Background concentrations of Argon-39 in shallow soil gas.

While radioisotopes of noble gases are known to be indicators of underground nuclear explosions (UNE), McIntyre et al. (2017) was the first to report the presence of 39Ar in shallow soil gas in association with a decades old UNE. While this finding hinted at the potential application of 39Ar to be used as an indicator of a UNE, doing so would also require an understanding of the natural concentrations of 39Ar present in soil gas. Without knowing the expected range and variability of naturally occurring concentrations of 39Ar, it is difficult to determine what measured concentrations would be indicative of an elevated concentration. This paper presents results from 16 soil gas samples and three atmospheric air samples collected from various locations across the western United States. Shallow soil gas samples were collected into self-contained underwater breathing apparatus (SCUBA) tanks using a custom-built soil gas sampling system and then processed and analyzed for 39Ar. The measured concentrations of 39Ar varied from atmospheric air concentrations to about 3.5 times atmospheric air concentrations (58 mBq/m3). The results presented here represent the first measurements of natural background 39Ar concentrations in shallow soil gas. This data will be necessary if 39Ar is to be used as an indicator of UNE.

Migration of noble gas tracers at the site of an underground nuclear explosion at the Nevada National Security Site.

As part of an underground gas migration study, two radioactive noble gases (37Ar and 127Xe) and two stable tracer gases (SF6 and PFDMCH) were injected into a historic nuclear explosion test chimney and allowed to migrate naturally. The purpose of this experiment was to provide a bounding case (natural transport) for the flow of radioactive noble gases following an underground nuclear explosion. To accomplish this, soil gas samples were collected from a series of boreholes and a range of depths from the shallow subsurface (3 m) to deeper levels (~160 m) over a period of eleven months. These samples have provided insights into the development and evolution of the subsurface plume and constrained the relative migration rates of the radioactive and stable gas species in the case when the driving pressure from the cavity is low. Analysis of the samples concluded that the stable tracer SF6 was consistently enriched in the subsurface samples relative to the radiotracer 127Xe, but the ratios of SF6 and 37Ar remained similar throughout the samples.

Measurements of Argon-39 at the U20az underground nuclear explosion site.

Pacific Northwest National Laboratory reports on the detection of 39Ar at the location of an underground nuclear explosion on the Nevada Nuclear Security Site. The presence of 39Ar was not anticipated at the outset of the experimental campaign but results from this work demonstrated that it is present, along with 37Ar and 85Kr in the subsurface at the site of an underground nuclear explosion. Our analysis showed that by using state-of-the-art technology optimized for radioargon measurements, it was difficult to distinguish 39Ar from the fission product 85Kr. Proportional counters are currently used for high-sensitivity measurement of 37Ar and 39Ar. Physical and chemical separation processes are used to separate argon from air or soil gas, yielding pure argon with contaminant gases reduced to the parts-per-million level or below. However, even with purification at these levels, the beta decay signature of 85Kr can be mistaken for that of 39Ar, and the presence of either isotope increases the measurement background level for the measurement of 37Ar. Measured values for the 39Ar measured at the site ranged from 36,000 milli- Becquerel/standard-cubic-meter-of-air (mBq/SCM) for shallow bore holes to 997,000 mBq/SCM from the rubble chimney from the underground nuclear explosion.

Development of a low-level (37)Ar calibration standard.

Argon-37 is an environmental signature of an underground nuclear explosion. Producing and quantifying low-level (37)Ar standards is an important step in the development of sensitive field measurement instruments. This paper describes progress at Pacific Northwest National Laboratory in developing a process to generate and quantify low-level (37)Ar standards, which can be used to calibrate sensitive field systems at activities consistent with soil background levels. This paper presents a discussion of the measurement analysis, along with assumptions and uncertainty estimates.

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.

Potential impact of releases from a new molybdenum-99 production facility on regional measurements of airborne xenon isotopes.

The monitoring of the radioactive xenon isotopes (131m)Xe, (133)Xe, (133m)Xe, and (135)Xe is important for the detection of nuclear explosions. While backgrounds of the xenon isotopes are short-lived, they are constantly replenished from activities dominated by the fission-based production of (99)Mo used for medical procedures. At present, one of the most critical locations on earth for the monitoring of nuclear explosions is the Korean peninsula where the Democratic People's Republic of Korea (DPRK) has announced that it conducted three nuclear tests between 2006 and 2013. This paper explores the backgrounds that would be caused by the medium to large scale production of (99)Mo in the region of the Korean peninsula.

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 PNNL's 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).

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.

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.

End-capping of the modified melanocortin tetrapeptide (p-Cl)Phe-D-Phe-Arg-Trp-NH2 as a route to hMC4R agonists.

Of the 42 R'-X-(p-Cl)Phe-D-Phe-Arg-Trp-NH(2) (X=CO, SO(2), PO, PS) tested at the human (h)MC1, hMC3, and hMC4 receptors (R), the most potent MC4R agonists (EC(50) of 8-20 nM) were obtained by end-capping with R'=CH(2)CHCH(2) (9), NCCH(2) (16), NH(2)COCH(2) (17), HCONHCH(2) (18), CH(3)NH (19), CH(2)CHCH(2)NH (21), 2-Th (23), PhCH(2) (30) and X=CO. These compounds possess 35-60-fold hMC4 versus hMC1Rs selectivity with urea LK-71 (19) being the most potent at hMC4R and MC4/1R selective (EC(50)=8.5 nM, MC4/1R=100). LK-75 (16) combines high potency at hMC4R and MC4/3R selectivity (EC(50)=10.5 nM, MC4/3R=290). SAR is discussed.

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).

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.