Cloudwater Deposition Process of Radionuclides Based on Water Droplets Retrieved from Pollen Sensor Data.

Radionuclides released during the Fukushima Daiichi nuclear accident caused altitude-dependent surface contamination in the mountainous areas of Japan. To explore the possible cloudwater deposition that formed a distinctive contamination profile, data from pollen sensors deployed nationwide were analyzed. Utilizing the polarization of scattered light, Cedar pollen and water droplets were distinguished. On March 15, when surface contamination was simulated in previous studies, dense clouds with high droplet number concentrations were observed outside the 137Cs surface deposition areas, indicating that the sensor sites were immersed amid cloud layers. In contrast, cloud droplets with moderate number concentrations were measured at altitudes of approximately 570-840 m, which overlapped with the surface contamination areas. Considering the existing knowledge on vertical gradients of cloudwater composition, these suggest that contaminated cloud droplets were localized near the cloud base where a moderate number concentration of cloud droplets was measured. A formation process was proposed for the observed vertical distribution, that is, surface contamination occurred intensively at the contact line between the cloud base and mountain slopes via cloudwater deposition, and the descending cloud base formed the contamination zone. This study sheds light on the deposition processes of radionuclides, which have not previously been clarified.

Altitude-dependent distribution of ambient gamma dose rates in a mountainous area of Japan caused by the fukushima nuclear accident.

Large amounts of airborne radionuclides were deposited over a wide area in eastern Japan, including mountainous regions, during the devastating Fukushima Dai-ichi nuclear power plant accident. Altitudinal distributions of ambient gamma dose rate in air were measured in a mountainous area at the northern rim of the Kanto Plain, Japan, using a portable instrument carried along the mountain trails. In the Nikko Mountain area, located 120 km north of Tokyo, the altitudinal distribution exhibited a maxima at ∼900-2000 m above sea level (ASL). This area was not affected by precipitation until 2300 Japan Standard Time (JST) on March 15, 2011. By that time, a substantial amount of radionuclides had been transported from the damaged reactor, according to the numerical simulations using transport models. Meteorological sounding data indicated that the corresponding altitudes were within the cloud layer. A visual-range monitor deployed in an unmanned weather station at 1292 m ASL also recorded low visibility on the afternoon of March 15. From these findings, it was deduced that the altitude-dependent radioactive contamination was caused by the cloud/fog deposition process of the radionuclides contained in aerosols acting as cloud condensation nuclei.

Transboundary secondary organic aerosol in western Japan indicated by the δ13C of water-soluble organic carbon and the m/z 44 signal in organic aerosol mass spectra.

The stable carbon isotope ratio (δ13C) of low-volatile water-soluble organic carbon (LV-WSOC) was measured in filter samples of total suspended particulate matter, collected every 24 h in the winter of 2010 at an urban site and two rural sites in western Japan. Concentrations of the major chemical species in fine aerosol (<1.0 µm) were also measured in real time by aerosol mass spectrometers. The oxidation state of organic aerosol was evaluated using f44; i.e., the proportion of the signal at m/z 44 (CO2+ ions from the carboxyl group) to the sum of all m/z signals in the organic mass spectra. A strong correlation between LV-WSOC and m/z 44 concentrations was observed, which suggested that LV-WSOC was likely to be associated with carboxylic acids in fine aerosol. Plots of δ13C of LV-WSOC versus f44 showed random variation at the urban site and systematic trends at the rural sites. The systematic trends qualitatively agreed with a simple binary mixture model of secondary organic aerosol with background LV-WSOC with an f44 of ∼0.08 and δ13C of -17‰ or higher. Comparison with reference values suggested that the source of background LV-WSOC was likely to be primary emissions associated with C4 plants.

Low blank sampling method for measurement of the nitrogen isotopic composition of atmospheric NOx.

The nitrogen isotopic composition of nitrogen oxide (NOx) is useful for estimating its sources and sinks. Several methods have been developed to convert atmospheric nitric oxide (NO) and/or nitrogen dioxide (NO2) to nitrites and/or nitrates for collection. However, the collection efficiency and blanks are poorly evaluated for many collection methods. Here, we present a method for collecting ambient NOx (NO and NO2 simultaneously) with over 90% efficiency collection of NOx and low blank (approximately 0.5 µM) using a 3 wt% hydrogen peroxide (H2O2) and 0.5 M sodium hydride (NaOH) solution. The 1σ uncertainty of the nitrogen isotopic composition was ± 1.2 ‰. The advantages of this method include its portability, simplicity, and the ability to collect the required amount of sample to analyze the nitrogen isotopic composition of ambient NOx in a short period of time. Using this method, we observed the nitrogen isotopic compositions of NOx at the Tsukuba and Yoyogi sites in Japan. The averaged δ15N(NOx) value and standard deviation (1σ) in the Yoyogi site was (-2.7 ± 1.8) ‰ and in the Tsukuba site was (-1.7 ± 0.9) ‰ during the sampling period. The main NOx source appears to be the vehicle exhaust in the two sites.

Sulfate aerosol as a potential transport medium of radiocesium from the Fukushima nuclear accident.

To date, areas contaminated by radionuclides discharged from the Fukushima Dai-ichi nuclear power plant accident have been mapped in detail. However, size of the radionuclides and their mixing state with other aerosol components, which are critical in their removal from the atmosphere, have not yet been revealed. We measured activity size distributions of (134)Cs and (137)Cs in aerosols collected 47 days after the accident at Tsukuba, Japan, and found that the activity median aerodynamic diameters of (134)Cs and (137)Cs in the first sample (April 28-May 12) were 0.54 and 0.53 µm, respectively, and those in the second sample (May 12-26) were both 0.63 µm. The activity size distributions of these radiocesium were within the accumulation mode size range and almost overlapped with the mass size distribution of non-sea-salt sulfate aerosol. From the analysis of other aerosol components, we found that sulfate was the potential transport medium for these radionuclides, and resuspended soil particles that attached radionuclides were not the major airborne radioactive substances at the time of measurement. This explains the relatively similar activity sizes of radiocesium measured at various sites during the Chernobyl accident. Our results can serve as basic data for modeling the transport/deposition of radionuclides.

A twenty-year deposition record of elemental carbon in Northern Japan retrieved from archived filters.

The black carbon or elemental carbon (EC) content in ice and snow has been a concern in climate change studies, but time-series records have mostly been obtained from glacier ice-core samples in limited geographical locations, such as the Arctic or high mountains. This is the first study to present decade-long records of EC deposition measured at urban (Sapporo) and background (Rishiri Island) sites in Japan, in the mid-latitude zone of the eastern edge of the Asian continent. By using archived membrane filters from an acid rain study, we retrieved monthly EC deposition records of 1993-2012 in Sapporo and intermittent deposition data in Rishiri. Annual EC deposition showed large fluctuations, with a maximum in 2000-2001 and a minor increase in 2010-2011. This interannual change was moderately related to the deposition of non-sea salt SO42- and the collected water volume but did not reflect the estimated emission history of China. High depositions in 2000-2001 were probably caused by the transport of Asian Dust accompanied by air pollutants, which were characteristically active in these years. The findings of this study have implications for the use of observational data in validating global aerosol transport models.

Comparative Analysis of PM2.5-Bound Polycyclic Aromatic Hydrocarbons (PAHs), Nitro-PAHs (NPAHs), and Water-Soluble Inorganic Ions (WSIIs) at Two Background Sites in Japan.

Daily PM2.5 (particulate matter with aerodynamic diameter ≤2.5 µm) samples were simultaneously collected at two background sites (Wajima Air Monitoring Station (WAMS) and Fukue-Jima Atmosphere and Aerosol Monitoring Station (FAMS)) in Japan in the East Asian winter and summer monsoon periods of 2017 and 2019, to compare the characteristics of air pollutants among different regions and to determine the possible variation during the long-range transport process. Polycyclic aromatic hydrocarbons (PAHs), nitro-PAHs (NPAHs), and water-soluble inorganic ions (WSIIs) were analyzed. Despite the PM2.5 concentrations at FAMS (8.90-78.5 µg/m3) being higher than those at WAMS (2.33-21.2 µg/m3) in the winter monsoon period, the average concentrations of ∑PAHs, ∑NPAHs, and ∑WSIIs were similar between the two sites. Diagnostic ratios indicated PAHs mainly originated from traffic emissions and mostly aged, whereas NPAHs were mostly secondarily formed during long-range transport. WSIIs at WAMS were mainly formed via the combustion process and secondary reactions, whereas those at FAMS mainly originated from sea salt and dust. Backward trajectories revealed the air masses could not only come from Asian continental coastal regions but also distant landlocked areas in the winter monsoon period, whereas most came from the ocean in the summer monsoon period. These findings can provide basic data for the establishment of prediction models of transboundary air pollutants in East Asia.

Altitudinal characteristics of atmospheric deposition of aerosols in mountainous regions: Lessons from the Fukushima Daiichi Nuclear Power Station accident.

To understand the formation process of radiologically contaminated areas in eastern Japan caused by the Fukushima Daiichi Nuclear Power Station (FDNPS) accident, the deposition mechanisms over complex topography are the key factors to be investigated. To characterize the atmospheric deposition processes of radionuclides over complex mountainous topography, we investigated the altitudinal distributions of the radiocesium deposited during the accident. In five selected areas, altitudinal characteristics of the air dose rates observed using airborne surveys were analyzed. To examine the deposition mechanisms, we supplementarily used vertical profiles of radiocesium deposition in each area calculated in the latest atmospheric dispersion model. In southern Iwate, the vertical profile of the observed air dose rate was uniform regardless of altitude. In western Tochigi, the areas with the highest levels of contamination were characteristically distributed in the middle of the mountains, while in southern Fukushima, the areas with the highest contamination levels were enhanced near the summits of mountains. In central Fukushima, high air dose rates were limited to the bottoms of basin-like valley. In the region northwest of FDNPS, the air dose rate was the highest at the bottom of valley topography and decreased gradually with altitude. The simulation results showed that calculated wet deposition and observed vertical profiles of total deposition were similar in areas of southern Iwate and northwest of FDNPS qualitatively, suggesting that the dominant deposition mechanism was wet deposition. In contrast, the atmospheric dispersion model failed to reproduce either the timing of precipitation events or vertical profiles of radiocesium deposition in three other areas. Although it was difficult to elucidate the deposition mechanisms in these areas due to uncertainties of the present model results, potential mechanisms such as cloud water deposition were still proposed based on circumstantial evidences of limited meteorological data during the early stage of the accident.

Weak size dependence of resuspended radiocesium adsorbed on soil particles collected after the Fukushima nuclear accident.

Most studies of the properties of airborne radionuclides emitted from the Fukushima Daiichi Nuclear Power Plant have focused on the relatively early stages of the accident, and little is known about the characteristics of radiocesium in the long-term. In this study, we analyzed activity size distributions of airborne radiocesium collected over 5 months in Tsukuba, Japan. Radiocesium in the accumulation mode size range (0.1-2 µm in aerodynamic diameter) was overwhelming in the early aerosol samples and decreased with time, while that associated with coarse aerosols remained airborne. We examined the radiocesium adsorbed onto airborne soil particles, and found that the size dependence of 137Cs surface density adsorbed on soil particles was weak. That is, radiocesium was distributed homogeneously throughout the aerodynamic diameter range of 2.1-11 µm. This characteristic may be related to the reported structure of radiocesium-bearing soil particles collected from the ground, which consisted of an aggregate of specific clay minerals and other non-cesium adsorbing particles. The resuspension factors for the first two aerosol samples collected during late April and May 2011 were close to those in European cities in the months following the Chernobyl accident, despite different soil and weather conditions.