The use of portable OSL and IRSL measurements of NaCl in low dose assessments following a radiological or nuclear emergency.

During recovery phases following a nuclear or radiological incident analyses of doses received by members of the public and responders are often required. Several methods have been investigated for use at different timescales after the incident, including assessments based on measurements of materials present at the time of the incident. Common salt has previously been shown to have potential for retrospective dosimetry in the mGy dose range using laboratory instrumentation. This preliminary study investigates the use of portable instruments, with unprepared commercially sourced salt, in dose ranges below 100 µGy. Responses from pulsed IRSL and portable OSL instruments were compared. For OSL measurements, detection limits of 7 µGy have been demonstrated, with detection limits of 30-340 µGy for the other instruments investigated. Dose responses in the 0-500 µGy range were determined for the most sensitive systems, which show a linear response over this dose range with a non-zero intercept representing doses received from environmental sources since manufacture of the salt. For use as a dosimeter, methods of removing or accounting for inherited signals will be required in this low dose range. The results demonstrate that salt has considerable potential for use in retrospective dosimetry below 100 µGy, and that measurements can be conducted with portable OSL instruments.

Assessment of the calibration of gamma spectrometry systems in forest environments.

A Monte Carlo simulation was used to develop a model of the response of a portable gamma spectrometry system in forest environments. This model was used to evaluate any corrections needed to measurements of 137Cs activity per unit area calibrated assuming an open field geometry. These were shown to be less than 20% for most forest environments. The model was also used to assess the impact of activity in the canopy on ground level measurements. For similar activity per unit area in the lower parts of the canopy as on the ground, 10-25% of the ground based measurement would be due to activity in the canopy, depending on the depth profile in the soil. The model verifies that an optional collimator cap can assess activity in the canopy by repeat survey.

Radiocarbon Releases from the 2011 Fukushima Nuclear Accident.

Radiocarbon activities were measured in annual tree rings for the years 2009 to 2015 from Japanese cedar trees (Cryptomeria japonica) collected at six sites ranging from 2.5-38 km northwest and north of the Fukushima Dai-ichi nuclear power plant. The 14C specific activity varied from 280.4 Bq kg-1 C in 2010 to 226.0 Bq kg-1 C in 2015. The elevated 14C activities in the 2009 and 2010 rings confirmed 14C discharges during routine reactor operations, whereas those activities that were indistinguishable from background in 2012-2015 coincided with the permanent shutdown of the reactors after the accident in 2011. High-resolution 14C analysis of the 2011 ring indicated 14C releases during the Fukushima accident. The resulted 14C activity decreased with increasing distance from the plant. The maximum 14C activity released during the period of the accident was measured 42.4 Bq kg-1 C above the natural ambient 14C background. Our findings indicate that, unlike other Fukushima-derived radionuclides, the 14C released during the accident is indistinguishable from ambient background beyond the local environment (~30 km from the plant). Furthermore, the resulting dose to the local population from the excess 14C activities is negligible compared to the dose from natural/nuclear weapons sources.

Carbon, cesium and iodine isotopes in Japanese cedar leaves from Iwaki, Fukushima.

Japanese cedar leaves from Iwaki, Fukushima were analyzed for carbon, cesium and iodine isotopic compositions before and after the 2011 nuclear accident. The Δ14C values reflect ambient atmospheric 14C concentrations during the year the leaves were sampled/defoliated, and also previous year(s). The elevated 129I and 134,137Cs concentrations are attributed to direct exposure to the radioactive fallout for the pre-fallout-expended leaves and to internal translocation from older parts of the tree for post-fallout-expended leaves. 134Cs/137Cs and 129I/137Cs activity ratios suggest insignificant isotopic and elemental fractionation during translocation. However, fractionation between radioiodine and radiocesium is significant during transportation from the source.

Evaluation of forest decontamination using radiometric measurements.

An experiment has been conducted to evaluate the additional dose reduction by clear felling contaminated forestry in Fukushima Prefecture, Japan, and using the timber to cover the areas with wood chips. A portable gamma spectrometry system, comprising a backpack containing a 3 × 3″ NaI(Tl) detector with digital spectrometer and GPS receiver, has been used to map dose rate and radionuclide activity concentrations before, after and at stages during this experiment. The data show the effect of the different stages of the experiment on dose rate at different locations around the site. The spectrometric data have allowed the assessment of the contributions of natural and anthropogenic radionuclides to the dose rate at different parts of the site before and after the experiment. This has clearly demonstrated the value of radiometric methods in evaluating remediation, and the effect of other environmental processes. The value of spectrometric methods which directly measure radionuclide concentrations has also been shown, especially through the identification of the contribution of natural and anthropogenic activity to the measured dose rate. The experiment has shown that clearing trees and applying wood chips can reduce dose rates by 10-15% beyond that achieved by just clearing the forest litter and natural redistribution of radiocaesium.

(14)C levels in the vicinity of the Fukushima Dai-ichi Nuclear Power Plant prior to the 2011 accident.

A 50-year-old Japanese cedar (Cryptomeria japonica) from Okuma, ∼1 km southwest of the Fukushima Dai-ichi Nuclear Power Plant, was cored and each annual ring was analysed for (14)C. The (14)C specific activity values varied from 330.4 Bq kg(-1) C in the tree ring formed in 1971 to 231.2 Bq kg(-1) C in the 2014 ring. During the periods 1971-1976 and 2011-2014, the (14)C specific activities are indistinguishable from the ambient background values. However, compared with the ambient atmospheric levels, the (14)C specific activities between 1977 and 2010 are significantly elevated, clearly indicating (14)C discharges from the reactors during their normal operations. In addition, the specific activities are positively correlated with the annual electricity generation values. The excess (14)C specific activities were <36 Bq kg(-1) C, corresponding to an additional annual effective dose of <2 µSv via the food ingestion pathway in the study location. The primary wind direction is east-southeast/southeast with a frequency of ∼30%, in comparison to ∼20% frequency for the direction of the site under study (north-northeast/northeast). This would tend to indicate a similar magnitude of additional effective dose and consequently no significant radiological impact of atmospheric (14)C discharges from the FDNPP during the entire period of normal operations. Additionally, no (14)C pulse in activity can be observed in the year 2011 ring. This might be caused by a limited (14)C release from the damaged reactors during the accident or that the prevailing wind during the short period of release (11th-25th March 2011) was not in the direction of Okuma.

Iodine isotopes in precipitation: Four-year time series variations before and after 2011 Fukushima nuclear accident.

Rainwater samples were collected monthly from Fukushima, Japan, in 2012-2014 and analysed for (127)I and (129)I. These are combined with previously reported data to investigate atmospheric levels and behaviour of Fukushima-derived (129)I before and after the 2011 nuclear accident. In the new datasets, (127)I and (129)I concentrations between October 2012 and October 2014 varied from 0.5 to 10 µg/L and from 1.2 × 10(8) to 6.9 × 10(9) atoms/L respectively, resulting in (129)I/(127)I atomic ratio ranges from 3 × 10(-8) to 2 × 10(-7). The (127)I concentrations were in good agreement with those in the previous period from March 2011 to September 2012, whereas the (129)I concentrations and (129)I/(127)I ratios followed declining trends since the accident. Although (129)I concentrations in five samples during the period of 2013-2014 have approached the pre-accident levels, (129)I concentrations in most samples remained higher values in winter and spring-summer. The high (129)I levels in winter and spring-summer are most likely attributed to local resuspension of the Fukushima-derived radionuclide-bearing fine soil particles deposited on land surfaces, and re-emission through vegetation taking up (129)I from contaminated soil and water, respectively. Long-term declining rate suggests that contribution of the Fukushima-derived (129)I to the atmosphere would become less since 2014.

Radiocarbon concentration in modern tree rings from Fukushima, Japan.

A 30-year-old Japanese cedar (Cryptomeria japonica), collected from Iwaki, Fukushima in 2014, was analyzed for the long-lived radionuclide (14)C. Values of Δ(14)C varied from 211.7‰ in 1984 to 16.9‰ in 2013. The temporal Δ(14)C variation can be described as an exponential decline, indistinguishable from the general Northern Hemisphere Zone 2 (NH Zone 2) values in the atmosphere, until at least 1994. Values of Δ(14)C for 1999 and 2004 are slightly depleted compared with NH Zone 2 values, while from 1999 to 2013 the data suggest a clear depletion with a 2-8 ppmV additional CO2 contribution from a (14)C-free (i.e. fossil carbon) source. This change coincides with local traffic increases since two nearby expressways were opened in the 1990's. In addition, the small but visible (14)C pulse observed in the 2011 tree-ring might be caused by release from the damaged reactors during the Fukushima nuclear accident.

Speciation of radiocesium and radioiodine in aerosols from Tsukuba after the Fukushima nuclear accident.

Aerosol samples were collected from Tsukuba, Japan, soon after the 2011 Fukushima nuclear accident and analyzed for speciation of radiocesium and radioiodine to explore their chemical behavior and isotopic ratios after the release. Most (134)Cs and (137)Cs were bound in organic matter (53­91%) and some in water-soluble fractions (5­15%), whereas a negligible proportion of radiocesium remained in minerals. This pattern suggests that sulfate salts and organic matter may be the main carrier of Cs-bearing particles. The (129)I in aerosol samples is contained in various proportions as soluble inorganic iodine (I(­) and IO3(­)), soluble organic iodine, and unextractable iodine. The measured mean (129)I/(131)I atomic ratio of 16.0 ± 2.2 is in good agreement with that measured from rainwater and consistent with ratios measured in surface soil samples. Together with other aerosols and seawater samples, an initial (129)I/(137)Cs activity ratio of ∼4 × 10(­7) was obtained. In contrast to the effectively constant (134)Cs/(137)Cs activity ratios (1.04 ± 0.04) and (129)I/(131)I atomic ratios (16.0 ± 2.2), the (129)I/(137)Cs activity ratios scattered from 3.5 × 10(­7) to 5 × 10(­6) and showed temporally and spatially different dispersion and deposition patterns between radiocesium and radioiodine. These findings confirm that (129)I, instead of (137)Cs, should be considered as a proxy for (131)I reconstruction.