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.

Numerical study of transport pathways of 137Cs from forests to freshwater fish living in mountain streams in Fukushima, Japan.

The accident at the Fukushima Dai-ichi Nuclear Power Plant in 2011 released a large quantity of radiocesium into the surrounding environment. Radiocesium concentrations in some freshwater fish caught in rivers in Fukushima Prefecture in October 2018 were still higher than the Japanese limit of 100 Bq kg-1 for general foodstuffs. To assess the uptake of 137Cs by freshwater fish living in mountain streams in Fukushima Prefecture, we developed a compartment model for the migration of 137Cs on the catchment scale from forests to river water. We modelled a generic forest catchment with Fukushima-like parameters to ascertain the importance of three export pathways of 137Cs from forests to river water for the uptake of 137Cs by freshwater fish. The pathways were direct litter fall into rivers, lateral inflow from the forest litter layer, and lateral transfer from the underlying forest soil. Simulation cases modelling only a single export pathway did not reproduce the actual trend of 137Cs concentrations in river water and freshwater fish in Fukushima Prefecture. Simulations allowing a combined effect of the three pathways reproduced the trends well. In the latter simulations, the decreasing trend of 137Cs in river water and freshwater fish was due to a combination of the decreasing trend in the forest leaves/needles and litter compartments, and the increasing trend in soil. The modelled 137Cs concentrations within the forest compartments were predicted to reach an equilibrium state at around ten years after the fallout due to the equilibration of 137Cs cycling in forests. The model suggests that long term 137Cs concentrations in freshwater fish in mountain streams will be controlled by the transfer of 137Cs to river water from forest organic soils.

Applicability of Kd for modelling dissolved 137Cs concentrations in Fukushima river water: Case study of the upstream Ota River.

A study is presented on the applicability of the distribution coefficient (Kd) absorption/desorption model to simulate dissolved 137Cs concentrations in Fukushima river water. The upstream Ota River basin was simulated using GEneral-purpose Terrestrial Fluid-flow Simulator (GETFLOWS) for the period 1 January 2014 to 31 December 2015. Good agreement was obtained between the simulations and observations on water and suspended sediment fluxes, and on particulate bound 137Cs concentrations under both base and high flow conditions. By contrast the measured concentrations of dissolved 137Cs in the river water were much harder to reproduce with the simulations. By tuning the Kd values for large particles, it was possible to reproduce the mean dissolved 137Cs concentrations during base flow periods (observation: 0.32 Bq/L, simulation: 0.36 Bq/L). However neither the seasonal variability in the base flow dissolved 137Cs concentrations (0.14-0.53 Bq/L), nor the peaks in concentration that occurred during storms (0.18-0.88 Bq/L, mean: 0.55 Bq/L), could be reproduced with realistic simulation parameters. These discrepancies may be explained by microbial action and leaching from organic matter in forest litter providing an additional input of dissolved 137Cs to rivers, particularly over summer, and limitations of the Kd absorption/desorption model. It is recommended that future studies investigate these issues in order to improve simulations of dissolved 137Cs concentrations in Fukushima rivers.

Simulation study of the effects of buildings, trees and paved surfaces on ambient dose equivalent rates outdoors at three suburban sites near Fukushima Dai-ichi.

The influence of buildings, trees and paved surfaces on outdoor ambient dose equivalent rates (H˙∗(10)) in suburban areas near to the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) was investigated with Monte Carlo simulations. Simulation models of three un-decontaminated sites in Okuma and Tomioka were created with representations of individual buildings, trees and roads created using geographic information system (GIS) data. The 134Cs and 137Cs radioactivity distribution within each model was set using in-situ gamma spectroscopy measurements from December 2014 and literature values for the relative radioactive cesium concentration on paved surfaces, unpaved land, building outer surfaces, forest litter and soil layers, and different tree compartments. Reasonable correlation was obtained between the simulations and measurements for H˙∗(10) across the sites taken in January 2015. The effect of buildings and trees on H˙∗(10) was investigated by performing simulations removing these objects, and their associated 134Cs and 137Cs inventory, from the models. H˙∗(10) were on average 5.0% higher in the simulations without buildings and trees, even though the total 134Cs and 137Cs inventory within each model was slightly lower. The simulations without buildings and trees were then modified to include 134Cs and 137Cs in the ground beneath locations where buildings exist in reality, and the inventory of paved surfaces modelled as if they had high retention of 134Cs and 137Cs fallout like soil areas. H˙∗(10) increased more markedly in these cases than when considering the shielding effect of buildings and trees alone. These results help clarify the magnitude of the effect of buildings, trees and paved surfaces on H˙∗(10) at the un-decontaminated sites within Fukushima Prefecture.

Applicability of Kd for modelling dissolved 137Cs concentrations in Fukushima river water: Case study of the upstream Ota River.

A study is presented on the applicability of the distribution coefficient (Kd) absorption/desorption model to simulate dissolved 137Cs concentrations in Fukushima river water. The upstream Ota River basin was simulated using GEneral-purpose Terrestrial Fluid-flow Simulator (GETFLOWS) for the period 1 January 2014 to 31 December 2015. Good agreement was obtained between the simulations and observations on water and suspended sediment fluxes, and on particulate bound 137Cs concentrations under both base and high flow conditions. By contrast the measured concentrations of dissolved 137Cs in the river water were much harder to reproduce with the simulations. By tuning the Kd values for large particles, it was possible to reproduce the mean dissolved 137Cs concentrations during base flow periods (observation: 0.32 Bq/L, simulation: 0.36 Bq/L). However neither the seasonal variability in the base flow dissolved 137Cs concentrations (0.14-0.53 Bq/L), nor the peaks in concentration that occurred during storms (0.18-0.88 Bq/L, mean: 0.55 Bq/L), could be reproduced with realistic simulation parameters. These discrepancies may be explained by microbial action and leaching from organic matter in forest litter providing an additional input of dissolved 137Cs to rivers, particularly over summer, and limitations of the Kd absorption/desorption model. It is recommended that future studies investigate these issues in order to improve simulations of dissolved 137Cs concentrations in Fukushima rivers.

Evaluation of sediment and 137Cs redistribution in the Oginosawa River catchment near the Fukushima Dai-ichi Nuclear Power Plant using integrated watershed modeling.

The Oginosawa River catchment lies 15 km south-west of the Fukushima Dai-ichi nuclear plant and covers 7.7 km2. Parts of the catchment were decontaminated between fall 2012 and March 2014 in preparation for the return of the evacuated population. The General-purpose Terrestrial Fluid-flow Simulator (GETFLOWS) code was used to study sediment and 137Cs redistribution within the catchment, including the effect of decontamination on redistribution. Fine resolution grid cells were used to model local features of the catchment, such as paddy fields adjacent to the Oginosawa River. The simulation was verified using monitoring data for river water discharge rates (r = 0.92), suspended sediment concentrations, and particulate 137Cs concentrations (r = 0.40). Cesium-137 input to watercourses came predominantly from land adjacent to river channels and forest gullies, e.g. the paddy fields in the Ogi and Kainosaka districts, as the ground in these areas saturates during heavy rain and is easily eroded. A discrepancy between the simulation and monitoring results on the sediment discharge rate following decontamination may be explained by fast erosion occurring after decontamination. Forested areas far from the channels only made a minor contribution to 137Cs input to watercourses, total erosion of between 0.001 and 0.1 mm from May 2011 to December 2015, as ground saturation is infrequent in these areas. The 2.3-6.9% y-1 decrease in the amount of 137Cs in forest topsoil over the study period can be explained by radioactive decay (approximately 2.3% y-1), along with a migration downwards into subsoil and a small amount of export. The amount of 137Cs available for release from land adjacent to rivers is expected to be lower in future than compared to this study period, as the simulations indicate a high depletion of inventory from these areas by the end of 2015. However continued monitoring of 137Cs concentrations in river water over future years is advised, as recultivation of paddy fields by returnees may again lead to fast erosion rates and release of the remaining inventory.

Using two detectors concurrently to monitor ambient dose equivalent rates in vehicle surveys of radiocesium contaminated land.

In response to the accident at Tokyo Electric Power Company's Fukushima Dai-ichi Nuclear Power Plant (FDNPP), vehicle-borne monitoring was used to map radiation levels for radiological protection of the public. By convention measurements from vehicle-borne surveys are converted to the ambient dose equivalent rate at 1 m height in the absence of the vehicle. This allows for comparison with results from other types of survey, including surveys with hand-held or airborne instruments. To improve the accuracy of the converted results from vehicle-borne surveys, we investigated combining measurements from two detectors mounted on the vehicle at different heights above the ground. A dual-detector setup was added to a JAEA monitoring car and compared against hand-held survey meter measurements in Fukushima Prefecture. The results obtained by combining measurements from two detectors were within ±20% of the hand-held reference measurements. The mean absolute percentage deviation from the reference measurements was 7.2%. The combined results from the two detectors were more accurate than those from either the roof-mounted detector, or the detector inside the vehicle, taken alone. One issue with vehicle-borne surveys is that ambient dose equivalent rates above roads are not necessarily representative of adjacent areas. This is because radiocesium is often deficient on asphalt surfaces, as it is easily scrubbed off by rain, wind and vehicle tires. To tackle this issue, we investigated mounting heights for vehicle-borne detectors using Monte Carlo gamma-ray simulations. When radiocesium is deficient on a road compared to the adjacent land, mounting detectors high on vehicles yields results closer to the values adjacent to the road. The ratio of ambient dose equivalent rates reported by detectors mounted at different heights in a dual-detector setup indicates whether radiocesium is deficient on the road compared to the adjacent land.

Coupling the advection-dispersion equation with fully kinetic reversible/irreversible sorption terms to model radiocesium soil profiles in Fukushima Prefecture.

Radiocesium is an important environmental contaminant in fallout from nuclear reactor accidents and atomic weapons testing. A modified Diffusion-Sorption-Fixation (mDSF) model, based on the advection-dispersion equation, is proposed to describe the vertical migration of radiocesium in soils following fallout. The model introduces kinetics for the reversible binding of radiocesium. We test the model by comparing its results to depth profiles measured in Fukushima Prefecture, Japan, since 2011. The results from the mDSF model are a better fit to the measurement data (as quantified by R2) than results from a simple diffusion model and the original DSF model. The introduction of reversible sorption kinetics means that the exponential-shape depth distribution can be reproduced immediately following fallout. The initial relaxation mass depth of the distribution is determined by the diffusion length, which depends on the distribution coefficient, sorption rate and dispersion coefficient. The mDSF model captures the long tails of the radiocesium distribution at large depths, which are caused by different rates for kinetic sorption and desorption. The mDSF model indicates that depth distributions displaying a peak in activity below the surface are possible for soils with high organic matter content at the surface. The mDSF equations thus offers a physical basis for various types of radiocesium depth profiles observed in contaminated environments.

Characteristics of radio-cesium transport and discharge between different basins near to the Fukushima Dai-ichi Nuclear Power Plant after heavy rainfall events.

This paper describes watershed modeling of catchments surrounding the Fukushima Dai-ichi Nuclear Power Plant to understand radio-cesium redistribution by water flows and sediment transport. We extended our previously developed three-dimensional hydrogeological model of the catchments to calculate the migration of radio-cesium in both sediment-sorbed and dissolved forms. The simulations cover the entirety of 2013, including nine heavy rainfall events, as well as Typhoon Roke in September 2011. Typhoons Man-yi and Wipha were the strongest typhoons in 2013 and had the largest bearing on radio-cesium redistribution. The simulated 137Cs discharge quantities over the nine events in 2013 are in good agreement with field monitoring observations. Deposition mainly occurs on flood plains and points where the river beds broaden in the lower basins, and within dam reservoirs along the rivers. Differences in 137Cs discharge ratios between the five basins are explained by differences in the initial fallout distribution within the basins, the presence of dam reservoirs, and the input supply to watercourses. It is possible to use these simulation results to evaluate future radioactive material distributions in order to support remediation planning.

Effect of Remediation Parameters on in-Air Ambient Dose Equivalent Rates When Remediating Open Sites with Radiocesium-contaminated Soil.

Calculations are reported for ambient dose equivalent rates [H˙*(10)] at 1 m height above the ground surface before and after remediating radiocesium-contaminated soil at wide and open sites. The results establish how the change in H˙*(10) upon remediation depends on the initial depth distribution of radiocesium within the ground, on the size of the remediated area, and on the mass per unit area of remediated soil. The remediation strategies considered were topsoil removal (with and without recovering with a clean soil layer), interchanging a topsoil layer with a subsoil layer, and in situ mixing of the topsoil. The results show the ratio of the radiocesium components of H˙*(10) post-remediation relative to their initial values (residual dose factors). It is possible to use the residual dose factors to gauge absolute changes in H˙*(10) upon remediation. The dependency of the residual dose factors on the number of years elapsed after fallout deposition is analyzed when remediation parameters remain fixed and radiocesium undergoes typical downward migration within the soil column.

Numerical study of sediment and 137Cs discharge out of reservoirs during various scale rainfall events.

Contamination of reservoirs with radiocesium is one of the main concerns in Fukushima Prefecture, Japan. We performed simulations using the three-dimensional finite volume code FLESCOT to understand sediment and radiocesium transport in generic models of reservoirs with parameters similar to those in Fukushima Prefecture. The simulations model turbulent water flows, transport of sediments with different grain sizes, and radiocesium migration both in dissolved and particulate forms. To demonstrate the validity of the modeling approach for the Fukushima environment, we performed a test simulation of the Ogaki Dam reservoir over Typhoon Man-yi in September 2013 and compared the results with field measurements. We simulated a set of generic model reservoirs systematically varying features such as flood intensity, reservoir volume and the radiocesium distribution coefficient. The results ascertain how these features affect the amount of sediment or 137Cs discharge downstream from the reservoirs, and the forms in which 137Cs is discharged. Silt carries the majority of the radiocesium in the larger flood events, while the clay-sorbed followed by dissolved forms are dominant in smaller events. The results can be used to derive indicative values of discharges from Fukushima reservoirs under arbitrary flood events. For example the generic model simulations indicate that about 30% of radiocesium that entered the Ogaki Dam reservoir over the flood in September 2015 caused by Typhoon Etau discharged downstream. Continued monitoring and numerical predictions are necessary to quantify future radiocesium migration in Fukushima Prefecture and evaluate possible countermeasures since reservoirs can be a sink of radiocesium.

Evaluation of ambient dose equivalent rates influenced by vertical and horizontal distribution of radioactive cesium in soil in Fukushima Prefecture.

The air dose rate in an environment contaminated with (134)Cs and (137)Cs depends on the amount, depth profile and horizontal distribution of these contaminants within the ground. This paper introduces and verifies a tool that models these variables and calculates ambient dose equivalent rates at 1 m above the ground. Good correlation is found between predicted dose rates and dose rates measured with survey meters in Fukushima Prefecture in areas contaminated with radiocesium from the Fukushima Dai-ichi Nuclear Power Plant accident. This finding is insensitive to the choice for modeling the activity depth distribution in the ground using activity measurements of collected soil layers, or by using exponential and hyperbolic secant fits to the measurement data. Better predictions are obtained by modeling the horizontal distribution of radioactive cesium across an area if multiple soil samples are available, as opposed to assuming a spatially homogeneous contamination distribution. Reductions seen in air dose rates above flat, undisturbed fields in Fukushima Prefecture are consistent with decrement by radioactive decay and downward migration of cesium into soil. Analysis of remediation strategies for farmland soils confirmed that topsoil removal and interchanging a topsoil layer with a subsoil layer result in similar reductions in the air dose rate. These two strategies are more effective than reverse tillage to invert and mix the topsoil.

Comment on 'Update of (40)K and (226)Ra and (232)Th series γ-to-dose conversion factors for soil'.

A comment on the recent Journal of Environmental Radioactivity article titled 'Update of (40)K and (226)Ra and (232)Th series γ-to-dose conversion factors for soil'.

Investigating isomorphs with the topological cluster classification.

Isomorphs are lines in the density-temperature plane of certain "strongly correlating" or "Roskilde simple" liquids where two-point structure and dynamics have been shown to be close to identical up to a scale transformation. Here we consider such a liquid, a Lennard-Jones glass former, and investigate the behavior along isomorphs of higher-order structural and dynamical correlations. We then consider an inverse power law reference system mapped to the Lennard-Jones system [Pedersen et al., Phys. Rev. Lett. 105, 157801 (2010)]. Using the topological cluster classification to identify higher-order structures, in both systems we find bicapped square antiprisms, which are known to be a locally favored structure in the Lennard-Jones glass former. The population of these locally favored structures is up to 80% higher in the Lennard-Jones system than the equivalent inverse power law system. The structural relaxation time of the two systems, on the other hand, is almost identical, and the four-point dynamical susceptibility is marginally higher in the inverse power law system. Upon cooling, the lifetime of the locally favored structures in the Lennard-Jones system is up to 40% higher relative to the reference system.

Identification of structure in condensed matter with the topological cluster classification.

We describe the topological cluster classification (TCC) algorithm. The TCC detects local structures with bond topologies similar to isolated clusters which minimise the potential energy for a number of monatomic and binary simple liquids with m ≤ 13 particles. We detail a modified Voronoi bond detection method that optimizes the cluster detection. The method to identify each cluster is outlined, and a test example of Lennard-Jones liquid and crystal phases is considered and critically examined.

Novel kinetic trapping in charged colloidal clusters due to self-induced surface charge organization.

Colloidal clusters are an unusual state of matter where tunable interactions enable a sufficient reduction in their degrees of freedom that their energy landscapes can become tractable - they form a playground for statistical mechanics and promise unprecedented control of structure on the submicron lengthscale. We study colloidal clusters in a system where a short-ranged polymer-induced attraction drives clustering, while a weak, long-ranged electrostatic repulsion prevents extensive aggregation. We compare experimental yields of cluster structures with theory which assumes simple addition of competing isotropic interactions between the colloids. Here we show that for clusters of size 4 ≤ m ≤ 7, the yield of minimum energy clusters is much less than expected. We attribute this to an anisotropic self-organized surface charge distribution which leads to unexpected kinetic trapping. We introduce a model for the coupling between counterions and binding sites on the colloid surface with which we interpret our findings.

Identification of long-lived clusters and their link to slow dynamics in a model glass former.

We study the relationship between local structural ordering and dynamical heterogeneities in a model glass-forming liquid, the Wahnström mixture. A novel cluster-based approach is used to detect local energy minimum polyhedral clusters and local crystalline environments. A structure-specific time correlation function is then devised to determine their temporal stability. For our system, the lifetime correlation function for icosahedral clusters decays far slower than for those of similarly sized but topologically distinct clusters. Upon cooling, the icosahedra form domains of increasing size and their lifetime increases with the size of the domains. Furthermore, these long-lived domains lower the mobility of neighboring particles. These structured domains show correlations with the slow regions of the dynamical heterogeneities that form on cooling towards the glass transition. Although icosahedral clusters with a particular composition and arrangement of large and small particles are structural elements of the crystal, we find that most icosahedral clusters lack such order in composition and arrangement and thus local crystalline ordering makes only a limited contribution to this process. Finally, we characterize the spatial correlation of the domains of icosahedra by two structural correlation lengths and compare them with the four-point dynamic correlation length. All the length scales increase upon cooling, but in different ways.

Lifetimes and lengthscales of structural motifs in a model glassformer.

We use a newly-developed method to identify local structural motifs in a popular model glassformer, the Kob-Andersen binary Lennard-Jones mixture. By measuring the lifetimes of a zoo of clusters, we find that 11-membered bicapped square antiprisms, denoted as 11A, have longer lifetimes on average than other structures considered. Other long-lived clusters are similar in structure to the 11A cluster. These clusters group into ramified networks that are correlated with slow particles and act to retard the motion of neighbouring particles. The structural lengthscale associated with these networks does not grow as fast as the dynamical lengthscale xi(4) as the system is cooled, in the range of temperatures our molecular dynamics simulations access. Thus we find a strong, but indirect, correlation between static structural ordering and slow dynamics.

The role of quench rate in colloidal gels.

Interactions between colloidal particles have hitherto usually been fixed by the suspension composition. Recent experimental developments now enable the control of interactions in situ. Here we use Brownian dynamics simulations to investigate the effect of controlling interactions upon gelation, by "quenching" the system from an equilibrium fluid to a gel. We find that, contrary to the normal case of an instantaneous quench, where the local structure of the gel is highly disordered, controlled quenching results in a gel with a much higher degree of local order. Under sufficiently slow quenching, local crystallisation is found, which is strongly enhanced when a monodisperse system is used. The higher the degree of local order, the smaller the mean squared displacement, indicating an enhancement of gel stability.

First-order phase transition in a model glass former: coupling of local structure and dynamics.

Recently, numerical evidence for a dynamical first-order phase transition in trajectory space [L.O. Hedges et al., Science 323, 1309 (2009)] has been found. In a model glass former in which clusters of 11 particles form upon cooling, we find that the transition has both dynamical and structural character. It occurs between an active phase with a high fraction of mobile and low fraction of cluster particles, and an inactive phase with few mobile but many cluster particles. The transition can be driven both dynamically and structurally with a chemical potential, showing that local order forms a mechanism for dynamical arrest.