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.

Chemical sequential extraction of O horizon samples from Fukushima forests: Assessment for degradability and radiocesium retention capacity of organic matters.

To investigate how radiocesium (137Cs) is retained in the O horizon via interactions with organic matter, we collected O horizon samples in Japanese cedar (Cryptomeria japonica) and konara oak (Quercus serrata) forest sites in Fukushima during the 8 years following the Fukushima Dai-ichi Nuclear Power Plant accident. To assess degradability and 137Cs retention capacity of organic matter, we conducted chemical sequential extraction with organic solvent and sulfuric acid, collecting the following fractions: organic solvent extractives (Fraction 1), acid-soluble carbohydrates (Fraction 3), and acid-insoluble residue (Fraction 4). In all samples, across sampling years and sites, 137Cs content in Fractions 1, 3, and 4, as a proportion of the total 137Cs content, was 0.0-23.6%, 18.4-42.9%, and 44.8-76.0%, respectively. Generally, 137Cs is considered to be electrostatically bound to organic matter and relatively mobile, making it easily extractable by sulfuric acid treatment. However, we observed a relatively high proportion of 137Cs in Fraction 4, suggesting strong retention of 137Cs and their immobility in the O horizon. Complex organic matter such as lignin or tannin may contribute this retention. We also noted that some part of 137Cs may be also retained by clay minerals in the O horizon. Although organic matter in Fractions 1 and 3 is considered to decompose faster than that in Fraction 4, over the observation period the 137Cs proportion and net rate of decrease in 137Cs content (in total and in each fraction) remained nearly constant. This result implies that decomposition of organic matter and the consequent release of bound 137Cs may be partly compensated by additional input of 137Cs from the canopy and 137Cs recycling by soil microorganisms. Our study highlights the potential role of organic matter in the O horizon as a temporary reservoir of 137Cs and a driver of the 137Cs cycle in forest ecosystems.

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.