P. Gross

Improvements of low-level radioxenon detection sensitivity by a state-of-the art coincidence setup

The ability to quantify isotopic ratios of 135, 133 m, 133 and 131 m radioxenon is essential for the verification of the Comprehensive Nuclear-Test Ban Treaty (CTBT). In order to improve detection limits, CEA has developed a new on-site setup using photon/electron coincidence (Le Petit et al., 2013. J. Radioanal. Nucl. Chem., DOI : 10.1007/s 10697-013-2525-8.). Alternatively, the electron detection cell equipped with large silicon chips (PIPS) can be used with HPGe detector for laboratory analysis purpose. This setup allows the measurement of β/γ coincidences for the detection of (133)Xe and (135)Xe; and K-shell Conversion Electrons (K-CE)/X-ray coincidences for the detection of (131m)Xe, (133m)Xe and (133)Xe as well. Good energy resolution of 11 keV at 130 keV and low energy threshold of 29 keV for the electron detection were obtained. This provides direct discrimination between K-CE from (133)Xe, (133m)Xe and (131m)Xe. Estimation of Minimum Detectable Activity (MDA) for (131m)Xe is in the order of 1mBq over a 4 day measurement. An analysis of an environmental radioxenon sample using this method is shown.

Spalax™ new generation: A sensitive and selective noble gas system for nuclear explosion monitoring

In the context of the verification regime of the Comprehensive nuclear Test ban Treaty (CTBT), CEA is developing a new generation (NG) of SPALAX™ system for atmospheric radioxenon monitoring. These systems are able to extract more than 6cm(3) of pure xenon from air samples each 12h and to measure the four relevant xenon radioactive isotopes using a high resolution detection system operating in electron-photon coincidence mode. This paper presents the performances of the SPALAX™ NG prototype in operation at Bruyères-le-Châtel CEA centre, integrating the most recent CEA developments. It especially focuses on an innovative detection system made up of a gas cell equipped with two face-to-face silicon detectors associated to one or two germanium detectors. Minimum Detectable activity Concentrations (MDCs) of environmental samples were calculated to be approximately 0.1 mBq/m(3) for the isotopes (131m)Xe, (133m)Xe, (133)Xe and 0.4 mBq/m(3) for (135)Xe (single germanium configuration). The detection system might be used to simultaneously measure particulate and noble gas samples from the CTBT International Monitoring System (IMS). That possibility could lead to new capacities for particulate measurements by allowing electron-photon coincidence detection of certain fission products.

An introduction to γ3 a new versatile ultralow background gamma spectrometer. Background description and analysis

The γ(3) setup has been designed as a versatile, high sensitivity spectrometry platform. State-of-the art techniques have been implemented to reduce its background to minimum level even though the system is installed at ground level. The shield design and background performance of the setup are presented. The spectrometer is composed of three identical HPGe detectors for high detection efficiency or coincidence measurement and can accommodate several sample geometries. Its shield includes three layers of increasing purity lead, a cosmic veto, an inner borated polyethylene layer, and a radon-free gas injection system. The spectrometer normalized background count rate is 4.4 counts per minutekgGe(-1) (in the 40-2500keV energy range). Its background characteristics, cosmic veto efficiency, and radon-free gas injection performances are discussed.

Characterization of Xe-133 global atmospheric background: Implications for the International Monitoring System of the Comprehensive Nuclear-Test-Ban Treaty

Monitoring atmospheric concentrations of radioxenons is relevant to provide evidence of atmospheric or underground nuclear weapon tests. However, when the design of the International Monitoring Network (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) was set up, the impact of industrial releases was not perceived. It is now well known that industrial radioxenon signature can interfere with that of nuclear tests. Therefore, there is a crucial need to characterize atmospheric distributions of radioxenons from industrial sources—the so-called atmospheric background—in the frame of the CTBT. Two years of Xe-133 atmospheric background have been simulated using 2013 and 2014 meteorological data together with the most comprehensive emission inventory of radiopharmaceutical facilities and nuclear power plants to date. Annual average simulated activity concentrations vary from 0.01 mBq/m3 up to above 5 mBq/m3 nearby major sources. Average measured and simulated concentrations agree on most of the IMS stations, which indicates that the main sources during the time frame are properly captured. Xe-133 atmospheric background simulated at IMS stations turn out to be a complex combination of sources. Stations most impacted are in Europe and North America and can potentially detect Xe-133 every day. Predicted occurrences of detections of atmospheric Xe-133 show seasonal variations, more accentuated in the Northern Hemisphere, where the maximum occurs in winter. To our knowledge, this study presents the first global maps of Xe-133 atmospheric background from industrial sources based on two years of simulation and is a first attempt to analyze its composition in terms of origin at IMS stations.

On the use of 127Xe standards for the quality control of CTBTO noble gas stations and support laboratories

(127)Xe has a longer half-life than (131m)Xe, it can be easily purely produced and it is present in the environment at very low level. For these reasons, (127)Xe is supposed to be a convenient quality control radionuclide for remote noble gas stations of the International Monitoring System (IMS) network. As CEA/DAM has recently developed two new photon/electron setups for low-level detection of (131m)Xe, (133m)Xe, (133)Xe and (135)Xe, we took the opportunity to test these setups for the measurement of a (127)Xe standard. The results and a detailed description of these measurements are presented in this paper. They illustrate the complexity of (127)Xe decay, emitting simultaneously several γ, X-rays, conversion electrons and Auger electrons; this results in highly summated coincidence spectra. The measurements performed provide precise electron energy calibration of the setups. The count rate of electrons in coincidence with iodine Kα X-rays was found to be surprisingly low, leading to the study of electron-gated photon spectrum. Finally, a comparison of three photon/electron coincidence spectra obtained with three different setups is given. The use of (127)Xe as a standard for energy calibration of IMS noble gas station is possible, but it appears to be quite complicated for efficiency check of noble gas station equipped with β/γ detectors.

Long-term performances of the 95ZR/95Nb chronometer for nuclear events dating

The present work reports on a long-term analysis of the performances of the (95)Zr/(95)Nb chronometer for dating a nuclear event. Taking benefit of a recent Profiency Test Exercise, a sample containing a standardized mixture of fission products has been measured repeatedly with a low background HPGe spectrometer during a period extending up to one year with the aim of assessing the accuracy of the various zero-time determinations. Evaluation of the uncertainties associated to these evaluations was performed using a Monte Carlo approach. Input parameters sensitivity has been investigated, especially the influence of the (95m)Nb decay branch. The (95)Zr/(95)Nb chronometer was found to be accurate for zero-time determination within one day and one week for a decay of 3 months and 10 months respectively. Sub-day uncertainties are achievable for a two months old sample whereas sub-week uncertainties are reached after a decay of six months. Limitations of the technique for dating a real event are investigated.

Ground surface ultralow background spectrometer: Active shielding improvements and coincidence measurements for the Gamma3 spectrometer

The ultralow background versatile spectrometer GAMMA3 has been optimized with the following shielding improvements: (i) optimized nitrogen injection flux of 300Lh-1, and (ii) cosmic veto configuration with 9 scintillating plates. These improvements allow a reduction of 39% of the normalized integral background count rate down to 2.7±0.2min-1kgGe-1 (40-2500keV energy range). Minimum Detectable Activities when performing direct γ-ray spectrometry or γ-γ coincidence spectrometry are compared.

Low-level laboratory measurement of xenon radionuclides: Electron-photon versus photon measurements

Radioactive xenon (mainly 131mXe, 133Xe, 133mXe and 135Xe) are tracked as markers of nuclear weapons testing. The CEA has developed the PIPSBox, a measurement cell able to detect electrons emitted by xenon nuclides. Combined with an ultra-low background γ spectrometer, electron detection capacities allow reaching minimum detectable activities (MDA) for a 3-day long measurement of about 0.5mBq for the four xenon radionuclides. Compared to a classical measurement cell, MDAs are improved by a factor of 2-4.

SPALAX NG: A breakthrough in radioxenon field measurement

Lessons-learned from 10 years of noble gas stations operation and dedicated R&D allowed the design of a New Generation of station. In order to produce 60m3 air equivalent Xenon samples every 8h, it implements: (i) larger sampler unit for Xenon extraction (2 compressors and 8 nitrogen membranes), (ii) new noble gas adsorbent (Ag@ZSM5), (iii) hardened components and (iv) new high resolution coincidence low background spectrometer (HPGe/PIPSBox). Station expected radioxenon sensitivity is lower than 0.3mBq/m3.