Plutonium concentration and 240Pu/239Pu atom ratio in biota collected from Amchitka Island, Alaska: recent measurements using ICP-SFMS

• Pu in biota near Amchitka Test Site was measured the first time in over a decade.
• 240Pu/239Pu ratios in terrestrial samples are within the range of global fallout.
• Elevated 240Pu/239Pu in marine samples was characteristic of North Pacific Ocean.
• Potential sources of enriched Pu to the marine environment regionally are suggested.
• Pu ratios cannot by themselves explain the enriched Pu in seawater around Amchitka.

Three underground nuclear tests, including the Unites States' largest, were conducted on Amchitka Island, Alaska. Monitoring of the radiological environment around the island is challenging because of its remote location. In 2008, the Department of Energy (DOE) Office of Legacy Management (LM) became responsible for the long term maintenance and surveillance of the Amchitka site. The first DOE LM environmental survey occurred in 2011 and is part of a cycle of activities that will occur every 5 years. The University of Alaska Fairbanks, a participant in the 2011 study, provided the lichen (Cladonia spp.), freshwater moss (Fontinalis neomexicanus), kelp (Eualaria fistulosa) and horse mussel (Modiolus modiolus) samples from Amchitka Island and Adak Island (a control site). These samples were analyzed for 239Pu and 240Pu concentration and 240Pu/239Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and 240Pu/239Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The 239+240Pu levels (mBq kg−1, dry weight) ranged from 3.79 to 57.1 for lichen, 167–700 for kelp, 27.9–148 for horse mussel, and 560–573 for moss. Lichen from Adak Island had higher Pu concentrations than Amchitka Island, the difference was likely the result of the higher precipitation at Adak compared to Amchitka. The 240Pu/239Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p < 0.001); lichen and moss averaged 0.184 ± 0.007, similar to the integrated global fallout ratio, whereas kelp and mussel (soft tissue) averaged 0.226 ± 0.003. These observations provide supporting evidence that a large input of isotopically heavier Pu occurred into the North Pacific Ocean, likely from the Marshall Island high yield nuclear tests, but other potential sources, such as the Kamchatka Peninsula Rybachiy Naval Base and Amchitka Island underground nuclear test site cannot be ruled out.