Long-term behaviour of Cs-137, Cs-133 and K in beech trees of French forests.

In the long-term after atmospheric deposit onto a forest ecosystem, Cs-137 becomes incorporated into the biogeochemical cycle of stable elements and progressively reaches a quasi-equilibrium state. This study aimed at determining to what extent Cs-137 activity distribution in tree vegetation could be predicted from that of stable caesium (Cs-133) and potassium (K), which are known to be stable chemical analogues and competitors for Cs-137 intake in tree organs. Field campaigns that focused on beech trees (Fagus sylvatica L.) were conducted in 2021 in three French forest stands with contrasted characteristics regarding either the contribution of global vs. Chornobyl fallouts, soil or climatic conditions. Decades after Cs-137 fallouts, it was found that more than 80% of the total radioactive inventory in the system remained confined in the top 20 cm mineral layers, while organic layers and beech vegetation (including roots) contributed each to less than 1.5%. The enhanced downward migration of Cs-137 in cambisol than podzol forest sites was presumably due to migration of clay particles and bioturbation. The distribution of Cs-137 and Cs-133 inventories in beech trees was very similar among sites but differed from that of K due a higher accumulation of Cs isotopes in roots (40-50% vs. < 25% for K). The aggregated transfer factor (Tag) of Cs-137 calculated for aerial beech organs were all lower than those reported in literature more than 20 years ago, this suggesting a decrease of bioavailability in soil due to ageing processes. Regarding their variability, Tags were generally lower by a factor 5 at the cambisol site, which was fairly well explained by a much higher value of RIP (radiocesium immobilisation potential). Cs-137 concentrations in trees organs normalized by the soil exchangeable fractions were linearly correlated to those of Cs-133 and the best fit was found for the linear regression model without intercept indicating that no more contribution of the foliar uptake could be observed on long term. Provided that the vertical distribution of caesium concentrations and fine root density are properly measured or estimated, Cs-133 was shown to be a much better proxy than K to estimate the root transfer of Cs-137.

Meta-analysis of radiocesium contamination data in Japanese cedar and cypress forests over the period 2011-2017.

Since Fukushima accident, dozens of field studies have been conducted in order to quantify and understand the behaviour of atmospheric radiocesium (137Cs) fallouts in contaminated forests of Fukushima and neighbouring prefectures. In this paper, we carry out a detailed review of data acquired over 2011-2017 in Japanese cedar and cypress plantations, focusing on aerial tree organs, soil layers and tree-to-soil depuration fluxes. To enable comparison and reinforce the consistency between sites, radiological measurements were normalized by the deposit and interpolated onto the same spatio-temporal frame. Despite some (poorly explained) residual variability, we derived a "mean" pattern by log-averaging data among sites. These "mean" results were analysed with the help of a simple mass-balance approach and discussed in the light of post-Fukushima literature. We demonstrated that the activity levels and dynamics in all compartments were consistent and generally well reproduced by the mass balance approach, for values of the interception fraction between 0.7 and 0.85. The analysis indicated that about 5% of the initial deposit remained in the aerial vegetation after 6 years, more than two thirds of intercepted 137Cs being transferred to the soil due to throughfall. The simulations indicated that foliar uptake might have contributed between 40% and 100% to the activity transferred to stem wood. The activity concentration in canopy organs rapidly decreased in the first few months then more slowly, according to an effective half-life of about 1.6 years. The activity level in the organic layer peaked in summer 2011 then decreased according to an effective half-life of 2.2 years. After a rapid increase in 2011, the contamination of mineral horizons continued to increase more slowly, 85% of 137Cs incoming through the organic layer being retained in the 0-5 cm layer according to a mean residence time longer than in the upper layer (7 against 1.5 years).

Behavior of 36Cl in agricultural soil-plant systems: A review of transfer processes and modelling approaches.

This article aims to review up-to-date knowledge and data acquired on 36Cl transfers to terrestrial soil-plant systems, evaluate the existing modelling approaches and identify priorities for future model improvements. This update has revealed the existence of fairly recent studies, whose results could be used for improving the modelling approaches which have been developed over the last decade. The priority areas include the consideration of the dry deposition process and the transfer of both gaseous and aerosol 36Cl to plants. The consideration of secondary processes such as the synthesis/mineralization of organochlorines and plant biomass litterfall is not recognized as a priority issue when assessing the impact of gaseous discharges. It was also identified that additional experimental studies had to be conducted to improve the understanding of the processes governing stable Cl and 36Cl dynamics in other terrestrial ecosystems (field crops, vegetables, grass) than forest environments on which most of the reported knowledge and data are reviewed.

Approaches to modelling radioactive contaminations in forests - Overview and guidance.

Modelling the radionuclide cycle in forests is important in case of contamination due to acute or chronic releases to the atmosphere and from underground waste repositories. This article describes the most important aspects to consider in forest model development. It intends to give an overview of the modelling approaches available and to provide guidance on how to address the quantification of radionuclide transport in forests. Furthermore, the most important gaps in modelling the radionuclide cycle in forests are discussed and suggestions are presented to address the variability of forest sites.

Meta-analysis of radiocesium contamination data in Japanese forest trees over the period 2011-2013.

The fate and dispersion of radiocesium in forests affected by the Fukushima atmospheric fallouts have been efficiently characterized by Japanese scientists thanks to monitoring surveys of radioactive contents in contaminated soil, water, and vegetation samples at numerous sites. In this paper, we carry out a meta-analysis of the field surveys conducted over the period 2011-2013 in evergreen coniferous and deciduous broadleaf forests of Fukushima or neighboring prefectures. The review focuses on contamination data acquired in tree vegetation - about 1500 spatio-temporal measurements of concentrations, inventories and depuration fluxes - with a particular interest for organs that were directly exposed to the atmospheric fallouts and subjected to depuration mechanisms (foliage, branches and outer bark). To reduce the spatial variability between the sites, radioactive data were normalized by the total deposit estimated at each site. Our analysis highlights the overall consistency of field observations despite the variety of experimental protocols, disparate sampling periods, differences in the forest stand characteristics and variability of the atmospheric deposition conditions. Assuming that the sites conformed to the same dynamics (within the range of residual variability), we then derive, discuss, and compare the mean representative evolutions of radiocesium contamination in the two categories of forest. Thanks to a simple mass balance approach, we finally demonstrate that: (i) about 90% of the radiocesium deposit was intercepted by evergreen coniferous vegetation, (ii) 80% of the deposit was gradually transferred to the forest floor in 3years, according to a well characterized depuration kinetics, and (iii) about 4% was readily absorbed by the foliage and translocated to internal organs (inner bark, stem wood and roots) at a rate of about 10-4d-1.

Interception of wet deposited atmospheric pollutants by herbaceous vegetation: Data review and modelling.

Better understanding and predicting interception of wet deposited pollutants by vegetation remains a key issue in risk assessment studies of atmospheric pollution. We develop different alternative models, following either empirical or semi-mechanistic descriptions, on the basis of an exhaustive dataset consisting of 440 observations obtained in controlled experiments, from 1970 to 2014, for a wide variety of herbaceous plants, radioactive substances and rainfall conditions. The predictive performances of the models and the uncertainty/variability of the parameters are evaluated under Hierarchical Bayesian modelling framework. It is demonstrated that the variability of the interception fraction is satisfactorily explained and quite accurately modelled by a process-based alternative in which absorption of ionic substances onto the foliage surfaces is determined by their electrical valence. Under this assumption, the 95% credible interval of the predicted interception fraction encompasses 81% of the observations, including situations where either plant biomass or rainfall intensity are unknown. This novel approach is a serious candidate to challenge existing empirical relationships in radiological or chemical risk assessment tools.

Modeling the early-phase redistribution of radiocesium fallouts in an evergreen coniferous forest after Chernobyl and Fukushima accidents.

Following the Chernobyl accident, the scientific community gained numerous data on the transfer of radiocesium in European forest ecosystems, including information regarding the short-term redistribution of atmospheric fallout onto forest canopies. In the course of international programs, the French Institute for Radiological Protection and Nuclear Safety (IRSN) developed a forest model, named TREE4 (Transfer of Radionuclides and External Exposure in FORest systems), 15 years ago. Recently published papers on a Japanese evergreen coniferous forest contaminated by Fukushima radiocesium fallout provide interesting and quantitative data on radioactive mass fluxes measured within the forest in the months following the accident. The present study determined whether the approach adopted in the TREE4 model provides satisfactory results for Japanese forests or whether it requires adjustments. This study focused on the interception of airborne radiocesium by forest canopy, and the subsequent transfer to the forest floor through processes such as litterfall, throughfall, and stemflow, in the months following the accident. We demonstrated that TREE4 quite satisfactorily predicted the interception fraction (20%) and the canopy-to-soil transfer (70% of the total deposit in 5 months) in the Tochigi forest. This dynamics was similar to that observed in the Höglwald spruce forest. However, the unexpectedly high contribution of litterfall (31% in 5 months) in the Tochigi forest could not be reproduced in our simulations (2.5%). Possible reasons for this discrepancy are discussed; and sensitivity of the results to uncertainty in deposition conditions was analyzed.

Evaluating variability and uncertainty in radiological impact assessment using SYMBIOSE.

SYMBIOSE is a modelling platform that accounts for variability and uncertainty in radiological impact assessments, when simulating the environmental fate of radionuclides and assessing doses to human populations. The default database of SYMBIOSE is partly based on parameter values that are summarized within International Atomic Energy Agency (IAEA) documents. To characterize uncertainty on the transfer parameters, 331 Probability Distribution Functions (PDFs) were defined from the summary statistics provided within the IAEA documents (i.e. sample size, minimal and maximum values, arithmetic and geometric means, standard and geometric standard deviations) and are made available as spreadsheet files. The methods used to derive the PDFs without complete data sets, but merely the summary statistics, are presented. Then, a simple case-study illustrates the use of the database in a second-order Monte Carlo calculation, separating parametric uncertainty and inter-individual variability.

Modelling the transfer of 14C from the atmosphere to grass: a case study in a grass field near AREVA-NC La Hague.

Radioactive (14)C is formed as a by-product of nuclear power generation and from operation of nuclear fuel reprocessing plants like AREVA-NC La Hague (North France), which releases about 15 TBq per year of (14)C into the atmosphere. Since the autumn of 2006, (14)C activity concentrations in samples from the terrestrial environment (air, grass and soil) have been monitored monthly on grassland 2 km downwind of the reprocessing plant. The monitoring data provides an opportunity to validate radioecology models used to assess (14)C transfer to grassland ecosystems. This article compares and discusses the ability of two different models to reproduce the observed temporal variability in grass (14)C activity in the vicinity of AREVA-NC La Hague. These two models are the TOCATTA model which is specifically designed for modelling transfer of (14)C and tritium in the terrestrial environment, and PaSim, a pasture model for simulating grassland carbon and nitrogen cycling. Both TOCATTA and PaSim tend to under-estimate the magnitude of observed peaks in grass (14)C activity, although they reproduce the general trends. PaSim simulates (14)C activities in substrate and structural pools of the plant. We define a mean turn-over time for (14)C within the plant, which is based on both experimental data and the frequency of cuts. An adapted PaSim result is presented using the 15 and 20 day moving average results for the (14)C activity in the substrate pool, which shows a good match to the observations. This model reduces the Root Mean Square Error (RMSE) by nearly 40% in comparison to TOCATTA.

TOCATTA: a dynamic transfer model of ¹4C from the atmosphere to soil-plant systems.

Many nuclear facilities release ¹4C into the environment, mostly as ¹4CO2, which mixes readily with stable CO2. This complete isotopic mixing (equilibrium) is often used as the basis for dose assessment models. In this paper, a dynamic compartment model (TOCATTA) has been investigated to describe ¹4C transfer in agricultural systems exposed to atmospheric ¹4C releases from nuclear facilities under normal operating or accidental conditions. The TOCATTA model belongs to the larger framework of the SYMBIOSE modelling and simulation platform that aims to assess the fate and transport of a wide range of radionuclides in various environmental systems. In this context, the conceptual and mathematical models of TOCATTA have been designed to be relatively simple, minimizing the number of compartments and input parameters required, appropriate to its use in an operational mode. This paper describes in detail ¹4C transfer in agricultural plants exposed to time-varying concentrations of atmospheric ¹4C, with a consideration also of the transfer pathways of ¹4C in soil. The model was tested against in situ data for ¹4C activity concentration measured over two years on a grass field plot located 2 km downwind of the AREVA NC La Hague nuclear reprocessing plant. The first results showed that the model roughly reproduced the observed month-to-month variability in grass ¹4C activity, but under-estimated (by about 33%) most of the observed peaks in the ¹4C activity concentration of grass. This tends to prove that it is not suitable to simulate intra-monthly variability, and a fortiori, the response of vegetation to accidental releases that may occur during the day. The need to increase the temporal resolution of the model has been identified in order to simulate the impact of intermittent ¹4C releases occurring either the day or night, such as those recorded by the AREVA NC plant.

Effects of radionuclide and rainfall characteristics on field loss parameters of grass.

The decrease of foliar activity in vegetation after its initial contamination by foliar deposition is termed "field loss" (Chamberlain, 1970). This work investigated further laboratory data concerning field loss of (134)Cs, (137)Cs, (85)Sr, (133)Ba and (123m)Te deposited on grassland (Madoz-Escande et al., 2005). Treatments consisted in rainfall scenarios cumulating 14 mm per week, combining two levels of intensity (8 or 30 mm/h) and two levels of frequency/precocity (late once or early twice-a-week). The time course of field loss was monitored in the edible tissues which were sampled by mowing between the rainfalls. Data were analyzed with an offset exponential loss model which is applicable to chronic contamination and is consistent with approaches adopted in radiological assessment models. Its parameters were estimated by the maximum-likelihood method, and their accuracy was determined by nonparametric bootstrap. Radionuclide and rainfall conditions significantly affected the estimated rate (lambda(1)) and extent (A(1)) of field loss. Field loss rate (lambda(1)) and nonentrainable fraction (1-A(1)) varied by a factor 1.5-3. Cesium was very mobile but persistent. On the contrary Tellerium was found less labile, but eventually was almost completely eliminated. Strontium and Barium had intermediate behaviors. Field loss was more efficient for moderate late once-a-week rainfalls (8mm/h). Higher rainfall intensity reduced more the radionuclides losses than higher rainfall frequency/precocity. This paper reports statistically relevant effects that should be considered for more realistic assessments.

An overview of BORIS: Bioavailability of Radionuclides in Soils.

The ability to predict the consequences of an accidental release of radionuclides relies mainly on the level of understanding of the mechanisms involved in radionuclide interactions with different components of agricultural and natural ecosystems and their formalisation into predictive models. Numerous studies and databases on contaminated agricultural and natural areas have been obtained, but their use to enhance our prediction ability has been largely limited by their unresolved variability. Such variability seems to stem from incomplete knowledge about radionuclide interactions with the soil matrix, soil moisture, and biological elements in the soil and additional pollutants, which may be found in such soils. In the 5th European Framework Programme entitled Bioavailability of Radionuclides in Soils (BORIS), we investigated the role of the abiotic (soil components and soil structure) and biological elements (organic compounds, plants, mycorrhiza, and microbes) in radionuclide sorption/desorption in soils and radionuclide uptake/release by plants. Because of the importance of their radioisotopes, the bioavailability of three elements, caesium, strontium, and technetium has been followed. The role of one additional non-radioactive pollutant (copper) has been scrutinised in some cases. Role of microorganisms (e.g., K(d) for caesium and strontium in organic soils is much greater in the presence of microorganisms than in their absence), plant physiology (e.g., changes in plant physiology affect radionuclide uptake by plants), and the presence of mycorrhizal fungi (e.g., interferes with the uptake of radionuclides by plants) have been demonstrated. Knowledge acquired from these experiments has been incorporated into two mechanistic models CHEMFAST and BIORUR, specifically modelling radionuclide sorption/desorption from soil matrices and radionuclide uptake by/release from plants. These mechanistic models have been incorporated into an assessment model to enhance its prediction ability by introducing the concept of bioavailability factor for radionuclides.