After the March 11, 2011, nuclear reactor meltdowns at Fukushima Dai-ichi, 180 samples of Japanese particulate matter (dusts and surface soils) and 235 similar U.S. and Canadian samples were collected and analyzed sequentially by gamma spectrometry, autoradiography, and scanning electron microscopy with energy dispersive X-ray analysis. Samples were collected and analyzed over a five-year period, from 2011 to 2016. Detectable levels of 134Cs and 137Cs were found in 142 of 180 (80%) Japanese particulate matter samples. The median radio-cesium specific activity of Japanese particulate samples was 3.2kBqkg-1±1.8kBqkg-1, and the mean was 25.7kBqkg-1 (σ=72kBqkg-1). The U.S. and Canadian mean and median radio‑cesium activity levels were <0.03kBqkg-1. U.S. and Canadian samples had detectable 134Cs and 137Cs in one dust sample out of 32 collected, and four soils out of 74. The maximum US/Canada radio-cesium particulate matter activity was 0.30±0.10kBqkg-1. The mean in Japan was skewed upward due to nine of the 180 (5%) samples with activities >250kBqkg-1. This skewness was present in both the 2011 and 2016 sample sets. >300 individual radioactively-hot particles were identified in samples from Japan; composed of 1% or more of the elements cesium, americium, radium, polonium, thorium, tellurium, or strontium. Some particles reached specific activities in the MBqμg-1 level and higher. No cesium-containing hot particles were found in the U.S. sample set. Only naturally-occurring radionuclides were found in particles from the U.S. background samples. Some of the hot particles detected in this study could cause significant radiation exposures to individuals if inhaled. Exposure models ignoring these isolated hot particles would potentially understate human radiation dose.
Keywords: Autoradiography; Gamma spectrometry; Radioactively-hot particles; SEM/EDS.
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