Mechanisms of 137Cs leaching based on long-term observations in forested headwater catchments in Yamakiya, Fukushima Prefecture, Japan

Dissolved radiocesium (mainly 134Cs and 137Cs) is thought to be leached mainly from suspended sediment in downstream rivers, while organic matter, such as leaf litter, contributes to catchments in forested headwater streams. It is also known that dissolved 137Cs in headwater streams exhibit seasonal variation with water tem-perature. Some mechanisms have been proposed as the causes: ionic competition of potassium ion (K+) and ammonium ion (NH4+), leaching associated with the decomposition of organic matter, and thermodynamic adsorption-desorption processes. We investigated the relationship between K+ and the dissolved organic carbon (DOC) concentrations and seasonal changes in dissolved 137Cs concentration using a large number of samples from a headwater's small catchments. We examined temporal trends in 137Cs concentrations in coarse organic matter, suspended sediments, and dissolved forms at four sites (one decontaminated site and three undeconta-minated sites) in the Yamakiya area since 2011. The distribution coefficients (Kdcss and Kdorg) of dissolved 137Cs concentrations relative to suspended sediment and coarse organic matter 137Cs concentrations were calculated, and differences in temporal changes due to decontamination were investigated. In addition, we examined the relationship between water temperature and DOC, K+, NH4+ and 137Cs concentrations in the headwater catch-ments. The suspended sediment 137Cs concentrations at the decontaminated headwater site (IBO) decreased significantly after decontamination and remained low thereafter. In contrast, dissolved 137Cs concentrations decreased temporarily during the decontamination period, but returned to pre-decontamination levels. Almost no NH4+ has been detected in headwater streams in our catchments. In the SET and ISH watersheds, where the distance from the groundwater spring is short, a correlation was found between DOC concentration and dissolved 137Cs concentration. In contrast, in the IBO watershed, where the distance from the groundwater spring is long, temperature dependence and a good correlation between K+ and 137Cs were observed. Therefore, microbial decomposition of organic matter may have a significant effect on the seasonal variation of dissolved 137Cs in forested headwater streams at short distances from the spring, but the influence of competing ions is expected to increase gradually as the water flows downstream.