GEOPHYSICS, VOL. 45, NO. 11 (NOVEMBER 1980); P. 1690-1694.

Radioactivity method

J. S. Duval*
Radioactivity measurementshave played an important role in geophysics since about 1935, and they have increasedin importance to the present. The most important areas of application have been in petroleum and uranium exploration. Radioactivity measurements have proved useful in geologic mapping, as well as in specialized applications such as reactor-site monitoring. The technological development of the method has reached a plateau, and the future of the method for some applications will depend upon development of more sophisticateddata processing and interpretation.
INTRODUCTION

The phrase radioactivity in geophysics could well include all techniquesinvolving the measurement of radiation. For the purposesof this paper, it is restricted to passive methods that measure gamma radiation from naturally occurring radioactive elements. The radioactive elements (radioelements) presentin the Earth s crust in sufficient quantity to be readily detected by measuring gamma radiation are the isotope 40K, members of the 238U decay series, and members of the 232Th decay series. Most of the gamma-ray measurement techniques applied in geophysics measuregamma rays from 4oK, 214Bi of the 238Useries,and20sTlofthe232Thseries. Theenergies and relative intensities of the gamma rays emitted by these elements were given by Kogan et al (197 1) and by Adams and Gasparini (1970). The theory and mathematics of radioactive decay were elegantly presented by Evans (1955). INSTRUMENTATION The instrumentation used to make radioactivity measurements has been consistently improved and refined through the rapid implementation of new technology. Some of the earliest radioactivity measurementswere made using ionization chambers and electrometers to obtain borehole measurements in 1935 (Howell and Frosch, 1939). Shortly thereafter, Geiger-Mueller tubes sensitive to gamma radiation were developed (Evans and Mugele, 1936) and quickly applied to geologic problems around the

world (Rothe and Kopcewicz, 1937; Gorshkov and Kurbatov, 1937; Landsberg, 1939). In the late 194Os, portable Geiger counters weighing about 10 kg became available (Test, 1947). About the same time research into the use of scintillation detectors was producing promising results which indicated that thallium-activated sodium-iodide crystals produced the greatest sensitivity to gamma radiation (Hofstadter, 1949). In 1949, R. W. Pringle and K. I. Roulston of the University of Manitoba developed a portable scintillation counter that could be used as a spectrometer to distinguish between uranium and thorium in ores by discriminating gamma rays with energies unique to each decay series, and a commercial version of the instrument became available in 1950 (Brownell, 1950). With the invention of the transistor in the early 1950s the instruments used for radioactivity measurementsbecame lighter, more compact, and more sophisticated. Portable gamma-ray spectrometers that made possible the in-situ measurement.of the concentrationsof potassium (K), equivalent uranium (eU), and equivalent thorium (eTh) were developed in the late 1950s and early 1960s (Schneider and Schwerdtel, 1960; Adams, 1961). By 1968 gammaray spectrometry was also being used for aerial surveys (Darnley, 1968). During the 1970s the trend in portable instruments was toward increasingly compact and versatile models. Currently available portable gamma-ray spectrometers have options for spectrum stabilization, automatic correction for

U.S. Geological Survey, Box 25046, M. S. 964, Denver Federal Center, Denver,CO 80225. 0016~8033/80/1101-1690 $03.00. This paper was prepared by an agencyof the U.S. government.

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Radioactivity Method Compton scattering, and analog and digital outputs for recording the data. These portable instruments can be usedfor hand-carried field surveys, auto-borne surveys, or aerial surveys. The 1970s trend in aerial gamma-ray spectrometerswas toward larger crystal volumes [up to 54.5 liters of NaI (Tl)], more rugged crystal design (as many as 512 spectral energy windows rather than the four energy windows normally used), and microprocessor and minicomputer data-acquisition systems. PETROLEUM EXPLORATION Radioactivity measurements were first used in petroleum exploration in boreholes in 1935, when an electrometerwith an amplifier and galvanometer were used (Howell and Frosch, 1939). High-pressure ionization chamberswere also used, but Geiger tubes proved to be better because of greater sensitivity and ease of use; Geiger tubes were used until more sensitive NaI (Tl) scintillation detectors became commercially available in the early 1950s. Since that time the gamma-ray sonde (borehole logging tool) has improved in mechanical construction, in temperature range, and in the type and stability of the electronics; however, the measurement, which is the total or gross gamma intensity, has not changed. The initial impetus behind the development of the gamma-ray sondewas the need to obtain logs of cased holes in order to locate cased-off production zones becauseelectrical methods could not be used (Sawdon, 1944). The potential of gamma-ray logs for stratigraphic correlation was quickly recognized (Landsberg, 1939) and has become one of the primary uses of the method. Other applications for which gamma-ray logs have been used include (1) clarification of other subsurface records (such as electric logs) by providing additional information to aid interpretation, (2) checking depths and thicknesses of strata, (3) location and delineation of camotite-doped cement behind casing (carnotite is a radioactive uranium mineral), and (4) lithologic logging. By 1949, radioactivity well logs had become commonplace in the petroleum industry, and some 18,000 gamma-ray logs had been made in United Stateswells alone (Fearon, 1949). Since that time the gamma-ray sonde has come to be one of the standard tools used in petroleum exploration and will undoubtedly continue to be used in the foreseeable future. Attempts also were made to use aerial gamma-ray surveys. Lundberg et al (1952) were among the first to advocate the use of gamma-ray surveys, and they made the claim that several new oil fields were found

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using radioactivity data. The use of this method and the mechanisms proposed to explain the apparent correlation of radioactivity data with deeply buried petroleum deposits were controversial, although various authors (Lobdell et al, 1954; Kellogg, 1957; Walker and Litzenberg, 1959; Langford, 1962) continued to support its use for some time Gregory (1956) made a careful comparison of aerial gammaray data over two oil fields with the geologic, pedological, and hydrological characteristics of the surface materials and concluded that the radiometric patternsreflected those characteristicsand had only a fortuitous correlation with the petroleum deposits. Alekseyev and Gottikh (1966) reached similar conclusions, except that they concluded radiometric surveys could be used to study and delineate tectonic features that might relate to petroleum occurrences. Foote (1969a) argued that previous radioactivity surveys were inadequate for petroleum exploration and that high-sensitivity gamma-ray spectrometric data properly corrected for cosmic radiation, airborne 214Bi, and pedologic features could provide a definitive test of the usefulnessof aerial radiometric surveys in petroleum exploration. Armstrong and Heemstra (1972a, b) argued for and presenteda geochemical model to explain the existence of radiometric anomalies over oil fields. Although the application of aerial radiometric surveys to petroleum exploration still has some proponents and has apparently been used with some successin the U.S.S.R., it has met with little acceptance in the petroleum industry becauseit has not been proven to work consistently. Because it has been extensively tested with inconclusive results and because other effective exploration techniques are available, a reexamination of the method for future exploration programs is not very likely. URANIUM EXPLORATION Prior to World War II, uranium exploration was essentially nonexistent except in finding high-grade uranium deposits as a source of radium and special uses, such as camotite for doping cement used in oil wells. After the war, uranium exploration became increasingly important, and aerial, ground, and borehole radioactivity methods were quickly developed. In the early ground surveys, portable GeigerMueller counters were used, and the prospectors using them frequently had little or no understanding of uranium geochemistry or radioactivity. Nevertheless, a number of uranium deposits were found using simple prospecting techniques (Ridland, 1945; Savage, 1949). When portable scintillation counters

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Duval U.S. Atomic Energy Commission (USAEC) led the way in developing probes specifically for uranium exploration (Comstock, 1956) and provided model boreholes and methods for calibration and quantitative interpretationof the logs (Scott et al, I96 I : Scott, 1963). Although Dodd et al ( 1970) suggested the need for borehole gamma-ray spectroscopy. gross-count gamma logs are the only type used extensively by industry. In recent years, however. the economic cut-off grades of uranium ores have decreasedto the point that radioactivity of natural concentrations of potassium and thorium have a significant effect on the calculated gross-count uranium grade. Hence, borehole spectroscopyis now being used to eliminate the effects of potassiumand thorium. High-resolution downhole gamma-ray spectromctcr probes are also being used to circumvent the problem of disequilibrium between uranium and its daughter products, which emit most of the gamma rays detected by gross-countmeasurements (Goldman and Marr, 1979; Senftle et al, 1976). OTHER APPLICATIONS In addition to petroleum and uranium exploration, radioactivity surveyshave been applied to a variety of problems. One of the most important of these has been as an aid to geologic mapping. The fact that gamma-ray intensitiesvary as a function of the lithology was recognized as early as 1939 (Landsberg, 1939). Since that time both ground and aerial gross-count gamma-ray surveys have been used to aid geologic mapping. In 1970, Darnley and Grasty (1971) presentedevidence that spectrometricsurveys offer distinct advantagesin mapping applications. but gross-count surveys continue to be used. Gamma-ray borehole logs have also been used in the exploration and evaluation of mineral deposits other than uranium. Tixier and Alger (1970) reviewed gamma-ray and other logging techniques as applied to coal and evaporite deposits. Bond et al (I 969) and Speranskii(1966) provided more detailed discussions of the application to coal exploration, and Costello and Norquay (1970) and Edwards et al (1967) described the application to evaporite and potash deposits. Bird (1965) described the use of gammaray logs to aid in the evaluation of salt deposits. Some other applicationsthat are not widely known include underwater applications for mineral exploration (Summerhayes et al, 1970) and for geologic mapping (Miller and Symons. 1973). monitoring the natural radioactivity at reactor sites (Bates, 1964; MacKallor, 1965), locating lost radioactive sources (Deal et al, 1972), measuring the water equivalent

became available in the 195Os,they quickly replaced the Geiger countersas a standardtool of the uranium explorationists. Brownell (1950) reported the results of a survey in Canada which was one of the first to use a portable scintillation counter. Portable grosscount scintillation counters are still popular for groundradiometric surveys and for ore-grade control surveysin uranium mines, although portable gammaray spectrometersare commonly used and their use will increase in future years. Experiments with aerial gamma-ray surveys were conducted beginning as early as 1948 in Canada (Godby et al, 1952), the United States (Stead, 1950), and England (Pierson and Franklin, 1951). Initially, aerial surveys measured total- or grosscount radioactivity, and numerous uranium deposits were discovered using aerial survey data (Boyle, 1956; Baranov, 1956; MacKevett, 1958; Loomis and Blair, 1959). During the 196Os, aerial gamma-ray spectrometers became more common because of their ability to discriminate the radioelements and because transistorized electronics made compact systems possible. In the late 196Os, large-volume [on the order of 50 liters of Nal(TI)] detectors, spectrometerswith multichannel analyzers, and complex data processing were developed in the United States (Foote, 1969b) and in Canada (Darnley. 1970). Beginning about 1970, the Geological Survey of Canada took the lead in researchand development of what has become known as high-sensitivity aerial gamma-ray spectrometry, and the Canadian government began a large-scale program to obtain aerial gamma-ray radioactivity data over most of Canada. Other countries have adopted similar programs; the National Uranium Resource Evaluation program (NURE) of the United States is one of the largest. Perhapsone of the most significant innovations for aerial and ground gamma-ray surveys was the establishment of calibration facilities in Canada (Grasty and Damley, 197 I) and in the United States (Ward, 1978). These calibration facilities have made it possible to report aerial survey data as apparent surface concentrationsof the radioelements. Laboratory analyses of surface samples can differ significantly from these aerial data because of effects of the averaging nature of the aerial measurements, soil moisture, and airborne bismuth. Nevertheless, the apparent surface concentration units are more meaningful to geologists, and they permit ready comparison between the results of different surveys. Borehole radioactivity logging in uranium exploration was quickly developed by adapting equipment and methods used in petroleum exploration. The

Radloactlvrity Method amountsof snow (Kogan et al, 1969; Grasty, 1973), and soil mapping (Schwarzer and Adams, 1973). THE FUTURE The measurementof natural radioactivity has been, and will continue to be, an important technique in exploration geophysics. In petroleum exploration, gross-countgamma-ray logs will continue to play a significant role but will remain technically stable except for minor improvements in equipment and interpretation. In uranium exploration, both surface and aerial equipmenthas reacheda plateauof sophistication and exploration equipment will continue the trend toward downhole spectroscopy. Because the interpretation of radioactivity data in uranium exploration has been largely confined to simple and obvious anomalies, and becausemost such anomalies have been found in many parts of the world, the future of surface radioactivity measurements in uranium exploration will depend upon the development of more sophisticateddata processingand interpretation. In geologic mapping, radioactivity data will continue to be used, and a trend toward the use of spectrometric data will develop. In particular, the massive data set produced by the National Uranium Resource Evaluation program of the U. S. Department of Energy should prove to be very useful for geologic mapping as well as mineral exploration for minerals other than uranium. Reactor site monitoring will continue as long as power reactors exist. Other specialized uses such as underwater applications, snow-water equivalent measurements, and soils mapping may continue, but any widespread use for these purposes seems unlikely. REFERENCES Adams, J. A. S., 1961, Radiometric determination of
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in a brine field, in Second symposium on salt, proc.: Northern Ohio Geol. Sot., v. 2, p. 57-69. Bond, L. O., Alger, R. P., and Schmidt, A. W., 1969, Well logging applications in coal mining and rock mechanics: AIME preprint no. 69-F-13. Boyle, T. L., 1956, Airborne radiometric surveying, in Peaceful uses of atomic energy, v. 6, Geology of Uranium and Thorium, Geneva, 19.55, Proceedings: New York, United Nations, p. 744-747. Brownell, G. M., 1950, Radiation surveys with a scintillation counter: Econ. Geol., v. 45, p. 167-174. Comstock, S. S., 1956, Scintillation drillhole logging, in Peaceful usesof atomic energy, v. 6, Geology of Uranium and Thorium, Geneva, 1955, Proceedings: New York, United Nations, p. 722-725. Costello, J. T., and Norquay, I. P., 1970, Logging the prairie evaporite formation in Saskatchewan, in Mining and groundwater geophysicsil967, Niagara Falls, 1967, proceedings:Ottawa, Geol. Surv. of Canada, econ. geol. rep. 26, p. 492-496. Damley, A. G., 1968, Helicopter tests with a gamma-ray spectrometer:Canadian Mining J., v. 89, p. 104-106. 1970, Airborne gamma-ray spectrometry: Can. Inst. of Mining and Metallurgy Trans., v. 73, p. 20-29. Damley, A. G., and Grasty, R. L., 1971, Mapping from the air by gamma-ray spectrometry, in Geochemical exploration, Toronto, 1970, Proceedings: Can. Inst. of Min. and Metal., special volume 11, p. 485-500. Deal, L. J., Doyle, I. F., Burson, Z. G., and Boyns, P. K., 1972, Locating the lost Athena rocket in Mexico by Aerial Radiological Measuring System (ARMS): Health Phys., v. 23, p. 95-98. Dodd, P. H., Droullard, R. F., and Lathan, C. P., 1970, Borehole logging methods for exploration and evaluation of uranium deposits, in Mining and groundwater geophysics, Niagara Falls, 1967, Proceedings: L. W. Morley, Ed., Ottawa, Geol. Sur. Can., econ. geol. rep. 26, p. 401-415. Edwards, J. M., Ottinger, N. H., and Haskell, R. E., 1967, Nuclear log evaluation of potash deposits, in SPWLA 8th Annual Logging Symposium, Denver, 1967, transactions: Houston, Texas, SPWLA, p. Ll-L12. Evans, R. D., 1955, The atomic nucleus: New York, McGraw-Hill Book Company, Inc., 972 p. Evans, R. D., and Mugele, R. A., 1936, Increased gammaray sensitivity of tube counters and the measurement ofthe~ thorium content of ordinary materiais: Rev. Sci. Instr., v. 7, p. 441-449. Fearon, R. E., 1949, Gamma-ray well logging: Nucleonics, v. 4, p. 67-75. Foote, R. S., 1969a, Review of radiometric techniques in petroleum exploration, in Unconventional methods in exploration for petroleum and natural gas, Symposium proceedings: W. B. Heroy, Ed., Dallas, Southern Methodist Univ., p. 43-55. 1969b, Improvement in airborne gamma-radiation data analyses for anomalous radiation by removal of environmental and pedologic radiation changes,, in Nuclear techniquesand mineral resources, Buenos Aires, 1968, Proceedings:Vienna, International Atomic Energy Agency, p. 187-194. Godby, E. A., Connock, S. H. G., Steljes, J. F., Cowper, G., and Carmichael, H., 1952, Aerial prospecting for radioactive materials: Atomic Energy of Can. rep. 13, 31 p. Goldman, L. H., and Marr, H. E., 1979, Application of high resolution gamma-ray spectroscopyto well logging, in SPWLA 20th Annual Logging Symposium, Tulsa, 1979, Transactions: Houston, Texas, Society of Professional Well Log Analysts, p. GGl-GGB. Gorshkov, G. V., and Kurbatov, L. M., 1937, An attempt to determine geological structure from the intensity of gamma emanation in boreholes: Arctica, v. 5, p. 9-44.

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Grasty, R. L., 1973, Snow water equivalent measurement using natural gamma emission: Nord. Hydrol., v. 4, p. l-16. Grasty, R. L., and Damley, A. G., 1971, The calibration of gamma-ray spectrometersfor ground and airborne use: Geol. Surv. of Can. paper 71-17, 27 p. Gregory, A. F., 1956, Analysis of radioactive sources in aeroradiometric surveys over oil fields: AAPG Bull., v. 40, p. 2457-2474. Hofstadter. R.. 1949. The detection of eamma ravs with thallium:activated sodium-iodide cry&ls: Phys: Rev., v. 75, p. 796-810. Howell, L. G., and Frosch, A., 1939, Gamma-ray well logging: Geophysics, v. 4, p. 106114. Kelloaa. W. C.. 1957. Observations and interpretation of radT;active patterns over some California oil fields: Mines Mag., v. 47, p. 26-28. Kogan, R. M., Kiforer, M. V., Fridman, S. D., Chirkov, N. P., and Yakslover, A. F., 1969, Determination of water equivalent snow cover by method of aerial gamma survey: Meteorol. and Hydrol., no. 4, p. 51-55. Ko an, R. M., Nazarov, I. M., and Fridman, S. D., 1971, 8 anuna spectrometryof natural environments and forrnations: Jerusalem, Israel Program for Scientific Translations, 337 p. (originally published in Russian, 1969). Landsberg, H., 1939, Radioactivity tests of rock samples for the correlation of sedimentary horizons: American Institute of Mining and Metallurgical Engineers Technical Publication no. 1103, 9 p. Langford, G. T., 1962, Radiation surveys aid oil search: World Oil, v. 154, p. 114-119. Lobdell, D. S., Buckley, E. F., and Merritt, J. W., 1954, Gamma-ray exploration comes of age: World Oil, v. 139, p. 107-l 12. Loomis, T. H. W., and Blair, R. G., 1959, Airborne radiometric reconnaissance in the Wind River Basin, Wyoming, 1954: U.S. Atomic Energy Comm. Rep. RME-1072, 34 p. Lundberg, H., Roulston, K. I., Pringle, R. W., and Brownell, G. W., 1952, Oil exploration with scintillation counters: Oil in Canada, v. 4, p, 40-46. MacKallor, J. A., 1965, Natural gamma aeroradioactivity map of Puerto Rico: U.S.G.S. geophys. invest. map GP-525. MacKevett, E. M., Jr., 1958, Geology of the Ross-Adams uranium-thorium deposit, Alaska, in Peaceful uses of atomic ener y. Y. 2, Survey of raw material resources, Geneva, 192 8, Proceedings: Geneva, United Nations, p. 502-508. Miller, J. M., and Symons, G. D., 1973, Radiometric traverse of the seabed off the Yorkshire coast: Nature, v. 242, p. 184-186. Pierson, D. H., and Franklin, E., 1951, Aerial prospecting