Variation analysis of atmospheric 7Be activity concentrations with respect to precipitation.

Beryllium-7 activity concentrations in the atmosphere and precipitation were continuously measured every day between April 2011 and December 2015 in Dazaifu, western Japan. The measured data were quantitatively analyzed to determine the precipitation-induced variation in 7Be activity concentrations. The average concentrations on nonprecipitation and precipitation days were 5.5 and 3.8 mBq/m3, respectively. This difference of 31% (1.7 mBq/m3) on average, was attributable to the washout effect, which was more significant in the summer. Regarding the association between 7Be activity concentration and precipitation, the concentration remained at a similar level for the small precipitation amount of <5.0 mm/day and showed a decreasing trend (but was insignificant) for the precipitation of 5.0-10.0 mm/day. A significant decrease in the concentration was observed for ≥10 mm/day. Furthermore, when precipitation occurred on two successive days, the 7Be activity concentrations on the second day significantly decreased regardless of precipitation.

TRITIUM IN THE ENVIRONMENT.

Environmental tritium are natural and anthropogenic origins, the distribution has spread in atmosphere, hydrosphere and biosphere as a variety of chemical forms. The natural tritium is produced by nuclear reactions of neutron with N and O in the upper atmosphere, the production rate changes with 11-year cycle of the solar activity. The production and radioactive decay of natural tritium is balanced on the whole earth, results in the inventory of about 1 EBq. Anthropogenic tritium by nuclear weapons testing had been released in 1950s-1960s, at highest intensity just before the Partial Test Ban Treaty in 1963, and the total release would be 186 EBq. In accordance with a peaceful use of nuclear energy, tritium has been releasing to the environment as airborne and liquid effluents from nuclear power plants and nuclear fuel reprocessing plants. The release from the nuclear power plants depends on the reactor type. Other sources are the tritium production facility of military purpose and the consumer products that use tritium as luminescent energy and disposed to landfill site. Internal dose is only concerned on tritium due to low decay energy, suggesting tritium concentrations in drinking water and food are critical for dose evaluation.

Analysis of Factors Contributing to the Increase in 7Be Activity Concentrations in the Atmosphere.

In March 2013, increased 7Be activity concentrations in the atmosphere were observed for successive days in Dazaifu, western Japan. The daily 7Be activity concentration ranged from 0.93 to 14 mBq/m3, with a monthly average of 8.3 mBq/m3. This average was the highest among the monthly averages observed between 1999 and 2015, and higher than the monthly average over this period (4.7 mBq/m3) plus twice the standard deviation. Also, this exceeded the monthly average (6.0 mBq/m3) only for March 1999-2015 (excluding 2013, when the cosmic-ray intensity, a component producing 7Be, decreased). Based on the backward trajectory analysis etc. results, the inflow of air from the stratosphere and upper troposphere at high latitudes that frequently occurred in March 2013 was considered the reason for the 7Be activity concentration increase.

Cosmogenic 7Be: Particle size distribution and chemical composition of 7Be-carrying aerosols in the atmosphere in Japan.

The particle size distributions of airborne aerosols with 7Be were measured using cascade impactors at Dazaifu, a city in western Japan, in 2018 to observe their seasonal variation. Beryllium-7 was found to be adsorbed to aerosols with a particle size of less than 2.1 µm; in general, particles sized 0.43-0.65 µm had the highest 7Be activity concentrations. The activity median aerodynamic diameter (AMAD) of 7Be fluctuated less over the year within the range of 0.40-0.52 µm, which is the size range of particles that can reach human alveoli, and had an annual mean of 0.43 ± 0.034 µm. The activity concentrations of 7Be were significantly lower in summer, which affected 7Be activity concentration for each particle size fraction. The particle size distribution of 7Be-carrying aerosols was also affected by that of the aerosol particles in the atmosphere. Finally, findings suggest that 7Be was mainly adsorbed to sulfate aerosols (particularly ammonium sulfate aerosols).

Tritium concentrations in the atmospheric environment at Rokkasho, Japan before the final testing of the spent nuclear fuel reprocessing plant.

This study aimed at obtaining background tritium concentrations in precipitation and air at Rokkasho where the first commercial spent nuclear fuel reprocessing plant in Japan has been under construction. Tritium concentration in monthly precipitation during fiscal years 2001-2005 had a seasonal variation pattern which was high in spring and low in summer. The tritium concentration was higher than that observed at Chiba City as a whole. The seasonal peak concentration at Rokkasho was generally higher than that at Chiba City, while the baseline concentrations of both were similar. The reason for the difference may be the effect of air mass from the Asian continent which is considered to have high tritium concentration. Atmospheric tritium was operationally separated into HTO, HT and hydrocarbon (CH(3)T) fractions, and the samples collected every 3 d-14 d during fiscal year 2005 were analyzed for these fractions. The HTO concentration as radioactivity in water correlated well with that in the precipitation samples. The HT concentration was the highest among the chemical forms analyzed, followed by the HTO and CH(3)T concentrations. The HT and CH(3)T concentrations did not have clear seasonal variation patterns. The HT concentration followed the decline previously reported by Mason and Östlund with an apparent half-life of 4.8 y. The apparent and environmental half-lives of CH(3)T were estimated as 9.2 y and 36.5 y, respectively, by combining the present data with literature data. The Intergovernmental Panel on Climate Change used the atmospheric lifetime of 12 y for CH(4) to estimate global warming in its 2007 report. The longer environmental half-life of CH(3)T suggested its supply from other sources than past nuclear weapon testing in the atmosphere.

An improved method for 85Kr analysis by liquid scintillation counting and its application to atmospheric 85Kr determination.

Atmospheric (85)Kr concentration at Fukuoka, Japan was determined by an improved (85)Kr analytical method using liquid scintillation counting (LSC). An average value of 1.54 +/- 0.05 Bq m(-3) was observed in 2008, which is about two times that measured in 1981 at Fukuoka, indicating a 29 mBq y(-1) rate of increase as an average for these 27 years. The analytical method developed involves collecting Kr from air using activated charcoal at liquid N(2) temperature and purifying it using He at dry ice temperature, followed by Kr separation by gas chromatography. An overall Kr recovery of 76.4 +/- 8.1% was achieved when Kr was analyzed in 500-1000 l of air. The Kr isolated by gas chromatography was collected on silica gel in a quartz glass vial cooled to liquid N(2) temperature and the activity of (85)Kr was measured with a low-background LS counter. The detection limit of (85)Kr activity by the present analytical method is 0.0015 Bq at a 95% confidence level, including all propagation errors, which is equivalent with (85)Kr in 1.3 l of the present air under the analytical conditions of 72.1% counting efficiency, 0.1597 cps background count rate, and 76.4% Kr recovery.

Isotopic evidence in tree rings for historical changes in atmospheric sulfur sources.

Little is understood about the usefulness of sulfur isotopic ratios (sigma 34S) in tree rings because the sulfur content in rings is generally insufficient for analysis using conventional methods. We present sigma 34S values of the water-soluble and the organically bound sulfur fractions in rings of coniferous trees grown in Japan, analyzed using a large-volume oxygen bomb. Comparing the sigma 34S values of the organically bound fraction in tree rings with past atmospheric sulfur concentrations and with those of their sources, we find clear evidence that the sigma 34S values of the organically bound fraction in the rings are dependent upon the values of the atmospheric sulfur sources. The evidence suggests that the sigma 34S values in tree rings are a useful chronological proxy for evaluating possible causes of past atmospheric sulfur pollution.