Creating high-precision reference gas standards of ⁸⁵Kr for groundwater age dating

Absolute gas counting (AGC) was applied to two gas blends of ⁸⁵Kr in argon-methane (P10) counting gas to establish a high-precision specific activity (Bq/cm³) reference value for characterizing ⁸⁵Kr detection efficiency for groundwater age dating measurements. The AGC or length-compensated technique has been utilized by the metrology community for decades and is an accepted method for developing radioactive gas standards. The AGC capability at Pacific Northwest National Laboratory (PNNL) uses a set of nine unequal-length proportional counters with precisely-measured internal volumes, and a gas loading system with high-precision pressure and temperature sensors. A series of AGC measurements were collected at multiple pressures to determine the inverse pressure relationship (1/P) for ⁸⁵Kr and define a wall-effect correction that accounts for events decaying into the detector wall and not depositing sufficient energy in the gas to be detected. In addition to the wall-effect, two additional corrections were evaluated and are discussed in detail. Specifically, the threshold effect which accounts for events deposited below the analysis threshold and a detection efficiency as a function of detector volume effect that was observed during analysis. A robust uncertainty model was developed using the Guide to the expression of Uncertainty in Measurements (GUM) approach. The combination of carefully scrutinized correction factors, precise measurements of pressure, temperature and detector volume, and robust counting statistics resulted in the determination of high-precision specific activity values with 0.50% or less total combined uncertainty for two Kr-in-P10 reference gas standards (KP10) that will enable new groundwater age-dating measurements at PNNL.