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Forests are important sources of dissolved radiocesium ( 137 Cs) discharge downstream. To improve understanding of dissolved 137 Cs discharge processes during rainstorms, we investigated the relationship between rainfall-runoff hydrological processes and the discharge of 137 Cs leached from litter. Leaching tests were conducted with broadleaf litter collected in the area where saturated overland flow was generated during rainstorms in a broadleaf-tree-dominated forest. According to the leaching test results, the 137 Cs leaching rate was higher in the early stage of the test and decreased afterward. There was no significant difference in the overall results between the agitation and non-agitation cases. The 137 Cs leaching rate from litter after the 24-h test was up to 33.7%. A large proportion of the original 137 Cs activity was present even after the tests, as leaching from litter during rainstorms in the headwater area could be an additional source of dissolved 137 Cs in the stream water. If mixing of 137 Cs originating from groundwater, soil water, and rainfall with the hydrological processes is assumed, differences between the observed and estimated 137 Cs in the surface runoff water became larger under high flow conditions. This analysis indicates additional 137 Cs loading on surface runoff water during rainstorms, where saturated surface area can expand as the surface runoff rate increases. Contact area between surface runoff and litter accumulated on the forest floor should increase and accelerate 137 Cs leaching from the litter. Therefore, 137 Cs leaching in the saturated surface area that is temporarily formed during rainstorms can play a principal role in dissolved 137 Cs discharge during rainfall-runoff events. Contaminated litter in the temporally saturated region of forested headwaters is an important factor contributing to elevated levels of dissolved 137 Cs during rainstorms in the Fukushima area., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Since headwater catchments are the source areas of 137 Cs for downstream river systems, 137 Cs discharge from headwater areas needs to be evaluated. Dissolved form (Dissolved), coarse organic matter (Org), and suspended sediments (SS) were sampled and 137 Cs concentrations were measured from June 2011 to November 2016 in four headwater catchments in Yamakiya District, located 35 km northwest of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP). The data up to September 2013 (2.5 y after the accident) have been already published (Iwagami et al., 2017a, b). The data up to November 2016 (5.7 y after the accident) are newly reported in the present paper together with data at a new sampling site. The whole data from June 2011 to November 2016 is discussed. The normalized 137 Cs concentrations ( 137 Cs concentrations normalized by the average deposition density of each catchment) in Dissolved, Org, and SS were in the order of 10 -6  m 2 /L, 10 -2  m 2 /kg, and 10 -1  m 2 /kg, respectively, before 2013 and declined to around 10 -8  m 2 /L, 10 -4  m 2 /kg, and 10 -2  m 2 /kg, respectively, in 2016. As a result of the decontamination program, the discharge of SS increased, whereas 137 Cs concentrations in SS declined significantly and the total flux of 137 Cs decreased. Although the clear effect of land use on decline trend in normalized 137 Cs concentrations in Dissolved was not found, more data are necessary for elucidating the relation between them., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Radionuclide contamination of groundwater causes critical impacts on water resources, human lives, and ecosystems. The intrusion of radionuclides into the groundwater flow system in Fukushima, Japan, could be illuminated by determining groundwater age and mixing processes. To do this, periodical field surveys were conducted in catchments contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident. Sampling began in May 2011, which was 2 months after the disaster, and continued through June 2012. Chlorofluorocarbon (CFCs), tritium, and oxygen and hydrogen stable isotopes were used as environmental tracers. The observed tritium concentrations suggested that the water contained accident-derived radionuclides that exceeded the natural background baseline. Groundwater ages in the selected two headwater catchments were estimated to be between 10 and 26 years by combined use of multiple CFCs concentrations. In addition, the governing groundwater flow system was mostly approximated by a piston flow model; however, modern water fraction was also suggested based on the relationship between CFC-11 and CFC-12. The estimated water age and isotopic signals among stream water, spring water, and groundwater revealed that the intrusion of radionuclides into the groundwater was caused by the mixing between groundwater and modern water sources such as soil water and precipitation with relatively high radionuclide concentrations. This mixing was facilitated by a weathered and fractured granite bedrock and a thin unsaturated subsurface layer in the study area. Continued long-term monitoring of radionuclides in the groundwater will be necessary for water resources management in the future. CAPSULE: Radionuclide intrusion into the groundwater is related to the mixing between radionuclide-poor groundwater and modern water with relatively high radionuclide concentration., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Radiocesium ( 137 Cs) migration from headwater forested areas to downstream rivers has been investigated in many studies since the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, which was triggered by a catastrophic earthquake and tsunami on 11 March 2011. The accident resulted in the release of a huge amount of radioactivity and its subsequent deposition in the environment. A large part of the radiocesium released has been shown to remain in the forest. The dissolved 137 Cs concentration and its temporal dynamics in river water, stream water, and groundwater have been reported, but reports of dissolved 137 Cs concentration in soil water remain sparse. In this study, soil water was sampled, and the dissolved 137 Cs concentrations were measured at five locations with different land-use types (mature/young cedar forest, broadleaf forest, meadow land, and pasture land) in Yamakiya District, located 35 km northwest of FDNPP from July 2011 to October 2012. Soil water samples were collected by suction lysimeters installed at three different depths at each site. Dissolved 137 Cs concentrations were analyzed using a germanium gamma ray detector. The dissolved 137 Cs concentrations in soil water were high, with a maximum value of 2.5 Bq/L in July 2011, and declined to less than 0.32 Bq/L by 2012. The declining trend of dissolved 137 Cs concentrations in soil water was fitted to a two-component exponential model. The rate of decline in dissolved 137 Cs concentrations in soil water (k 1 ) showed a good correlation with the radiocesium interception potential (RIP) of topsoil (0-5 cm) at the same site. Accounting for the difference of 137 Cs deposition density, we found that normalized dissolved 137 Cs concentrations of soil water in forest (mature/young cedar forest and broadleaf forest) were higher than those in grassland (meadow land and pasture land)., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

The concentration of dissolved 137 Cs in groundwater and stream water in the headwater catchments in Yamakiya district, located ∼35 km north west of Fukushima Dai-ichi Nuclear Power Plant (FDNPP), was monitored from June 2011 to July 2013, after the earthquake and tsunami disaster. Groundwater and stream water were sampled at intervals of approximately 2 months at each site. Intensive sampling was also conducted during rainstorm events. Compared with previous data from the Chernobyl NPP accident, the concentration of dissolved 137 Cs in stream water was low. In the Iboishi-yama catchment, a trend was observed for the concentration of dissolved 137 Cs in stream water to decline, which could be divided into two phases by October 2011 (a fast flush of activity as a result of rapid washoff and a slow decline as a result of soil fixation and redistribution processes). The highest 137 Cs concentration recorded at Iboishi-yama was 1.2 Bq/L on August 6, 2011, which then declined to 0.021-0.049 Bq/L during 2013 (in stream water under normal water-flow conditions). During the rainfall events, the concentration of dissolved 137 Cs in stream water increased temporarily. The concentration of dissolved 137 Cs in groundwater at a depth of 30 m at Iboishi-yama displayed a decreasing trend from 2011 to 2013, with a range from 0.039 Bq/L to 0.0025 Bq/L. The effective half-lives of stream water in the initial fast flush and secondary phases were 0.10-0.21 and 0.69-1.5 y, respectively in the three catchments. The effective half-life of groundwater was 0.46-0.58 y at Koutaishi-yama and 0.50-3.3 y at Iboishi-yama. The trend for the concentration of dissolved 137 Cs to decline in groundwater and stream water was similar throughout 2012-2013, and the concentrations recorded in deeper groundwater were closer to those in stream water. The declining trend of dissolved 137 Cs concentrations in stream water was similar to that of the loss of canopy 137 Cs by throughfall, as shown in other reports of forest sites in the Yamakiya district., (Copyright © 2016. Published by Elsevier Ltd.)

Radiocesium ( 137 Cs) migration from headwaters in forested areas provides important information, as the output from forest streams subsequently enters various land-use areas and downstream rivers. Thus, it is important to determine the composition of 137 Cs fluxes (dissolved fraction, suspended sediment, or coarse organic matter) that migrate through a headwater stream. In this study, the 137 Cs discharge by suspended sediment and coarse organic matter from a forest headwater catchment was monitored. The 137 Cs concentrations in suspended sediment and coarse organic matter, such as leaves and branches, and the amounts of suspended sediment and coarse organic matter were measured at stream sites in three headwater catchments in Yamakiya District, located ∼35 km northwest of Fukushima Dai-ichi Nuclear Power Plant (FDNPP) from August 2012 to September 2013, following the earthquake and tsunami disaster. Suspended sediment and coarse organic matter were sampled at intervals of approximately 1-2 months. The 137 Cs concentrations of suspended sediment and coarse organic matter were 2.4-49 kBq/kg and 0.85-14 kBq/kg, respectively. The 137 Cs concentrations of the suspended sediment were closely correlated with the average deposition density of the catchment. The annual proportions of contribution of 137 Cs discharge by suspended sediment, coarse organic matter, and dissolved fraction were 96-99%, 0.0092-0.069%, and 0.73-3.7%, respectively. The total annual 137 Cs discharge from the catchment was 0.02-0.3% of the deposition., (Copyright © 2016 Elsevier Ltd. All rights reserved.)