A pilot study of radiocesium activity concentration in the stemflow of deciduous broad-leaved trees: Its relationship with leaves and outer bark as of 2022-2023.

The radiocesium (137Cs) activity concentration in stemflow, which is an element of the 137Cs cycle in the forest, is determined by the supply of 137Cs from the outer bark and leaves. Long-term monitoring data of deciduous broad-leaved trees since the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident have shown the 137Cs activity concentration in the outer bark decreasing exponentially, while that in the leaves has remained nearly constant. Therefore, it is expected that the contribution of the outer bark to 137Cs in stemflow eventually becomes smaller than that of leaves over time. We hypothesized that as of 2022-2023 (i.e., more than 10 years after the FDNPP accident), the main source of 137Cs in the stemflow of deciduous broad-leaved trees is mainly leaching from leaves. We tested this hypothesis by conducting two surveys in the autumn of 2022 (September-October) and early summer of 2023 (May-June) in Kawauchi Village, Fukushima Prefecture. Samples consisted of stemflow, leaves, and outer bark from a total of 10 deciduous broad-leaved trees (three konara oaks, three mizunara oaks, two Japanese chestnuts, and two cherry blossoms). Our statistical analyses (correlation, linear and multilinear regression analyses) showed that the 137Cs activity concentrations in stemflow were significantly positively correlated to those in leaves, with no positive correlation detected with the outer bark, suggesting that at the time of the survey, the 137Cs activity concentration in stemflow was mainly influenced by the 137Cs activity concentration in leaves. In addition, we propose a method for estimating the stemflow 137Cs activity concentration in konara oak using data from leaves. Although the method's prediction accuracy is low from 2011 to 2013, it is able to estimate the stemflow 137Cs activity concentration in konara oak. Thus, it can help determine one of the model parameters of 137Cs dynamics within deciduous broad-leaved forests.

Effect of litter removal five years after the Fukushima accident on 137Cs uptake by Japanese cedar.

Removal of litter-associated 137Cs from the forest floor (litter removal) can reduce the 137Cs uptake by plants; however, the proposed effective period for litter removal was 1-2 years after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. This is because the 137Cs in forest soil migrates rapidly from the litter to surface mineral soil layers in Japanese forests, and thus the effectiveness of litter removal will quickly become limited. However, it is unknown whether this approach can be applied to forests whose vertical migration of 137Cs in the forest soil is relatively slow. Herein, we compared the 137Cs activity concentration in the inner bark of the Japanese cedar (Cryptomeria japonica) between litter removal (conducted in September and October 2016, 5 years after the accident) and in control areas in Kawauchi Village, Fukushima Prefecture, where the vertical migration of 137Cs was relatively slow from the litter to surface mineral soil layers. Air dose rates (ambient dose equivalent) in the litter removal area were significantly lower than those in the control area in 2022, and the 137Cs inventory in the forest soil in litter removal area also tended to be lower than that in the control area. In Japanese cedars with similar levels of outer bark contamination, the 137Cs activity concentration in the inner bark in the litter removal area was significantly lower than that in the control area, and consistent trends were also found when comparing the 137Cs activity concentration in the leaves of Stephanandra incisa and Wisteria floribunda obtained from the same forest. Thus, the litter removal 5 years after the FDNPP accident may have reduced the 137Cs uptake in Japanese cedar in an evergreen coniferous forest where the vertical migration of 137Cs is relatively slow in the forest soil.

Factors influencing the difference in dissolved ion inputs to the forest floor between deciduous and coniferous stands: comparison under high and low atmospheric deposition conditions.

It is necessary to clear the relationship between physical and vegetation factors on the processes governing dissolved ion inputs to the forest floor to estimate correctly the values of atmospheric input to the forest. This study identified the factors influencing the differences in dissolved ion inputs to the forest floor between coniferous evergreen and broad-leaved deciduous species by analyzing the phenological variations of dry deposition and canopy exchange calculated by the canopy budget model under a high-deposition site near the city of Tokyo and a low-deposition site 84 km further away. At low-deposition site, vegetation factors such as capture efficiency did not explain the differences in Na+ or Cl- dry deposition. Leaf physiological characteristics influenced the differences in the Mg2+ and Ca2+ canopy leaching values, and phenology, leaf wettability, and diffusion processes from water film into leaves influenced the differences in NH4+ and NO3- input processes between tree types. At the high-deposition site, differences in the dry deposition of Na+, SO42-, Cl-, Mg2+, Ca2+, NH4+, and NO3- between tree types were influenced by differences in capture efficiency between coniferous and broad-leaved canopies in the leafed period and by the absence of leaves in deciduous species after leaf fall. These results indicated that atmospheric deposition affected the capture efficiency of coniferous trees for dry deposition and enhanced the difference of dissolved ion inputs to the forest floor between coniferous and deciduous species.

Radiocesium mobility in different parts of the two major tree species in Fukushima.

Radiocesium (137Cs) released in the Fukushima Dai-ichi Nuclear Power Plant accident is still cycling in the forest ecosystem. We examined the mobility of 137Cs in the external parts-leaves/needles, branches, and bark-of the two major tree species in Fukushima, Japanese cedar (Cryptomeria japonica) and konara oak (Quercus serrata). This variable mobility will likely lead to spatial heterogeneity of 137Cs and difficulty in predicting its dynamics for decades. We conducted leaching experiments on these samples by using ultrapure water and ammonium acetate. In Japanese cedar, the 137Cs percentage leached from current-year needles was 26-45% (ultrapure water) and 27-60% (ammonium acetate)-similar to those from old needles and branches. In konara oak, the 137Cs percentage leached from leaves was 47-72% (ultrapure water) and 70-100% (ammonium acetate)-comparable to those from current-year and old branches. Relatively poor 137Cs mobility was observed in the outer bark of Japanese cedar and in organic layer samples from both species. Comparison of the results from corresponding parts revealed greater 137Cs mobility in konara oak than in Japanese cedar. We suggest that more active cycling of 137Cs occurs in konara oak.

Ten-year trends in vertical distribution of radiocesium in Fukushima forest soils, Japan.

To elucidate interannual changes in the vertical distribution of 137Cs in forest ecosystems contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident, we investigated 137Cs inventories in forest soils (both organic and mineral soil horizons) at 10 sampling plots with different 137Cs deposition levels and dominant species for up to 10 years after the accident. We examined the temporal variation of the 137Cs inventories by depth with exponential regression models (assuming that the transition and partitioning of 137Cs are still active) and exponential offset regression models (assuming a shift to a stable 137Cs distribution, defined as the "quasi-equilibrium steady-state" in the Chernobyl accident). In the organic horizon, the 137Cs inventories were exponentially decreasing, and it might take more time to converge in the quasi-equilibrium steady-state at most plots. In the mineral soil horizon, most of 137Cs was found in the surface layer of the mineral soil horizon (0-5 cm). In this layer, the inventories first increased and then become relatively constant, and the exponential offset model was selected at most plots, suggesting entry into the quasi-equilibrium steady-state over the observation period. Although we also observed exponentially increasing trends in a lower layer (5-10 cm) of the mineral soil horizon, there was no clear increasing or decreasing trend of 137Cs inventory in the deeper mineral soil layers (10-15 and 15-20 cm). Our calculation of the relaxation depth and migration center revealed that downward migration of 137Cs is not significant in terms of the overall 137Cs distribution in the mineral soil horizon over 10 years.

Dynamics of radiocaesium within forests in Fukushima-results and analysis of a model inter-comparison.

Forests cover approximately 70% of the area contaminated by the Fukushima Daiichi Nuclear Power Plant accident in 2011. Following this severe contamination event, radiocaesium (137Cs) is anticipated to circulate within these forest ecosystems for several decades. Since the accident, a number of models have been constructed to evaluate the past and future dynamics of 137Cs in these forests. To explore the performance and uncertainties of these models we conducted a model inter-comparison exercise using Fukushima data. The main scenario addressed an evergreen needleleaf forest (cedar/cypress), which is the most common and commercially important forest type in Japan. We also tested the models with two forest management scenarios (decontamination by removal of soil surface litter and forest regeneration) and, furthermore, a deciduous broadleaf forest (konara oak) scenario as a preliminary modelling study of this type of forest. After appropriate calibration, the models reproduced the observed data reliably and the ranges of calculated trajectories were narrow in the early phase after the fallout. Successful model performances in the early phase were probably attributable to the availability of comprehensive data characterizing radiocaesium partitioning in the early phase. However, the envelope of the calculated model end points enlarged in long-term simulations over 50 years after the fallout. It is essential to continue repetitive verification/validation processes using decadal data for various forest types to improve the models and to update the forecasting capacity of the models.

Estimation of the rate of 137Cs root uptake into stemwood of Japanese cedar using an isotopic approach.

Japanese cedar (Cryptomeria japonica) is the main timber species in Japan. The prediction of the temporal changes in the 137Cs concentration in the stemwood of Japanese cedar after the Fukushima nuclear accident is essential for optimizing forest management in contaminated areas. However, it is difficult to estimate the respective contributions of root and foliar uptake to 137Cs accumulation in stemwood from simple field measurements, especially in trees that contain the residue of initially-deposited 137Cs. In this study, we devised a method for estimating the rate of 137Cs root uptake into stemwood using the 133Cs content in stemwood and the 137Cs/133Cs ratio in the exchangeable fraction of soil. As a trial, the method was applied to a cedar stand in Fukushima Prefecture, using available monitoring data from prior studies over 5 years from August 2011 to August 2016. The mean annual rate of 137Cs root uptake into stemwood over this period was estimated as 53 ± 20 Bq m-2 yr-1. We note that our method likely provided a maximum estimate, because it is based on the assumptions that 133Cs in wood is exclusively supplied by root uptake, and that Cs isotopes are taken up by roots in the top 5 cm of mineral soil. Moreover, the mean annual increase of the 137Cs inventory in stemwood during the study period was measured as 108 Bq m-2 yr-1, although this value was associated with considerable uncertainty (95% confidence interval from -109 to 324 Bq m-2 yr-1). As a result, the maximum estimated rate of 137Cs root uptake into stemwood accounted for around half of the measured rate of 137Cs accumulation in stemwood. Our results show that the Cs isotopic approach has potential to distinguish the main pathway of stemwood contamination (i.e., root vs. foliar uptake) following radioactive fallout.

Calculations for ambient dose equivalent rates in nine forests in eastern Japan from 134Cs and 137Cs radioactivity measurements.

Understanding the relationship between the distribution of radioactive 134Cs and 137Cs in forests and ambient dose equivalent rates (H˙∗(10)) in the air is important for researching forests in eastern Japan affected by the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. This study used a large number of measurements from forest samples, including 134Cs and 137Cs radioactivity concentrations, densities and moisture contents, to perform Monte Carlo radiation transport simulations for H˙∗(10) between 2011 and 2017. Calculated H˙∗(10) at 0.1 and 1 m above the ground had mean residual errors of 19% and 16%, respectively, from measurements taken with handheld NaI(Tl) scintillator survey meters. Setting aside the contributions from natural background radiation, 134Cs and 137Cs in the organic layer and the top 5 cm of forest soil generally made the largest contributions to calculated H˙∗(10). The contributions from 134Cs and 137Cs in the forest canopy were calculated to be largest in the first two years following the accident. Uncertainties were evaluated in the simulation results due to the measurement uncertainties in the model inputs by assuming Gaussian measurement errors. The mean uncertainty (relative standard deviation) of the simulated H˙∗(10) at 1 m height was 11%. The main contributors to the total uncertainty in the simulation results were the accuracies to which the 134Cs and 137Cs radioactivities of the organic layer and top 5 cm of soil, and the vertical distribution of 134Cs and 137Cs within the 5 cm soil layers, were known. Radioactive cesium located in the top 5 cm of soil was the main contributor to H˙∗(10) at 1 m by 2016 or 2017 in the calculation results for all sites. Studies on the 137Cs distribution within forest soil will therefore help explain radiation levels henceforth in forests affected by the FDNPP accident. The merits of this study are that it modelled multiple forests for a long time period, with the important model inputs being informed by field measurements, and it quantified how the measurement uncertainties in these inputs affected the calculation results.

A dataset of 137Cs activity concentration and inventory in forests contaminated by the Fukushima accident.

The majority of the area contaminated by the Fukushima Daiichi Nuclear Power Plant accident is covered with forests. We developed a dataset for radiocaesium (137Cs) in trees, soil, and mushrooms measured at numerous forest sites. The 137Cs activity concentration and inventory data reported in scientific journal papers written in English and Japanese, governmental reports, and governmental monitoring data on the web were collated. The ancillary information describing the forest stands were also collated, and further environmental information (e.g. climate) was derived from the other databases using longitude and latitude coordinates of the sampling locations. The database contains 8593, 4105, and 3189 entries of activity concentration data for trees, soil, and mushrooms, and 471 and 3521 entries of inventory data for trees and soil, respectively, which were collected from 2011 to 2017, and covers the entire Fukushima prefecture. The data can be used to document and understand the spatio-temporal dynamics of radiocaesium in the affected region and to aid the development and validation of models of radiocaesium dynamics in contaminated forests.

Vertical distributions of radiocesium in Japanese forest soils following the Fukushima Daiichi Nuclear Power Plant accident: A meta-analysis.

This study investigated the temporal change in vertical distributions of radiocesium inventories in Japanese forest soils during the early phase (from 2011 to 2017) following the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, using three simple parameters. We calculated the fraction in the organic layer (Fl/t), the migration center (Xc) and the relaxation depth (α) using 99 soil inventory data sets. Fl/t decreased significantly from 2011 to 2017 (logistic analysis, p < 0.001). In addition, Fl/t in the FDNPP zone rapidly decreased compared to that in the Chernobyl Nuclear Power Plant (ChNPP) zone from the first year to the second year. Different migration rates from organic to mineral soil layers between previous studies in the ChNPP and this study have several possible causes such as organic litter features, climate and physico-chemical forms of initial deposition. In mineral soil layers in the FDNPP zone, only Xc increased significantly with time according to generalized mixed model analysis (p < 0.01). However, Xc and α in the ChNPP zone decreased from two to five years after the accident in 1986, which shows a high 137Cs retention in the organic layer even in the fifth year after the accident. The vertical migration of 137Cs in the mineral soil layer in the FDNPP zone appears to be due to low input of 137Cs from organic to surface mineral soil layer after the second year. These results indicate that 137Cs retention capacity of the organic layer can affect the apparent vertical migration of 137Cs in the underlying mineral soil layer.

Temporal changes in the spatial patterns of air dose rate from 2012 to 2016 at forest floors in Fukushima, Japan.

This study investigates temporal changes in the distribution of air dose rates at forest floors from 2012 to 2016 by measuring air dose rates at a height of 10 cm. The study was conducted at four different topography forest sites in Fukushima Prefecture, Japan. At each forest site, the air dose rate was found to have decreased by 7%-22% over time from 2012 to 2016 owing to the movement of radiocesium from organic layers to mineral soil layers in the forest site. However, the spatial distribution patterns of air dose rates did not change at these forest sites over five years. Besides, high correlations between air dose rates and organic plus surface mineral soil inventories were found at these forest sites during most of study years. Therefore, little changes in the spatial distribution of air dose rates could be caused by radiocesium retention at the same location in these forest sites. No statistical correlation between air dose rates and slope gradients was found in the two hilly forest sites with steep slopes above 35°. Accordingly, this study shows that the distribution patterns of air dose rates in the forest floors remained stable depending on the spatial distribution of radiocesium, which formed in the early phase after the Fukushima Daiichi Nuclear Power Plant accident.

New predictions of 137Cs dynamics in forests after the Fukushima nuclear accident.

Most of the area contaminated by the Fukushima Daiichi Nuclear Power Plant accident is covered by forest. In this paper, we updated model predictions of temporal changes in the 137Cs dynamics using the latest observation data and newly provided maps of the predicted 137Cs activity concentration for wood, which is the most commercially important part of the tree body. Overall, the previous prediction and latest observation data were in very good agreement. However, further validation revealed that the migration from the soil surface organic layer to the mineral soil was overestimated for evergreen needleleaf forests. The new prediction of the 137Cs inventory showed that although the 137Cs distribution within forests differed among forest types in the first 5 years, the difference diminished in the later phase. Besides, the prediction of the wood 137Cs activity concentrations reproduced the different trends of the 137Cs activity concentrations for cedar, oak, and pine trees. Our simulation suggests that the changes of the wood 137Cs activity concentration over time will slow down after 5-10 years. Although the model uncertainty should be considered and monitoring and model updating must continue, the study provides helpful information on the 137Cs dynamics within forest ecosystems and the changes in wood contamination.

Six-year trends in exchangeable radiocesium in Fukushima forest soils.

We investigated the changes in 137Cs exchangeable fraction in the soils of contaminated forest ecosystems until 6 years after the Fukushima radioactive atmospheric deposits. For this investigation, we performed chemical extractions of 137Cs from both organic and mineral soil layer sampled from two forest stands, Japanese cedar (Cryptomeria japonica) and broadleaf deciduous, mainly konara oak (Quercus serrata), which are located 26-27 km inland from the Fukushima Dai-ichi Nuclear Power Plant. The exchangeable 137Cs as a proportion of the total 137Cs inventory was only 10% in the organic layer and 6.1% in the mineral soil layer about 5 months after the accident at the Japanese cedar site. We observed an exponential decrease in the proportion of exchangeable 137Cs in both organic and mineral soil layer samples over the 6-years observation period at both sites. The proportion significantly decreased within 2-4 years after the accident, becoming almost constant (2-4%). These results support the interpretation that contaminated forests have entered a steady-state phase of 137Cs cycling, although we need more integration for an improved vision of the future of Fukushima forests.

Effects of radiocesium fixation potentials on 137Cs retention in volcanic soil profiles of Fukushima forests.

Radiocesium is well-known to be stabilized by clay minerals in soils, while volcanic soils could typically be poor in micaceous clays that fix 137Cs effectively. We investigated 137Cs fixation potentials [radiocesium interception potential (RIP)] and depth distribution of 137Cs stocks in volcanic soils to analyze effects of clay content and mineralogy on soil retention and migration of 137Cs after the Fukushima nuclear accident. Clay minerals of the volcanic soils were dominated by hydroxy-interlayered vermiculite (HIV) and short-range-order minerals, irrespective of bedrocks. The soil RIPs were positively correlated with mass of clay fraction among the HIV-dominated volcanic soils, but RIP per clay content in the HIV-dominated volcanic soils were lower than in the soils rich in illite or vermiculitic clays. The small RIPs in the organic horizons resulted in rapid 137Cs migration from the organic horizons and their accumulation in the upper 0-5 cm mineral soil. Although RIPs of the studied volcanic soils fall within the lower class among major soil types, vertical 137Cs migration in the mineral soil is small unless RIP is less than 300-400 mmol kg-1 due to the low clay contents and shortage of illite or vermiculite.

Calibration of forest 137Cs cycling model "FoRothCs" via approximate Bayesian computation based on 6-year observations from plantation forests in Fukushima.

Predicting the environmental fate of 137Cs in forest ecosystems along with the concentrations of 137Cs in tree parts are important for the managements of radioactively contaminated forests. In this study, we calibrate the Forest RothC and Cs model (FoRothCs), a forest ecosystem 137Cs dynamics model, using observational data obtained over six years from four forest sites with different levels of 137Cs contamination from Fukushima Prefecture. To this end, we applied an approximate Bayesian computation (ABC) technique based on the observed 137Cs concentrations (Bq kg-1) of five compartments (leaf, branch, stem, litter, and soil) in a Japanese cedar plantation. The environmental decay (increment) constants of the five compartments were used as the summary statistics (i.e., the metric for model performance) to infer the five parameters related to 137Cs transfer processes in FoRothCs. The ABC technique successfully reconciled the model outputs with the observed trends in 137Cs concentrations at all sites during the study period. Furthermore, the estimated parameters are in agreement with the literature values (e.g., the root uptake rates of 137Cs). Our study demonstrates that model calibration with ABC based on the trends in 137Cs concentrations of multi compartments is useful for reducing the prediction uncertainty of 137Cs dynamics in forest ecosystems.

Temporal changes in the radiocesium distribution in forests over the five years after the Fukushima Daiichi Nuclear Power Plant accident.

To elucidate the temporal changes in the radiocesium distribution in forests contaminated by the Fukushima Daiichi Nuclear Power Plant accident, we monitored the 137Cs concentration and inventory within forests from 2011 to 2015 across nine plots containing variable tree species and different contamination levels. The 137Cs concentrations in needles and branches decreased exponentially at all coniferous plots, with effective ecological half-lives of 0.45-1.55 yr for needles and 0.83-1.69 yr for branches. By contrast, the 137Cs concentration in deciduous konara oak leaves did not change over the five years. The concentration of 137Cs in oak wood increased by 37-75%, whereas that in Japanese red pine decreased by 63% over the five years. In Japanese cedar and hinoki cypress, the 137Cs concentration in wood showed an increasing trend in half of the plots. The changes in 137Cs in the organic and mineral soil layers were not strongly related to the tree species or contamination level. Our multi-site, multi-species monitoring results revealed that the pattern of temporal changes in radiocesium in the 9 forest plots was similar overall; however, changes in 137Cs in needles/leaves and wood differed among tree species.

Stemflow-induced spatial heterogeneity of radiocesium concentrations and stocks in the soil of a broadleaved deciduous forest.

The transport of radiocesium from the canopy and quantification of the spatial distribution of radiocesium in the soil of konara oak forests are important to better understand the variability of 137Cs stocks in the soil between proximal and distal stem areas as well as fine-scale variations around the tree trunk. Moreover, a better understanding of fine-scale spatial variabilities of 137Cs concentrations and stocks will provide insights for optimizing soil sampling strategies to provide a more robust estimation of contamination at the stand scale. This study aims to elucidate the transport of 137Cs by stemflow in a radioactively contaminated konara oak forest in Tsukuba, Japan by describing and quantifying the fine-scale spatial distribution of 137Cs in the soil and preferential flowpaths of stemflow on the tree stem by a dye tracing experiment. 137Cs concentrations and stocks were higher in the soils of the proximal stem area than distal stem area when they corresponded with the preferential flowpaths of stemflow. There was a significant relationship between canopy projection area of individual trees and average soil 137Cs concentrations and stocks, even though canopies of the trees overlapped. Our results demonstrate that the spatiality of 137Cs concentrations and stocks in the soil of the proximal stem area are governed (at least partially) by the preferential flowpaths of stemflow along the tree trunk. In addition, higher 137Cs concentrations and stocks in the near-trunk soils of trees with larger crown areas might be caused by an enhanced ability to capture dry deposition.

Nitrate isotopic composition reveals nitrogen deposition and transformation dynamics along the canopy-soil continuum of a suburban forest in Japan.

RATIONALE: Heavy nitrogen (N) deposition often causes high nitrate (NO3(-)) accumulation in soils in temperate forested ecosystems. To clarify the sources and production pathways of this NO3(-), we investigated NO3(-) isotope signatures in deposition processes along the canopy-soil continuum of a suburban forest in Japan. METHODS: The stable isotopes of N and oxygen (O) were used to trace the source and transformation dynamics of nitrate (NO3(-)) in two forest stands: a plantation of Cryptomeria japonica (coniferous tree; CJ) and a natural secondary forest of Quercus acutissima (broadleaf, deciduous tree; QA). The NO3(-) and ammonium (NH4(+)) concentrations were measured, as well as the δ(15)N and δ(18)O values of NO3(-), in rainfall, throughfall, stem flow, litter layer water, and soil water (10, 30, and 70 cm depths). RESULTS: Seasonal variations were observed in the δ(15)N values of throughfall and stem flow NO3(-) at both sites, and in the δ(18)O values of throughfall and stem flow NO3(-) at the QA site. The range in the δ(18)O values of rainfall and throughfall NO3(-) was large (65-70‰) but decreased dramatically to 2-5‰ in soil water at both sites. At the QA site, the δ(18)O values of stem flow NO3(-) decreased to 40‰ during several rain events, especially in the growing season. CONCLUSIONS: NO3(-) from atmospheric deposition was replaced by microbially generated NO3(-) mainly in the organic horizon and surface portion of the mineral soil under excess N deposition in this suburban forest. Microbial activity, including both immobilization and nitrification in organic-rich horizons near the surface, contributed to incorporating atmospheric NO3(-) quickly into the internal microbial N cycle. We also found evidence of microbial nitrification in the canopy of the QA stand during the growing season.