Evaluation of semi-mechanistic models to predict soil to grass transfer factor of 137Cs based on long term observations in French pastures.

The aim of this study was to evaluate and improve the accuracy of the semi-mechanistic models used in regulatory exposure assessment tools, to describe the transfer factors of 137Cs from pasture soils to grass observed in different grazing areas of France between 2004 and 2017. This involved a preliminary parameterization step of the dynamic factor describing the ageing of radiocesium in the root zone using a Bayesian approach. A data set with mid-term (10 years about) and long term (more than 20 years) field and literature data from 4 European countries was used. A double kinetics of the bioavailability decay was evidenced with two half-life periods equal to 0.46 ± 0.11 yr and 9.57 ± 1.12 yr for the fast and slow declining rates respectively. We, then, tested a few existing alternative models proposed in literature. The comparison with field data showed that these models always underestimated the observations by one to two orders of magnitude, suggesting that the solid-liquid partition coefficient (Kd) was overestimated by models. The results suggest that semi mechanistic models might fail in the long-term prediction of the radionuclide transfer from soil-to-plant in the food chain. They highlight the need to calculate Kd using easily exchangeable 137Cs (i.e. labile fraction) rather than total soil 137Cs.

Dose reconstruction supports the interpretation of decreased abundance of mammals in the Chernobyl Exclusion Zone.

We re-analyzed field data concerning potential effects of ionizing radiation on the abundance of mammals collected in the Chernobyl Exclusion Zone (CEZ) to interpret these findings from current knowledge of radiological dose-response relationships, here mammal response in terms of abundance. In line with recent work at Fukushima, and exploiting a census conducted in February 2009 in the CEZ, we reconstructed the radiological dose for 12 species of mammals observed at 161 sites. We used this new information rather than the measured ambient dose rate (from 0.0146 to 225 µGy h-1) to statistically analyze the variation in abundance for all observed species as established from tracks in the snow in previous field studies. All available knowledge related to relevant confounding factors was considered in this re-analysis. This more realistic approach led us to establish a correlation between changes in mammal abundance with both the time elapsed since the last snowfall and the dose rate to which they were exposed. This relationship was also observed when distinguishing prey from predators. The dose rates resulting from our re-analysis are in agreement with exposure levels reported in the literature as likely to induce physiological disorders in mammals that could explain the decrease in their abundance in the CEZ. Our results contribute to informing the Weight of Evidence approach to demonstrate effects on wildlife resulting from its field exposure to ionizing radiation.

Particulate organic matter in rivers of Fukushima: An unexpected carrier phase for radiocesiums.

The role of particulate organic matter in radiocesium transfers from soils to rivers was investigated in areas contaminated by the Fukushima Daiichi Nuclear Power Plant accident. Suspended and deposited sediments, filtered water, macro organic debris and dead leaves were sampled along the six most contaminated coastal river catchments of the Fukushima prefecture in the early autumns 2013 and 2014. Radiocesium concentrations of river samples and total organic carbon concentrations in suspended and deposited sediments were measured. Radiocesium concentrations of suspended and deposited sediments were significantly correlated to 137Cs inventories in soils and total organic carbon. The distributions of radiocesium between the organic and mineral phases of both types of sediment were assessed by using a modelling approach. The results suggest that, during the early autumn season, the organic fraction was the main phase that carried the radiocesiums in deposited sediments and in suspended sediments for suspended loads <25mg·L-1. For higher suspended loads like those occurring during typhoon periods, the mineral fraction was the main carrier phase. Thus, high apparent distribution coefficient values noted by various authors in Fukushima could be attributed to the high radiocesium contents of particulate organic matter. Since it is well known that organic compounds generally do not significantly adsorb radiocesium onto specific sites, several hypotheses are suggested: 1) Radiocesiums may have been absorbed into organic components at the early stage of atmospheric radioactive deposits and/or later due to biomass recycling and 2) Those elements would be partly carried by glassy hot particles together with organic matter transported by rivers in Fukushima. Both hypotheses would lead to conserve the amount of radiocesiums associated with particles during their transfers from the contaminated areas to the marine environment. Finally, such organically bound radiocesium would lead to significant deliveries of bioavailable radiocesium for living organisms at Fukushima.

Behaviour of radiocaesium in coastal rivers of the Fukushima Prefecture (Japan) during conditions of low flow and low turbidity--Insight on the possible role of small particles and detrital organic compounds.

To investigate riverine transfers from contaminated soils of the Fukushima Prefecture in Japan to the marine environment, suspended sediments, filtered water, sediments and detrital organic macro debris deposited onto river beds were collected in November 2013 within small coastal rivers during conditions of low flow rates and low turbidity. River waters were directly filtered on the field and high efficiency well-type Ge detectors were used to analyse radiocaesium concentrations in very small quantities of suspended particles and filtered water (a few mg to a few g). For such base-flow conditions, our results show that the watersheds studied present similar hydro-sedimentary behaviours at their outlets and that the exports of dissolved and particulate radiocaesium are comparable. Moreover, the contribution of these rivers to the instantaneous export of radiocaesium to the ocean is similar to that of the Abukuma River. Our preliminary results indicate that, in the estuaries, radiocaesium concentrations in suspended sediments would be reduced by more than 80%, while radiocaesium concentration in filtered waters would be maintained. Significant correlations between radiocaesium concentrations and radiocaesium inventories in the soils of the catchments indicate that there was at that time little intra and inter-watershed variability in the transfer processes of radiocaesium from lands to rivers at this regional scale. The apparent liquid-solid partition coefficient (KD) values acquired for the lowest loads/finest particles complement the values acquired by using sediment traps and highlight the strong capacity of the smallest particles to transfer radiocaesium. Finally, but not least, our observations suggest that there could be a significant transfer of highly contaminated detrital biomass from forest litter to the downstream rivers in a rather conservative way.

Radiological dose reconstruction for birds reconciles outcomes of Fukushima with knowledge of dose-effect relationships.

We reconstructed the radiological dose for birds observed at 300 census sites in the 50-km northwest area affected by the accident at the Fukushima Daiichi nuclear power plant over 2011-2014. Substituting the ambient dose rate measured at the census points (from 0.16 to 31 µGy h(-1)) with the dose rate reconstructed for adult birds of each species (from 0.3 to 97 µGy h(-1)), we confirmed that the overall bird abundance at Fukushima decreased with increasing total doses. This relationship was directly consistent with exposure levels found in the literature to induce physiological disturbances in birds. Among the 57 species constituting the observed bird community, we found that 90% were likely chronically exposed at a dose rate that could potentially affect their reproductive success. We quantified a loss of 22.6% of the total number of individuals per increment of one unit log10-tansformed total dose (in Gy), over the four-year post-accident period in the explored area. We estimated that a total dose of 0.55 Gy reduced by 50% the total number of birds in the study area over 2011-2014. The data also suggest a significant positive relationship between total dose and species diversity.

137Cs in French soils: deposition patterns and 15-year evolution.

Around 2000 surface samples have been taken from French soil at around twenty stations over the last fifteen years. Caesium 137, the only artificial radionuclide in the terrestrial environment currently detectable with gamma spectroscopy, was measured in the samples. The levels of caesium activity were compared to deposition estimates for deposits from atmospheric weapons tests and Chernobyl fallout. Since the start of data acquisition, specific activity in the samples has decreased with a mean effective half-life of between 8 and 11 y, for meadow soil and agricultural soil respectively. These field observations confirm that the conventional soil migration-retention model, which uses distribution coefficient Kd, is insufficient for modelling caesium distribution in the surface soil layer. Although the differences between sites tend to diminish with time, surface specific activity in agricultural and meadow soil varies on average from a few Bq to several tens of Bq per kg of dry matter.

Mapping of 137Cs deposition over eastern France 16 years after the Chernobyl accident.

We observed the relationship between present-day 137Cs surface activity and the rainfall in May 1986 to establish a relevant map of 137Cs deposition over eastern France. This study was performed in an area of the lower Rhône valley where clayey soils are assumed to trap caesium efficiently. Based on the rainwater/airborne activity ratio deduced from this relationship, we verified that present-day activities, measured in clayey soils of this type, are relatively representative of the initial depositions. The interlocked contaminated areas of the resulting map can be related to rainfall occurrences, as is the case for all countries affected by the Chernobyl fallout. This map can be reasonably compared with those obtained for countries bordering France in terms of both activity levels and extent of homogeneous activity areas. Lastly, we demonstrate that it would not be possible to produce a coherent map of initial fallout by extending the campaign over the whole of the eastern territory based on present-day soil activity measurements alone. Hence, only the relationship between 137Cs deposition and the rainfall of the first week of May 1986 can be used to construct a map depicting the Chernobyl fallout over eastern France.