Uranium, Thorium and Anthropogenic Radionuclides as Atmospheric Tracers

  • K. HiroseEmail author
Part of the Advances in Isotope Geochemistry book series (ADISOTOPE)


Anthropogenic radionuclides (137Cs, 90Sr, Pu isotopes and others) and uranium and thorium in rainwater and airborne dust are useful tracers for better understanding of atmospheric transport processes, micrometeorological processes, and natural and human induced environmental changes. Typically, analyses on spatial and temporal changes of anthropogenic radonuclides have aided to constrain the time scale of atmospheric transport of aerosols, such as stratosphere and troposphere residence times of aerosols. Although uranium and thorium in the atmosphere are used primarily as tracers of soil dust, their levels and isotope ratios have been significantly perturbed by anthropogenic sources, (e.g., fly ash and accidental releases of uranium). Therefore, uranium, thorium and their isotope ratios in airborne dust and rainwater reflect environmental changes caused by human activities and climate change. Taking into account that rates of anthropogenic radioactive fallout have recently been boosted by the resuspension of radionuclides in deposited particles, recent variations of anthropogenic radionuclides in rainwater and surface air, as well as thorium and uranium isotopes, is important tracers to study ongoing terrestrial environmental changes due to human activities.


Deposition Sample Meteorological Research Institute Anthropogenic Radionuclide Washout Ratio Thorium Isotope 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.



We thank Pavel P. Povinec of Comenius University and Michio Aoyama and Yasuhito Igarashi of the Geochemical Research Department, MRI, for their help in preparing the manuscript. We also thank two reviewers (Gi-Hoon Hong and Paul Martin) and the editor (Mark Baskaran) for their constructive comments and suggestions.


  1. Aoyama M (1988) Evidence of stratospheric fallout of caesium isotopes from the Chernobyl accident. Geophys Res Lett 15:327–330Google Scholar
  2. Aoyama M (1999) Geochemical studies on behavior of anthropogenic radionuclides in the atmosphere, PhD Thesis, Kanazawa UniversityGoogle Scholar
  3. Aoyama M, Hirose K, Suzuki Y, Inoue H, Sugimura Y (1986) High level radioactive nuclides in Japan in May. Nature 321:819–820Google Scholar
  4. Aoyama M, Hirose K, Sugimura Y (1991) The temporal variation of stratospheric fallout derived from the Chernobyl accident. J Environ Radioact 13:103–115Google Scholar
  5. Aoyama M, Hirose K, Takatani S (1992) Particle size dependent dry deposition velocity of the Chernobyl radioactivity. In: Schwartz SE, Slinn WGN (eds) Precipitation scavenging and atmospheric-surface exchange processes: fifth international conference, hemisphere, vol 3., pp 1581–1593Google Scholar
  6. Aoyama M, Hirose K, Igarashi Y (2006) Re-construction and updating our understanding on the global weapons tests 137Cs fallout. J Environ Monitor 8:431–438Google Scholar
  7. Arimoto R, Webb JL, Conley M (2005) Radioactive contamination of atmospheric dust over southeastern New Mexico. Atmos Environ 39:4745–4754Google Scholar
  8. Barrie LA (1985) Scavenging ratios, wet deposition, and in-cloud oxidation: an application to the oxides of sulphur and nitrogen. J Geophys Res 90:5789–5799Google Scholar
  9. Baskaran M, Coleman CH, Santschi PH (1993) Atmospheric depositional fluxes of 7Be and 210Pb at Galveston and College Station, Texas. J Geophys Res 98:20, 555–520, 571Google Scholar
  10. Baskaran M, Hong GH, Santschi PH (2009) Radionuclide analysis in seawater. In: Wurl O (ed) Practical guidelines for the analysis of seawater. CRC Press, Boca Raton, pp 259–304Google Scholar
  11. Berne A (1995) Use of EICroM TRU RESIN in the determination of americium, plutonium and uranium in air filter and water samples. USDOE Report EML-575Google Scholar
  12. Cambray RS, Fisher EMR et al (1968) Radioactive fallout in air and rain: Result to the middle of 1968. AERE-R 5899 HMSO, LondonGoogle Scholar
  13. Chamizo E, Jimenez-Romos MC et al (2008) Isolation of Pu-isotopes from environmental samples using ion chromatography for accelerator mass spectrometry and alpha spectrometry. Anal Chim Acta 606:239–245Google Scholar
  14. Crecelius EA, Robertson DE et al (1978) Atmospheric deposition of 7Be and other elements on the Washington coast. Pacific Northwest Laboratory Annual Report for 1977 to the DOE Assistant Secretary for Environment: Ecological Sciences, PNL-2500 PT-2, Battelle, Pacific Northwest Laboratory, pp 7.25–7.26Google Scholar
  15. Englemann RJ (1971) Scavenging prediction using ratios of concentrations in air and precipitation. J Appl Meteorol 10:493–497Google Scholar
  16. Faure G (1986) Principles of isotope geology, 2nd edn. Wiley, New YorkGoogle Scholar
  17. Feng J-L, Zhu L-P et al (2008) Heavy dust fall in Beijing, on April 16–17, 2006: geochemical properties and indications of the dust provenance. Geochem J 42:221–236Google Scholar
  18. Fujiwara H, Fukuyama T et al (2007) Deposition of atmospheric 137Cs in Japan associated with the Asian dust event of March 2002. Sci Total Environ 384:306–315Google Scholar
  19. Grabowska S, Mietelski JW et al (2003) Gamma emitters on micro-Becquerel activity level in air at Krakow (Poland). J Atmos Chem 46:103–116Google Scholar
  20. Hardy EPJr (1977) Final tabulation of monthly 90Sr data, 1954–1976. USERDE Report HASL-329Google Scholar
  21. Harley JH (1980) Plutonium in the environment– a review. J Radiat Res 21:83–104Google Scholar
  22. Harvey MJ, Matthews KM (1989) 7Be deposition in a high-rainfall area of New Zealand. J Atmos Chem 8:299–306Google Scholar
  23. Hirose K (1995) Geochemical studies on the Chernobyl radioactivity in environment. J Radioanal Nucl Chem Articles 197:315–335Google Scholar
  24. Hirose K (2000) Dry and wet deposition behaviors of thorium isotopes. J Aerosol Res Jpn 15:256–263Google Scholar
  25. Hirose K, Aoyama M et al (1987) Annual deposition of Sr-90, Cs-137 and Pu-239,240 from the 1961–1980 nuclear explosions: a simple model. J Meteor Soc Japan 65:259–277Google Scholar
  26. Hirose K, Takatani S, Aoyama M (1993) Wet deposition of radionuclides derived from the Chernobyl accident. J Atmos Chem 17:61–71Google Scholar
  27. Hirose K, Igarashi Y et al (2001) Long-term trends of plutonium fallout observed in Japan. In: Kudo A (ed) Plutonium in the environment. Elsevier Science, Amsterdam, pp 251–266Google Scholar
  28. Hirose K, Igarashi Y et al (2003) Recent trends of plutonium fallout observed in Japan: plutonium as a proxy for desertification. J Environ Monitor 5:1–7Google Scholar
  29. Hirose K, Kim CK et al (2004) Plutonium deposition observed in Daejeon, Korea: wet and dry depositions of plutonium. Sci Total Environ 332:243–252Google Scholar
  30. Hirose K, Igarashi Y, Aoyama M (2007) Recent trends of plutonium fallout observed in Japan: comparison with natural lithogenic radionuclides, thorium isotopes. J Radioanal Nucl Chem 273:115–118Google Scholar
  31. Hirose K, Igarashi Y, Aoyama M (2008) Analysis of 50 years records of atmospheric deposition of long-lived radionuclides in Japan. Appl Radiat Isot 66:1675–1678Google Scholar
  32. Hirose K, Igarashi Y et al (2010) Depositional behaviors of plutonium and thorium at Tsukuba and Mt Haruna in Japan indicate the sources of atmospheric dust. J Environ Radioact 101:106–112Google Scholar
  33. Hirota M, Nemoto K et al (2004) Spatial and temporal variations of atmospheric 85Kr observing during 1995–2001 in Japan: estimation of atmospheric 85Kr inventory in the northern hemisphere. J Rad Res 45:405–413Google Scholar
  34. Hong G-H et al (2011) Applications of anthropogenic radionuclides as tracers to investigate marine environmental processes. In: Baskaran M (ed) Handbook of environmental isotope geochemistry. Springer, HeidelbergGoogle Scholar
  35. IAEA (1986) Summary Report on the Post-Accident Review Meeting on the Chernobyl Accident. Safety Series No. 75-INSAG-1, International Atomic Energy Agency, ViennaGoogle Scholar
  36. IAEA (2006) Experimental consequences of Chernobyl accident and their mediation: twenty years of experience. Report of the Chernobyl Forum Expert Group ‘Environment’, Radiological assessment reports series, International Atomic Energy Agency, ViennaGoogle Scholar
  37. IAEA/AQ/11 (2009) A procedure for the rapid determination of Pu isotopes and Am-241 in soil and sediment samples by alpha spectrometry, IAEA Analytical Quality in Nuclear Application Series No. 11, International Atomic Energy Agency, ViennaGoogle Scholar
  38. Igarashi Y, Otsuji-Hatori M, Hirose K (1996) Recent deposition of 90Sr and 137Cs observed in Tsukuba. J Environ Radioact 31:157–169Google Scholar
  39. Igarashi Y, Aoyama M et al (2001) Is it possible to use 90Sr and 137Cs as tracers for the aeolian transport? Water Air Soil Poll 130:349–354Google Scholar
  40. Igarashi Y, Aoyama M et al (2003) Resuspension: decadal monitoring time series of the anthropogenic radioactivity deposition in Japan. J Rad Res 44:319–328Google Scholar
  41. Igarashi Y, Inomata Y et al (2009) Possible change in Asian dust source suggested by atmospheric anthropogenic radionuclides during the 2000s. Atmos Environ 43:2971–2980Google Scholar
  42. Karlsson L, Hernandez F et al (2008) Using 137Cs and 40K to identify natural Saharan dust contributions to PM10 concentrations and air quality impairment in the Canary Islands. Atoms Environ 42:7034–7042Google Scholar
  43. Katsuragi Y (1983) A study of 90Sr fallout in Japan. Papers Meteor Geophys 33:277–291Google Scholar
  44. Katsuragi Y, Aoyama M (1986) Seasonal variation of Sr-90 fallout in Japan through the end of 1983. Pap Meteor Geophys 37:15–36Google Scholar
  45. Katsuragi Y, Hirose K, Sugimura Y (1982) A study of plutonium fallout in Tokyo through the end of 1966. Papers Meteor Geophys 33:85–93Google Scholar
  46. Kikawada Y, Oda K et al (2009) Anomalous uranium isotope ratio in atmospheric deposits in Japan. J Nucl Sci Tech 46:1094–1098Google Scholar
  47. Kim CS, Kim CK et al (2000) Rapid determination of Pu isotopes and atom ratios in small amounts of environmental samples by an on-line sample pre-treatment system and isotope dilution high resolution inductively coupled plasma spectrometry. J Anal At Spectrom 15:247–255Google Scholar
  48. Kim CS, Kim CK et al (2007) Determination of Pu isotope concentrations and isotope ratio by inductively coupled plasma mass spectrometry: a revies of analytical methodology. J Anal At Spectrom 22:827–841Google Scholar
  49. Kolb W (1989) Seasonal fluctuations of the uranium and thorium contents of aerosols in ground-level air. J Environ Radioact 9:61–75Google Scholar
  50. Krey PW, Krajewksi BT (1970) Comparison of atmospheric transport model calculations with observations of radioactive debris. J Geophys Res 75:2901–2908Google Scholar
  51. Krey PW, Leifer R et al (1979) Atmospheric burn-up of the Cosmos-954 reactor. Science 205:583–585Google Scholar
  52. Kurosaki Y, Mikami M (2003) Recent frequent dust events and their relation to surface wind in East Asia. Geophys Res Lett 30:1736. doi: 10.1029/2003GL017261 CrossRefGoogle Scholar
  53. Lee SH, Pham MK, Povinec PP (2002) Radionuclide variations in the air over Monaco. J Radioanal Nucl Chem 254:445–453Google Scholar
  54. Lee HN, Igarashi Y et al (2006) Global model simulations of the transport of Asian and Sahara dust: total deposition of dust mass in Japan. Water Air Soil Poll 169:137–166Google Scholar
  55. Lu X, Jia X, Wang F (2006) Natural radioactivity of coal and its by-products in the Baoji coal-fire power plant, China. Cur Sci 91:1508–1511Google Scholar
  56. Lujaniené G, Aninkevicius V, Lujanas V (2009) Artificial radionuclides in the atmosphere over Lithuania. J Environ Radioact 100:108–119Google Scholar
  57. Martin P (2003) Uranium and thorium series radionuclides in rainwater over several tropical storms. J Environ Radioact 65:1–18Google Scholar
  58. Matsunami T, Mamuro T (1975) Study of uranium deposition by basin method. Ann Rep Radiat Cen Osaka Pref 16:22–24Google Scholar
  59. McNeary D, Baskaran M (2003) Depositional characteristics of 7Be and 210Pb in southeastern Michigan. J Geophy Res 108: D7, 4201, doi: 10.1029/2002JD003021.
  60. Nicholson KW (1988) A review of particle resuspension. Atmos Environ 22:2639–2651Google Scholar
  61. Otsuji-Hatori M, Igarashi Y, Hirose K (1996) Preparation of a reference fallout material for activity measurements. J Environ Radioact 31:143–155Google Scholar
  62. Papastefanou C (2010) Escaping radioactivity from coal-fired plants (CPPs) due to coal burning and associated hazards: a review. J Environ Radioact 101:191–200Google Scholar
  63. Pennannen AS, Sillanpää M et al (2007) Performance of a high-volume cascade impactor in six European urban environments: mass measurement and chemical characterization of size segregated particulate samples. Sci Total Environ 15:297–310Google Scholar
  64. Reiter ER, Bauer E (1975) Residence times of atmospheric pollutant. CIAP Monogr.1, US Department of Transportation, Washington DCGoogle Scholar
  65. Roos P (2008) Analysis of radionuclides using ICP-MS. In: Povinec PP (ed) Analysis of environmental radionuclides, Elsevier Science, Amsterdam, pp 295–330Google Scholar
  66. Rosner G, Winkler R (2001) Long-term variation (1986–1998) of post-Chernobyl 90Sr, 137Cs, 238Pu and 239,240Pu concentrations in air, depositions to ground, resuspension factors and resuspension rates in south Germany. Sci Total Environ 273:11–25Google Scholar
  67. Sakuragi Y, Meason JL, Kuroda PK (1983) Uranium and plutonium isotopes in the atmosphere. J Geophys Res 88:3718–3724Google Scholar
  68. Schmel GA (1980) Particle and gas dry deposition: a review. Atmos Environ 14:983–1011Google Scholar
  69. Slinn WGN (1978) Parametrizations for resuspension and for wet and dry deposition of particles and gases for use in radiation dose calculations. Nucl Saf 19:205–219Google Scholar
  70. Tadmor J (1986) Radoactivity from coal-fired plants. A review. J Environ Radioact 4:177–204Google Scholar
  71. Turekian KK, Cochran JK (1981) 210Pb in surface air at Enewetak and the Asian dust to the Pacific. Nature 292:522–524Google Scholar
  72. Turekian KK, Graustein WC, Cochran JK (1989) Lead-210 in the SEAREX Program: an aerosol tracer across the Pacific. In: Duce RA (ed) Chemical oceanography, vol 10. Academic, San Diego, pp 51–80Google Scholar
  73. UNSCEAR (2000) Sources and effects of ionizing radiation, vol. 1: Sources, United Nations Scientific Committee on the Effects of Atomic Radiation, United Nations, New YorkGoogle Scholar
  74. Warneke T, Croudace IW et al (2002) A new ground-level fallout record of uranium and plutonium isotopes for northern temperate latitudes. Earth Planet Sci Lett 203:1047–1057Google Scholar
  75. Weiss W, Sittkus A et al (1983) Large-scale atmospheric mixing derived from meridional profiles of krypton 85. J Geophys Res 88:8574–8578Google Scholar
  76. Weyer S, Anbar AD et al (2008) Natural fractionation of 238U/235U. Geochim Cosmochim Acta 72:345–359Google Scholar
  77. Yang J (2007) Concentration and distribution of uranium in Chinese coals. Energy 32:203–212Google Scholar
  78. Yoschenko VI, Kashparov AV et al (2006) Resuspension and redistribution of radionuclides during grassland and forest fires in the Chernobyl exclusion zone: part I, Fire experiments. J Environ Radioact 86:143–163Google Scholar
  79. Zhang Y, Zheng J et al (2010) Characterization of Pu concentration and its isotopic composition in a reference fallout material. Sci Total Environ 408:1139–1144Google Scholar

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© Springer-Verlag Berlin Heidelberg 2012

Authors and Affiliations

  1. 1.Department of Materials and Life SciencesSophia UniversityTokyoJapan

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