Brian E. Zimmerman

Development of a Traceable Calibration Methodology for Solid 68Ge/68Ga Sources Used as a Calibration Surrogate for 18F in Radionuclide Activity Calibrators

We have developed a methodology for calibrating 68Ge radioactivity content in a commercially available calibration source for activity calibrators in a way that is traceable to the national standard. Additionally, the source was cross-calibrated for equivalent 18F content by direct comparison with the national standard for 18F in the same geometry. Methods: Sources containing standardized 68GeCl4 or 18F-FDG solutions were prepared at the National Institute of Standards and Technology (NIST) with mock syringe blanks used in the construction of a commercially available epoxy-based 68Ge calibration source. These sources and several NIST-constructed epoxy-based 68Ge mock syringes were then used as artifact standards to determine calibration factors for NIST-maintained activity calibrators and secondary standard ionization chambers to enable calibration of the actual commercial sources. A direct comparison between the solution-based 68Ge sources and the 18F-FDG sources allowed for an empiric determination of the relative response for these radionuclides in several commercial activity calibrators. Potential measurement effects due to differences between the solution composition and the epoxy and theoretic 68Ge-to-18F response ratios were studied by Monte Carlo simulation. Results: The calibration factors developed in this study enabled NIST to calibrate epoxy-based mock syringe sources with a relative combined standard uncertainty of 0.52%. The direct comparisons of the 68Ge and 18F standards in the various ionization chambers allowed the activity to be expressed in terms of equivalent 18F activity with a relative combined standard uncertainty of about 0.9%. Conclusion: The ability for NIST to calibrate these epoxy-based mock syringes enabled, for the first time to our knowledge, the direct traceability to the national 68Ge standard to be established for this type of source. Through a direct comparison with the NIST 18F standard, the determination of the relative response ratios in activity calibrators enabled the equivalent 18F activity to be determined in a way that was also traceable to the national 18F activity standard.

Standardization of 68Ge/68Ga using three liquid scintillation counting-based methods

A solution containing 68Ge in equilibrium with its daughter, 68Ga, has been standardized for the first time at the National Institute of Standards and Technology (NIST) using 3 liquid scintillation-based techniques: live-timed 4πβ -γ anticoincidence (LTAC) counting, the Triple-to-Double Coincidence Ratio (TDCR) method, and 3H-standard efficiency tracing with the CIEMAT1/NIST (CNET) method. The LTAC technique is much less dependent on level scheme data and model-dependent parameters and was thus able to provide a reference activity concentration value for the master solution with a combined standard uncertainty of about 0.3 %. The other two methods gave activity concentration values with respective differences from the reference value of +1.2 % and −1.5 %, which were still within the experimental uncertainties. Measurements made on the NIST “4π”γ secondary standard ionization chamber allowed for the determination of calibration factors for that instrument, allowing future calibrations to be made for 68Ge/68Ga without the need for a primary measurement. The ability to produce standardized solutions of 68Ge presents opportunities for the development of a number of NIST-traceable calibration sources with very low (<1 %) relative standard uncertainties that can be used in diagnostic medical imaging.

The standardization of the potential bone palliation radiopharmaceutical 117mSn(+4)DTPA

Solutions containing the potential bone pain palliation radionuclide 117mSn, in chloride form and as a diethylenetriaminepentaacetate (DTPA) complex, have been standardized by 4 pi beta liquid scintillation (LS) spectrometry and 4 pi gamma-ray spectrometry. Massic activities of the stock solutions were measured in order to determine dose calibrator settings for the solutions using commercial dose calibrators. Excellent agreement in the measurement of solution massic activity between the two techniques was achieved. The massic activity of 117mSnCl4 stock solution was found to be 38.62 +/- 0.23 MBq g-1 and 38.81 +/- 0.94 MBq g-1 with LS spectrometry and 4 pi gamma-ray spectrometry respectively. The respective values of the massic activity of the 117mSnDTPA stock solution with LS spectrometry and 4 pi gamma-ray spectrometry were 39.35 +/- 0.23 MBq g-1 and 39.70 +/- 0.96 MBq g-1. Impurities were analyzed in several solutions and found to have emission rates on the order of 10(-4) to 10(-6) of the rate of the 117mSn emission at the end-of-bombardment. The largest impurities came from 113Sn and 125Sn, the activation products of isotopic impurities present in the 117Sn target. The relative proportions of the various impurities were found to be highly dependent upon the source of 117Sn target material. The implications of choice of half-life used in the decay correction of 117mSn are discussed.

Revision of the NIST Standard for (223)Ra: New Measurements and Review of 2008 Data.

After discovering a discrepancy in the transfer standard currently being disseminated by the National Institute of Standards and Technology (NIST), we have performed a new primary standardization of the alpha-emitter 223Ra using Live-timed Anticoincidence Counting (LTAC) and the Triple-to-Double Coincidence Ratio Method (TDCR). Additional confirmatory measurements were made with the CIEMAT-NIST efficiency tracing method (CNET) of liquid scintillation counting, integral γ-ray counting using a NaI(Tl) well counter, and several High Purity Germanium (HPGe) detectors in an attempt to understand the origin of the discrepancy and to provide a correction. The results indicate that a −9.5 % difference exists between activity values obtained using the former transfer standard relative to the new primary standardization. During one of the experiments, a 2 % difference in activity was observed between dilutions of the 223Ra master solution prepared using the composition used in the original standardization and those prepared using 1 mol·L−1 HCl. This effect appeared to be dependent on the number of dilutions or the total dilution factor to the master solution, but the magnitude was not reproducible. A new calibration factor (“K-value”) has been determined for the NIST Secondary Standard Ionization Chamber (IC “A”), thereby correcting the discrepancy between the primary and secondary standards.

Traceability in nuclear medicine

Accurate, reproducible measurement of radioactivity in nuclear medicine applications is vital to ensure the safety and effectiveness of disease diagnosis and treatment using unsealed radioactive sources. The need to maintain a high degree of confidence in those measurements requires that they be carried out so as to be traceable to national and international standards. In addition, measurement traceability for radioactivity in medicine helps ensure international consistency in measurement at all levels of practice (national measurement laboratories, research institutions, isotope producers, radiopharmaceutical manufacturers and clinics). This paper explores the importance of radioactivity measurement in nuclear medicine and demonstrates how traceability can be extended from international standards to the quantity of the drug administered to the patient.

Cocktail volume effects in 4πβ Liquid scintillation spectrometry with 3H-standard efficiency tracing for low-energy β-emitting radionuclides

Abstract The effect of total liquid scintillation (LS) cocktail volume (or mass) in the 4πβ LS spectrometry of β-emitting radionuclides has been investigated. The magnitude of such possible volume effects on the apparent activity of low-energy β-emitting radionuclides, as determined by the CIEMAT/NIST 3H-standard efficiency tracing method, as well as any systematic trends in the relative detection efficiencies of low-ebergy β-emitters were studied. The radionuclides chosen for the study, 63Ni and 36Cl, were traced against 3H. Detection efficiency losses, as a function of total LS cocktail volume, were found to be energy-dependent. Because of the low Eβmax for the decay of 3H and 63Ni, systematic losses in efficiency with increasing cocktail mass, as well as at extremely low (

A compendium on the NIST radionuclide assays of the massic activity of {sup 63}Ni and {sup 55}Fe solutions used for an international intercomparison of liquid scintillation spectrometry techniques

The National Institute of Standards and Technology recently participated in an international measurement intercomparison for 63Ni and 55Fe, which was conducted amongst principal national radionuclidic metrology laboratories. The intercomparison was sponsored by EUROMET, and was primarily intended to evaluate the capabilities of liquid scintillation (LS) spectrometry techniques for standardizing nuclides that decay by low-energy β-emission (like 63Ni) and by low-Z (atomic number) electron capture (like 55Fe). The intercomparison findings exhibit a very good agreement for 63Ni amongst the various participating laboratories, including that for NIST, which suggests that the presently invoked LS methodologies are very capable of providing internationally-compatible standardizations for low-energy β-emitters. The results for 55Fe are in considerably poorer agreement, and demonstrated the existence of several unresolved problems. It has thus become apparent that there is a need for the various international laboratories to conduct rigorous, systematic evaluations of their LS capabilities in assaying radionuclides that decay by low-Z electron capture.

63NI HALF-LIFE : A NEW EXPERIMENTAL DETERMINATION AND CRITICAL REVIEW

Abstract The 63Ni half-life has been determined to be 101.06 ± 1.97 a based on three independent measurements, conducted over the past 27 years, of the massic activity of gravimetrically-related 63Ni sources. The 63Ni assays were performed initially (in 1968) by microcalorimetry using an assumed mean β− energy per decay, and subsequently (in 1984 and 1995) by 4πβ liquid scintillation spectrometry with 3H-standard efficiency tracing. The present result is the first and only determination of the 63Ni half-life which is based on actually following the radioactive decay of 63Ni. All previously reported determinations were derived from specific activity evaluations. These earlier determinations have been scutinizingly reviewed as part of this work. Some of these previous values can be revised in lieu of more recent nuclear data and on consideration of the experimental details. Based on a critical evaluation of the extant data set, a 63Ni half-life value of T=101.1 ± 1.4 a is recommended.

Uncertainty determination for activity measurements by means of the TDCR method and the CIEMAT/NIST efficiency tracing technique

Liquid scintillation counting is a very powerful technique for the activity determination of a number of radionuclides. In radionuclide metrology, the TDCR method and the CIEMAT/NIST efficiency tracing technique are widely used in many laboratories.Both methods require rather complex calculation techniques to derive the counting efficiency of the nuclide under study.This article explores the various sources of uncertainty that should be considered when applying these two techniques, and focuses on possible ways to evaluate them. Concrete examples are provided within the paper.

National radioactivity standards for β-emitting radionuclides used in intravascular brachytherapy

The uses of beta-particle emitting radionuclides in therapeutic medicine are rapidly expanding. To ensure the accurate assays of these nuclides prior to administration, radioactivity standards are needed. The National Institute of Standards and Technology (NIST), the national metrological standards laboratory for the United States, uses high-efficiency liquid scintillation counting to standardize solutions of such beta emitters, including 32P, 90Sr/90Y, and 188Re. Additional measurements are made on radionuclidic impurities, half lives, and other decay-scheme parameters (such as branching decay ratios or gamma-ray abundances) using HPGe detectors and reentrant ionization chambers. Following such measurements at NIST, standards are disseminated in three ways: Standard Reference Materials (SRMs), calibrations for source manufacturers, and calibration factors for commercial instruments. Uncertainties in the activity calibrations for these nuclides are of the order of +/-0.5% (at approximately 1-standard deviation confidence intervals).