James C. Hayes

Detection and analysis of xenon isotopes for the comprehensive nuclear-test-ban treaty international monitoring system.

The use of the xenon isotopes for detection of nuclear explosions is of great interest for monitoring compliance with the comprehensive nuclear-test-ban treaty (CTBT). Recently, the automated radioxenon sampler-analyzer (ARSA) was tested at the Institute for Atmospheric Radioactivity (IAR) in Freiburg, Germany to ascertain its use for the CTBT by comparing its results to laboratory-based analyses, determining its detection sensitivity and analyzing its results in light of historical xenon isotope levels and known reactor operations in the area. Xe-133 was detected nearly every day throughout the test at activity concentrations ranging between approximately 0.1 mBq/m3 to as high as 120 mBq/m3. Xe-133m and 135Xe were also detected occasionally during the test at concentrations of less than 1 to a few mBq/m3.

Measurements of ambient radioxenon levels using the automated radioxenon sampler/analyzer (ARSA)

The Pacific Northwest National Laboratory has developed an Automated Radioxenon Sampler/Analyzer (ARSA) in support of the Comprehensive Nuclear-Test-Ban-Treaty (CTBT) to measure four radioxenon isotopes: 131mXe, 133mXe, 133gXe, and 135gXe. This system uses a beta-gamma coincidence counting detector to produce two-dimensional plots of gamma-energy versus beta-energy. Betas and conversion electrons (CE) are detected in a cylindrical plastic scintillation cell and gamma and X-rays are detected in a surrounding NaI(Tl) scintillation detector. The ARSA has been field tested at several locations to measure the radioxenon concentrations. Most recently it has been deployed at the Institut für Atmosphärische Radioaktivität in Freiburg, Germany. During the first 4 months of 2000 the measured 133Xe oncentrations have varied between 0.0±0.1 and 110±10 mBq/m3 air. The longer lived 131mXe (T1/2 = 11.9 d) and short lived 135Xe (T1/2 = 9.1 h) have also been detected in small quantities, while 133mXe concentrations have been consistent with zero. Minimum detectable concentration (MDC) calculations for 133gXe fell well below the 1 mBq per standard-cubic-meter of air requirement adopted by the CTBT Preparatory Commission.1 A description of the radioxenon detector, the concentration and MDC calculations and preliminary results of the field test in Germany are presented.

Analysis of data from sensitive U.S. monitoring stations for the Fukushima Dai-ichi nuclear reactor accident

The March 11, 2011 9.0 magnitude undersea megathrust earthquake off the coast of Japan and subsequent tsunami waves triggered a major nuclear event at the Fukushima Dai-ichi nuclear power station. At the time of the event, units 1, 2, and 3 were operating and units 4, 5, and 6 were in a shutdown condition for maintenance. Loss of cooling capacity to the plants along with structural damage caused by the earthquake and tsunami resulted in a breach of the nuclear fuel integrity and release of radioactive fission products to the environment. Fission products started to arrive in the United States via atmospheric transport on March 15, 2011 and peaked by March 23, 2011. Atmospheric activity concentrations of (131)I reached levels of 3.0×10(-2) Bqm(-3) in Melbourne, FL. The noble gas (133)Xe reached atmospheric activity concentrations in Ashland, KS of 17 Bqm(-3). While these levels are not health concerns, they were well above the detection capability of the radionuclide monitoring systems within the International Monitoring System of the Comprehensive Nuclear-Test-Ban Treaty.

Redox-Active Metal–Organic Composites for Highly Selective Oxygen Separation Applications

A redox-active metal-organic composite material shows improved and selective O2 adsorption over N2 with respect to individual components (MIL-101 and ferrocene). The O2 sensitivity of the composite material arises due to the formation of maghemite nanoparticles with the pore of the metal-organic framework material.

The science case for 37Ar as a monitor for underground nuclear explosions

A new calculation of the production of 37Ar from nuclear explosion neutron interactions on 40Ca in a suite of common sub-surface materials (rock, etc) is presented. Even in mineral structures that are relatively low in Ca, the resulting 37Ar signature is large enough for detection in cases of venting or gaseous diffusion driven by barometric pumping. Field and laboratory detection strategies and projected sensitivities are presented.

Noble gas migration experiment to support the detection of underground nuclear explosions

A Noble Gas Migration Experiment injected 127Xe, 37Ar, and sulfur hexafluoride into a former underground nuclear explosion shot cavity. These tracer gases were allowed to migrate from the cavity to near-surface and surface sampling locations and were detected in soil gas samples collected using various on-site inspection sampling approaches. Based on this experiment we came to the following conclusions: (1) SF6 was enriched in all of the samples relative to both 37Ar and 127Xe. (2) There were no significant differences in the 127Xe to 37Ar ratio in the samples relative to the ratio injected into the cavity. (3) The migratory behavior of the chemical and radiotracers did not fit typical diffusion modeling scenarios.

Atmospheric plume progression as a function of time and distance from the release point for radioactive isotopes

The radionuclide network of the International Monitoring System comprises up to 80 stations around the world that have aerosol and xenon monitoring systems designed to detect releases of radioactive materials to the atmosphere from nuclear explosions. A rule of thumb description of plume concentration and duration versus time and distance from the release point is useful when designing and deploying new sample collection systems. This paper uses plume development from atmospheric transport modeling to provide a power-law rule describing atmospheric dilution factors as a function of distance from the release point. Consider the plume center-line concentration seen by a ground-level sampler as a function of time based on a short-duration ground-level release of a nondepositing radioactive tracer. The concentration C (Bq m(-3)) near the ground varies with distance from the source with the relationship C=R×A(D,C) ×e (-λ(-1.552+0.0405×D)) × 5.37×10(-8) × D(-2.35) where R is the release magnitude (Bq), D is the separation distance (km) from the ground level release to the measurement location, λ is the decay constant (h(-1)) for the radionuclide of interest and AD,C is an attenuation factor that depends on the length of the sample collection period. This relationship is based on the median concentration for 10 release locations with different geographic characteristics and 365 days of releases at each location, and it has an R(2) of 0.99 for 32 distances from 100 to 3000 km. In addition, 90 percent of the modeled plumes fall within approximately one order of magnitude of this curve for all distances.

Development of an absolute gas-counting capability for low to medium activities.

Pacific Northwest National Laboratory (PNNL) is developing a capability to measure the absolute activity concentration of gaseous radionuclides using length-compensated proportional-counting. This capability will enable the validation of low-level calibration standards for use in PNNLs new shallow underground laboratory. Two sets of unequal length proportional counters have been fabricated; one set has been fabricated using ultra-low background (ULB) electroformed copper and a second set fabricated from Oxygen-Free High-Conductivity Copper (OFHC).

Alternative treaty monitoring approaches using ultra-low background measurement technology

The International Monitoring System (IMS) of the Comprehensive Test Ban Treaty includes a network of stations and laboratories for collection and analysis of radioactive aerosols. Alternative approaches to IMS operations are considered as a method of enhancing treaty verification. Ultra-low background (ULB) detection promises the possibility of improvements to IMS minimum detectable activities (MDAs) well below the current approach, requiring MDA < or = 30 microBq/m(3) of air for (140)Ba, or about 10(6) fissions per daily sample.

Abatement of xenon and iodine emissions from medical isotope production facilities.

The capability of the International Monitoring System (IMS) to detect xenon from underground nuclear explosions is dependent on the radioactive xenon background. Adding to the background, medical isotope production (MIP) by fission releases several important xenon isotopes including xenon-133 and iodine-133 that decays to xenon-133. The amount of xenon released from these facilities may be equivalent to or exceed that released from an underground nuclear explosion. Thus the release of gaseous fission products within days of irradiation makes it difficult to distinguish MIP emissions from a nuclear explosion. In addition, recent shortages in molybdenum-99 have created interest and investment opportunities to design and build new MIP facilities in the United States and throughout the world. Due to the potential increase in the number of MIP facilities, a discussion of abatement technologies provides insight into how the problem of emission control from MIP facilities can be tackled. A review of practices is provided to delineate methods useful for abatement of medical isotopes.