Composition optimization of scintillating rare-earth nanocrystals in oxide glass-ceramics for radiation spectroscopy.

Glass-ceramic nanocomposites comprising GdBr3/CeBr3 loaded sodium-aluminosilicate glasses in which scintillating crystallites are precipitated in situ from a host glass matrix were studied. This materials system shows promise as an alternative to single-crystal scintillators, with potential to be fabricated into a wide variety of sizes, shapes, and compositions. Batch compositions containing 15-18 mol. % GdBr3 and 3-4 mol. % CeBr3 were prepared and analyzed for photoluminescent light yield. Light yield peaked with rare-earth content of 15 mol. % GdBr3 and 4 mol. % CeBr3. Preliminary ceramization studies on this composition found that the precipitated phase more closely matched a Gd2O3-CeO2 mixture rather than the GdBr3(Ce) that was targeted.

GdBr3: CE in a glass wafer as a nuclear radiation monitor.

A glass wafer that contains cerium-activated gadolinium-based scintillator has been tested as a nuclear radiation monitor. The detector is prepared by mixing powdered gadolinium and cerium (3+) bromides with alumina, silica, and lithium fluoride, melting the mixture at 1,400°C, and then quenching and annealing the glass. The resulting clear glass matrix emits stimulated blue light that can be collected by a conventional photomultiplier tube. Spectral analysis of radionuclides with this detector shows the energy peaks for alpha particles, the energy continuum for beta particles, the Compton continuum and full-energy peaks for gamma rays, and an energy continuum with specific reaction-product peaks for neutrons. Energy resolution for the 5.5-MeV alpha particle and 0.662-MeV gamma-ray peaks is about 20%. This resolution, although threefold poorer than for single-crystal NaI(Tl) scintillators, contributes to radionuclide identification and quantification. Application of this detector to radiation monitoring is proposed, as well as approaches for improving light collection and energy resolution that will facilitate radionuclide identification and monitoring, especially for alpha particles, beta particles, and low-energy gamma rays.

Long-term selective retention of natural Cs and Rb by highly weathered coastal plain soils.

Naturally occurring Cs and Rb are distinctly more abundant relative to K in the highly weathered upland soils of the Savannah River Site, South Carolina, than in average rock of Earth's upper continental crust (UCC), by factors of 10 and 4, respectively. Naturally occurring Cs has been selectively retained during soil evolution, and Rb to a lesser extent, while K has been leached away. In acid extracts of the soils, the Cs/K ratio is about 50 times and the Rb/K ratio about 15 times the corresponding ratios for the UCC, indicating that relatively large amounts of natural Cs and Rb have been sequestered in soil microenvironments that are highly selective for these elements relative to K. Cation exchange favoring Cs and Rb ions, and subsequent fixation of the ions, at sites in interlayer wedge zones within hydroxy-interlayered vermiculite particles may account for the observations. The amounts of stable Cs retained and the inferred duration of the soil evolution, many thousands of years, provide new insights regarding long-term stewardship of radiocesium in waste repositories and contaminated environments. Study of natural Cs in soil adds a long-term perspective on Cs transport in soils not available from studies of radiocesium.

Radiation background in a LaBr3(Ce) gamma-ray scintillation detector.

Gamma-ray spectral analyses with a 5-cm × 5-cm LaBr3(Ce) detector and a NaI(Tl) detector of the same size show that the LaBr3(Ce) has much better gamma-ray peak resolution and full-energy peak counting efficiency but worse detection sensitivity. The LaBr3(Ce) detector has relatively high intrinsic radiation background due to the naturally occurring La radioisotope in lanthanum. Although this La background is entirely below the energy of 1,500 keV, additional background is in the energy region between 1,500 keV and 2,750 keV. The manufacturer attributes this radiation to alpha particles emitted by the five short-lived progeny of an Ac impurity. Comparative values for peak resolution, full-energy peak counting efficiency, and detection sensitivity are reported for Am, Co, and Cs. Results of counting Cs sources at two activity levels demonstrate the impact of background on detection sensitivity.

Freundlich and dual Langmuir isotherm models for predicting 137Cs binding on Savannah River Site soils.

Distribution of 137Cs and stable cesium between aqueous solution and near-surface soil samples from five locations at the Savannah River Site was measured in order to develop a predictive model for 137Cs uptake by the soils. Sorption of 137Cs in these soils appears to be mostly by hydroxy-interlayered vermiculite. Batch sorption studies with 4 d for equilibration were conducted at three cesium concentrations and at two backing electrolyte (NaNO3) concentrations. The soil-solution mixtures were pH-adjusted to evaluate the effects of pH on cesium sorption. Sorbed cesium was related to the equilibrium aqueous cesium concentrations by a Freundlich isotherm model. Model fits on logarithmic scales have a common slope of 0.60 +/- 0.03 for acidic mixtures and 0.69 +/- 0.04 for neutralized mixtures but have unique intercepts that are influenced by backing electrolyte concentration and pH. An ion-exchange model is proposed that pertains to all five soils and relates the Freundlich isotherms to the cation exchange capacity of soil and the aqueous concentrations of cesium, sodium, and a third ionic species that was hydrogen in the acidic mixtures and potassium in the neutralized mixtures. Model fits are consistent with Kd values in the entire range of 5-2,300 L kg(-1) determined for the five soil types. As an alternate model, dual Langmuir isotherms were fitted to the data. The results suggest cesium sorption by (1) relatively few interlayer-wedge sites, highly selective for cesium, and (2) much more abundant but less selective sites on internal and external planar surfaces.