John N. Rosholt

EVOLUTION OF THE ISOTOPIC COMPOSITION OF URANIUM AND THORIUM IN SOIL PROFILES.

Mass-spectrometric and alpha-spectrometric analyses for the isotopic composition of U 238 , U 235 , U 234 , Th 232 , and Th 230 have been made on several soils and soil profiles in glacial-derived parent material, volcanic rock, and shale. Three deep profiles from Minnesota represent typical well-developed soils on till and loess of Wisconsin age continuously sampled to depths of 6, 7, and 10 feet, respectively. Results on individual soil horizons, in these three profiles, show similar trends in the variation of U 234 /U 238 and Th 230 /U 238 ratios, the predominant features being excess Th 230 and deficient U 234 compared to U 238 . The other soils and soil profiles have different variations which can be correlated by use of a model to describe uranium migration. The data collected provided information for interpreting the causes of uranium migration in soils and for constructing a tentative model to explain the isotopic evolution of uranium and thorium in soil profiles. The proposed model indicates that (1) uranium was leached at depth in the profile, (2) preferential leaching of U 234 was continuous in the soil, and (3) upward capillary migration of a fraction of the uranium with above-normal U 234 /U 238 ratio tended to make uranium of high U 234 ratio available for isotopic exchange in upper soil horizons and for assimilation in organic complexes in surface soils which are rich in organic matter. Thus some of the organic-rich surface soils, which have had considerable time to develop, contain uranium with excess U 234 compared to U 238 . Interpretations from this model suggest that remixing of radioisotopes by geochemical processes contributes significantly, along with the usual physical processes of radioactive growth and decay, toward producing an isotopic composition near radioactive equilibrium.

Lead Isotope Systematics and Uranium Depletion in the Granite Mountains, Wyoming

Isotopic composition and concentration of lead in whole rock and microcline and concentration of uranium and thorium in whole-rock samples of granite from the Granite Mountains, Wyoming, have been determined. The lead isotopic composition in the whole rocks was found to be highly radiogenic with a range in Pb 206 /Pb 204 of 19.58 to 42.27; the corresponding range in microclines is 15.39 to 22.44. A Pb 206 /Pb 204 versus Pb 207 /Pb 204 plot of the whole-rock data yields an apparent isochron age of 2,790 ± 80 m.y. as the time of crystallization of the granite. Chemically determined values of U 238 /Pb 204 in the whole rocks lie between 3.3 and 18.4 and are too low to account for the amount of radiogenic lead observed. A material balance of lead, thorium, and uranium components indicates that an average of approximately 75 percent of the amount of uranium required to produce the radiogenic lead was removed from the rocks, whereas, on the average, there was no apparent loss of thorium. Loss of uranium from the granite is demonstrated to extend at least to a depth of 165 ft in a drill core. The average uranium loss from the samples analyzed represents about 20 g uranium per 1,000 kg of rock that apparently was removed during the Cenozoic and that probably constitutes the major source of uranium now in ore deposits in central Wyoming basins. The lead isotopic composition of the microclines indicates that lead was mobilized within the granite and was isolated in the feldspar during a thermal event about 1,640 + 120 m.y. ago. However, there is no evidence that the whole rocks themselves became open systems at that time. Whole-rock and microcline isochrons intersect at Pb 206 /Pb 204 and Pb 207 /Pb 204 of 13.77 and 14.86, respectively, indicating a characteristic U 238 /Pb 204 of 8.96 in the source region of the granite magma.

Isotopic fractionation of uranium in sandstone

Relatively unoxidized black uranium ores from sandstone deposits in the western United States show deviations in the uranium-235 to uranium-234 ratio throughout a range from 40 percent excess uranium-234 to 40 percent deficient uranium-234 with respect to a reference uranium-235 to uranium-234 ratio. The deficient uranium-234 is leached preferentially to uranium-238 and the excess uranium-234 is believed to result from deposition of uranium-234 enriched in solutions from leached deposits.

Accumulation rates of Th-230, Pa-231, and some transition metals on the Bermuda Rise

Abstract Measurements of 238U, 234U, 230Th, 232Th, 231Pa, Mn, Fe, Co, Ni, Cu, and Zn were made on 23 samples from core GPC-5, a 29-m giant piston core from a water depth of 4583 m on the northeastern Bermuda Rise (33°41.2′N, 57°36.9′W). This area is characterized by rapid deposition of sediment transported by abyssal currents. Unsupported 230Th and 231Pa are present throughout the core but, because of large variations in the sedimentation rate, show marked departures from exponential decay with depth. The trend with depth of the 231 Pa ex 230 Th ex ratio is consistent with the average accumulation rate of 36 cm/1000 y reported earlier on the basis of radiocarbon dating and CaCO3 stratigraphy. When expressed on a carbonate-free basis, concentrations of Mn, Co, Ni, Cu, Zn, 230Thex, and 231Paex all show cyclic variations positively correlated with those of CaCO3. The correlations can be explained by a model in which all of these constituents, including CaCO3, are supplied to the sediments from the water column at a constant rate. Concentration variations are controlled mainly by varying inputs of terrigenous detritus, with low inputs occurring during interglacials and high inputs during glacials. Relationships between the metal and 230Thex concentrations permit estimates of the rates at which the metals are removed to the sediment by scavenging from the water column. The results, in μg/cm2-1000 y, are: 4300 ± 1100 for Mn, 46 ± 16 for Ni and 76 ± 26 for Cu. These rates are somewhat larger than ocean-wide averages estimated by other methods, and the absolute rate of 230Th accumulation in GPC-5 averages about nine times higher than production in the overlying water column. This part of the Bermuda Rise and similar bottom-current deposits may act as important accumulators of elements scavenged from seawater.

Dating methods applicable to the Quaternary

Includes 5 topical chapters covering paleoclimates, dating methods, volcanism, tephrochronology, and Pacific margin tephrochronologic correlation, and 15 chapters of regional synthesis covering: the Pacific margin; the Columbia Plateau; the Snake River Plain; the major pluvial lakes of the Great Basin; the Basin and Range in California, Arizona, and New Mexico; the Colorado Plateau; the Southern and Central Rocky Mountains; the Northern and Southern Great Plains, Osage Plains, and Interior Highlands; the Lower Mississippi Valley; the Gulf of Mexico Coastal Plain and Florida; the Appalachian Highlands and Interior Low Plateaus; and the Atlantic Coastal Plain. A large, full-color geologic map of the Quaternary deposits of the Lower Mississippi Valley, in addition to correlation charts, tables, and cross-sections relating to other chapters, is also included.

Age of the moon: An isotopic study of uranium-thorium-lead systematics of lunar samples

Concentrations of U, Th, and Pb in Apollo 11 samples studied are low (U. 0.16 to 0.87; Th, 0.53 to 3.4; Pb, 0.29 to 1.7, in ppm) but the extremely radiogenic lead in samples allows radiometric dating. The fine dust and the breccia have a concordant age of 4.66 billion years on the basis of 207Pb/206Pb, 206Pb/238U, 207Pb/235U, and208Pb/232Th ratios. This age is comparable with the age of meteorites and with the age generally accepted for the earth. Six crystalline and vesicular samples are distinctly younger than the dust and breccia. The 238U/235U ratio is the same as that in earth rocks, and 234U is in radioactive equilibrium with parent 238U.

The distribution and mobility of uranium in glassy and zeolitized tuff, Keg Mountain area, Utah, U.S.A.

Abstract The distribution and mobility of uranium in a diagenetically altered, 8 Ma old tuff in the Keg Mountain area, Utah, are modelled in this study. The modelling represents an improvement over similar earlier studies in that it: (1) considers a large number of samples (76) collected with good geologic control and exhibiting a wide range of alteration; (2) includes radiometric data for Th, K and RaeU (radium equivalent uranium) as well as U; (3) considers mineralogic and trace-element data for the same samples; and (4) analyzes the mineral and chemical covariation by multivariate statistical methods. The variation of U in the tuff is controlled mainly by its primary abundance in glass and by the relative abundance of non-uraniferous detritus and uraniferous accessory minerals. Alteration of glass to zeolite, even though extensive, caused no large or systematic change in the bulk concentration of U in the tuff. Some redistribution of U during diagenesis is indicated by association of U with minor alteration products such as opal and hydrous Fe−Mn oxide minerals. Isotopic studies indicate that the zeolitized tuff has been open to migration of U decay products during the last 0.8 Ma. The tuff of Keg Mountain has not lost a statistically detectable fraction of its original U, even though it has a high (≈ 9 ppm) trace U content and has been extensively altered to zeolite. Similar studies in a variety of geological environments are required in order to identify the particular combination of conditions most favorable for liberation and migration of U from tuffs.

The Uranium-trend dating method: Principles and application for southern California marine terrace deposits

Abstract Uranium-trend dating is an open-system method for age estimation of Quaternary sediments, using disequilibrium in the 238 U 234 U 230 Th decay series. The technique has been applied to alluvium, colluvium, loess, till, and marine sediments. In this study we tested the U-trend dating method on calcareous marine terrace deposits from the Palos Verdes Hills and San Nicolas Island, California. Independent age estimates indicate that terraces in these areas range from ∼80 ka to greater than 1.0 Ma. Two low terraces on San Nicolas Island yielded U-trend plots that have a clustered array of points and the ages of these deposits are indeterminate or highly suspect. Middle Pleistocene terraces and one early Pleistocene terrace on San Nicolas Island and all terraces on the Palos Verdes Hills gave reasonably linear U-trend plots and estimated ages that are stratigraphically consistent and in agreement with independent age estimates. We conclude that many marine terrace deposits are suitable for U-trend dating, but U-trend plots must be carefully evaluated and U-trend ages should be consistent with independent geologic control.

Uranium series disequilibrium in a young surficial uranium deposit, northeastern Washington, U.S.A.

A recently discovered ore-grade accumulation of U in organic-rich sediments of late Quaternary age provides an opportunity for studying the early association of U, U-daughters, and organic matter in a natural setting. The U occurs in valley-fill sediments of peat, peaty clay, silt, and sand along the north fork of Flodelle Creek, Stevens County, Washington. Radiometric techniques (delayed neutron, high-resolution gamma-ray spectrometry, thin-source alpha spectrometry) were employed to determine the abundance and distribution of U-series nuclides, the extent of secular equilibrium within the U decay series, and the apparent U-series ages of U incorporation. Sixteen lithologically distinct intervals were sampled from a 292 cm core. Uranium contents range from 140 to 2790 ppm and are positively correlated with organic contents. Measured alpha activity ratios of 234U/238U (1.31–1.38) are very similar to those reported in coexisting waters, suggesting a rather constant isotopic composition of introduced U. Much lower Th contents of <10–40 ppm are controlled by the type and abundance of silicate detritus. The youth of the host sediments (<15 000 a) and the paucity of associated radioactivity suggested large excesses of U relative to radioactive daughters and such excesses were observed, particularly in the shallowest intervals. Apparent ages of U emplacement determined by the (alpha) activity ratio of 230Th daughter to 234U parent show a general increase with depth and fair agreement with estimated depositional ages. This observation suggests dominantly syndepositional or early post depositional emplacement of U followed by decay-generated buildup of 230Th daughter with time. However, interval by interval comparisons of the relative abundances of other daughters, particularly 226Ra and 210Pb, indicate variability caused by processes other than closed-system growth and decay, probably because chemically diverse daughters that are decay-generated in situ have differing mobilities and because upwelling ground water continuously adds more U and minor amounts of daughters. If 230Th is considered the least susceptible to these modifications, the data suggest some addition of 234U in the deepest intervals and some loss of 226Ra and/or gain of 222Rn throughout the studied core.

Radioisotope dilution analyses of geological samples using 236U and 229Th

Abstract The use of 236U and 229Th in alpha spectrometric measurements has some advantages over the use of other tracers and measurement techniques in isotope dilution analyses of most geological samples. The advantages are: (1) these isotopes do not occur in terrestrial rocks, (2) they have negligible decay losses because of their long half lives, (3) they cause minimal recoil contamination to surface-barrier detectors, (4) they allow for simultaneous determination of the concentration and isotopic composition of uranium and thorium in a variety of sample types, and (5) they allow for simple and constant corrections for spectral inferences, 0.5% of the 238U activity is subtracted for the contribution of 235U in the 236U peak and 1% of the 229Th activity is subtracted from the 230Th activity. Disadvantages in using 236U and 229Th are: (1) individual separates of uranium and thorium must be prepared as very thin sources for alpha spectrometry, (2) good resolution in the spectrometer system is required for thorium isotopic measurements where measurement times may extend to 300 h, and (3) separate calibrations of the 236U and 229Th spike solution with both uranium and thorium standards are required. The use of these tracers in applications of uranium-series disequilibrium studies has simplified the measurements required for the determination of the isotopic composition of uranium and thorium because of the minimal corrections needed for alpha spectral interferences.