Update of NIST half-life results corrected for ionization chamber source-holder instability.

As reported at the ICRM 2011, it was discovered that the source holder used for calibrations in the NIST 4πγ ionization chamber (IC) was not stable. This has affected a large number of half-life measurement results previously reported and used in compilations of nuclear data. Corrections have been made on all of the half-life data based on the assumption that the changes to the ionization chamber response were gradual. The corrections are energy dependent and therefore radionuclide specific. This presentation will review our results and present the recommended changes in half-life values and/or uncertainties.

Unexpected bias in NIST 4πγ ionization chamber measurements.

In January of 2010, it was discovered that the source holder used for calibrations in the NIST 4πγ ionization chamber (IC) has not been stable. The positioning ring that determines the height of the sample in the reentrant tube of the IC has slowly shifted during 35 years of use. This has led to a slow change in the calibration factors for the various radionuclides measured by this instrument. The changes are dependent on γ-ray energy and the time the IC was calibrated for a given radionuclide. A review of the historic data with regard to when the calibrations were done has enabled us to approximate the magnitude of the changes with time. This requires a number of assumptions, and corresponding uncertainty components, including whether the changes in height were gradual or in steps as will be shown in drawings of sample holder. For calibrations the changes in calibration factors have been most significant for low energy gamma emitters such as (133)Xe, (241)Am, (125)I and (85)Kr. The corrections to previous calibrations can be approximated and the results corrected with an increase in the overall uncertainty. At present we are recalibrating the IC based on new primary measurements of the radionuclides measured on the IC. Likewise we have been calibrating a new automated ionization-chamber system. A bigger problem is the significant number of half-life results NIST has published over the last 35 years that are based on IC measurements. The effect on half-life is largest for long-lived radionuclei, especially low-energy γ-ray emitters. This presentation will review our results and recommend changes in values and/or uncertainties. Any recommendation for withdrawal of any results will also be undertaken.

A new large-area 2pi proportional counting system at NIST.

A new large-area gas flow multi-wire proportional counter has been developed to replace the large-area counting system that is currently in use at the National Institute of Standards and Technology (NIST) and several Department of Defense counting facilities for calibrating large-area alpha and beta sources. The current systems are over 20 years old and part replacement is very difficult. The new systems have been built using specifications that will improve on the current systems and allow collecting data at pressures up to 0.2MPa. The ability to operate at higher pressures will increase the beta efficiency of the counter and lead to improved precision in the final measured results. Comparison of the results from the old and new systems is presented for both alpha and beta sources.

Ionization chamber measurements of the half-lives of 24Na, 42K, 76As and 198Au.

Samples of 24Na, 42K, 76As and 198Au were produced by irradiation in the National Institute of Standards and Technology (NIST) reactor, and examined for impurities before and after measurement. Half-life measurements were carried out in the NIST 4pigamma pressurized ionization chamber. The results are compared to presently accepted values and previous NIST measurements.

Establishment of transfer standard for holmium-166-DOTMP.

The measurement of 166Ho, both as a chloride solution and as [166Ho]-1,4,7,10-tetraazacyclododecane-1,4,7,10-tetramethylenephoonic acid (DOTMP), was examined for four models of radionuclide calibrators: Capintec CRC-35R (two chambers), Capintec 712MX, AtomLab 100 (two chambers), and a Capintec CRC-12. Holmium-166 chloride was measured as 16 ml in 20-ml glass dose vials. Diagnostic imaging level [166Ho]DOTMP solutions, nominally 400 MBqg(-1), were measured as 12 ml in 20-ml dose vials. Finally, therapeutic level [166Ho]DOTMP solutions, nominally 9GBqg(-1), were measured as aliquots of 100-500 microl in sealed plastic vials of 10-ml saline. Single calibration factors for each instrument manufacturer are recommended for 12-16-ml of either solution in 20-ml glass dose vials, (673+/-9) x 10 and 72.7+/-0.7, for the Capintec and AtomLab models, respectively. Calibration factors recommended for the therapeutic dose geometry are (706+/-6) x 10 and 68.7+/-1.3, for the Capintec and AtomLab models, respectively. The calibration factors recommended for an NIST 5-ml ampoule are (686+/-5) x 10 and 70.9+/-0.4 for the Capintec and AtomLab models, respectively.

Half-life measurements at the National Institute of Standards and Technology.

For nearly half a century the half-lives of many radionuclides have been measured with increasing precision. The results of these measurements for many long-lived radionuclides, such as 60Co, 137Cs, 85Kr, 133Ba, 207Bi, 152Eu, 154Eu, and 155Eu, have been updated recently by the Radioactivity Group of NIST. These long-lived radionuclides are used extensively to calibrate various nuclear counting and monitoring systems. The long-term precision of these calibrations can be greatly affected by the uncertainties in the calibrant half-lives. Results for the half-lives of many radionuclides measured over the last four decades are tabulated. In addition, values of the half-lives of several short-lived radionuclides used in nuclear medicine are addressed, which are critical in determining the correct dosage given in patient treatment, are addressed. Comparisons with the recommended values from the International Atomic Energy Agency Coordinated Research Program and the Evaluated Nuclear Structure Data File from Brookhaven National Laboratory are presented and any apparent disagreements noted.

The standardization of 177Lu by 4pibeta liquid scintillation spectrometry with 3H-standard efficiency tracing.

Solutions containing the potential radiotherapy radionuclide 177Lu have been standardized at the National Institute of Standards and Technology (NIST) by 4pibeta liquid scintillation (LS) counting with 3H-standard efficiency tracing using the CIEMAT/NIST method. Confirmatory measurements were made with 4pi NaI(TI) gamma-ray spectrometry. Activity determinations were made on 4 solutions over the course of 10 months with an expanded (k = 2) uncertainty on the activity of 0.8%. Half-life measurements were carried out using the NIST "4pi" gamma ionization chamber (IC) and LS counting and gave a new value of 6.65+/-0.01 d, which is shorter than the current ENSDF-recommended value by 1.3%. Impurity analyses were performed by high-purity germanium (HPGe) gamma-ray spectrometry and indicated only the presence of 177mLu at a level of 0.02% that of the 177Lu as of the respective reference times for the four solutions. Calibration factors for the NIST IC and Vinten 671 ionization chambers were developed, as were dial settings for the NIST-maintained Capintec CRC-12.

Comprehensive Review and Critical Evaluation of the Half-Life of Tritium.

As part of the preparation and calibration of three new National Institute of Standards and Technology (NIST) tritiated-water radioactivity Standard Reference Materials (SRMs), we have performed a comprehensive review and critical evaluation of the half-life of tritium (hydrogen-3). Twenty three experimentally-determined values of the half-life of tritium, reported between 1936 and 2000, were found. Six of these values were updated by later values. Two values were limits. Two values were deemed to be outliers. The 13 remaining values were evaluated in several ways. The results are compared with the results of other recent evaluations and all are found to be in good agreement. Our final recommended value for the half-life of tritium is the average of the adopted values from the four most recent evaluations, (4500 ± 8) d, where 8 d corresponds to one standard uncertainty.

A new experimental determination of the dose calibrator setting for 188Re.

UNLABELLED: Accurate activity measurements of radionuclides using commercial dose calibrators requires that the correct dial setting (or calibration factor) be applied. The dose calibrator setting for the medical radionuclide 188Re (as 188ReO4-) has been determined experimentally using solution sources prepared and calibrated at the National Institute of Standards and Technology (NIST). METHODS: The specific activity of two sources (in units of MBq/g) in the standard 5-mL NIST ampoule and in a 5-mL SoloPak dose vial were calibrated using 4pibeta liquid scintillation counting with 3H-standard efficiency tracing and gamma-ray/bremmstrahlung counting in the NIST "4pi" gamma ionization chamber on gravimetrically related sources. RESULTS: The newly determined settings for the NIST Capintec CRC-12 dose calibrator are (631+/-4) x 10 and (621+/-3) x 10 for the respective ampoule and dose vial geometries with an expanded (at a presumed 95% confidence level) uncertainty of 0.4%-0.5% in the activity determination. The setting for the dose vial geometry was independently confirmed using a Capintec CRC-15R at Cedars-Sinai Medical Center using sources calibrated against a NIST standard. CONCLUSION: These new settings result in activity readings 28%-30% lower than those obtained using the previously recommended setting of 496 x 10. This discrepancy most likely results from underestimating the total radiation yield from 188Re decay when calculating the dose calibrator response. This study emphasizes the need for experimental determinations of dose calibrator settings in the geometry in which the measurements will be performed.

An International Marine-Atmospheric 222Rn Measurement Intercomparison in Bermuda Part I: NIST Calibration and Methodology for Standardized Sample Additions.

As part of an international 222Rn measurement intercomparison conducted at Bermuda in October 1991, NIST provided standardized sample additions of known, but undisclosed ("blind") 222Rn concentrations that could be related to U.S. national standards. The standardized sample additions were obtained with a calibrated 226Ra source and a specially-designed manifold used to obtain well-known dilution factors from simultaneous flow-rate measurements. The additions were introduced over sampling periods of several hours (typically 4 h) into a common streamline on a sampling tower used by the participating laboratories for their measurements. The standardized 222Rn activity concentrations for the intercomparison ranged from approximately 2.5 Bq · m-3 to 35 Bq · m-3 (of which the lower end of this range approached concentration levels for ambient Bermudian air) and had overall uncertainties, approximating a 3 standard deviation uncertainty interval, of about 6 % to 13 %. This paper describes the calibration and methodology for the standardized sample additions.

An International Marine-Atmospheric 222Rn Measurement Intercomparison in Bermuda Part II: Results for the Participating Laboratories.

As part of an international measurement intercomparison of instruments used to measure atmospheric 222Rn, four participating laboratories made nearly simultaneous measurements of 222Rn activity concentration in commonly sampled, ambient air over approximately a 2 week period, and three of these four laboratories participated in the measurement comparison of 14 introduced samples with known, but undisclosed ("blind") 222Rn activity concentration. The exercise was conducted in Bermuda in October 1991. The 222Rn activity concentrations in ambient Bermudian air over the course of the intercomparison ranged from a few hundredths of a Bq · m-3 to about 2 Bq · m-3, while the standardized sample additions covered a range from approximately 2.5 Bq · m-3 to 35 Bq · m-3. The overall uncertainty in the latter concentrations was in the general range of 10 %, approximating a 3 standard deviation uncertainty interval. The results of the intercomparison indicated that two of the laboratories were within very good agreement with the standard additions, and almost within expected statistical variations. These same two laboratories, however, at lower ambient concentrations, exhibited a systematic difference with an averaged offset of roughly 0.3 Bq · m-3. The third laboratory participating in the measurement of standardized sample additions was systematically low by about 65 % to 70 %, with respect to the standard addition which was also confirmed in their ambient air concentration measurements. The fourth laboratory, participating in only the ambient measurement part of the intercomparison, was also systematically low by at least 40 % with respect to the first two laboratories.

Construction and Calibration of the NIST Large-Area-Source X-Ray Counting System.

This paper describes the construction and calibration of the NIST large area x-ray counting system. 238Pu sources 8 in (20.32 cm) by 5 in (12.70 cm) thick, emitting L x rays in the range of 12-20 keV are calibrated for total emission rate and also for rate through a centrally located 3 in (7.63 cm) diameter aperture. Alpha particle emission rates are obtained using the known x-ray to alpha particle abundances. The sources will be used to calibrate alpha-particle surface monitors.

The NIST Primary Radon-222 Measurement System.

Within the United States, the national standard for radon measurements is embodied in a primary radon measurement system that has been maintained for over 50 years to accurately measure radon (222Rn) against international and national radium (226Ra) standards. In turn, all of the radon measurements made at the National Institute of Standards and Technology (NIST) and the radon transfer calibration standards and calibration services provided by NIST are directly related to this national radon standard. This primary radon measurement system consists of pulse ionization chambers and ancillary gas handling and gas purification equipment. The system is currently undergoing a significant upgrading and expansion which will replace the extant outdated system.

The standardization of samarium-153.

Samarium-153 has been standardized by 4 pi beta liquid-scintillation counting, with an uncertainty of 0.4%. The probability per decay for the 103.2-keV gamma ray was measured, using two germanium detectors, to be 0.298 +/- 0.004. The half life, based on liquid-scintillation measurements over 6.4 half lives and pressurized-ionization-chamber measurements over four half lives, was found to be 46.27 +/- 0.02 h. The uncertainties given are one estimated standard deviation (of the mean when applicable) for random and non-random components.