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This report presents previously unpublished radiochemical data for approximately 3,000 ground-water and surface-water samples collected from 47 states during mid-1954 through 1965. Data are reported for approximately 1,900 ground-water and 1,100 surface-water samples. Data for gross alpha, gross beta, gross radium as radium-226, and natural uranium concentrations are given for most samples. These data provide information regarding the background radioactivity levels in many of the Nation's waters before much of the large scale testing of nuclear weapons by the major world powers. These data also may be useful for identifying and evaluating long-term variations and trends. INTRODUCTION The late 1940's and early 1950's were a time of rapid nuclear weapon development and testing (Smyth, 1946; Jungk, 1958). These tests resulted in the widespread distribution of shortand long-lived radionuclides in the environment (Fradkin, 1989). Concern about the presence of these radionuclides in the environment, especially in ground and surface waters, resulted in the development of laboratory capabilities for analyzing radionuclides in water by the U.S. Geological Survey. The first U.S. Geological Survey laboratory capabilities were developed (about 1953) in Washington, D.C., for the determination of tritium and uranium in water samples. A second laboratory capability was developed (about 1954) at the Denver Federal Center in Colorado for the determination of gross alpha, gross beta, and gross radium in water samples. From mid-1954 through 1965, the U.S. Geological Survey collected several thousand natural groundand surface-water samples from across the United States for analysis of selected radionuclides. Results of radium and uranium analyses for 561 ground-water samples were published by Scott and Barker (1962). Analytical results for most of the samples collected during the 1954-1965 period, however, were not published. This report presents the previously unpublished radiochemical data obtained by analyzing approximately 3,000 groundand surface-water samples collected from 47 states during mid-1954 through 1965. No samples were collected from Delaware, New Hampshire, or Vermont. Sample-site and radiochemical data are presented for about 1,900 ground-water samples and 1,100 surface-water samples. Although the data presented in this report may not meet present-day criteria for sample identification and analytical quality assurance, these analyses nevertheless constitute a valuable historical data base and may be useful for identifying and evaluating long-term variations and trends. The samples generally were collected from natural, relatively pristine sources. During the initial phases of the radiochemical-data-acquisition efforts, sampling locations were only vaguely identified for many of the samples that were collected. In addition, new analytical instrumentation was being acquired and tested, and new analytical methods were being developed. These reasons may explain, in part, why these data were not published at that time. Beginning in 1964, radiochemical data of a comparable nature were collected monthly for many of the Nation's major rivers, as part of a Radiochemical Surveillance Network project conducted by the U.S. Geological Survey. Additional radiochemical data also were collected by the same project at more than 50 Hydrologic Benchmark Network stations on small, relatively pristine streams. These data are available through the National Water Data Storage and Retrieval System (WATSTORE), the U.S. Geological Survey's automated datastorage and data-retrieval system. SAMPLE COLLECTION AND PRESERVATION Collection of ground-water samples generally was accomplished by allowing the tap or pump to run for several minutes before collecting a sample, preferably without visible turbidity. All samples were collected in 1-gal borosilicate glass bottles. From about the mid-1950's through the early 1960's, samples were preserved by the addition of 2 to 3 mL of a glacial acetic acid and chloroform mixture. The preservative was added to minimize precipitate formation and algal and bacterial growth. Surface-water samples were collected by dipping water from a well-mixed, representative part of the stream. Turbid ground-water and all surface-water samples were filtered in the laboratory prior to analysis, and samples were usually analyzed within 1 to 2 months after collection. In the early 1960's, water sampling bottles were changed from glass to polyethylene. This was done to reduce costs, eliminate breakage in shipment, and to simplify handling. In the mid-1960's, unpublished laboratory studies indicated that most well aerated surface-water samples remained stable for 6 months or more without the use of the acetic acid-chloroform preservative. Preservative use was, therefore, discontinued for most surface-water samples, but they were stored in the dark to reduce algal and bacterial growth. Ground-water samples also were generally collected and stored without preservatives. Occasionally, however, ground-water samples containing reduced iron or other salts required the addition of hydrochloric or nitric acid to decrease the pH to 1 or less. This usually prevented the formation of precipitates. Extremely saline thermal ground-water samples occasionally required the addition of measured quantities of distilled water to prevent salt precipitation. RADIOCHEMICAL CALIBRATION STANDARDS AND ANALYSES A variety of calibration standards have been recommended and used by various agencies throughout the years for gross-alpha and gross-beta (betagamma) determinations. Problems inherent in the use of multiple calibration standards, and the lack of comparability of sample analyses obtained when using different standards, were described in detail by Janzer (1980). The practice of multiple calibration-standard use, however, continues. Analyzing laboratories rarely indicate the calibration standards used when gross radiochemical data are reported. Reliable conversion factors generally are not known or applicable to compensate for the differences of the alpha and beta energies associated with various isotopes, and the differences of the absorption characteristics of dissolved-solids residues that are obtained from water samples of different composition. Since 1954, the U.S. Geological Survey has used natural uranium as the standard of choice for gross-alpha calibration and measurements, and all gross-alpha results in this report are based on the use of this calibration standard. Natural uranium (acetate) with the equilibrium, undepleted isotopic abundances of uranium-234, uranium-235, and uranium-238 were used for the preparation of calibration counting planchets. Uranium isotope abundances were determined by alpha spectrometry as described by Edwards (1968). Grossalpha concentrations were expressed in terms of the weight equivalent of natural uranium (micrograms of natural uranium per liter), which would yield the same activity in the water sample. Scott and Barker (1962) noted that gross-beta concentrations given in their report were determined and reported in terms of thallium-204 as the calibration standard. Strontium-90/yttrium-90 became the standard of choice for the U.S. Geological Survey about or shortly after 1957. Details of the analytical procedures used for determining gross-beta radioactivity were described by Barker and Robinson (1963). Cesium-137 became more commonly used as a gross-beta calibration standard beginning in the early 1960's. U.S. Geological Survey gross-beta results were reported in terms of both of the commonly used calibration standards strontium-90/yttrium-90 and cesium-137 after about mid-1965. Thallium-204 decays by beta emission O~) with a maximum energy of 0.766 MeV. Strontium-90 decays by beta emission O~) with a maximum energy of 0.546 MeV. The strontium-90 decay is accompanied by simultaneous p~ decay of an equilibrium amount of the short-lived yttrium-90 daughter, which decays with a p~ maximum energy of 2.27 MeV. Cesium-137 decays 6.5 percent by p~ with a 1.176 MeV maximum and 93.5 percent with a 0.514 MeV maximum (Lederer and others, 1968). There is no simple direct way of converting gross beta measurement results based on one standard to results obtained using other standards. Janzer (1980) reported experimental results, using natural uranium and americium-241 as gross-alpha calibration standards, which showed that grossalpha measurements differed by as much as 100 percent when equivalent water samples were analyzed. Differences in gross-beta measurements of equivalent water samples, as a result of using strontium-90/yttrium-90 versus cesium-137 standards, varied from 0 to 25 percent depending on the evaporated dissolvedsolids-residue thickness in the counting planchets. There may be some concern regarding the validity and comparability of gross-radioactivity analyses made in the mid-1950's with analyses made at later dates. Comparing the variety of calibration standards in use today with those used in the mid-1950's, differences of as much as 100 percent in the analytical results obtained for the same sample by different laboratories may not be uncommon. Even with differences of these magnitudes, however, gross-radioactivity analyses can be quite useful as indicators of change or to identify areas where water is possibly contaminated by radionuclides. A lack of appreciable gross radioactivity in water samples from a specific area commonly obviates the need for repetitive sampling and more complex and costly analyses. ANALYTICAL PROCEDURES Gross-alpha and gross-beta analyses given in tables 1 and 2 of this report were performed by evaporating measured aliquots of the filtered samples to dryness in platinum or Teflon1 evaporating dishes. On the basis of the specific conductance of the untreated sample, an aliquot volume was selected to yield a weight of no more than 150 mg of dissolved-solids residue after ev

Data for gross alpha, gross beta, gross radium as radium-226, and uranium in ground and surface waters in the United States, mid-1954 through 1965