Micro- and nanochamber array system for single enzyme assays.

Arrays of small reaction containers, ranging from 624 femtoliters (10-15 L) to 270 attoliters (10-18 L), for capturing a single enzyme molecule and measuring the activity were developed along with a new reversible sealing system based on a pneumatic valve actuator made of polydimethylsiloxane (PDMS). The valve was actuated by PBS solution, effectively preventing evaporation of the solution from the micro- and nanochambers and allowing the assay to be performed over a long period of time. The hydrolysis rates of ß-D-galactosidase (ß-gal), kcat, were decreased according to the decrease of the chamber size, and the overall tendency seems to be symmetrically related to the specific surface area of the chambers even under the prevented condition of non-specific adsorption. The spatial localization of the protons in the chambers, which might could affect the dissociation state of the proteins, was also investigated to explain the decrease in the hydrolysis rate. The developed chamber system developed here may be useful for artificially reproducing the confined intracellular environment and molecular crowding conditions.

Simulation study on 3H behavior in the Fukushima coastal region: Comparison of influences of discharges from the Fukushima Daiichi and rivers.

The release of tritium (3H) to the ocean is planned on the coastal environment in the Fukushima coastal region from Spring or Summer of 2023. Before its release, we evaluate the effect of 3H discharges from the port of Fukushima Daiichi and rivers in the Fukushima coastal region using a three-dimensional hydrodynamic model (3D-Sea-SPEC). The simulation results showed that discharges from the port of Fukushima Daiichi dominantly affected the 3H concentrations in monitoring points within approximately 1 km. Moreover, the results indicate that the effect of riverine 3H discharge was limited around the river mouth under base flow conditions. However, its impact on the Fukushima coastal regions under storm flow conditions was found, and the 3H concentrations in seawater in the Fukushima coastal region were formed around 0.1 Bq/L (mean 3H concentrations in seawater in the Fukushima coastal region) in the near shore.

Accumulation mechanisms of radiocaesium within lichen thallus tissues determined by means of in situ microscale localisation observation.

Many lichens are well known to accumulate radiocaesium and, thus acting as biomonitors of contamination levels. However, the actual localisation and chemical forms of radiocaesium in contaminated lichens have not yet been elucidated because, despite their high radioactivity, these forms are present in trace amounts as chemical entities. Here, we use autoradiography and demonstrate for the first time in situ microscale localisation of radiocaesium within thallus tissues to investigate the radiocaesium forms and their accumulation mechanism. Radiocaesium distributions showed similar trends in lichen tissues collected two and six years after the Fukushima nuclear accident. The radiocaesium was localised in the brown pigmented parts i.e., melanin-like substances, in the lower cortex of lichen thallus. Quantum chemical calculations showed that functional group of melanin-like substances can chelate Cs+ ion, which indicates that the Cs+ ions form complexes with the substances. Based on these findings, we suggest that radiocaesium ions may be retained stably in melanin-like substances for long periods (two to six years) due to steric factors, such as those seen in porphyrin-like structures and via multimer formation in the lower cortex. In addition, electron microscopy and autoradiography were used to observe radiocaesium-bearing microparticles (CsMPs) on/in the upper cortex and around the medullary layer. Micron-sized particles appeared to adhere to the surface tissue of the thallus, as shown by electron microscopy, suggesting that the particles were trapped by development of an adhesive layer; that is, CsMPs were trapped both physically and physiologically. These findings provide information on in situ localisation of two chemical forms of radiocaesium, cations and particles, in lichen thallus tissues and their accumulation mechanisms.

A modeling approach to estimate 3H discharge from rivers: Comparison of discharge from the Fukushima Dai-ichi and inventory in seawater in the Fukushima coastal region.

Estimation of 3H discharge from river catchments is important to evaluate the effect of Fukushima Dai-ichi discharge and future planned 3H release to the ocean on the coastal environment. Using a previously developed model based on the tank model and observed 3H concentration in river water, the 3H discharge from the Abukuma River and 13 other rivers in the Fukushima coastal region were estimated from June 2013 to March 2020. The 3H discharge from catchments of the Abukuma River and 13 other rivers in the Fukushima coastal region during 2014-2019 were estimated to be 1.2-4.0 TBq/y. These values were approximately 2-22 times larger than the annual 3H discharge from the Fukushima Dai-ichi after 2016, indicating the significance of 3H discharge from the catchments through the rivers. This estimation is expected to be useful to evaluate and predict 3H concentrations and inventories in the Fukushima coastal region for consideration of planned 3H release to the ocean.

Radiocaesium accumulation capacity of epiphytic lichens and adjacent barks collected at the perimeter boundary site of the Fukushima Dai-ichi Nuclear Power Station.

We investigated the radiocaesium content of nine epiphytic foliose lichens species and the adjacent barks of Zelkova serrata (Ulmaceae, "Japanese elm") and Cerasus sp. (Rosaceae, "Cherry tree") at the boundary of the Fukushima Dai-ichi Nuclear Power Station six years after the accident in 2011. Caesium-137 activities per unit area (the 137Cs-inventory) were determined to compare radiocaesium retentions of lichens (65 specimens) and barks (44 specimens) under the same growth conditions. The 137Cs-inventory of lichens collected from Zelkova serrata and Cerasus sp. were respectively 7.9- and 3.8-times greater than the adjacent barks. Furthermore, we examined the radiocaesium distribution within these samples using autoradiography and on the surfaces with an electron probe micro analyzer (EPMA). Autoradiographic results showed strong local spotting and heterogeneous distributions of radioactivity in both the lichen and bark samples, although the intensities were lower in the barks. The electron microscopy analysis demonstrated that particulates with similar sizes and compositions were distributed on the surfaces of the samples. We therefore concluded that the lichens and barks could capture fine particles, including radiocaesium particles. In addition, radioactivity was distributed more towards the inwards of the lichen samples than the peripheries. This suggests that lichen can retain 137Cs that is chemically immobilised in particulates intracellularly, unlike bark.

Key factors controlling radiocesium sorption and fixation in river sediments around the Fukushima Daiichi Nuclear Power Plant. Part 1: Insights from sediment properties and radiocesium distributions.

In order to elucidate the radiocesium transport behaviors in natural environment, we systematically investigated sediments from the highly contaminated rivers of Ukedo and Odaka around the Fukushima Daiichi Nuclear Power Plant. We focused on determining the key factors controlling the radiocesium sorption and fixation, such as variations in the particle size, clay mineralogy, and organic matter (OM). The distribution patterns of the 137Cs concentration and particle size fractions were found to be similar for the two rivers, indicating that both clay and silt fractions contributed almost equally to the Cs sorption. The clay mineralogical composition evaluated using X-ray diffraction analysis showed that the relative contents of micaceous minerals were higher in the Ukedo River samples, whereas the relative contents of smectite and kaolinite were higher in the Odaka River samples. This implies that the sediments in both rivers were likely at different weathering stages due to the different geological settings in both catchments. The effects of OM on the sediment properties were also investigated by comparing the cation exchange capacity (CEC) and the radiocesium interception potential (RIP) of the two samples both with and without OM present. The CEC values were controlled by both the clay minerals and OM, and the RIP values increased significantly in the absence of OM. Such trends were correlated to the total organic carbon values, which may be used to understand the direct and indirect roles of OM in the sorption and fixation of Cs. These key differences in river sediment were attributed to the differences in the geological settings and weathering stages. These properties may contribute to the different sorption and fixation behaviors of radiocesium. In the second part paper, we further examined these behaviors and identified key factors by investigating their relationship to the sediment properties of both rivers.

Key factors controlling radiocesium sorption and fixation in river sediments around the Fukushima Daiichi Nuclear Power Plant. Part 2: Sorption and fixation behaviors and their relationship to sediment properties.

We systematically investigated the sorption and fixation behaviors of radiocesium (137Cs) for sediments taken from the rivers of Ukedo and Odaka around the Fukushima Daiichi Nuclear Power Plant. By comparing the Cs sorption and sequential desorption results at various Cs concentrations, across a range of sediment properties, we were able to understand the different contributions at frayed edge sites (FESs) and regular exchange sites (RESs) of the clay minerals, and their relationships with the Cs concentrations and the contents of organic matter (OM). The Cs sorption and fixation were dominated by FESs at trace Cs concentrations, and by ion exchange at RES and the collapse of interlayers at higher Cs concentrations. The Cs sorption at lower Cs concentration was strongly related to radiocesium interception potential (RIP); however, Cs fixation was more related to clay mineralogy (i.e. contents of mica, vermiculite and hydroxy-interlayered vermiculite) rather than the RIP. The first-order kinetic constants for time-dependent Cs sorption at low Cs concentrations were correlated negatively to the ratio between the total organic carbon and RIP values. This implies that Cs access to FESs requires a relatively long duration that is dependent on the contents of the OM. From these results, the sorption and fixation mechanisms were confirmed to be significantly different at different Cs concentrations. Then, the prediction of Cs transport should be based on the key mechanisms that are dominant at the actual trace levels of Cs. A significant difference between the Cs fixation behaviors at the Ukedo River and Odaka River may be understood by considering the differences in their clay mineralogy, due to the different geological settings and weathering stages of both catchments.

Mineral composition characteristics of radiocesium sorbed and transported sediments within the Tomioka river basin in Fukushima Prefecture.

The deposited radiocesium in the Fukushima river basin is transported in the river systems by soil particles and redistributed in the downstream areas. Although predicting the behaviors of minerals that adsorb radiocesium and of radiocesium dissolved in river water within the river systems is essential, the dominant mineral species that adsorb radiocesium have not yet been comprehensively identified. We identify herein such mineral species by investigating the 137Cs distribution and the mineral species in each size fraction that are found in the bedload sediments from an upstream reservoir to an estuary within the Tomioka river basin located east of Fukushima Prefecture in Japan. In the fine sand sediment, which is the dominant fraction in terms of the 137Cs quantity in the river bedload, the 137Cs concentrations of the felsic and mafic minerals are comparable to that of micas. The mafic minerals contain 62% of the 137Cs in the fine sand fraction in the upstream area, while the felsic minerals contain the highest quantities of 137Cs in the downstream area. These results suggest that the quantification of the mineral species and the 137Cs concentration of each size fraction are critically important in predicting the behaviors of the minerals and radiocesium within the Fukushima river basin in the future.

Specificity and Continuity of Schizophrenia and Bipolar Disorder: Relation to Biomarkers.

Schizophrenia and bipolar disorder overlap considerably in terms of symptoms, familial patterns, risk genes, outcome, and treatment response. This article provides an overview of the specificity and continuity of schizophrenia and mood disorders on the basis of biomarkers, such as genes, molecules, cells, circuits, physiology and clinical phenomenology. Overall, the discussions herein provided support for the view that schizophrenia, schizoaffective disorder and bipolar disorder are in the continuum of severity of impairment, with bipolar disorder closer to normality and schizophrenia at the most severe end. This approach is based on the concept that examining biomarkers in several modalities across these diseases from the dimensional perspective would be meaningful. These considerations are expected to help develop new treatments for unmet needs, such as cognitive dysfunction, in psychiatric conditions.

Temporal decrease in air dose rate in the sub-urban area affected by the Fukushima Dai-ichi Nuclear Power Plant accident during four years after decontamination works.

Trends of air dose rate decrease after decontamination works and factors which affect them constitute essential information for radiation protection, such as prediction of external exposure to the public and implementation of measures to reduce such exposure. This study investigated the decrease of air dose rate (ambient dose rate at 1 m above the ground) at 163 points across sub-urban areas in the evacuation zone around the Fukushima Dai-ichi Nuclear Power Plant over the period of four years following the decontamination works carried out in November 2012. The air dose rate on the asphalt pavement decreased faster than on soil surfaces. In addition, air dose rates near the forest decreased at a slower pace than in open fields. These results suggest that the air dose rate in urbanized areas can decrease faster than in other types of land, even after decontamination. Based on comparisons with decrease rates obtained in other studies, the air dose rate tends to decrease faster outside the evacuation zone than inside it. The decrease in air dose rate after decontamination was slower than before decontamination. The contribution of the weathering effect and human activity was estimated to be about 80% and 20% of the ecological decrease rate, respectively.

A Decision-Theoretic Model of Behavior Change.

Undesirable habitual or addictive behaviors are often difficult to change. The issue of "behavior change" has long been studied in various research fields. Several models for behavior change have converged to the hypothesis that attitudes, norms, and self-efficacy are important determinants of intentions and behavior. To improve the accuracy of behavior-change models, some researchers have tried to combine behavioral economics models with existing models for behavior change. However, these attempts have failed because the existing models [e.g., Theory of Planned Behavior (TPB)] are not consistent with Expected Utility Theory (EUT), which underlies various behavioral economics models. In the present paper, we clarify the corresponding components between existing models for behavior change and EUT, and propose a new model, the Decision-Theoretic Model of behavior change (DTM), which is a natural extension of ordinary EUT.

Dissolution behaviour of radiocaesium-bearing microparticles released from the Fukushima nuclear plant.

Radiocaesium-bearing microparticles (CsMPs) composed of silicate glass were released by the Fukushima Daiichi Nuclear Power Plant accident in March 2011. Since CsMPs contain a high concentration of radiocaesium, their dynamics and fate in the environment are urgent issues to be investigated. Here, we show that CsMPs are dissolved by weathering in the environment and that their radioactivity is more rapidly decreased by dissolution than the physical decay of radiocaesium. We conducted dissolution experiments with CsMPs in pure water that absorbed CO2 from the atmosphere and in artificial seawater at several temperatures. The dissolution progress was monitored by the decrease in the 137Cs radioactivity in CsMPs, and the dissolution rate was estimated. The activation energy for the dissolution of CsMPs was estimated to be 65 and 88 kJ/mol and the dissolution rate at 13 °C (approximate annual mean temperature in Fukushima City) was 0.014 and 0.140 µm/y for pure water and seawater, respectively, assuming that radiocaesium is uniformly distributed in spherical CsMPs. The shapes of the CsMPs dissolved in pure water were considerably altered, suggesting that the dissolution proceeded without maintaining the geometry. Tin oxide and iron oxide nanoparticulates formed on the surfaces. Such features were similar to those observed in CsMPs recently collected in Fukushima Prefecture, indicating that weathering dissolution of CsMPs is also occurring in the environment. For the CsMPs dissolved in seawater, a crust of secondary Mg- and Fe-rich minerals was formed, and the glass matrix inside the crust decreased, creating space between the crust and the glass matrix.

Inner structure and inclusions in radiocesium-bearing microparticles emitted in the Fukushima Daiichi Nuclear Power Plant accident.

Radiocesium-bearing microparticles (CsMPs), consisting substantially of silicate glass, were released to the environment during the Fukushima Daiichi Nuclear Power Plant accident in March 2011. Since the CsMPs were formed inside the damaged reactors during the accident, we investigate the inner structures of several CsMPs by transmission electron microscopy to understand the events within the reactors. Elemental mapping of the CsMPs shows a distinct radial distribution of Cs with a higher concentration near the surface of the CsMPs, implying that Cs was in a gaseous state in the reactor atmosphere and diffused into the glass matrix after formation of the glass particles. In some CsMPs, Zn and Fe also showed a similar radial distribution to Cs, suggesting that those elements may have diffused outward where Cs was abundant. In addition, submicron crystals were present as inclusions in several of the CsMPs and were identified as chromium spinels ((Fe2+,Zn)(Cr,Fe3+)2O4), acanthite (Ag2S), molybdenite (MoS2) and hessite (Ag2Te). The spinels contained ferrous iron (Fe2+), suggesting that the atmosphere inside the reactors was reductive to some extent. Also, boron was not detected in the glass matrix of the CsMPs despite using electron energy-loss spectroscopy, indicating that most of the control rods made of B4C might have created a eutectic alloy without vaporization. These detailed investigations of the inner structures in the CsMPs may offer information on the damaged reactors that are difficult to access because of the high radiation fields.

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.

Loss of radioactivity in radiocesium-bearing microparticles emitted from the Fukushima Dai-ichi nuclear power plant by heating.

Radiocesium-bearing microparticles (CsPs) substantially made of silicate glass are a novel form of radiocesium emitted from the broken containment vessel of Fukushima Dai-ichi nuclear power plant. CsPs have a potential risk of internal radiation exposure caused by inhalation. Radiation-contaminated waste including CsPs is being burned in incinerators; therefore, this study has investigated the responses of CsPs to heating in air. The radioactivity of CsPs gradually decreased from 600 °C and was almost lost when the temperature reached 1000 °C. The size and spherical morphology of CsPs were almost unchanged after heating, but cesium including radiocesium, potassium and chlorine were lost, probably diffused away from the CsPs. Iron, zinc and tin originally dissolved in the glass matrix were crystallized to oxide nanoparticles inside the CsPs. When the CsPs were heated together with weathered granitic soil that is common in Fukushima, the radiocesium released from CsPs was sorbed by the surrounding soil. From these results, it is expected that the radioactivity of CsPs will be lost when radiation-contaminated waste including CsPs is burned in incinerators.

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.

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.

Deposition of radiocesium on the river flood plains around Fukushima.

The environment in the area around Fukushima Daiichi Nuclear Power Plant has been contaminated by widely deposited significant amount of radioactive materials, which were released to the atmosphere caused by the Fukushima Daiichi Nuclear Power Plant accident due to the Great East Japan Earthquake, which occurred on March 11, 2011. The radiocesium released in the accident mainly affects radiation dose in the environment. Decontamination work in the contaminated area except a mountain forests has been conducted to decrease the radiation dose. However, there are concerns that the redistribution of this radiation due to water discharge will occur due to the resulting transport of radiocesium. In particular, the deposition of soil particles containing radiocesium on the flood plains in the downstream areas of Fukushima's rivers can potentially increase the local radiation dose. Therefore, it is important to understand the influence of the deposition behavior of radiocesium on the radiation dose. Investigations of rivers have been performed to enhance the understanding of the mechanisms by which radiocesium is deposited on these flood plains. It was found that the spatial distribution of the radiocesium concentration on the flood plain along the river is heterogeneous with a dependence on the depositional condition and that the number of points with high air dose rates is limited. In detail, the radiocesium concentration and air dose rates in flood channels are higher than those at the edges of the river channels. Based on these heterogeneity and hydrological events, the deposition and transport mechanisms of the radiocesium due to water discharge at rivers were also interpreted, and a conceptual model was constructed.

High-Density Dielectrophoretic Microwell Array for Detection, Capture, and Single-Cell Analysis of Rare Tumor Cells in Peripheral Blood.

Development of a reliable platform and workflow to detect and capture a small number of mutation-bearing circulating tumor cells (CTCs) from a blood sample is necessary for the development of noninvasive cancer diagnosis. In this preclinical study, we aimed to develop a capture system for molecular characterization of single CTCs based on high-density dielectrophoretic microwell array technology. Spike-in experiments using lung cancer cell lines were conducted. The microwell array was used to capture spiked cancer cells, and captured single cells were subjected to whole genome amplification followed by sequencing. A high detection rate (70.2%-90.0%) and excellent linear performance (R2 = 0.8189-0.9999) were noted between the observed and expected numbers of tumor cells. The detection rate was markedly higher than that obtained using the CellSearch system in a blinded manner, suggesting the superior sensitivity of our system in detecting EpCAM- tumor cells. Isolation of single captured tumor cells, followed by detection of EGFR mutations, was achieved using Sanger sequencing. Using a microwell array, we established an efficient and convenient platform for the capture and characterization of single CTCs. The results of a proof-of-principle preclinical study indicated that this platform has potential for the molecular characterization of captured CTCs from patients.

Radiocaesium activity concentrations in parmelioid lichens within a 60 km radius of the Fukushima Dai-ichi Nuclear Power Plant.

Radiocaesium activity concentrations ((134)Cs and (137)Cs) were measured in parmelioid lichens collected within the Fukushima Prefecture approximately 2 y after the Fukushima Dai-ichi Nuclear Power Plant accident. A total of 44 samples consisting of nine species were collected at 16 points within a 60 km radius of the Fukushima Dai-ichi Nuclear Power Plant. The activity concentration of (134)Cs ranged from 4.6 to 1000 kBq kg(-1) and for (137)Cs ranged from 7.6 to 1740 kBq kg(-1). A significant positive correlation was found between the (137)Cs activity concentration in lichens and the (137)Cs deposition density on soil (n = 44), based on the calculated Spearman's rank correlation coefficients as r = 0.90 (P < 0.01). The two dominant species, Flavoparmelia caperata (n = 12) and Parmotrema clavuliferum (n = 11), showed strong positive correlations, for which the r values were calculated as 0.92 (P < 0.01) and 0.90 (P < 0.01) respectively. Therefore, Flavoparmelia caperata and Parmotrema clavuliferum are suggested as biomonitoring species for levels of radiocaesium fallout within the Fukushima Prefecture.