A Comparative Study of Mercury Bioaccumulation in Bivalve Molluscs from a Shallow Estuarine Embayment.

In estuarine food webs, bivalve molluscs transfer nutrients and pollutants to higher trophic levels. Mercury (Hg) pollution is ubiquitous, but it is especially elevated in estuaries historically impacted by industrial activities, such as those in the U.S. Northeast. Monomethylmercury (MeHg), the organic form of Hg, is highly bioaccumulative and transferable in the food web resulting in the highest concentrations in the largest and oldest marine predators. Patterns of Hg concentrations in marine bivalve molluscs, however, are poorly understood. In this study, inorganic Hg (iHg), MeHg, and the total Hg (THg) in soft tissues of the northern quahogs (Mercenaria mercenaria), eastern oysters (Crassostrea virginica), and ribbed mussels (Geukensia demissa) from eastern Long Island sound, a temperate estuary of the western North Atlantic Ocean was investigated. In all three species, concentrations of THg remained similar between the four sampling months (May, June, July, and September), and were mostly independent of animal size. In quahogs, MeHg and iHg displayed significant (p < 0.05) positive (iHg in May and June) and negative (MeHg in July and September) changes with shell height. Variability in concentrations of THg, MeHg, and iHg, both inter- and intra-specifically was high and greater in quahogs and oysters (THg: 37, 39%, MeHg: 28, 39%, respectively) than in mussels (THg: 13%, MeHg: 20%). The percentage of THg that was MeHg (%MeHg) was also highly variable in the three species (range: 10-80%), highlighting the importance of measuring MeHg and not only THg in molluscs.

Dissolved organic matter thiol concentrations determine methylmercury bioavailability across the terrestrial-marine aquatic continuum.

The most critical step for methylmercury (MeHg) bioaccumulation in aquatic food webs is phytoplankton uptake of dissolved MeHg. Dissolved organic matter (DOM) has been known to influence MeHg uptake, but the mechanisms have remained unclear. Here we show that the concentration of DOM-associated thiol functional groups (DOM-RSH) varies substantially across contrasting aquatic systems and dictates MeHg speciation and bioavailability to phytoplankton. Across our 20 study sites, DOM-RSH concentrations decrease 40-fold from terrestrial to marine environments whereas dissolved organic carbon (DOC), the typical proxy for MeHg binding sites in DOM, only has a 5-fold decrease. MeHg accumulation into phytoplankton is shown to be directly linked to the concentration of specific MeHg binding sites (DOM-RSH), rather than DOC. Therefore, MeHg bioavailability increases systematically across the terrestrial-marine aquatic continuum as the DOM-RSH concentration decreases. Our results strongly suggest that measuring DOM-RSH concentrations will improve empirical models in phytoplankton uptake studies and will form a refined basis for modeling MeHg incorporation in aquatic food webs under various environmental conditions.

Riverine Discharge Fuels the Production of Methylmercury in a Large Temperate Estuary.

Estuaries are an important food source for the world's growing population, yet human health is at risk from elevated exposure to methylmercury (MeHg) via the consumption of estuarine fish. Moreover, the sources and cycling of MeHg in temperate estuarine ecosystems are poorly understood. Here, we investigated the seasonal and tidal patterns of mercury (Hg) forms in Long Island Sound (LIS), in a location where North Atlantic Ocean waters mix with the Connecticut River. We found that seasonal variations in Hg and MeHg in LIS followed the extent of riverine Hg delivery, while tides further exacerbated the remobilization of earlier deposited riverine Hg. The net production of MeHg near the river plume was significant compared to that in other locations and enhanced during high tide, possibly resulting from the enhanced microbial activity and organic carbon remineralization in the river plume. Statistical models, driven by our novel data, further support the hypothesis that the river-delivered organic matter and inorganic Hg drive net MeHg production in the estuarine water column. Our study sheds light on the significance of water column biogeochemical processes in temperate tidal estuaries in regulating MeHg levels and inspires new questions in our quest to understand MeHg sources and dynamics in coastal oceans.

Nutrient Inputs Stimulate Mercury Methylation by Syntrophs in a Subarctic Peatland.

Climate change dramatically impacts Arctic and subarctic regions, inducing shifts in wetland nutrient regimes as a consequence of thawing permafrost. Altered hydrological regimes may drive changes in the dynamics of microbial mercury (Hg) methylation and bioavailability. Important knowledge gaps remain on the contribution of specific microbial groups to methylmercury (MeHg) production in wetlands of various trophic status. Here, we measured aqueous chemistry, potential methylation rates (k meth ), volatile fatty acid (VFA) dynamics in peat-soil incubations, and genetic potential for Hg methylation across a groundwater-driven nutrient gradient in an interior Alaskan fen. We tested the hypotheses that (1) nutrient inputs will result in increased methylation potentials, and (2) syntrophic interactions contribute to methylation in subarctic wetlands. We observed that concentrations of nutrients, total Hg, and MeHg, abundance of hgcA genes, and rates of methylation in peat incubations (k meth ) were highest near the groundwater input and declined downgradient. hgcA sequences near the input were closely related to those from sulfate-reducing bacteria (SRB), methanogens, and syntrophs. Hg methylation in peat incubations collected near the input source (FPF2) were impacted by the addition of sulfate and some metabolic inhibitors while those down-gradient (FPF5) were not. Sulfate amendment to FPF2 incubations had higher k meth relative to unamended controls despite no effect on k meth from addition of the sulfate reduction inhibitor molybdate. The addition of the methanogenic inhibitor BES (25 mM) led to the accumulation of VFAs, but unlike molybdate, it did not affect Hg methylation rates. Rather, the concurrent additions of BES and molybdate significantly decreased k meth , suggesting a role for interactions between SRB and methanogens in Hg methylation. The reduction in k meth with combined addition of BES and molybdate, and accumulation of VFA in peat incubations containing BES, and a high abundance of syntroph-related hgcA sequences in peat metagenomes provide evidence for MeHg production by microorganisms growing in syntrophy. Collectively the results suggest that wetland nutrient regimes influence the activity of Hg methylating microorganisms and, consequently, Hg methylation rates. Our results provide key information about microbial Hg methylation and methylating communities under nutrient conditions that are expected to become more common as permafrost soils thaw.

The impact of the Three Gorges Dam on the fate of metal contaminants across the river-ocean continuum.

The Three Gorges Dam (TGD) is the world's largest hydropower construction. It can significantly impact contaminant transport in the Yangtze River-East China Sea Continuum (YR-ECSC). In addition to evaluating the impact of the TGD on the deposition of contaminants in the reservoir, we also address their cycles in the river below the dam and in the coastal East China Sea. A comprehensive study of metal contaminant transport along the YR-ECSC has not been previously attempted. We quantified the fates of mercury (Hg), arsenic (As), lead (Pb), cadmium (Cd) and chromium (Cr) within the YR-ECSC, and the impacts of the TGD, by sampling water and suspended particles along the Yangtze River during spring, summer, fall, and winter and by modeling. We found that the Yangtze River transports substantial amounts of heavy metals into the coastal ocean. In 2016, riverine transport amounted to 48, 5900, 11,000, 230, and 15,000 megagrams (Mg) for Hg, As, Pb, Cd, and Cr, respectively, while other terrestrial contributions were negligible. Metal flux into the coastal ocean was primarily derived from the downstream portion of the river (84-97%), while metals transported from upstream were largely trapped in the Three Gorges Reservoir (TGR, 72%-96%). For example, 34 Mg of Hg accumulated in the TGR owing to river damming, large-scale soil erosion, and anthropogenic point source releases, while 21 Mg of Hg was depleted from the riverbed downstream owing to the altered river hydrology caused by the TGD. Overall the construction of TGD resulted in a 6.9% net decrease in the Hg burden of the East China Sea, compared to the pre-TGD period.

Formalin-preserved zooplankton are not reliable for historical reconstructions of methylmercury bioaccumulation.

Time-series measurements of methylmercury (MeHg) concentrations in short-lived planktic animals, such as copepods, could allow for an evaluation of mercury (Hg) inputs and transferability to organisms in marine environments. If reliable, MeHg measurements in formalin-preserved marine animals could offer insights into past environmental MeHg levels. In the present study, we examined whether the amount of MeHg changed over time in formalin-preserved copepods for two species, Acartia tonsa, and Temora longicornis. Over a 51 (A. tonsa) and 7 (T. longicornis) week incubation, we found significant changes in MeHg content in both copepods, while the timing of these changes differed between species. Furthermore, we investigated the mechanism behind these temporal changes through a separate incubation experiment of formalin spiked with two levels of organic matter (OM), and stable-isotope-enriched Hg tracers. We found that the methylation of an inorganic 199Hg tracer was significantly higher in OM-enriched solutions in comparison to a control seawater-formalin solution. Our results suggest that formalin-preserved copepods are not fit for studies of past trends due to ongoing and unpredictable abiotic transformations of Hg in chemically preserved animal tissue.

An assessment of the impact of artisanal and commercial gold mining on mercury and methylmercury levels in the environment and fish in Cote d'Ivoire.

Artisanal and small-scale gold mining (ASGM) activities are an important source of mercury (Hg) to the atmosphere globally, and in most countries in West Africa, where gold production has increased dramatically in the last decade from both commercial and ASGM activities. This study focused on examining the concentrations of Hg and methylmercury (MeHg) in water, sediments and fish in four regions associated with gold mining activities in Cote d'Ivoire to assess the potential exposure of the local communities to MeHg from fish consumption. Concentrations of dissolved total Hg and MeHg in water and sediment were elevated at some locations sample and were indicative of local contamination. Several locations had sediment total Hg above 100 ng g-1 and sediment %MeHg ranged from 0.03 to 4.4%. Fish concentrations exceeded 0.3 µg/ g wet wt., especially for carnivores and fish caught in the western region of the country. Bioaccumulation factors, relative to dissolved MeHg, were higher for carnivores than omnivores and varied with region, suggesting other factors besides MeHg concentration alone were impacting uptake and trophic transfer. Given that people in Cote d'Ivoire consume fish at a higher level than other countries, the levels in fish were sufficient to exceed the US EPA's guidance criteria even at average consumption levels, and particularly for people consuming fish at a higher rate. Overall, this study provides compelling evidence that ASGM activities in Cote d'Ivoire are leading to elevated exposure and likely impacting the health of the local populations in regions where such activity is occurring.

Impacts of farmed fish consumption and food trade on methylmercury exposure in China.

The global pollutant mercury (Hg), especially as methylmercury (MeHg), threatens human and ecosystem health. But major contributors of MeHg exposure to people in China remain highly debated. We developed the China Mercury Exposure Assessment (CMEA) model, which incorporates human exposure pathways for MeHg and total Hg (THg), the interregional, including international and interprovincial, food trading as well as human physiology to provide a comprehensive system that can evaluate the pathway of Hg forms to human consumers in China. Based on the CMEA model that employed the most comprehensive and recent data, we have found that the Probable Daily Intake (PDI) of MeHg for the Chinese population was 0.057 (range: 0.036-0.091 as 60% confidence interval) µg·kg-1·day-1, while that of THg was 0.35 (range: 0.22-0.55) µg·kg-1·day-1. MeHg exposure was dominated by fish intake, especially by farm-raised freshwater fish due to higher consumption of these fish. In 2011, fish intake contributed to 56% to the total MeHg exposure, followed by rice (26%). Consumption of farm-raised fish reduced human exposure to MeHg by 33%. On the other hand, interregional food trading increased MeHg exposure of the Chinese population, as a whole, by 7.6%. The international and interprovincial food trades contributed to 5.1% and 22% of MeHg intake, respectively. For the whole China, fish intake related exposure to MeHg was highest for the Eastern and Northeastern populations, while Tibetans were chronically exposed to the highest MeHg from other sources. Our findings highlight the importance of farmed fish and food trade for MeHg exposure.

Traditional Tibetan Medicine Induced High Methylmercury Exposure Level and Environmental Mercury Burden in Tibet, China.

Highly elevated concentrations of total mercury (THg) and methylmercury (MeHg) were found in the municipal sewage in Tibet. Material flow analysis supports the hypothesis that these elevated concentrations are related to regular ingestion of Hg-containing Traditional Tibetan Medicine (TTM). In Tibet in 2015, a total of 3600 kg of THg was released from human body into the terrestrial environment as a result of TTM ingestion, amounting to 45% of the total THg release into the terrestrial environment in Tibet, hence substantially enhancing the environmental Hg burden. Regular ingestion of TTM leads to chronic exposure of Tibetans to inorganic Hg (IHg) and MeHg, which is 34 to 3000-fold and 0-12-fold higher than from any other known dietary sources, respectively. Application of a human physiology model demonstrated that ingestion of TTM can induce high blood IHg and MeHg levels in the human body. Moreover, 180 days would be required for the MeHg to be cleared out of the human body and return to the initial concentration i.e. prior to the ingestion of 1 TTM pill. Our analysis suggests that high Hg level contained in TTM could be harmful to human health and elevate the environmental Hg burden in Tibet.

Mercury Stable Isotopes Reveal Influence of Foraging Depth on Mercury Concentrations and Growth in Pacific Bluefin Tuna.

Pelagic ecosystems are changing due to environmental and anthropogenic forces, with uncertain consequences for the ocean's top predators. Epipelagic and mesopelagic prey resources differ in quality and quantity, but their relative contribution to predator diets has been difficult to track. We measured mercury (Hg) stable isotopes in young (<2 years old) Pacific bluefin tuna (PBFT) and their prey species to explore the influence of foraging depth on growth and methylmercury (MeHg) exposure. PBFT total Hg (THg) in muscle ranged from 0.61 to 1.93 µg g-1 dw (1.31 µg g-1 dw ±0.37 SD; 99% ± 6% MeHg) and prey ranged from 0.01 to 1.76 µg g-1 dw (0.13 µg g-1 dw ±0.19 SD; 85% ± 18% MeHg). A systematic decrease in prey δ202Hg and Δ199Hg with increasing depth of occurrence and discrete isotopic signatures of epipelagic prey (δ202Hg: 0.74 to 1.49‰; Δ199Hg: 1.76-2.96‰) and mesopelagic prey (δ202Hg: 0.09 to 0.90‰; Δ199Hg: 0.62-1.95‰) allowed the use of Hg isotopes to track PBFT foraging depth. An isotopic mixing model was used to estimate the dietary proportion of mesopelagic prey in PBFT, which ranged from 17% to 55%. Increased mesopelagic foraging was significantly correlated with slower growth and higher MeHg concentrations in PBFT. The slower observed growth rates suggest that prey availability and quality could reduce the production of PBFT biomass.

Mercury bioaccumulation increases with latitude in a coastal marine fish (Atlantic silverside, Menidia menidia).

Human exposure to the neurotoxic methylmercury (MeHg) occurs primarily via the consumption of marine fish, but the processes underlying large-scale spatial variations in fish MeHg concentrations [MeHg], which influence human exposure, are not sufficiently understood. We used the Atlantic silverside (Menidia menidia), an extensively studied model species and important forage fish, to examine latitudinal patterns in total Hg [Hg] and [MeHg]. Both [Hg] and [MeHg] significantly increased with latitude (0.014 and 0.048 µg MeHg g-1 dw per degree of latitude in juveniles and adults, respectively). Four known latitudinal trends in silverside traits help explain these patterns: latitudinal increase in MeHg assimilation efficiency, latitudinal decrease in MeHg efflux, latitudinal increase in weight loss due to longer and more severe winters, and latitudinal increase in food consumption as an adaptation to decreasing length of the growing season. Given the absence of a latitudinal pattern in particulate MeHg, a diet proxy for zooplanktivorous fish, we conclude that large-scale spatial variation in growth is the primary control of Hg bioaccumulation in this and potentially other fish species.

Assessing Fukushima-Derived Radiocesium in Migratory Pacific Predators.

The 2011 release of Fukushima-derived radionuclides into the Pacific Ocean made migratory sharks, teleosts, and marine mammals a source of speculation and anxiety regarding radiocesium (134+137Cs) contamination, despite a lack of actual radiocesium measurements for these taxa. We measured radiocesium in a diverse suite of large predators from the North Pacific Ocean and report no detectable (i.e., ≥ 0.1 Bq kg-1 dry wt) Fukushima-derived 134Cs in all samples, except in one olive ridley sea turtle (Lepidochelys olivacea) with trace levels (0.1 Bq kg-1). Levels of 137Cs varied within and across taxa, but were generally consistent with pre-Fukushima levels and were lower than naturally occurring 40K by one to one to two orders of magnitude. Predator size had a weaker effect on 137Cs and 40K levels than tissue lipid content. Predator stable isotope values (δ13C and δ15N) were used to infer recent migration patterns, and showed that predators in the central, eastern, and western Pacific should not be assumed to accumulate detectable levels of radiocesium a priori. Nondetection of 134Cs and low levels of 137Cs in diverse marine megafauna far from Fukushima confirms negligible increases in radiocesium, with levels comparable to those prior to the release from Fukushima. Reported levels can inform recently developed models of cesium transport and bioaccumulation in marine species.

Contaminated Marine Sediments As a Source of Cesium Radioisotopes for Benthic Fauna near Fukushima.

Marine animals, seawater, and sediment near Fukushima, Japan have become contaminated with 134Cs and 137Cs released in March 2011 from the damaged Fukushima Dai-ichi nuclear power plant. Radiocesium concentrations in some benthic fauna declined more slowly than in pelagic fish in the same region. We tested the hypothesis that benthic fish remained more contaminated due to the bioavailability of radiocesium in sediments. Laboratory experiments demonstrated that the assimilation efficiency of 137Cs was 16% in polychaetes ingesting Fukushima sediment, up to 55% in crabs ingesting polychaetes, and about 80% in fish ingesting worms. In addition, all animals acquired Cs directly from the aqueous phase, but this accounted for only 1.2-2.5% of their total body burden. Thus, diet accounted for nearly all of the total body burden of Cs in these animals. Rate constants of Cs loss from animal tissues were 20% d-1 for polychaetes, 10% d-1 for crabs, and 6% d-1 for fish after acquisition of Cs from water; rate constants following dietary uptake were 45% d-1, 14% d-1, and 5% d-1 for polychaetes, crabs, and fish, respectively. A bioaccumulation model indicated that the transfer factors of Cs from sediments and the trophic transfer factors from worms to predators were about 1. Overall, sediment-bound Cs is sufficiently bioavailable to deposit-feeding polychaetes, and macrofauna assimilate Cs from these polychaetes to account for >90% of their body burden. This helps to explain the longer retention of Cs in bottom-dwelling fish near Fukushima.

Reconstructing transoceanic migration patterns of Pacific bluefin tuna using a chemical tracer toolbox.

Large pelagic predators play important roles in oceanic ecosystems, and may migrate vast distances to utilize resources in different marine ecoregions. Understanding movement patterns of migratory marine animals is critical for effective management, but often challenging, due to the cryptic habitat of pelagic migrators and the difficulty of assessing past movements. Chemical tracers can partially circumvent these challenges by reconstructing recent migration patterns. Pacific bluefin tuna (Thunnus orientalis; PBFT) inhabit the western and eastern Pacific Ocean, and are in steep decline due to overfishing. Understanding age-specific eastward transpacific migration patterns can improve management practices, but these migratory dynamics remain largely unquantified. Here, we combine a Fukushima-derived radiotracer (134Cs) with bulk tissue and amino acid stable isotope analyses of PBFT to distinguish recent migrants from residents of the eastern Pacific Ocean. The proportion of recent migrants to residents decreased in older year classes, though the proportion of older PBFT that recently migrated across the Pacific was greater than previous estimates. This novel toolbox of biogeochemical tracers can be applied to any species that crosses the North Pacific Ocean.

Methylmercury in dried shark fins and shark fin soup from American restaurants.

Consumption of meat from large predatory sharks exposes human consumers to high levels of toxic monomethylmercury (MMHg). There also have been claims that shark fins, and hence the Asian delicacy shark fin soup, contain harmful levels of neurotoxic chemicals in combination with MMHg, although concentrations of MMHg in shark fins are unknown. We measured MMHg in dried, unprocessed fins (n=50) of 13 shark species that occur in the international trade of dried shark fins as well as 50 samples of shark fin soup prepared by restaurants from around the United States. Concentrations of MMHg in fins ranged from 9 to 1720 ng/g dry wt. MMHg in shark fin soup ranged from <0.01 to 34 ng/mL, with MMHg averaging 62 ± 7% of total Hg. The highest concentrations of MMHg and total Hg were observed in both fins and soup from large, high trophic level sharks such as hammerheads (Sphyrna spp.). Consumption of a 240 mL bowl of shark fin soup containing the average concentration of MMHg (4.6 ng/mL) would result in a dose of 1.1 µg MMHg, which is 16% of the U.S. EPA's reference dose (0.1 µg MMHg per 1 kg per day in adults) of 7.4 µg per day for a 74 kg person. If consumed, the soup containing the highest measured MMHg concentration would exceed the reference dose by 17%. While shark fin soup represents a potentially important source of MMHg to human consumers, other seafood products, particularly the flesh of apex marine predators, contain much higher MMHg concentrations and can result in substantially greater exposures of this contaminant for people.

Evaluation of radiation doses and associated risk from the Fukushima nuclear accident to marine biota and human consumers of seafood.

Radioactive isotopes originating from the damaged Fukushima nuclear reactor in Japan following the earthquake and tsunami in March 2011 were found in resident marine animals and in migratory Pacific bluefin tuna (PBFT). Publication of this information resulted in a worldwide response that caused public anxiety and concern, although PBFT captured off California in August 2011 contained activity concentrations below those from naturally occurring radionuclides. To link the radioactivity to possible health impairments, we calculated doses, attributable to the Fukushima-derived and the naturally occurring radionuclides, to both the marine biota and human fish consumers. We showed that doses in all cases were dominated by the naturally occurring alpha-emitter (210)Po and that Fukushima-derived doses were three to four orders of magnitude below (210)Po-derived doses. Doses to marine biota were about two orders of magnitude below the lowest benchmark protection level proposed for ecosystems (10 µGy⋅h(-1)). The additional dose from Fukushima radionuclides to humans consuming tainted PBFT in the United States was calculated to be 0.9 and 4.7 µSv for average consumers and subsistence fishermen, respectively. Such doses are comparable to, or less than, the dose all humans routinely obtain from naturally occurring radionuclides in many food items, medical treatments, air travel, or other background sources. Although uncertainties remain regarding the assessment of cancer risk at low doses of ionizing radiation to humans, the dose received from PBFT consumption by subsistence fishermen can be estimated to result in two additional fatal cancer cases per 10,000,000 similarly exposed people.

Radiocesium in Pacific bluefin tuna Thunnus orientalis in 2012 validates new tracer technique.

The detection of Fukushima-derived radionuclides in Pacific bluefin tuna (PBFT) that crossed the Pacific Ocean to the California Current Large Marine Ecosystem (CCLME) in 2011 presented the potential to use radiocesium as a tracer in highly migratory species. This tracer requires that all western Pacific Ocean emigrants acquire the (134)Cs signal, a radioisotope undetectable in Pacific biota prior to the Fukushima accident in 2011. We tested the efficacy of the radiocesium tracer by measuring (134)Cs and (137)Cs in PBFT (n = 50) caught in the CCLME in 2012, more than a year after the Fukushima accident. All small PBFT (n = 28; recent migrants from Japan) had (134)Cs (0.7 ± 0.2 Bq kg(-1)) and elevated (137)Cs (2.0 ± 0.5 Bq kg(-1)) in their white muscle tissue. Most larger, older fish (n = 22) had no (134)Cs and only background levels of (137)Cs, showing that one year in the CCLME is sufficient for (134)Cs and (137)Cs values in PBFT to reach pre-Fukushima levels. Radiocesium concentrations in 2012 PBFT were less than half those from 2011 and well below safety guidelines for public health. Detection of (134)Cs in all recent migrant PBFT supports the use of radiocesium as a tracer in migratory animals in 2012.

Pacific bluefin tuna transport Fukushima-derived radionuclides from Japan to California.

The Fukushima Dai-ichi release of radionuclides into ocean waters caused significant local and global concern regarding the spread of radioactive material. We report unequivocal evidence that Pacific bluefin tuna, Thunnus orientalis, transported Fukushima-derived radionuclides across the entire North Pacific Ocean. We measured γ-emitting radionuclides in California-caught tunas and found (134)Cs (4.0 ± 1.4 Bq kg(-1)) and elevated (137)Cs (6.3 ± 1.5 Bq kg(-1)) in 15 Pacific bluefin tuna sampled in August 2011. We found no (134)Cs and background concentrations (~1 Bq kg(-1)) of (137)Cs in pre-Fukushima bluefin and post-Fukushima yellowfin tunas, ruling out elevated radiocesium uptake before 2011 or in California waters post-Fukushima. These findings indicate that Pacific bluefin tuna can rapidly transport radionuclides from a point source in Japan to distant ecoregions and demonstrate the importance of migratory animals as transport vectors of radionuclides. Other large, highly migratory marine animals make extensive use of waters around Japan, and these animals may also be transport vectors of Fukushima-derived radionuclides to distant regions of the North and South Pacific Oceans. These results reveal tools to trace migration origin (using the presence of (134)Cs) and potentially migration timing (using (134)Cs:(137)Cs ratios) in highly migratory marine species in the Pacific Ocean.