Elwood A. Lepel

Rare earth elements in chloride-rich groundwater, Palo Duro Basin, Texas, USA

Rare earth element (REE) data for groundwater samples from the Deep-Basin Brine aquifer of the Palo Duro Basin, Texas, USA, illustrates the potential use of REE for inferring groundwater flow paths through different geologic materials. The REE content of the groundwaters range over 2.5 orders of magnitude and are depleted by 102 to 105 relative to aquifer materials. The shale-normalized REE patterns for groundwater that have primarily interacted with arkosic sandstones (granite wash) are flat with similar heavy REE (HREE) enrichments [(LuLa)n = 0.60 to 0.80]. The samples with highest REE contents and REE patterns, which are enriched in the intermediate REEs (IREEs; Sm-Tb) reflect variable degrees of interaction with carbonate rocks. The IREE enrichment is the result of fluid interaction with Fe-Mn coatings on carbonate minerals and/or secondary minerals in fractures and vugs. The chloride complex, [LnCl2+] and free-ions are the predominant REE species, accounting for over 95% of the REEs. Carbonate and sulfate species account for the other 5% and have very little influence on the behavior of the REEs. Although this study indicates a potentially important role for the REEs in understanding geochemical transport and groundwater movement, it also indicates the necessity for developing a better understanding of REE speciation in high ionic strength solutions.

Precise trace rare earth analysis by radiochemical neutron activation

A rare earth group separation scheme followed by normal Ge(Li), low energy photon detector (LEPD), and Ge(Li)−NaI(Tl) coincidence-noncoincidence spectrometry significantly enhances the detection sensitivity of individual rare earth elements (REE) at or below the ppb level. Based on the selected γ-ray energies, normal Ge(Li) counting is favored for140La,170Tb and169Yb; LEPD is favored for low γ-ray energies of147Nd,153Sm,166Ho and169Yb; and noncoincidence counting is favored for141Ce,143Ce,142Pr,153Sm,171Er and175Yb. The detection of radionuclides152mEu,159Gd and177Lu is equally sensitive by normal Ge(Li) and noncoincidence counting;152Eu is equally sensitive by LEPD and normal Ge(Li); and153Gd and170Tm is equally favored by all the counting modes. Overall, noncoincidence counting is favored for most of the REE. Precise measurements of the REE were made in geological and biological standards.

Nuclear archeology in a bottle: evidence of pre-Trinity U.S. weapons activities from a waste burial site.

During World War II, the Hanford Site in Washington became the location for U.S. plutonium production. In 2004, a bottle containing a sample of plutonium was recovered from a Hanford waste trench. Here, state-of-the-art instrumental analyses, reactor model simulations, and investigative science techniques were used to provide insights as to the origin of this unknown sample, a process collectively termed as nuclear archeology. Isotopic age dating conducted on the sample in 2007 indicated the sample was separated from the spent fuel 61.6 +/- 4.5 years earlier. The isotope (22)Na, a detectable product of a secondary nuclear reaction, proved useful as a powerful tool for nuclear forensic analysis as (1) an easily detectable signifier of the presence of alpha emitting actinides, (2) an indicator of sample splitting, and (3) a measure of the time since sample splitting. Analytical results of minor actinide isotopes and reactor model simulations confirmed the material originated from the X-10 reactor in Oak Ridge, TN. Corroborated by historical documents, we concluded this sample was part of the first batch of Pu separated at T-Plant, Hanford, the worlds first industrial-scale reprocessing facility, on December 9, 1944. This sample represents the oldest known collection of man-made (239)Pu in the world.

Rare earth element patterns in biotite, muscovite and tourmaline minerals

Rare earth element concentrations in the minerals biotite and muscovite from the mica schist country rocks of the Etta pegmatite and tourmalines from the Bob Ingersoll pegmatite have been measured by INAA and CNAA. The concentrations range from 10−4 g/g to 10−10 g/g. The REE patterns of biotite, muscovite and tourmaline reported herein are highly fractionated from light to heavy REE. The REE concentrations in biotite and muscovite are high and indigenous. The pegmatite tourmalines contain low concentrations of REE. Variations in tourmaline REE patterns reflect the geochemical evolution of pegmatite melt/fluid system during crystallization.

Adaptation and implementation of the RAYGUN gamma-ray analysis code on the IBM PC

The RAYGUN gamma-ray analysis code (a descendant of GAMANAL and GRPANL) has been converted from FORTRAN IV to RATFOR and ported to the IBM PC environment. The history of the code and some of the problems encountered during the conversion are discussed. The converted code was then used to analyze the IAEA G-1 Intercomparison Spectra as one measure of the codes performance. The results of the analyses showed that although the intrinsic peak finding and multiplet resolution capabilities of the code are a bit weak, the UPPER-LIMIT and LIBRARY-SEARCH options work quite well. When appropriate gamma-ray libraries are created, the overall performance of the code is quite satisfactory. The RAYGUN code runs on an IBM PC or clone with 256 Kbytes of RAM.

Trace Rare-Earth Element analysis of briny groundwaters

Rare-Earth Element (REE) concentrations in briny groundwaters are very low, and range from ppb to ppt levels. REE can be measured at these low levels using prechemistry to concentrate the REE, postchemistry as an REE group separation following neutron activation, and reactivation for chemical yields. The brine solutions appear to be stable with respect to trace elements (such as the REE) over the four years of sample storage. The brine REE patterns are highly fractionated from light REE to heavy REE, including a negative Eu anomaly. The REE patterns appear to be characteristic of each formation and its source region.

Naturally Occurring Radioactive Materials in Cargo at US Borders

Abstract In the USA and other countries large numbers of vehicles pass through border crossings each day. The illicit movement of radioactive sources is a concern that has resulted in the installation of radiation detection and identification instruments at border crossing points. This activity is judged to be necessary because of the possibility of an act of terrorism involving a radioactive source that may include any number of dangerous radionuclides. The problem of detecting, identifying and interdicting illicit radioactive sources is complicated by the fact that many materials present in cargo are somewhat radioactive. Some cargo contains naturally occurring radioactive material that may trigger radiation portal monitor alarms. Such nuisance alarms can be an operational limiting factor for screening of cargo at border crossings. Information about the nature of the radioactive materials in cargo that can interfere with the detection of radionuclides of concern is necessary to help anticipate and recognise likely sources of these nuisance alarms.

A field-deployable, aircraft-mounted sensor for the environmental survey of radionuclides

The Environmental Radionuclide Sensor System (ERSS)3 is an extremely sensitive sensor, which has been cooperatively developed by Pacific Northwest National Laboratory (PNNL) and Special Technologies Laboratory (STL) for environmental surveys of radionuclides. The ERSS sensors fit in an airborne pod and include twenty High-Purity Germanium (HPGe) detectors for the high-resolution measurement of gamma-ray emitting radionuclides, twenty-four3He detectors for possible neutron measurements, and two video cameras for visual correlation. These acrial HPGe sensors provide much better gamma-ray energy resolution than can be obtained with NaI(TI) detectors. The associated electronics fit into three racks. The system can be powered by the 28 V DC electrical supply of typical aircraft or 120 V AC. The data acquisition hardware is controlled by customized software and a real-time display is provided. Each gamma-ray event is time stamped and stored for later analysis. This paper will present the physical design, discuss the software used to control the system, and provide some examples of its use.

Nuclear Resonance Fluorescence of /sup 235/U

Nuclear resonance fluorescence is a physical process that provides an isotopic-specific signature that can be used for the identification and characterization of materials. The technique involves the detection of prompt discrete-energy photons emitted from a sample which is exposed to photons in the MeV energy range. Potential applications of the technique range from detection of high explosives to characterization of special nuclear materials. One isotope of significant interest is 235U. Pacific Northwest National Laboratory and Passport Systems have collaborated to conduct measurements searching for nuclear resonance fluorescence signatures of 235U below 3 MeV using a 220 g sample of highly enriched uranium. Nine 235U resonances between 1650 and 2010 keV were identified in the preliminary analysis. Analysis of the measurement data to determine the integrated cross sections of the resonances is in progress.

Location of neutron sources using moderator-free directional thermal neutron detectors

The use of neutron detectors designed to record only those thermalized neutrons coming from a highly specific direction can provide enhanced capability for applications such as locating nuclear weapons material or monitoring storage vaults containing special nuclear materials. Such a detection system should be as free of moderator as possible to assure effective directionality. We provide evidence from computer modeling and experimental tests that this technique allows the identification and localization of neutron sources at greater distances and narrower angular resolution than would be possible with conventional moderating neutron detectors.