Information about source points of anthropogenic radioactivity

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The first atomic explosion at Alamogordo, New Mexico at 5:29 A.M., July 16, 1945, ushered in an era of the systemic release of biologically significant radionuclides from anthropogenic sources. Those who created these devices of destruction never imagined the silent efficiency or the hemispheric thoroughness of the biogeochemical cycling which now make these effluents available to all the inhabitants of the biosphere.

A proliferation of anthropogenic sources of nuclear contamination, including the development of nuclear weapons, followed this first test explosion in 1945. The most obvious sources of contamination were the many nuclear weapons tests (1945-1980), but equally significant release sources were the weapons production facilities and fuel reprocessing sites which evolved with the development of military nuclear capabilities (See RAD 11 for a summary of major nuclear waste source points). The creation of atomic power stations was the inexorable result of the exploitation of the fission process for military purposes and constitutes an unfortunate footnote to the Cold War. These nuclear generating facilities provide an additional opportunity for the release of low levels of radioactivity to the environment; whether there will be another accident at a nuclear power station as severe as the one that occurred at Chernobyl remains to be seen.

The nuclear effluents released from these anthropogenic source points follow pathways, and create a baseline of nuclear contamination which can and must be documented to allow evaluation of the environmental impact of nuclear accidents such as Chernobyl as well as the future impact of releases from thousands of other potential source points of radioactive contamination.
 

PATHWAY MODELS: Nuclear weapons testing (1945-1978) resulted in local, tropospheric and stratospheric fallout patterns. Initially the low-yield "fat man" atomic weapons had only a modest input on stratospheric transport routes, but after the development of more powerful thermonuclear weapons in the mid-1950's (hydrogen bombs), stratospheric fallout became the principle mode of hemispheric transport of weapons tests fallout. Weapons testing stratospheric fallout occurred not only in a primary pulse in conjunction with a tropospheric component, but also as long-term fallout which continued in decreasing intensity over a period of decades, as documented by the Riso National Laboratories (Denmark) summary of cumulative fallout data in the next section of RADNET (RAD 8: Baseline Data).

In contrast to weapons testing pathways, Chernobyl contamination occurred primarily as a tropospheric injection of smoke and radionuclides which produced much higher than expected contamination in distant locations, as well as less than expected close-in fallout at the reactor accident site. The Chernobyl accident, which was hemispheric in its impact, serves as a model for the tropospheric dispersion of any major nuclear accident plume, given the caveat that weather conditions and reactor design help dissipate the local impact of the fallout pattern. Weapons testing fallout, Sellafield fuel reprocessing facility effluents, and later, the Chernobyl plume illustrate a fundamental reality about the biogeochemical pathways of effluents from a nuclear accident: radioactive contamination occurs not as one incident but as a series of pulses in time and space, impacting pathways to human consumption

primary pulse: direct deposition of anthropogenic nuclear effluents in the form of rapidly moving air-borne pulses of radioiodine and vaporized radionuclides (e.g. radiocesium) resulting from major nuclear accidents such as Chernobyl, with total global tropospheric transport times of as little as two weeks. Fallout from such events is associated with and maximized by rainfall (or snowfall) events which allow rapid transfer to human diet of radionuclides deposited directly in forage pathways (e.g. foliar deposition). Such transfer can occur within several days of the plume passage. Immersion, absorption and inhalation are other exposure pathways. See the EPA summary of pathway exposure in the previous section of RADNET, RAD 6.

secondary pulse: the slower movement of radioactive contamination in the abiotic environment including delayed particulate fallout, the mobilization and uptake of existing fallout, and its bioaccumulation in pathways to human consumption. Passage and uptake of the secondary (indirect) pulse of contamination from abiotic media to biological media can vary in time from weeks to years.

tertiary pulse: the delayed redistribution of wind-blown deposition, the remobilization of existing fallout, the transport of surface contamination by human activities (vehicles, foot traffic, train, marine, and air transport, on clothing, and in manufacturing processes, etc.), and the incorporation of multiple modes of pathway contamination into processed foods and consumer products which may be transferred to areas unaffected by the primary and secondary pulses of an accident plume (For an example of a tertiary pulse, see the Peak Pulse Analysis of Chernobyl Derived Radiocesium in Imported Foods in Section 9: Dietary Intake). Redistribution of wind-blown plutonium and other long-lived radionuclides from Chernobyl and military source points will continue for millenniums (²³⁹Pu 1/2T = 24,131 years).

Liquid releases from facilities such as Sellafield follow plume pathways involving a slower dispersion of the primary pulse with less obvious secondary and tertiary pulses of delayed contamination of pathways to human consumption.

Post-Chernobyl World Health Organization (WHO) Pathways Summary:

Following the Chernobyl accident, WHO issued this outline of pathways exposure:
 

Cloud Shine-Ground Shine:

Another angle from which to consider pathway exposure, cloud shine and ground shine are airborne and deposited radioactivity characterizing a nuclear accident. They provide pathways to external exposure (skin irradiation and absorption). Cloud shine and ground shine assure the presence of internal exposure pathways (inhalation, ingestion). These rapidly moving pathway pulses, which have complex radionuclide composites, are a formidable challenge to accurate biological monitoring, the prerequisite of credible dose assessment.
 

Nuclear effluents are deposited in the abiotic environment (air, water, sediment or soil) and are soon transferred to biological media and follow one or more of the above pathways to human consumption. Radioactive contamination doesn't respect national or political boundaries; just because contamination is not reported by the media of a given country does not mean it is unable to cross national boundaries invisibly and impact widely separated and often isolated population groups.

Nuclear effluents move not only in space but also in time. The rapid tropospheric transfer of radionuclides as volatile gaseous and aerosol forms occurs much more quickly than the slower dispersion of stratospheric fallout. Resuspension and remobilization of long-lived radionuclides occur long after the shorter lived radionuclides have decayed, and their movement through the biosphere can continue for thousands of years. In the first few days of a nuclear accident, the presence of ¹³¹I and other short-lived nuclides overshadows the presence of all other radionuclides. As these nuclides decay, longer-lived isotopes such as ¹³⁷Cs emerge as the principle source of exposure. The surprising lesson of the Chernobyl accident is that in between the overwhelming domination of the radioiodine isotopes and in conjunction with the dispersion of radiocesium (¹³⁷Cs: 1/2T = 30.14 years), numerous other biologically significant radionuclides such as ruthenium and tellurium also characterize an accident plume pathway as it silently moves across national boundaries. The list of indicator nuclides in the Plume Pathway Timetable, though incomplete, helps denote the complexity and duration of nuclear accidents which then can subject large population groups to low but biologically significant exposure to long-lived radionuclides for generations. The indicator nuclides listed in column one are present from the beginning of a release and provide exposure even while masked by the more intense activity levels of the shorter-lived nuclides. Long term exposure is a function of radioactive and biological half-life as well as biological and mercantile availability. In the secondary and tertiary stages of a plume pulse, exposure is primarily from inhalation and ingestion of long-lived radionuclides. The total nuclide inventory of any source term release in a major nuclear accident will vary widely depending on the type of facility at which the accident occurs. The total nuclide inventory listed below is within the same order of magnitude as the Chernobyl source term.
 

The following unannotated citations are basic information sources for understanding the fundamentals of the biogeochemical cycling of radioactive contamination in the environment.  Other biological monitoring citations are found in RAD11: Anthropogenic Radioactivity: Nuclear Power Plants: Biological Monitoring.

Aarkrog, A. (1971). Prediction models for strontium-90 and cesium-137 levels in the human food chain. Health Physics. 20. pg. 297-311.

Aarkrog, A. et al. (1987). Technetium-99 and cesium-134 as long distance tracers in Arctic waters. Estuarine, Coastal Shelf Sci. 24. pg. 637-647.

Agency for Toxic Substances and Disease Registry. (1990). Toxicological profile for plutonium. Public Health Service, U.S. Department of Health and Human Services, ATSDR, Atlanta, GA.

Assimakopoulos, P.A., Ioannides, K.G., Pakou, A.A., Mantzios, A.S. and Pappas, C.P. (August 15, 1993). Transport of radiocaesium from a sheep's diet to its tissues. Sci. Total Environ. 136(1-2). pg. 1-11.

Barber, Ruth, Plumb, Mark A., Boulton, Emma, Roux, Isabelle and Dubrova, Yuri E. (May 14, 2002). Elevated mutation rates in the germ line of first- and second-generation offspring of irradiated male mice. Proceedings of the National Academy of Sciences. 10. pg. 1073. http://www.pnas.org/cgi/content/abstract/102015399v1

Belot, Y. (1986). Transfer of long-lived radionuclides through marine food chains: A review of transfer data. J. Environ. Radioactivity. 4. pg. 83-90.

Benoit, G., Rozan, T.F., Patton, P.C. and Arnold, C.L. (March 1999). Trace metals and radionuclides reveal sediment sources and accumulation rates in Jordan Cove, Connecticut. Estuaries. 22(1). pg. 65-80.

Boelskifte, S. and Dahlgaard, H. (1985). Concentration factor of ⁶⁰Co for Fucus vesiculosus estimated by integrated water sampling. Report No. DK-4000. Riso National Laboratory, Roskilde, Denmark.

Bunzl, K., Kracke, W. and Schimmack, W. (1992). Vertical Migration of plutonium-239 and -240, americium-241 and cesium-137 fallout in a forest soil under spruce. Analyst. 117. pg. 469-474.

Carvalho, F.P. and Fowler, S.W. (1985). Americium adoption on the surfaces of macrophytic algae. J. Environ. Radioactivity. 2. pg. 311-317.

Chamberlain, A.C. (1970). Interception and retention of radioactive aerosols by vegetation. Atmos. Environ. 4. pg. 57-78.

Churchill, J.H., Hess, C.T. and Smith, C.W. (1980). Measurement and computer modeling of radionuclide uptake by marine sediments near a nuclear power reactor. Health Physics. 38. pg. 327-340.

Comans, R.N.J., Middelburg, J.J., Zonderhuis, J., Woittiez, J.R.W., De Lange, G.J., Das, H.A. and Van Der Weijden, C.H. (1989). Mobilization of radiocesium in pore water of lake sediments. Nature. 339. pg. 367-369.

Cooke, A.I., Green, N., Rimmer, D.L., Weekes, T.E.C., Wilkins, B.T., Beresford, N.A. and Fenwick, J.D. (1996). Absorption of radiocaesium by sheep after ingestion of contaminated soils. Science of the Total Environment. 192(1). pg. 21-29.

Croom, J.M. and Ragsdale, H.L. (1980). A model of radiocesium cycling in a sand hills- Turkey Oak (quercus laevis) ecosystem. Ecological Modeling. 11. pg. 55-65.

Dahlgaard, H. and Boelskifte, S. (1985). "SENSI": A model describing the accumulation and time-integration of radioactive discharges in bioindicators (Fucus and Mytilus) including seasonal variation. Riso National Laboratory, Roskilde, Denmark.

Dahlgaard, H. and Boelskifte, S. (1992). SENSI: A model describing the accumulation and time-integration of radioactive discharges in the bioindicator Fucus vesiculosus. Journal of Environmental Radioactivity. 16(1). pg. 49-64.

Diabate, S. and Strack, S. (1993). Organically bound tritium. Health Physics. 65. pg. 698-712.

Ennis, E.M., Ward, G.M., Johnson, J.E. and Boamah, K.N. (1988). Transfer coefficients of selected radionuclides to animal products. II. Hen eggs and meat. Health Physics. 54. pg. 167-170.

Fisher, N.S., Olson, B.L. and Bowen, V.T. (1980). Plutonium uptake by marine phytoplankton in culture. Limnol. Oceanogr. 25(5). pg. 823-839.

Fisher, N.S., Cochran, J.K., Krishnaswami, S. and Livingston, H.D. (1988). Predicting the oceanic flux of radionuclides on sinking biogenic debris. Nature. 335(13). pg. 622-625.

Franke, B. (1986). Development of an adequate program of environmental radiation monitoring for the TMI nuclear power facility. Institute for Energy and Environmental Research, Takoma Park, MD.

Fulker, M.J., Jackson, D., Leonard, D.R., McKay, K. and John, C. (March 1998). Doses due to man-made radionuclides in terrestrial wild foods near Sellafield. J. Radiological Protection. 18(1), pg. 3-13.

Garten, C.T. (1995). Dispersal of radioactivity by wildlife from contaminated sites in a forested landscape. Journal of Environmental Radioactivity. 29(2). pg. 137-156.

Grytsyuk, N., Arapis, G., and Davydchuk, V. (2006). Root uptake of ¹³⁷Cs by natural and semi-natural grasses as a function of texture and moisture of soils. Journal of Environmental Radioactivity, Volume 85, Issue 1, Amsterdam, The Netherlands. pg. 48-58.

Gutknecht, J. (1961). Mechanism of radioactive zinc uptake by ulva lactuca. Limnol. Oceanogr. 6. pg. 426-431.

Hakanson, L., Andersson, T. and Nilsson, A. (1992). Radioactive cesium in fish in Swedish lakes 1986-1988 - General pattern related to fallout and lake characteristics. Journal of Environmental Radioactivity. 15(3). pg. 207-230.

Hakonson, T.E., Watters, P.L. and Hanson, W.C. (1981). The transport of plutonium in terrestrialecosystems. Health Phys. 40. pg. 63-69.

Handl, J. and Pfau, A. (1987). Feed-milk transfer of fission products following the Chernobyl accident. Atomkernenergie. 49(3). pg. 171-173.

Harvey, R.S. (1964). Uptake of radionuclides by fresh water algae and fish. Health Physics. 10. pg. 243-247.

Harvey, R.S. (1973). Temperature effects on the sorption of radionuclides by aquatic organisms. Report No. DP-MS-73-8. Prepared in connection with work under Contract No. AT(07-2)-1 with the U.S. Atomic Energy Commission, Washington, D.C.

Hess, C.T., Smith, C.W. and Price, A.H. (1975). Model for the accumulation of radionuclides in oysters and sediments. Nature. 258(5532). pg. 225-226.

Hetherington, J.A. (1978). The uptake of plutonium nuclides by marine sediments. Mar. Sci. Commun. 4. pg. 239-274.

Hinton, T.G., McDonald, M., Ivanov, Y., Arkhipov, N. and Arkhipov, A. (1996). Foliar absorption of resuspended ¹³⁷Cs relative to other pathways of plant contamination. Journal of Environmental Radioactivity. 30(1). pg. 15-30.

Hinton, T.G., Stoll, J.M. and Tobler, L. (1995). Soil contamination of plant surfaces from grazing and rainfall interactions. Journal of Environmental Radioactivity. 29(1). pg. 11-26.

Honjo, S., Manganini, S.J. and Cole, J.J. (1982). Sedimentation of biogenic matter in the deep ocean. Deep-Sea Research. 29(5). pg. 609-625.

Hunt, G.J. (1998). Transfer across the human gut of environmental plutonium, americium, cobalt, caesium and technetium:  Studies with cockles (Cerostoderma edule) from the Irish Sea. J. Radiol. Prot. 18(1). pg. 1-9.

Hunt, G.J., and Kershaw, P.J. (1990). Remobilisation of artificial radionuclides from the sediment of the Irish Sea. J. Radiol. Prot. 10(2). pg. 147-151.

Hunt, G.J., Hewitt, C.J. and Shepherd, J.G. (1982). The identification of critical groups and its application to fish and shellfish consumers in the coastal area of the north-east Irish Sea. Hlth. Phys. 43. pg. 875-889.

Hunt, G.J., Leonard, D.R.P. and Lovett, M.B. (1990). Transfer of environmental plutonium and americium across the human gut. Sci. Total Environ. 90. pg. 273-283.

Johanson, K.J., Bergstrom, R.V., Bothmer, S. and Karlen, G. (1990). Radiocesium in wildlife of a forest ecosystem in central Sweden. Transfer of radionuclides in natural and seminatural environments. Elsevier Applied Science, London. pg. 183-193.

Johnson, J.E., Ward, G.M., Ennis, M.E. and Boamah, K.N. (1988). Transfer coefficients of selected radionuclides to animal products. I. Comparison of milk and meat from dairy cows and goats. Health Physics. 54. pg. 161-166.

Kammerer, L., Hiersche, L. and Wirth, E. (1994). Uptake of radiocesium by different species of mushrooms. Journal of Environmental Radioactivity. 23(2). pg. 135-150.

Knowles, J.F., Smith, D.L. and Winpenny, K. (1998). A comparative study of the uptake, clearance and metabolism of technetium in lobster (Homarus gammarus) and edible crab (Cancer pagurus). Radiation Protection Dosimetry. 75. pg. 125-129.

Kudo, A., Ed. (2001). Radioactivity in the environment: Plutonium in the environment: Edited proceedings of the Second Invited International Symposium. Volume 1. Elsevier, NY, NY.

Larsen, R.J., Haagenson, P.L. and Reiss, N.M. (1989). Transport processes associated with the initial elevated concentrations of Chernobyl radioactivity in surface air in the United States. Journal of Environmental Radioactivity 10(1). 1-18.

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McCarthy, J.F., Sanford, W.E. and Stafford, P.L. (November 11, 1998). Lanthanide field tracers demonstrate enhanced transport of transuranic radionuclides by natural organic matter. Environmental Science and Technology. Web edition <http://acsinfo.acs.org>. ASAP article.

Monte, L., Quaggia, S., Pompei, F. and Fratarcangeli, S. (1990). The Behavior of ¹³⁷Cs in some edible fruits. Journal of Environmental Radioactivity. 11(3). pg. 207-214.

Murphy, C.E., Jr. (1993). Tritium transport and cycling in the environment. Health Phys. 65(6). pg. 683-697.

Murphy, C.E. and Pendergast, M.M. (1979). Environmental transport and cycling of tritium in the vicinity of atmospheric releases.Behavior of tritium in the environment. IAEA-SM-232/80. International Atomic Energy Agency, Vienna.

Murphy, G.E. (1993). Tritium transport and cycling in the environment. Health Physics. 65. pg. 683-697.

Nelson, V.A. and Seymour, A.H. (1972). Oyster research with radionuclides: A review of selected literature. Proceedings of the National Shellfisheries Association. 62. pg. 89-93.

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Patton, T.L. and Penrose, W.R. (1989). Fission product tin in sediments. Journal of Environmental Radioactivity. 10(3). pg. 201-212.

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Platt, R. B., Palms, J.M., Ragsdale, H.L., Shure, D.J., Mayer, P.G. and Mohrbacher, J. A. (1973). Empirical benefits derived from an ecosystem approach to environmental monitoring of a nuclear fuel reprocessing plant. Environmental behavior of radionuclides released in the nuclear industry. International Atomic Energy Agency, Vienna.

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Prosser, S.L., Popplewell, D.S. and Lloyd, N.C. (1994). The radiological significance of ²³⁷Np in the environment. Journal of Environmental Radioactivity. 23(2). pg. 123-134.

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