Emily K. Mace

A shallow underground laboratory for low-background radiation measurements and materials development.

Pacific Northwest National Laboratory recently commissioned a new shallow underground laboratory, located at a depth of approximately 30 meters-water-equivalent. This new addition to the small class of radiation measurement laboratories located at modest underground depths houses the latest generation of custom-made, high-efficiency, low-background gamma-ray spectrometers and gas proportional counters. This paper describes the unique capabilities present in the shallow underground laboratory; these include large-scale ultra-pure materials production and a suite of radiation detection systems. Reported data characterize the degree of background reduction achieved through a combination of underground location, graded shielding, and rejection of cosmic-ray events. We conclude by presenting measurement targets and future opportunities.

Signatures and Methods for the Automated Nondestructive Assay of

International Atomic Energy Agency (IAEA) inspectors currently perform periodic inspections at uranium enrichment plants to verify UF6 cylinder enrichment declarations. Measurements are typically performed with handheld high-resolution sensors on a sampling of cylinders taken to be representative of the facilitys entire cylinder inventory. These measurements are time-consuming, expensive, and assay only a small fraction of the total cylinder volume. An automated nondestructive assay system capable of providing enrichment measurements over the full volume of the cylinder could improve upon current verification practices in terms of manpower and assay accuracy. The 185-keV emission from U-235 is utilized in todays cylinder measurements, but augmenting this “traditional” signature with more-penetrating “non-traditional” signatures could help to achieve full-volume assay in an automated system. This paper describes the study of non-traditional signatures that include neutrons produced by F-19 (α, n) reactions (spawned primarily from U-234 alpha emission) and the high-energy gamma rays (extending up to 8 MeV) induced by those neutrons when they interact in the cylinder wall and nearby materials. The potential of these non-traditional signatures and assay methods for automated cylinder verification is explored using field measurements on a small population of cylinders ranging from 2.0% to 5% in U-235 enrichment. The standard deviation of the non-traditional high-energy gamma-ray assay approach was 4.7% relative to the declared cylinder enrichments; the standard deviation of the traditional enrichment meter approach using a well-collimated high-resolution spectrometer was 4.3%. The prospect of using the non-traditional high-energy gamma-ray signature in concert with the traditional 185-keV signature to reduce the uncertainty of automated cylinder assay is discussed.

{\rm UF}_{6}

A new ultra-low-background proportional counter was recently developed with an internal volume of 100 cm(3) and has been characterized at pressures from 1-10 atm with P-10 (90% Ar, 10% methane) gas. This design, along with a counting system providing event digitization and passive and active shielding, has been developed to complement a new shallow underground laboratory (30 m water-equivalent). Backgrounds and low-level reference materials have been measured, and system sensitivity for (37)Ar has been calculated.

Cylinders at Uranium Enrichment Plants

A deuterium-tritium (DT) associated particle neutron generator (APNG) with active focusing has been operated using an alpha particle detector made of a ZnO:Ga phosphor with decay time of approximately 1 ns. The APNG is capable of producing 109 neutrons per second. The DT beam spot diameter was adjusted and measured from 7 mm to 2.1 mm with the possibility of achieving 1 mm subject to the removal of a safety interlock protecting the APNG tritiated target. In addition, the alpha detector was found to have a detection efficiency of 88% and sub-nanosecond time resolution (<0.7 ns) using a Burle 8850 bialkali photocathode. Lastly, the neutron beam was obstructed using various amounts of lead shielding to study the generators imaging contrast capability for neutron radiography. The APNG provides high-rate capability and a large solid angle with acceptance of 8%.

A new shallow underground gas-proportional counting lab—First results and Ar-37 sensitivity

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.

Characterization of an Associated Particle Neutron Generator With ZnO:Ga Alpha-Detector and Active Focusing

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).

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

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.

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

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.

Development of a Low-Level Ar-37 Calibration Standard

Characterization of two sets of custom unequal length proportional counters is underway at Pacific Northwest National Laboratory (PNNL). These detectors will be used in measurements to determine the absolute activity concentration of gaseous radionuclides (e.g., 37Ar). A set of three detectors has been fabricated based on previous PNNL ultra-low-background proportional counter designs and now operate in PNNLs shallow underground counting laboratory. A second set of four counters has also been fabricated using clean assembly of Oxygen-Free High-Conductivity copper components for use in a shielded above-ground counting laboratory. Characterization of both sets of detectors is underway with measurements of background rates, gas gain, and energy resolution. These results will be presented along with a shielding study for the above-ground cave.

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

Development of ultra low background gas proportional counters has made the contribution from naturally occurring radioactive isotopes - primarily α and β activity in the uranium and thorium decay chains - inconsequential to instrumental sensitivity levels when measurements are performed in above ground surface laboratories. Simple lead shielding is enough to mitigate against gamma rays as gas proportional counters are already relatively insensitive to naturally occurring gamma radiation. The dominant background in these surface laboratory measurements using ultra low background gas proportional counters is due to cosmic ray generated muons, neutrons, and protons. Studies of measurements with ultra low background gas proportional counters in surface and underground laboratories as well as radiation transport Monte Carlo simulations suggest a preferred conceptual design to achieve the highest possible sensitivity from an array of low background gas proportional counters when operated in a surface laboratory. The basis for a low background gas proportional counter array and the preferred shielding configuration is reported, especially in relation to measurements of radioactive gases having low energy decays such as (37)Ar.