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Compton suppression gamma-counting: The effect of count rate

Past research has shown that anti-coincidence shielded Ge(Li) spectrometers enhanced the signal-to-background ratios for gamma-photopeaks, which are situated on high Compton backgrounds. Ordinarily, an anti- or non-coincidence spectrum (A) and a coincidence spectrum (C) are collected simultaneously with these systems. To be useful in neutron activation analysis (NAA), the fractions of the photopeak counts routed to the two spectra must be constant from sample to sample to variations must be corrected quantitatively. Most Compton suppression counting has been done at low count rate, but in NAA applications, count rates may be much higher. To operate over the wider dynamic range, the effect of count rate on the ratio of the photopeak counts in the two spectra (A/C) was studied. It was found that as the count rate increases, A/C decreases for gammas not coincident with other gammas from the same decay. For gammas coincident with other gammas, A/C increases to a maximum and then decreases. These results suggest that calibration curves are required to correct photopeak areas so quantitative data can be obtained at higher count rates. ?? 1984.

Nuclear Instruments and Methods In Physics Researc↗

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

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. ?? 1984.

Nuclear Instruments and Methods In Physics Researc↗

Synchrotron radiation determination of elemental concentrations in coal

The variations with depth of the elemental concentrations in vitrinites in a series of vitrites have been determined using radiation from the Cornell high energy synchrotron source. All of the vitrites were selected from a single drill core sample of coal from the Emery coalfield, Utah. The results are compared with similar determinations using the Heidelberg proton microprobe. The advantages and disadvantages of the two techniques are discussed. Results are reported for S, Ca, Ti, Fe, Zn, Br, and Sr. For example, it is found that Fe increases from top to bottom of the coal bed in contrast to S, which decreases from top to bottom of the bed. Other features of the two data sets are also described. ?? 1984.

Nuclear Instruments and Methods in Physics Researc↗

36Cl: A tracer in groundwater in the aquia formation of Southern Maryland

The Aquia Formation (Paleocene) of Southern Maryland, a marine unit consisting predominantly of quartz sands, but containing 20-40% glauconite, represents one of the many productive, heavily pumped aquifers of the Southeastern Coastal Plain. An unusually high 36Cl activity ( ~ 15 ?? modem water) measured in an outcrop sample is interpreted as a result of the bomb pulse input. About 25 km downdip from the recharge area, a minimum in total chloride concentration occurs. This minimum is thought to correlate with the latest low-stand of sea-level, and thus to provide time information which is in general agreement with ages calculated from hydrodynamic data. However, significant increases in the 36Cl concentrations are observed along the flow path which may be due to ion filtration or to leakage of modem, bomb-contaminated water into the Aquia aquifer. ?? 1987.

Nuclear Instruments and Methods in Physics Researc↗

Determination of the occurrence of gold in an unoxidized Carlin-type ore sample using synchrotron radiation

The occurrence of the so-called invisible gold in two unoxidized Carlin-type gold samples from Nevada has been determined using synchrotron X-ray fluorescence (SXRF) analysis at the National Synchrotron Light Source, Brookhaven National Laboratory. A bedded sample from the East ore zone of the Carlin deposit and a breccia sample from Horse Canyon were analyzed. Preliminary results show that gold is found only in the Horse Canyon breccia sample. Experimental details including other X-ray line and diffraction peak interferences, standards used, and minimum detection limits (MDLs) are discussed. Gold, with a MDL range of 0.8 to 3 ppm, was not detected in euhedral pyrite crystals except in the interior porous portion of one grain. Gold was detected in some parts of the matrix. The phase which contains gold has not yet been identified. The highest content of gold so far analyzed is about 40 ppm. There are interesting implications of these new findings. ?? 1987.

Nuclear Instruments and Methods in Physics Researc↗

The uses of synchrotron radiation sources for elemental and chemical microanalysis

Synchrotron radiation sources offer important features for the analysis of a material. Among these features is the ability to determine both the elemental composition of the material and the chemical state of its elements. For microscopic analysis synchrotron X-ray fluorescence (SXRF) microprobes now offer spatial resolutions of 10 ??m with minimum detection limits in the 1-10 ppm range depending on the nature of the sample and the synchrotron source used. This paper describes the properties of synchrotron radiation and their importance for elemental analysis, existing synchrotron facilities and those under construction that are optimum for SXRF microanalysis, and a number of applications including the high energy excitation of the K lines of heavy elements, microtomography, and XANES and EXAFS spectroscopies. ?? 1990.

Nuclear Instruments and Methods in Physics Researc↗

36C1 measurements and the hydrology of an acid injection site

In an area in western Tennessee (United States), an industrial firm is injecting acidic (pH = 0.1) iron chloride into permeable zones of carbonate rocks at depths ranging from 1000 to 2200 m below land surface. Overlying the injection zone at a depth of approximately 500 m below land surface is a regional fresh-water aquifer, the Knox aquifer. A study is currently underway to investigate whether the injection wells are hydraulically isolated from the fresh-water aquifer. Drilling of a test well that will reach a total depth of 2700 m has been initiated. The 36Cl content of 15 samples from the Knox aquifer, from monitor wells in the vicinity of the injection site, and from the test well have been analyzed. ?? 1990.

Nuclear Instruments and Methods in Physics Researc↗

Rare earth element concentrations in geological and synthetic samples using synchrotron X-ray fluorescence analysis

The concentrations of rare earth elements (REEs) in specific mineral grains from the Bayan Obo ore deposit and synthetic high-silica glass samples have been measured by synchrotron X-ray fluorescence (SXRF) analysis using excitation of the REE K lines between 33 and 63 keV. Because SXRF, a nondestructive analytical technique, has much lower minimum detection limits (MDLs) for REEs, it is an important device that extends the in situ analytical capability of electron probe microanalysis (EPMA). The distribution of trace amounts of REEs in common rock-forming minerals, as well as in REE minerals and minerals having minor quantities of REEs, can be analyzed with SXRF. Synchrotron radiation from a bending magnet and a wiggler source at the National Synchrotron Light Source, Brookhaven National Laboratory, was used to excite the REEs. MDLs of 6 ppm (La) to 26 ppm (Lu) for 3600 s in 60-??m-thick standard samples were obtained with a 25-??m diameter wiggler beam. The MDLs for the light REEs were a factor of 10-20 lower than the MDLs obtained with a bending magnet beam. The SXRF REE concentrations in mineral grains greater than 25 ??m compared favorably with measurements using EPMA. Because EPMA offered REE MDLs as low as several hundred ppm, the comparison was limited to the abundant light REEs (La, Ce, Pr, Nd). For trace values of medium and heavy REEs, the SXRF concentrations were in good agreement with measurements using instrumental neutron activation analysis (INAA), a bulk analysis technique. ?? 1993.

Nuclear Instruments and Methods in Physics Researc↗

Active neutron interrogation experiments and simulation verification using the SIngle-scintillator Neutron and Gamma-Ray spectrometer (SINGR) for geosciences

We present a new SIngle-scintillator Neutron and Gamma Ray spectrometer (SINGR) instrument for use with both passive and active measurement techniques. Here we discuss the application of SINGR for planetary exploration missions, however, hydrology, nuclear non-proliferation, and resource prospecting are all potential areas where the instrument could be applied. SINGR uses an elpasolite scintillator, Cs 2 YLiCl 6 :Ce (CLYC), that has been shown to have high neutron efficiency even at small volumes, with a gamma-ray energy resolution of approximately 4% full-width-at-half-maximum at 662 keV. Active gamma-ray and neutron (GRNS) measurements were performed with SINGR at the NASA Goddard Space Flight Center (GSFC) Goddard Geophysical and Astronomical Observatory (GGAO) outdoor test site using a pulsed neutron generator (PNG) to interrogate geologically relevant materials (basalt and granite monuments). These experimental results, combined with simulations, demonstrate that SINGR is capable of generating neutron die-away curves that can be used to reconstruct the bulk hydrogen abundance and the depth distribution of hydrogen within the monuments. We compare our experimental results with Monte Carlo N-Particle (MCNP) 6.1 transport simulations to constrain the uncertainties in depth and hydrogen abundance from the neutron die-away data generated by SINGR. For future planetary exploration missions, SINGR provides a single detector system for interrogating the shallow subsurface to characterize the presence and abundance of hydrated phases and to provide bulk elemental analysis.

Nuclear Instruments and Methods in Physics Researc↗

Determination of the optimum-size californium-252 neutron source for borehole capture gamma-ray analysis

The fast- and thermal-neutron fluence rates from a 3.7 ??g 252Cf neutron source in a simulated borehole have been measured as a function of the source-to-detector distance using air, water, coal, iron ore-concrete mix, and dry sand as borehole media. Gamma-ray intensity measurements were made for specific spectral lines at low and high energies for the same range of source-to-detector distances in the iron ore-concrete mix and in coal. Integral gamma-ray counts across the entire spectrum were also made at each source-to-detector distance. From these data, the specific neutron-damage rate, and the critical count-rate criteria, we show that in an iron ore-concrete mix (low hydrogen concentration), 252Cf neutron sources of 2-40 ??g are suitable. The source size required for optimum gamma-ray sensitivity depends on the energy of the gamma ray being measured. In a hydrogeneous medium such as coal, similar measurements were made. The results show that sources from 2 to 20 ??g are suitable to obtain the highest gamma-ray sensitivity, again depending on the energy of the gamma ray being measured. In a hydrogeneous medium, significant improvement in sensitivity can be achieved by using faster electronics; in iron ore, it cannot. ?? 1979 North-Holland Publishing Co.

Nuclear Instruments and Methods↗

Use of chlorine-36 to determine regional-scale aquifer dispersivity, eastern Snake River Plain aquifer, Idaho/USA

Chlorine-36 (36Cl) derived from processed nuclear waste that was disposed at the US Department of Energy's Idaho National Engineering and Environmental Laboratory (INEEL) through a deep injection well in 1958, was detected 24-28 yr later in groundwater monitoring wells approximately 26 km downgradient from the source. Groundwater samples covering the period 1966-1995 were selected from the US Geological Survey's archived-sample library at the INEEL and analyzed for 36Cl by accelerator mass spectrometry (AMS). The smaller 36Cl peak concentrations in water from the far-field monitoring wells relative to the input suggest that aquifer dispersivity may be large. However, the sharpness of the 1958 disposal peak of 36Cl is matched by the measured 36Cl concentrations in water from these wells. This implies that a small aquifer dispersivity may be attributed to preferential groundwater flowpaths. Assuming that tracer arrival times at monitoring wells are controlled by preferential flow, a 1-D system-response model was used to estimate dispersivity by comparing the shape of predicted 36Cl-concentration curves to the shape of 36Cl-concentration curves measured in water from these observation wells. The comparisons suggest that a 1-D dispersivity of 5 m provides the best fit to the tracer data. Previous work using a 2-D equivalent porous-media model concluded that longitudinal dispersivity (equivalent to 1-D dispersivity in our model) was 90 m (Ackerman, 1991). A 90 m dispersivity value eliminates the 1958 disposal peak in our model output curves. The implications of the arrival of 36Cl at downgradient monitoring wells are important for three reasons: (1) the arrival times and associated 36Cl concentrations provide quantitative constraints on residence times, velocities, and dispersivities in the aquifer; (2) they help to refine our working hypotheses of groundwater flow in this aquifer and (3) they may suggest a means of estimating the distribution of preferential flowpaths in the aquifer. ?? 2000 Elsevier Science B.V. All rights reserved.

Nuclear Instruments and Methods in Physics Researc↗

Chlorine-36 and cesium-137 in ice-core samples from mid-latitude glacial sites in the Northern Hemisphere

Chlorine-36 (36Cl) concentrations, 36Cl/Cl ratios, and 36Cl fluxes in ice-core samples collected from the Upper Fremont Glacier (UFG) in the Wind River Mountain Range, Wyoming, United States and the Nangpai Gosum Glacier (NGG) in the Himalayan Mountains, Nepal, were determined and compared with published results from the Dye-3 ice-core drilling site on the Greenland Ice Sheet. Cesium-137 (137Cs) concentrations in the NGG also were determined. The background fluxes for 36Cl for each glacial site were similar: (1.6??0.3)??10-2 atoms/cm2 s for the UFG samples, (0.7??0.1)??10-2 atoms/cm2 s for the NGG samples, and (0.4??0.1)??10-2 atoms/cm2 s for the Dye-3 samples. The 36Cl fluxes in ice that was deposited as snow during peak atmospheric nuclear weapon test (1957-1958) were (33??1)??10-2 atoms/cm2 s for the UFG site, (291??3)??10-2 atoms/cm2 s for the NGG site, and (124??5)??10-2 atoms/ cm2 s for the Dye-3 site. A weapon test period 137Cs concentration of 0.79??0.05 Bq/kg in the NGG ice core also was detected in the same section of ice that contained the largest 36Cl concentration. ?? 2000 Elsevier Science B.V. All rights reserved.

Nuclear Instruments and Methods in Physics Researc↗

Identification of bomb-produced chlorine-36 in mid-latitude glacial ice of North America

In 1991, the U.S. Geological Survey collected a 160-meter (m) ice core from the Upper Fremont Glacier (43??07???N, 109??36???W) in the Wind River Mountain Range of Wyoming in the western United States [1]. In 1994-95, ice from this core was processed at the National Ice Core Laboratory in Denver, Colorado, and analyzed for chlorine-36 (36Cl) by accelerator mass spectrometry at PRIME Laboratory, Purdue University. A tritium bomb peak identified in the work by [1] was used as a marker to estimate the depth of bomb-produced 36Cl. Tritium concentrations ranged from 0 tritium units (TU) for older ice to more than 300 TU at 29 m below the surface of the glacier, a depth that includes ice that was deposited as snow during nuclear-weapons tests through the early 1960's. Maximum 36Cl production during nuclear-weapons tests was in the late 1950's; therefore, the analyses were performed on ice from a depth of 29.8 to 32 m. Calculated flux for 36Cl in ice deposited in the late 1950's ranged from 1.2 ?? 0.1 ?? 10-1 atoms/cm2 s for ice from 29.8 to 30.4 m, to 2.9 ?? 0.1 ?? 10-1 atoms/cm2 s for ice from 31.5 to 32.0 m. Ice samples from a depth of 104.7 to 106.3 m were selected to represent pre-weapons tests 36Cl flux. Calculated flux for 36Cl in this deeper ice was 4.6 ?? 0.8 ?? 10-3 atoms/cm2 s for ice from 104.7 to 105.5 m and 2.0 ?? 0.2 ?? 10-2 atoms/cm2 s for ice from 105.5 to 106.3 m. These flux calculations from the Upper Fremont Glacier analyses are the first for bomb-produced 36Cl in ice from a mid-latitude glacier in North America. It may now be possible to fully quantify the flux of 36Cl from nuclear-weapons tests archived in mid-latitude glacial ice and to gain a better understanding of the distribution of 36Cl and other cosmogenic nuclides.

Nuclear Instruments and Methods in Physics Researc↗

Ion irradiation damage in ilmenite at 100 K

A natural single crystal of ilmenite (FeTiO3) was irradiated at 100 K with 200 keV Ar2+. Rutherford backscattering spectroscopy and ion channeling with 2 MeV He+ ions were used to monitor damage accumulation in the surface region of the implanted crystal. At an irradiation fluence of 1 ?? 1015 Ar2+/cm2, considerable near-surface He+ ion dechanneling was observed, to the extent that ion yield from a portion of the aligned crystal spectrum reached the yield level of a random spectrum. This observation suggests that the near-surface region of the crystal was amorphized by the implantation. Cross-sectional transmission electron microscopy and electron diffraction on this sample confirmed the presence of a 150 nm thick amorphous layer. These results are compared to similar investigations on geikielite (MgTiO3) and spinel (MgAl2O4) to explore factors that may influence radiation damage response in oxides.

Nuclear Instruments and Methods in Physics Researc↗

Quantitative analysis of major elements in silicate minerals and glasses by micro-PIXE

The Guelph micro-PIXE facility has been modified to accommodate a second Si(Li) X-ray detector which records the spectrum due to light major elements (11 ??? Z ??? 20) with no deleterious effects from scattered 3 MeV protons. Spectra have been recorded from 30 well-characterized materials, including a broad range of silicate minerals and both natural and synthetic glasses. Sodium is mobile in some of the glasses, but not in the studied mineral lattices. The mean value of the instrumental constant H for each of the elements Mg, Al, and Si in these materials is systematically 6-8% lower than the H-value measured for the pure metals. Normalization factors are derived which permit the matrix corrections requisite for trace-element measurements in silicates to be based upon pure metal standards for Mg, Al and Si, supplemented by well-established, silicate mineral standards for the elements Na, K and Ca. Rigorous comparisons of electron microprobe and micro-PIXE analyses for the entire, 30-sample suite demonstrate the ability of micro-PIXE to produce accurate analysis for the light major elements in silicates. ?? 1997 Elsevier Science B.V.

Nuclear Instruments and Methods in Physics Researc↗

Nuclear methods applied to uranium geochemistry

Stable and radioactive daughter products produced from nuclear disintegrations of uranium have proved useful in fundamental studies of the geochemistry of uranium in igneous rock and sedimentary environments and in ore deposits. Information gained from geochemical studies of uranium migration has been used to develop models for attempts to date archeological, geological, and oceanographic environments represented by samples of bone, wood, charcoal, continental and marine carbonates, marine sediments, and glacially derived soils. Recent improvements of nuclear instrumentation and techniques allowed accurate measurements of natural radioactive isotopes, and it is now believed that radioactive equilibrium between the long-lived isotopes of the two uranium decay series is more the exception than the rule in nature. It was assumed that the 234U and 238U isotopes were in equilibrium until Thurber confirmed that considerable separation between 234U daughter and 238U parent exists in nature. It now has been documented that the 234U content may range from 60% deficient to 500% in excess relative to 238U. An excess of 15% of 234U isotope in sea water is well documented. A summary of previous work has shown that geochemical fractionation of the radioactive nuclides in 238U and 235U decay series takes place in the hydrologic environment, resulting in depletion of 230Th and 231Pa with respect to their parents, 238U, 234U, and 235U, in water and a complementary enrichment of these daughter nuclides in some sediments. Subsequent assimilation of Uranium, essentially free of radioactive daughters, occurs in some specific types of deposits such as carbonates and phosphates.

IEEE Transactions on Nuclear Science↗

A practical method of estimating standard error of age in the fission track dating method

A first-order approximation formula for the propagation of error in the fission track age equation is given by PA = C[P2s+P2i+P2??-2rPsPi] 1 2, where PA, Ps, Pi and P?? are the percentage error of age, of spontaneous track density, of induced track density, and of neutron dose, respectively, and C is a constant. The correlation, r, between spontaneous are induced track densities is a crucial element in the error analysis, acting generally to improve the standard error of age. In addition, the correlation parameter r is instrumental is specifying the level of neutron dose, a controlled variable, which will minimize the standard error of age. The results from the approximation equation agree closely with the results from an independent statistical model for the propagation of errors in the fission-track dating method. ?? 1979.

Nuclear Tracks↗

Low-field nuclear magnetic resonance characterization of organic content in shales

Low-field nuclear magnetic resonance (LF-NMR) relaxometry is a non-invasive technique commonly used to assess hydrogen-bearing fluids in petroleum reservoir rocks. Longitudinal T 1 and transverse T 2 relaxation time measurements made using LF-NMR on conventional reservoir systems provides information on rock porosity, pore size distributions, and fluid types and saturations in some cases. Recent improvements in LF-SNMR instrument electronics have made it possible to apply these methods to assess highly viscous and even solid organic phases within reservoir rocks. T 1 and T 2 relaxation responses behave very differently in solids and liquids, therefore the relationship between these two modes of relaxation can be used to differentiate organic phases in rock samples or to characterize extracted organic materials. Using T 1 -T 2 correlation data, organic components present in shales, such as kerogen and bitumen, can be examined in laboratory relaxometry measurements. In addition, implementation of a solid-echo pulse sequence to refocus some types of T 2 relaxation during correlation measurements allows for improved resolution of solid phase photons. LF-NMR measurements of T 1 and T 2 relaxation time correlations were carried out on raw oil shale samples from resources around the world. These shales vary widely in mineralogy, total organic carbon (TOC) content and kerogen type. NMR results were correlcated with Leco TOC and geochemical data obtained from Rock-Eval. There is excellent correlation between NMR data and programmed pyrolysis parameters, particularly TOC and S2, and predictive capability is also good. To better understand the NMR response, the 2D NMR spectra were compared to similar NMR measurements made using high-field (HF) NMR equipment.

Conference Paper↗