Time-series variations in 129I concentrations and 129I/137Cs ratios in suspended particulate matter collected in eastern Japan immediately after the 2011 nuclear accident in Fukushima, Japan

Abstract

We have determined the hourly atmospheric concentrations of ¹²⁹I in aerosols dispersed into the atmosphere by the nuclear accident at the Fukushima Daiichi Nuclear Power Plant (FD1NPP) on March 11, 2011. Data were obtained by measuring the quantity of ¹²⁹I in suspended particulate matter (SPM) collected on filter tapes at 41 SPM monitoring stations in Fukushima and other prefectures in eastern Japan, including the metropolitan area of Tokyo and the surrounding area. After scrutiny, 500 out of 920 hourly SPM samples were determined to be reliable (i.e., devoid of cross-contamination), and these were subjected to further analysis and discussion. Based on the data from these samples, especially data from the four SPM sampling sites located close to the FD1NPP (Futaba, Naraha, Haramachi and Nihonmatsu), the time-series variations in the atmospheric concentration of ¹²⁹I and the activity ratio of ¹²⁹I/¹³⁷Cs were reconstructed by using ¹³⁷Cs concentration data in the literature. ¹²⁹I and ¹³⁷Cs were observed to be continuously and sometimes explosively dispersed into the atmosphere in aerosols transported by radioactive plumes from the FD1NPP. The highest activity concentrations of ¹²⁹I and ¹³⁷Cs were observed in the SPM sample at the Futaba SPM station (3.2 km west-northwest of the FD1NPP) at 14:00-15:00 on March 12 after the venting of Unit 1. Systematically high ¹²⁹I/¹³⁷Cs activity ratios were observed at the Futaba and Haramachi stations from March 12 to 14, suggesting that radioactive masses released from the FD1NPP during the first few days after the nuclear accident were relatively enriched in radioiodine. High activity ratios of ¹²⁹I/¹³⁷Cs were also measured starting on March 21 at Naraha (17.5 km south of FD1NPP) and from March 22-23 in the metropolitan area which must have been caused by a different type of emission event(s) on those days at the FD1NPP, as previously reported. The ¹²⁹I data from this study are highly effective in the validation and elaboration of the modelling of the atmospheric dispersion of radioiodine. They further contribute to assessing the internal exposure due to inhalation of ¹³¹I estimated by means of such elaborate atmospheric diffusion models.

Keywords: (129)I; (131)I. Fukushima nuclear accident. Suspended particulate matter.