Comparison of measured and simulated concentrations of 133Xe in the shallow subsurface.

Radioactive isotopes of the noble gases xenon and argon are considered primary indicators of an underground nuclear explosion. However, high atmospheric concentrations from other anthropogenic sources may lead to an elevation in the underground levels of these gases, particularly in times of increasing atmospheric pressure. In 2014, a week long sampling campaign near Canadian Nuclear Laboratories in the Ottawa River Valley resulted in first of their kind measurements of atmospheric 133Xe that had been pressed into the subsurface. In an effort to better understand this imprinting process, a second follow-up sampling campaign was conducted in the same location in 2016. The results of the second sampling campaign, where samples were collected at depths of 1 m and 2 m over a 14 day period and measured for their 133Xe concentration, are presented here. Gas transport and sample concentrations were predicted using the Subsurface Transport over Multiple Phases (STOMP) simulator. These results are examined and compared to the corresponding experimental results.

Xenon adsorption on geological media and implications for radionuclide signatures.

The detection of radioactive noble gases is a primary technology for verifying compliance with the pending Comprehensive Nuclear-Test-Ban Treaty. A fundamental challenge in applying this technology for detecting underground nuclear explosions is estimating the timing and magnitude of the radionuclide signatures. While the primary mechanism for transport is advective transport, either through barometric pumping or thermally driven advection, diffusive transport in the surrounding matrix also plays a secondary role. From the study of primordial noble gas signatures, it is known that xenon has a strong physical adsorption affinity in shale formations. Given the unselective nature of physical adsorption, isotherm measurements reported here show that non-trivial amounts of xenon adsorb on a variety of media, in addition to shale. A dual-porosity model is then discussed demonstrating that sorption amplifies the diffusive uptake of an adsorbing matrix from a fracture. This effect may reduce the radioxenon signature down to approximately one-tenth, similar to primordial xenon isotopic signatures.

Measuring the noble metal and iodine composition of extracted noble metal phase from spent nuclear fuel using instrumental neutron activation analysis.

Masses of noble metal and iodine nuclides in the metallic noble metal phase extracted from spent fuel are measured using instrumental neutron activation analysis. Nuclide presence is predicted using fission yield analysis, and radionuclides are identified and the masses quantified using neutron activation analysis. The nuclide compositions of noble metal phase derived from two dissolution methods, UO2 fuel dissolved in nitric acid and UO2 fuel dissolved in ammonium-carbonate and hydrogen-peroxide solution, are compared.

Source term estimation of radioxenon released from the Fukushima Dai-ichi nuclear reactors using measured air concentrations and atmospheric transport modeling.

Systems designed to monitor airborne radionuclides released from underground nuclear explosions detected radioactive fallout across the northern hemisphere resulting from the Fukushima Dai-ichi Nuclear Power Plant accident in March 2011. Sampling data from multiple International Modeling System locations are combined with atmospheric transport modeling to estimate the magnitude and time sequence of releases of (133)Xe. Modeled dilution factors at five different detection locations were combined with 57 atmospheric concentration measurements of (133)Xe taken from March 18 to March 23 to estimate the source term. This analysis suggests that 92% of the 1.24 × 10(19) Bq of (133)Xe present in the three operating reactors at the time of the earthquake was released to the atmosphere over a 3 d period. An uncertainty analysis bounds the release estimates to 54-129% of available (133)Xe inventory.

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.

Elevated radioxenon detected remotely following the Fukushima nuclear accident.

We report on the first measurements of short-lived gaseous fission products detected outside of Japan following the Fukushima nuclear releases, which occurred after a 9.0 magnitude earthquake and tsunami on March 11, 2011. The measurements were conducted at the Pacific Northwest National Laboratory (PNNL), (46°16'47″N, 119°16'53″W) located more than 7000 km from the emission point in Fukushima Japan (37°25'17″N, 141°1'57″E). First detections of (133)Xe were made starting early March 16, only four days following the earthquake. Maximum concentrations of (133)Xe were in excess of 40 Bq/m(3), which is more than ×40,000 the average concentration of this isotope is this part of the United States.

Total potential source contribution function analysis of trace elements determined in aerosol samples collected near Lake Huron.

Aerosol samples were collected at the rural Burnt Island Ontario Integrated Air Deposition Network air sampling station on the northern shore of Lake Huron from 1992 through 1994. The samples were analyzed for trace elements by neutron activation analysis, and the air concentrations of over 30 elements were determined. Total potential source contribution function analysis (TPSCF) was used to determine the most probable geographical location of these aerosols' origin. The TPSCF results for As, In, Sb, Se, Sn, and Zn are highlighted in this paper. Source regions for these elements ranged from Alma, Quebec, Canada to Carrollton, GA. Because of large seasonal variations in the concentrations of the atmospheric concentrations of these elements, TPSCFvalues were calculated for the summer and winter halves of the year as well as the entire year.

Optimizing the removal of carbon phases in soils and sediments for sequential chemical extractions by coulometry.

We have developed a coulometric technique to optimize the removal of the carbonate and organic fractions for sequential chemical extractions of soils and sediments. The coulometric system facilitates optimizing these two fractions by direct real-time measurement of carbon dioxide (CO2) evolved during the removal of these two fractions. Further analyses by ICP-MS and alpha-spectrometry aided in interpreting the results of coulometry experiments. The effects of time, temperature, ionic strength and pH were investigated. The sensitivity of the coulometric reaction vessel/detection system was sufficient even at very low total carbon content (< 0.1 mol kg-1). The efficiency of the system is estimated to be 96% with a standard deviation of 8%. Experiments were carried out using NIST Standard Reference Materials 4357 Ocean Sediment (OS), 2704 Buffalo River Sediment (BRS), and pure calcium carbonate. Carbonate minerals were dissolved selectively using an ammonium acetate-acetic acid buffer. Organic matter was then oxidized to CO2 using hydrogen peroxide (H2O2) in nitric acid. The carbonate fraction was completely dissolved within 120 min under all conditions examined (literature suggests up to 8 h). For the OS standard, the oxidation of organic matter self-perpetuates between 45 and 50 degrees C, a factor of two less than commonly suggested, while organic carbon in the BRS standard required 80 degrees C for the reaction to proceed to completion. For complete oxidation of organic matter, we find that at least three additions of H2O2 are required (popular methods suggest one or two).