No abstract

In the EXILL campaign a highly efficient array of high purity germanium (HPGe) detectors was operated at the cold neutron beam facility PF1B of the Institut Laue-Langevin (ILL) to carry out nuclear structure studies, via measurements of γ-rays following neutron-induced capture and fission reactions. The setup consisted of a collimation system producing a pencil beam with a thermal capture equivalent flux of about 108 n s−1cm−2 at the target position and negligible neutron halo. The target was surrounded by an array of eight to ten anti-Compton shielded EXOGAM Clover detectors, four to six anti-Compton shielded large coaxial GASP detectors and two standard Clover detectors. For a part of the campaign the array was combined with 16 LaBr3:(Ce) detectors from the FATIMA collaboration. The detectors were arranged in an array of rhombicuboctahedron geometry, providing the possibility to carry out very precise angular correlation and directional-polarization correlation measurements. The triggerless acquisition system allowed a signal collection rate of up to 6 × 105 Hz. The data allowed to set multi-fold coincidences to obtain decay schemes and in combination with the FATIMA array of LaBr3:(Ce) detectors to analyze half-lives of excited levels in the pico- to microsecond range. Precise energy and efficiency calibrations of EXILL were performed using standard calibration sources of 133Ba, 60Co and 152Eu as well as data from the reactions 27Al(n,γ)28Al and 35Cl(n,γ)36Cl in the energy range from 30 keV up to 10 MeV.

The performance of the diffusive gradient in thin film technique (DGT) was evaluated as a tool for the long-term monitoring of water quality, using uranium as a case study. DGTs with a Metsorb™ (TiO2) sorbent were deployed consecutively at two alkaline freshwater sites, the River Enborne and the River Lambourn, UK for seven-day intervals over a five-month deployment period to obtain time weighted average concentrations. Weekly spot samples were taken to determine physical and chemical properties of the river water. Uranium was measured in these spot samples and after extraction from the DGT devices. The accuracy of the DGT device time weighted average concentrations to averaged spot water samples in both rivers was 86% (27 to 205%). The DGT diffusive boundary layer (DBL) (0.037-0.141 cm - River Enborne and 0.062-0.086 cm - River Lambourn) was affected by both water flow and biofouling of the diffusion surface. DBL thicknesses found at both sites were correlated with flow conditions with an R(2) value of 0.614. Correlations were also observed between the DBL thickness and dissolved organic carbon (R(2) = 0.637) in the River Lambourn, indicating the potential presence of a complex zone of chemical interactions at the surface of the DGT. The range of DBL thicknesses found at the River Lambourn site were also attributed to of the development of macro-flora on the active sampling surface, indicating that the DBL thickness cannot be assumed to be water flow dependant only. Up to a 57% under-estimate of uranium DGT concentration was observed compared to spot sample concentrations if the DBL was neglected. This study has shown that the use of DGT can provide valuable information in environmental monitoring schemes as part of a 'tool-box' approach when used alongside conventional spot sampling methods.

Sudden increases in the background gamma-radiation dose may occur due to the removal of (222)Rn and (220)Rn progeny from the atmosphere by wet deposition mechanisms. This contribution has been measured using a Geiger-Muller detector at the Atomic Weapons Establishment (Aldermaston, UK) during July 2005-April 2006. The results are approximated by a log-normal distribution and there were nine separate occurrences of the gamma-radiation dose exceeding 125% of the geometric mean value. The increases were associated with periods of heavy rainfall, although no correlation was evident between the dose rate and the amount of rainfall, as increased rainfall dilutes the activity further rather than increasing its atmospheric removal. The events were preceded by periods of fine weather and atmospheric stability that allow for the build-up of (222)Rn and (220)Rn progeny. Similar increases in gamma-radiation dose have been measured at a nearby monitoring station situated approximately 11 miles from Aldermaston. Increases in gamma-radiation dose during heavy rainfall have also been observed throughout the UK, that followed the trajectory of an air mass. All events decreased to typical values within 1-2 h as the water permeated into the ground below and the radioactivity decayed away.

Commercially available Diphonix(®) resin (TrisKem International) was evaluated as a receiving phase for use with the diffusive gradients in thin-films (DGT) passive sampler for measuring uranium. This resin has a high partition coefficient for actinides and is used in the nuclear industry. Other resins used as receiving phases with DGT for measuring uranium have been prone to saturation and significant chemical interferences. The performance of the device was evaluated in the laboratory and in field trials. In laboratory experiments uptake of uranium (all 100% efficiency) by the resin was unaffected by varying pH (4-9), ionic strength (0.01-1.00 M, as NaNO3) and varying aqueous concentrations of Ca(2+) (100-500 mg L(-1)) and HCO3(-) (100-500 mg L(-1)). Due to the high partition coefficient of Diphonex(®), several elution techniques for uranium were evaluated. The optimal eluent mixture was 1M NaOH/1M H2O2, eluting 90% of the uranium from the resin. Uptake of uranium was linear (R(2)=0.99) over time (5 days) in laboratory experiments using artificial freshwater showing no saturation effects of the resin. In field deployments (River Lambourn, UK) the devices quantitatively accumulated uranium for up to 7 days. In both studies uptake of uranium matched that theoretically predicted for the DGT. Similar experiments in seawater did not follow the DGT theoretical uptake and the Diphonix(®) appeared to be capacity limited and also affected by matrix interferences. Isotopes of uranium (U(235)/U(238)) were measured in both environments with a precision and accuracy of 1.6-2.2% and 1.2-1.4%, respectively. This initial study shows the potential of using Diphonix(®)-DGT for monitoring of uranium in the aquatic environment.