernobyl fallout in Lithuania, and the trends of incidence of thyroid cancer from 1991 to 2015 in different regions. Averaged age-dependent thyroid doses were estimated for every municipality based on radioiodine activity in milk, reconstructed from available 131I activity measurements in the grass. Thyroid cancer incidence rates were calculated for the entire population and for two age at the time of exposure groups: 0-19 years and 0-9 years. Thyroid cancer relative risk (RR) was estimated for three municipality-specific thyroid dose (for 0-year-old babies) categories: less than 100 mGy (reference group), 100-199 mGy, and ≥200 mGy. Over the study period (1991-2015), a total of 5664 cases of thyroid cancer were registered in the entire Lithuanian population; 817 cases in the age group from 0 to 19 years at the time of the Chernobyl accident, and 266 cases in the age group from 0 to 9 years. Age-standardized thyroid cancer incidence rates have notably increased since 2000, peaked in 2009 (especially in females), and then slightly decreased and stabilized. The estimated average municipality-specific age-dependent thyroid doses ranged from 270 mGy in western Lithuania to 1.5 mGy in central and northern Lithuania. For the age group of 0-19 years at the time of the accident, in the period 1991-1995, the thyroid cancer relative risk was significantly increased (RR 3.91; 95 % CI: 1.27-10.29, p=0.01) in the highest dose category, compared to the lowest (although based on a small number of cases). For the age group 0-9 years at the time of the accident, a tendency of increased RR in the highest dose category appeared in the most recent period, 2011-2015. Our observations need to be confirmed by further following trends of thyroid cancer incidence in the cohort of 0-19-year-old Lithuanians at the time of the Chernobyl accident.

Glacier mice as a temporary sink for fallout radionuclides and heavy metals on the Norwegian glacier Austerdalsbreen.

Glacier mice are peculiar rolling or stationary moss balls found on the surface of some glaciers. They may harbour an ecological habitat for cold-adapted invertebrates and microorganisms, but little is known about their potential to accumulate and disseminate harmful elements and substances. In this study, we investigate the presence of fallout radionuclides (137Cs, 238Pu, 239Pu, 240Pu, 210Pb) and heavy metals (Pb, As, Hg, Cd) in glacier mice and compare the results to bryophytes from adjacent glacier ecosystems. Samples were collected at Austerdalsbreen, a Norwegian outlet glacier from Jostedalsbreen ice cap. Maximum activity concentrations for bryophytes are 552 ± 12 Bq kg-1 for 137Cs, 3485 ± 138 Bq kg-1 for 210Pb, 0.0223 ± 0.065 Bq kg-1 for 238Pu and 4.34 ± 0.43 Bq kg-1 for 239+240Pu while maximum heavy metals concentrations are 70.5 mg kg-1 for Pb, 1.0 mg kg-1 for As, 1.6 mg kg-1 for Hg and 0.13 mg kg-1 for Cd. Maximum activity concentrations in cryconite are 1973.4 ± 5.0 Bq kg-1 for 137Cs, 3632 ± 593 Bq kg-1 for 210Pb, 0.51 ± 0.11 Bq kg-1 for 238Pu and 13.1 ± 1.4 Bq kg-1 for 239+240Pu and maximum heavy metal concentrations are 50.4 mg kg-1 for Pb, 3.4 mg kg-1 for As, 1.5 mg kg-1 for Hg and 0.082 mg kg-1 for Cd. We find that glacier mice show lower activity concentrations of radionuclides compared to cryoconite. The major source of plutonium isotopes is related to global fallout, whereas detected radio-cesium may be additionally affected by post-Chernobyl fallout to an unknown extent. Comparison between glacier surface and adjacent glacial habitats shows higher concentrations of heavy metals in glacier mice on the glacier ice surface and medial moraines compared to bryophytes in the glacier forefield. Glacier mice exported from a receding glacier may affect the cycling of radioactive and metal pollutants in developing proglacial ecosystems.

Characterization of typical transuranic nuclides in a reference fallout material using SF-ICP-MS.

For the quality control in determining transuranic nuclides in fallout samples, this work first reported the 237Np activity concentration in a reference fallout material and further calculated the activity ratios of 237Np/239+240Pu and 237Np/241Am, and the atom ratio of 237Np/239Pu in it. The reference fallout material prepared by the Meteorological Research Institute was collected at 14 stations throughout Japan in 1963-1979. The 237Np and Pu isotopes (239Pu and 240Pu) were separated and purified using AG MP-1M anion-exchange resin, quantified using 242Pu as an isotope dilution tracer, and determined by the SF-ICP-MS. The analytical method was validated by the analysis of 4 sediment reference materials. The activity concentrations of 237Np, 239Pu and 240Pu were (25.9 ± 0.6) × 10-3, 4.10 ± 0.01 and 2.89 ± 0.04 Bq/kg, respectively, in the investigated reference fallout material. The activity ratio of 237Np/239+240Pu (3.7 ± 0.1) × 10-3 was consistent with the global fallout evaluation value. The 237Np/239Pu atom ratio of 0.561 ± 0.014 was higher than the average global fallout value of 0.41 ± 0.010, indicating the necessity of establishing regional characteristic global fallout value of 237Np/239Pu atom ratio for assessment of radioactive contamination. Comparison of the 237Np/239+240Pu activity ratios between in the reference fallout material and in soils over several decades indicated that 237Np has stronger migration capability than Pu isotopes in soils because 237Np was depleted compared to reference fallout material.

Modeling Fallout from Nuclear Weapon Detonations: Efficient Activity and Dose Calculation of Radionuclides and Their Progeny.

ABSTRACT: The purpose of this paper is to present a practical method for quick determination of potential radiological doses and contaminations by fallout from nuclear detonations, or other releases, that includes the contributions from all nuclides. We precalculate individual (total) activities of all radionuclides from any initial cocktail and all their ingrowing progeny at a set of pinpoints in time with a logarithmic time-spacing. This is combined with the set of dose conversion factors (DCC) for any exposure pathway to obtain a time-dependent cocktail for the whole release as if it is one substance. An atmospheric dispersion model then provides the thinning coefficient of the released material to give local concentrations and dose rates. Progeny ingrowth is illustrated for pure 238 U and for a nuclear reactor that has been shut down. Efficient dose assessment is demonstrated for fallout from nuclear detonations and compared with the traditional approach of preselecting nuclides for specific endpoints and periods-of-interest. The compound cocktail DCC reduces the assessment of contaminations and potential dose-effects from fallout after a nuclear detonation to (the atmospheric dispersion of) only one tracer substance, representing any cocktail of nuclides and their progeny. This removes the need to follow all separate nuclides or an endpoint-specific preselection of "most important nuclides." As the cocktail DCCs can be precalculated and the atmospheric dispersion of only one tracer substance has to be modelled, our method is fast. The model for calculating cocktail DCCs is freely available, easily coupled to any regular atmospheric dispersion model, and therefore ready for operational use by others.

Effects on local atmospheric environment of volcanic ash from Sakurajima volcano, inferred from atmospheric deposition of Potassium-40 at Kagoshima City, Japan.

In this study, we statistically demonstrated that an anomalous high of 40K fallout in the atmospheric fallout in Kagoshima City is caused by heavy ashfall associated with eruptions of Sakurajima volcano. Sakurajima is one of the most active volcanoes in Japan, and its repeated explosive eruptions cause large amounts of ash to fall on Kagoshima City. The fallout of crust-derived natural radionuclides, 40K, 212Pb, and 214Bi, from the atmosphere in Kagoshima City showed a significant correlation with the number of eruptions of Sakurajima volcano and the amount of ashfall in Kagoshima City. In contrast, no significant correlation was found between 40K and 7Be fallout. The 40K fallout indicates that almost all of the atmospheric fallout in Kagoshima City is composed of volcanic ash particles. The contribution from mineral and sea salt particles other than volcanic ash is minimal. The mass balance of the observed 40K fallout, ashfall, and atmospheric fallout yield indicates that there is a significant amount of volcanic ash deposition that is not accounted for as ashfall. In most cases, the ash deposition observed as ashfall is only 30-70 wt% of the total deposition collected as atmospheric fallout samples, and the remaining portion is fine-grained and behaves as suspended volcanic ash particles, which significantly impact the atmospheric environment.

Source, preservation and re-suspension of 239,240Pu in a well dated peat core collected from northwest China.

Owning to the high radiotoxicity in high concentrations, as well as the irreplaceability in quantifying soil erosion rates, demarcating the Anthropocene, and dating of sediment, anthropogenic 239,240Pu have drawn high attention. However, the source in specific areas, preservation characteristics in different environment media, and re-distribution process after the cessation of atmospheric nuclear weapons tests, have not been fully understood, which obscures the exact start year, temporal variation, and deposition flux of 239,240Pu in sedimentary records, and hinders the wide application of 239,240Pu in environment study. A sediment core from the Yiwu peat bog with dominance of atmospheric deposition in the source material, simple sedimentary environment, and high dust deposition flux, was collected to examine the 239,240Pu, and explore the source, preservation, and re-distribution process. The double peaks of 239,240Pu in 1952 CE and 1963 CE, as well as 240Pu/239Pu ratios of 0.163-0.190 with an average of 0.177 ± 0.010 confirmed that the 239,240Pu source originated predominantly from global fallout. The minimal vertical migration of plutonium in the Yiwu peat core was attributed to the near-neutral pH condition. The high inventory of 128 ± 7 Bq m-2, as well as the atypical negative correlation between 239,240Pu concentrations and organic matter content (r = - 0.79, P < 0.01), was attributed to the contribution of 239,240Pu re-suspended with dust from the neighboring Gobi Desert, particularly in the cold and dry years. The total re-suspended 239,240Pu was estimated to be 77 Bq m-2, exceeding the direct fallout level of 51 Bq m-2 during 1945-2016 CE. In this study, the specified deposition pattern of 239,240Pu after the cessation of atmospheric nuclear weapons was established, providing an important standard for multiple environmental studies, and the re-suspended amount of 239,240Pu in a typical arid area was quantified for the first time.

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.

Level, distribution and sources of Np, Pu and Am isotopes in Peter the Great Bay of Japan sea.

Transuranium elements such as Np, Pu and Am, are considered to be the most important radioactive elements in view of their biological toxicity and environmental impact. Concentrations of 237Np, Pu isotopes and 241Am in two sediment cores collected from Peter the Great Bay of Japan Sea were determined using radiochemical separation combined with inductively coupled plasma mass spectrometry (ICP-MS) measurement. The 239,240Pu and 241Am concentrations in all sediment samples range from 0.01 Bq/kg to 2.02 Bq/kg and from 0.01 Bq/kg to 1.11 Bq/kg, respectively, which are comparable to reported values in the investigated area. The average atomic ratios of 240Pu/239Pu (0.20 ± 0.02 and 0.21 ± 0.01) and 241Am/239+240Pu activity ratios (3.32 ± 2.76 and 0.45 ± 0.17) in the two sediment cores indicated that the sources of Pu and Am in this area are global fallout and the Pacific Proving Grounds through the movement of prevailing ocean currents, and no measurable release of Np, Pu and Am from the local K-431 nuclear submarine incident was observed. The extremely low 237Np/239Pu atomic ratios ((2.0-2.5) × 10-4) in this area are mainly attributed to the discrepancy of their different chemical behaviors in the ocean due to the relatively higher solubility of 237Np compared to particle active plutonium isotopes. It was estimated using two end members model that 23% ± 6% of transuranium radionuclides originated from the Pacific Proving Grounds tests, and the rest (ca. 77%) from global fallout.

Comparison of external dose estimates using different retrospective dosimetry methods in the settlements located near Semipalatinsk Nuclear Test Site, Republic of Kazakhstan.

For correct assessment of health risks after low-dose irradiation, calculation of radiation exposure estimates is crucial. To verify the calculated absorbed doses, instrumental methods of retrospective dosimetry are used. We compared calculated and instrumental-based estimates of external absorbed doses in the residents of Dolon, Mostik and Cheremushki villages, Kazakhstan, affected by the first nuclear weapon test performed at the Semipalatinsk Nuclear Test Site (SNTS) on August 29, 1949. The 'instrumental' doses were retrospectively estimated using the Luminescence Retrospective Dosimetry (LRD) and Electron Spin Resonance (ESR) methods. Correlation between the calculated individual cumulative external absorbed whole-body doses based on typical input data and ESR-based individual doses in the same people was strong (r = 0.782). It was even stronger between the calculated doses based on individual questionnaires' input data and the ESR-based doses (r = 0.940). Application of the LRD method is useful for validation of the calculated settlement-average cumulated external absorbed dose to air. Reconstruction of external exposure can be supplemented with the data from later measurements of soil contamination with long-lived radionuclides, such as, 137Cs. Our results show the reliability of the calculational method used for the retrospective assessment of individual external doses.

Important role of turbulence on the distribution of particle radioactivity in the nuclear explosions.

The distribution of particle radioactivity is one of the most important source items of radioactive fallout prediction model for nuclear explosion. For radioactive particles with the diameter larger than 0.5 µm, the influence of turbulent coagulation cannot be ignored. However, few scholars have considered the role of turbulence in the study of the distribution of particle radioactivity. The General Dynamic Equation (GDE), which is solved using the Multi-Monte Carlo method, is used in this study to establish a new model of the distribution of particle radioactivity that takes the impact of turbulent coagulation into account. The results present that the surface and volume distributions of particle radioactivity are closer to those of the Defense Land Fallout Interpretative Code (DELFIC) model, and the relative error of the surface (volume) distribution reduces from 1.243 (0.687) to 0.945 (0.284) when compared to the previous model that simply takes Brownian coagulation into account. The geometric median diameter of total particle radioactivity increases as the solidification temperature increases and as the particle size range increases when considering the influence of various geological conditions. When considering the effects of turbulent coagulation, the differences in the particle radioactivity produced under different geological conditions are smaller than those only considering the Brownian coagulation. This study highlights the importance of turbulent coagulation on the distribution of particle radioactivity in the nuclear explosions.

Spatial distribution, source identification, and transportation paths of plutonium in the Beibu Gulf, South China Sea.

To investigate the spatial distribution and source of plutonium isotopes in the Beibu Gulf, surface sediments were collected and analyzed using sector field inductively coupled plasma mass spectrometry (SF-ICP-MS). The activities of 239+240Pu in surface sediments ranged from 0.012 to 0.451 mBq/g (mean: 0.171 ± 0.138 mBq/g, n = 36), indicating a decreasing trend in a counterclockwise direction from the southern bay mouth. The counterclockwise decreasing trend in the south of the bay mouth is similar to the current in the Beibu Gulf. The 240Pu/239Pu atom ratios in surface sediments ranged from 0.156 to 0.283 (mean: 0.236 ± 0.031, n = 36), slightly higher than that of the global fallout value of 0.18. This suggests that the Pu in the Beibu Gulf was a combination of global fallout and Pacific Proving Ground (PPG). The average contribution of the plutonium (Pu) derived from the PPG in the sediment was estimated to be 52 % ± 24 %.

LARCalc, a tool to estimate sex- and age-specific lifetime attributable risk in populations after nuclear power plant fallout.

A tool called LARCalc, for calculating the radiological consequences of accidental large scale nuclear power plant releases based on estimates of 137Cs ground deposition, is presented. LARCalc is based on a previously developed models that has been further developed and packaged into an easy-to-use decision support tool for training of decision makers. The software visualises the radiological impact of accidental nuclear power plant releases and the effects of various protective measures. It is thus intended as a rapid alternative for planning protective measures in emergency preparedness management. The tool predicts projected cumulative effective dose, projected lifetime attributable cancer risk, and residual dose for some default accidental release scenarios. Furthermore, it can predict the residual dose and avertable cumulative lifetime attributable risk (LAR) resulting from various protective measures such as evacuation and decontamination. It can also be used to predict the avertable collective dose and the increase in cancer incidence within the specified population. This study presents the theoretical models and updates to the previous models, and examples of different nuclear fallout scenarios and subsequent protective actions to illustrate the potential use of LARCalc.

Examining the effects of soil entrainment during nuclear cloud rise on fallout predictions using a multiscale atmospheric modeling framework.

Current operational models for nuclear cloud rise over land were developed and validated using observations from shallow-buried or surface detonations, where lofted soil quickly mixed with fission products from the detonation. These models poorly predict fallout from elevated detonations near the fallout-free height of burst (FFHOB), where interactions with the ground are limited and the mixing of fission products and lofted soil is incomplete. Fallout-free is a misnomer at this HOB, as fallout was observed in these cases, but was below the levels of concern, especially off-grounds of the nuclear test site. To correctly characterize and model fallout from detonations near the FFHOB, models must be developed which can capture the stratified nature of the particle and activity-size distributions within the cloud. Previously, it was shown that the Weather Research and Forecasting (WRF) model can accurately simulate nuclear cloud rise for airbursts with little to no ground interactions (Arthur et al., 2021). That work is expanded here by (1) using a radiation-hydrodynamics code to improve the fireball initialization in WRF, (2) further developing an aerosol package from WRF-Chem to simulate lofted soil, and (3) combining the WRF cloud rise simulations with the operational models used at the National Atmospheric Release Advisory Center (NARAC) for fallout modeling. Using this combination of codes, the Upshot-Knothole Grable detonation, which was just below the FFHOB, is simulated from seconds after detonation through cloud rise and fallout, and results are compared to historical test data. The results show improved prediction of dose rate and highlight the need to correctly characterize the entrainment of material into the cloud and the subsequent mixing of fission products with entrained material.

Long-term study (1987-2023) on the distribution of 137Cs in soil following the Chernobyl nuclear accident: a comparison of temporal migration measurements and compartment model predictions.

After the Chernobyl accident, a designated area of ~1000 m2 within the University farm of Aristotle University of Thessaloniki in Northern Greece was utilized as a test ground for radioecological measurements. The profile of 137Cs in the soil was monitored from 1987 to 2023, with soil samples collected in 5-cm-thick slices (layers) down to a depth of 30 cm. The mean total deposition of 137Cs in the area, backdated to the time of the Chernobyl accident, was determined to be 18.6 ± 1.8 kBq m-2 based on four follow-up profile measurements of 137Cs in the soil for the years 2022 and 2023. It is noteworthy that this value is similar the total deposition at the site, which was independently measured to be about 20 kBq m-2 during the first year after the Chernobyl accident. The fractional contribution of each soil layer (e.g., 0-5 cm, 5-10 cm, 10-15 cm, etc.) to the total deposition of 137Cs (0-30 cm) is presented and analyzed. A compartment model was utilized to forecast the temporal evolution of fractional contributions of the different soil layers to the total deposition of 137Cs (0-30 cm). In this model, each soil layer is represented as a separate compartment. The model assumes that the transfer rates between adjacent compartments are equal. The agreement between the measured fractional contributions and the model predictions suggests that the compartment model with equal transfer rates can capture the broad patterns of 137Cs migration within the soil layers over the long period of 1987-2023. However, the use of a second compartment model with increasing transfer rates between consecutive soil layers did not align with the observed outcomes. This indicates that diffusion may not be the primary migration mechanism over the 36-y period covered by our study.

Restoring areas after a radioactive fallout: A multidisciplinary study on decontamination.

Land remediation is an important part of restoration measures after a radioactive fallout containing long-lived fission products such as 137Cs. In this multidisciplinary study, we focused on three main issues related to remediation of contaminated urban areas. First, we assessed how much decontamination contributes to reducing resident radiation exposure and how much this reduction depends on the timing of implemented measures. Second, we calculated direct and indirect costs of decontamination in an industrialized country such as Sweden. Finally, in a survey study, we considered reactions of Swedish citizens to being given the hypothetical option of moving to a site decontaminated after radioactive fallout and how this predicted response might influence the design of contingency plans. The main findings are that clean-up operations must be done within the first few years after a fallout to contribute significantly to reducing residual dose. If conducted within 1-2 years, large-scale decontamination can, on average, avert 20-200 manSv per km2 residential area and unit ground deposition of 137Cs (1 MBq). The estimated direct costs (in 2020 purchasing power) would amount to 100 million Euro per km2 decontaminated residential area (comparable to Japanese estimates after the Fukushima accident), generating 39,000 m3 of radioactive waste on average, mainly in the form of 137Cs-contaminated topsoil. In our survey study of 2291 Swedish respondents about their willingness to return to decontaminated homes, women, families with resident children, and high-income earners exhibited more skepticism about returning, even if authorities were to deem it safe. The demographic pattern in attitudes was similar to that found among evacuees in the Fukushima prefecture after 2011. We conclude that predefined ranges of measured 137Cs ground deposition can be used as guidance for rescue leaders in the early post-accident phase in long-term planning for affected areas. This planning should include timing and intensity of decontamination measures, duration of evacuation, and risk communication to citizens. Because some citizens expressed both high risk perception and risk aversion, however, timely and dialogic communication is unlikely to limit a shift after the incident to an older and more male-dominated population composition. There is a risk that those who can afford to do so will move away, whereas people whose wealth is locked in property (houses or businesses) will feel stuck. Perceptions of unfairness may fray the social fabric and complicate resettlement, which in some cases may mean inefficient outlay of decontamination costs. We believe that the issue of monetary compensation to affected residents requires priority in future work.

Plutonium in sediments of the Eastern Guangdong coast-its sources and their contribution.

The 239+240Pu activities and 240Pu/239Pu atom ratios of surface sediments from the Eastern Guangdong coast (EGDC) were determined by sector field ICP-MS in order to examine the sources of plutonium (Pu) and quantify their contributions. The 239+240Pu activities in the EGDC ranged from 0.113 to 0.451 Bq kg-1, with an average of 0.225 ± 0.090 Bq kg-1 (n = 17). Consistently high 240Pu/239Pu atom ratios, ranging from 0.218 to 0.274 (average = 0.254 ± 0.014, n = 17), indicate a non-global fallout Pu source in the EGDC. The horizontal distribution of the 240Pu/239Pu atom ratios in the EGDC sediment suggests the non-global fallout Pu is sourced from close-in fallout from the Pacific Proving Grounds (PPG). Using a simple two end-member mixing model, we calculated the relative proportions of Pu from the PPG and global fallout in the EGDC to be 57 ± 9 % and 43 ± 9 %, respectively. Moreover, from the well-defined relationship between 239+240Pu activity and total organic carbon content in sediments and a two end-member mixing model using δ13C, we further calculated the Terr-global fallout (riverine input) and Mar-global fallout (direct atmospheric deposition) to be 11 ± 2 % and 32 ± 6 %, respectively. Finally, from the activity levels and atom ratios of Pu isotopes in the EGDC, we established a baseline for future use in environmental risk assessment related to nuclear power plant operations.

Plutonium isotopes in the ground air layer in southern Poland (2010-2016): Source terms, seasonal variability and correlations with meteorological conditions.

In this study, the results of the analysis of Pu-238 and Pu-239 + 240 activity concentrations on aerosol filters collected from 2010 to 2016 in Krakow (Southern Poland) are presented and discussed. For the first time, the temporal variation of Pu-239 + 240 activity concentration in surface air in Poland was studied using Fourier analysis. The analysis clearly showed that the Pu-239 + 240 content in the near-ground air layer is subject to seasonal variations and demonstrates annual periodicity. Pu analyses were performed using alpha spectrometry. The measured values ranged from 1.93∙10-10 Bq/m3 to 1.31∙10-8 Bq/m3 with an average of 2.07∙10-9 Bq/m3 for Pu-239 + 240 and from 9.07∙10-11 Bq/m3 to 1.27∙10-9 Bq/m3 with the average 1.52∙10-10 Bq/m3 for Pu-238. The analysis of the potential sources of plutonium isotopes in the air aerosols samples indicated that only two samples are uniquely characterized by the ratio corresponding to spent nuclear fuel: February 2012 (0.59 ± 0.18) and February 2015 (0.68 ± 0.19). The remaining samples showed mixed origins, with global radioactive fallout appearing to contribute more than spent nuclear fuel. To study the relationship between Pu-239 + 240 and meteorological conditions, Pearson's correlation and circulation pattern analyses were performed. The analyses showed that the Pu-239 + 240 activity concentration depends on air temperature (R = 0.51), the sum of ice and snowfall (R = -0.45), relative humidity (R = -0.54) and mean total cloud cover (R = -0.56). High concentrations of Pu-239 + 240 were positively correlated with air advection from the southern and eastern sectors, whereas low concentrations were observed during dynamic weather conditions with intense circulation from the western sector. In case of Pu-238 no significant correlation was observed.

Assessment of Differentiated Thyroid Carcinomas in French Polynesia After Atmospheric Nuclear Tests Performed by France.

Importance: Due to the amount of iodine 131 released in nuclear tests and its active uptake by the thyroid, differentiated thyroid carcinoma (DTC) is the most serious health risk for the population living near sites of nuclear tests. Whether low doses to the thyroid from nuclear fallout are associated with increased risk of thyroid cancer remains a controversial issue in medicine and public health, and a misunderstanding of this issue may be associated with overdiagnosis of DTCs. Design, Setting, and Participants: This case-control study was conducted by extending a case-control study published in 2010 that included DTCs diagnosed between 1984 and 2003 by adding DTCs diagnosed between 2004 and 2016 and improving the dose assessment methodology. Data on 41 atmospheric nuclear tests conducted by France between 1966 and 1974 in French Polynesia (FP) were assessed from original internal radiation-protection reports, which the French military declassified in 2013 and which included measurements in soil, air, water, milk, and food in all FP archipelagos. These original reports led to an upward reassessment of the nuclear fallout from the tests and a doubling of estimates of the mean thyroid radiation dose received by inhabitants from 2 mGy to nearly 5 mGy. Included patients were diagnosed from 1984 to 2016 with DTC at age 55 years or younger and were born in and resided in FP at diagnosis; 395 of 457 eligible cases were included, and up to 2 controls per case nearest by birthdate and matched on sex were identified from the FP birth registry. Data were analyzed from March 2019 through October 2021. Exposure: The radiation dose to the thyroid gland was estimated using recently declassified original radiation-protection service reports, meteorological reports, self-reported lifestyle information, and group interviews of key informants and female individuals who had children at the time of these tests. Main Outcomes and Measures: The lifetime risk of DTC based on Biological Effects of Ionizing Radiation (BEIR) VII models was estimated. Results: A total of 395 DTC cases (336 females [85.1%]; mean [SD] age at end of follow-up, 43.6 [12.9] years) and 555 controls (473 females [85.2%]; mean [SD] age at end of follow-up, 42.3 [12.5] years) were included. No association was found between thyroid radiation dose received before age 15 years and risk of DTC (excess relative risk [ERR] per milligray, 0.04; 95% CI, -0.09 to 0.17; P = .27). When excluding unifocal noninvasive microcarcinomas, the dose response was significant (ERR per milligray, 0.09; 95% CI, -0.03 to 0.02; P = .02), but several incoherencies with the results of the initial study reduce the credibility of this result. The lifetime risk for the entire FP population was 29 cases of DTC (95% CI, 8-97 cases), or 2.3% (95% CI, 0.6%-7.7%) of 1524 sporadic DTC cases in this population. Conclusions and Relevance: This case-control study found that French nuclear tests were associated with an increase in lifetime risk of PTC in FP residents of 29 cases of PTC. This finding suggests that the number of thyroid cancer cases and the true order of magnitude of health outcomes associated with these nuclear tests were small, which may reassure populations of this Pacific territory.

Statistical modeling of trends in infant mortality after atmospheric nuclear weapons testing.

The global fallout from atmospheric nuclear weapons testing in the 1950s and 1960s caused by far the greatest exposure of mankind to ionizing radiation. Surprisingly few epidemiological studies of the possible health effects of atmospheric testing have been conducted. Here, long-term trends in infant mortality rates in the United States (U.S.) and five major European countries (EU5) were examined: The United Kingdom, Germany, France, Italy, and Spain. Bell-shaped deviations from a uniformly decreasing secular trend were found beginning in 1950, with maxima around 1965 in the U.S. and 1970 in EU5. From the difference between observed and predicted infant mortality rates, in the period 1950-2000, the overall increase in infant mortality rates was estimated to be 20.6 (90% CI: 18.6 to 22.9) percent in the U.S. and 14.2 (90% CI: 11.7 to 18.3) percent in EU5 which translates to 568,624 (90% CI: 522,359 to 619,705) excess infant deaths in the U.S. and 559,370 (90% CI: 469,308 to 694,589) in the combined five European countries. The results should be interpreted with caution because they rely on the assumption of a uniformly decreasing secular trend if there had been no nuclear tests, but this cannot be verified. It is concluded that atmospheric nuclear weapons testing may be responsible for the deaths of several million babies in the Northern Hemisphere.