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.

Innovative concept for a major breakthrough in atmospheric radioactive xenon detection for nuclear explosion monitoring.

The verification regime of the comprehensive test ban treaty (CTBT) is based on a network of three different waveform technologies together with global monitoring of aerosols and noble gas in order to detect, locate and identify a nuclear weapon explosion down to 1 kt TNT equivalent. In case of a low intensity underground or underwater nuclear explosion, it appears that only radioactive gases, especially the noble gas which are difficult to contain, will allow identification of weak yield nuclear tests. Four radioactive xenon isotopes, 131mXe, 133mXe, 133Xe and 135Xe, are sufficiently produced in fission reactions and exhibit suitable half-lives and radiation emissions to be detected in atmosphere at low level far away from the release site. Four different monitoring CTBT systems, ARIX, ARSA, SAUNA, and SPALAX™ have been developed in order to sample and to measure them with high sensitivity. The latest developed by the French Atomic Energy Commission (CEA) is likely to be drastically improved in detection sensitivity (especially for the metastable isotopes) through a higher sampling rate, when equipped with a new conversion electron (CE)/X-ray coincidence spectrometer. This new spectrometer is based on two combined detectors, both exhibiting very low radioactive background: a well-type NaI(Tl) detector for photon detection surrounding a gas cell equipped with two large passivated implanted planar silicon chips for electron detection. It is characterized by a low electron energy threshold and a much better energy resolution for the CE than those usually measured with the existing CTBT equipments. Furthermore, the compact geometry of the spectrometer provides high efficiency for X-ray and for CE associated to the decay modes of the four relevant radioxenons. The paper focus on the design of this new spectrometer and presents spectroscopic performances of a prototype based on recent results achieved from both radioactive xenon standards and air sample measurements. Major improvements in detection sensitivity have been reached and quantified, especially for metastable radioactive isotopes 131mXe and 133mXe with a gain in minimum detectable activity (about 2 × 10-3 Bq) relative to current CTBT SPALAX™ system (air sampling frequency normalized to 8 h) of about 70 and 30 respectively.

Measurement and modelling of radioxenon plumes in the Ottawa Valley.

Since 2001 a real-time radiation monitoring network of Canadian nuclear facilities and major population centres has been implemented for response to nuclear incidents including a possible terrorist attack. Unshielded NaI(Tl) spectroscopic detectors are employed to measure gamma radiation from airborne radioactivity and radioactivity deposited on the ground. These detectors are composed of a standard 3''x3'' cylindrical NaI(Tl) spectrometers with data storage and integrated telemetry. Some of the detectors have been deployed in the Ottawa Valley near Chalk River Laboratories and Ottawa, which has a complex radioxenon environment due to the proximity of nuclear power reactors, and medical isotope facilities. Although not a health threat, these releases have provided an opportunity for the Canadian Meteorological Centre and the Commissariat à l'Energie Atomique to validate their meteorological models. The meteorological models of the two organizations are in good agreement on the origin and the source terms of these releases.

Automated radioxenon monitoring for the comprehensive nuclear-test-ban treaty in two distinctive locations: Ottawa and Tahiti.

In preparation for verification of the Comprehensive Nuclear-Test-Ban-Treaty, automated radioxenon monitoring is performed in two distinctive environments: Ottawa and Tahiti. These sites are monitored with SPALAX (Systeme de Prelevement d'air Automatique en Ligne avec l'Analyse des radioXenons) technology, which automatically extracts radioxenon from the atmosphere and measures the activity concentrations of (131m,133m,133,135)Xe. The resulting isotopic concentrations can be useful to discern nuclear explosions from nuclear industry xenon emissions. Ambient radon background, which may adversely impact analyser sensitivity, is discussed. Upper concentration limits are reported for the apparently radioxenon free Tahiti environment. Ottawa has a complex radioxenon background due to proximity to nuclear reactors and medical isotope facilities. Meteorological models suggest that, depending on the wind direction, the radioxenon detected in Ottawa can be characteristic of the normal radioxenon background in the Eastern United States, Europe, and Japan or distinctive due to medical isotope production.

Atmospheric xenon radioactive isotope monitoring.

The Comprehensive Nuclear Test Ban Treaty (CTBT) organisation is implementing a world-wide monitoring network in order to check that the State Signatories comply with the treaty. One of the monitoring facilities consists of an atmospheric noble gas monitoring equipment. According to the requirements annexed in the treaty, the French Atomic Energy Commission (CEA) developed a device, called SPALAX, which automatically extracts xenon from ambient air and makes in situ measurements of the activities of four xenon radioisotopes (131mXe, 133mXe, 133Xe, 135Xe). The originality of this device is noticeable essentially in the gas sample processing method: thanks to the coupling of a gas permeator and of a noble gas specific adsorbent, it can selectively extract and concentrate xenon to more than 3 x 10 E6. This process is carried out continuously without cryogenic cooling, without any regeneration time. The detection of the xenon radioactive isotopes is done automatically by high spectral resolution gamma spectrometry, a robust technology well-suited for on-field instrumentation. In the year 2000, a prototype was involved in an international evaluation exercise directed by the CTBT organisation (CTBTO). This exercise demonstrated that the SPALAX equipment perfectly met the requirements of the CTBTO for such systems. On the basis of the continuous 24-h resolution record of the atmospheric xenon radioactive isotopes concentrations, the SPALAX system also demonstrated that ambient levels of 133Xe can fluctuate quickly from less than the detection limit to over 40 x 10(-3) Bq m(-3). In order to build an industrial version of this equipment, the CEA entered into a partnership with a French engineering company (S.F.I., Marseille, France), which is now able to produce an industrial version of SPALAX, i.e. more compact and more efficient than the prototypes. The 133Xe minimum detectable concentration is 0.15 x 10(-3) Bq m(-3) air per 24 h sampling cycle.

Intercomparison experiments of systems for the measurement of xenon radionuclides in the atmosphere.

Radioactive xenon monitoring is one of the main technologies used for the detection of underground nuclear explosions. Precise and reliable measurements of (131m)Xe, (133g)Xe, (133m)Xe, and (135g)Xe are required as part of the International Monitoring System for compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT). For the first time, simultaneous testing of four highly sensitive and automated fieldable radioxenon measurement systems has been performed and compared to established laboratory techniques. In addition to an intercomparison of radioxenon monitoring equipment of different design, this paper also presents a set of more than 2000 measurements of activity concentrations of radioactive xenon made in the city of Freiburg, Germany in 2000. The intercomparison experiment showed, that the results from the newly developed systems agree with each other and the equipment fulfills the fundamental requirements for their use in the verification regime of the CTBT. For 24-h measurements, concentrations as low as 0.1 mBqm(-3) were measured for atmospheric samples ranging in size from 10 to 80 m(3). The (133)Xe activity concentrations detected in the ambient air ranged from below 1 mBqm(-3) to above 100 mBqm(-3).