Jeffrey T. Cessna

Radioassays of yttrium-90 used in nuclear medicine

Yttrium-90 radioassays are required in nuclear medicine at the gigabecquerel activity level (GBq) for measuring injected activity, and at the becquerel level for measuring individual tissue samples in biodistribution studies. A method of standardizing 90Y for activity using high-efficiency liquid-scintillation counting is described. Solution standards were used to establish the calibration factors for commercial radionuclide calibrators. Detection efficiencies are also presented for liquid-scintillation counting, NaI(T1) bremsstrahlung counting and Cerenkov counting.

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.

Liquid-scintillation counting techniques for the standardization of radionuclides used in therapy

Abstract Radionuclides are increasingly used in therapeutic nuclear medicine. The CIEMAT/NIST method of standardizing high-energy beta-particle emitters is being applied to a list of candidate radionuclides developed by the US nuclear medicine community. Standards and standard methods are needed by the pharmaceutical manufacturers in North America before these nuclides can be widely distributed. Solutions standardized by liquid-scintillation counting are used to establish counting efficiencies for Cerenkov counting and NaI(T1) well crystals, and potentiometer settings for commercial radionuclide calibrators. Results are presented for a number of beta-particle-emitting radionuclides.

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.

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).

Radionuclide calibrator measurements of 18F in a 3 ml plastic syringe

This paper discusses the calibration of Capintec radionuclide calibrators for the measurement of (18)F in the pharmacy and clinic. In support of a planned regional comparison, a secondary laboratory was set up at Oak Ridge National Laboratories in Oak Ridge, TN. The laboratory was used to prepare 1mL (18)F-fluorodeoxyglucose sources in 3mL plastic BD syringes (Becton, Dickinson and Company, Franklin Lakes, New Jersey, USA) and to determine dial settings in three models of radionuclide calibrators. Measurements were verified by comparing radionuclide calibrator measurements of a 5mL ampoule source with previous results. The CIEMAT/NIST method of tritium efficiency tracing was used for activity determinations.

Experimental Investigation of Dose Calibrator Response for 125I Brachytherapy Solutions Contained in 5 ml Plastic Syringes and 2 ml Conical Glass V-vials as a Function of Filling Mass

The effect of measurement geometry on the determination of the activity of solutions containing 125I for use in brachytherapy applications has been investigated for 5 mL plastic syringes and 2 mL conical glass dose vials as a function of filling mass. New dial settings for the syringes over a filling mass range of 1 to 3 g have been determined to be 497+/-8 and 469+/-8 (expanded, k = 2, uncertainties) for the NIST Capintec CRC- 12 and Capintec CRC-35R, respectively, with any effect due to the filling mass lying within the uncertainty in the activity calibration. A filling mass effect was observed in the dose vials, causing a 10.5% reduction in the chamber response from a 2 g filling mass to 1 g. Dial settings at 2 g were experimentally found to be 143+/-2 and 135+/-2 (expanded uncertainties) for the NIST Capintec CRC-12 and Capintec CRC-35R, respectively. The appropriate dial settings for the same vials with a 1 g filling mass were found to be 120+/-2 and 114+/-2 for CRC-12 and CRC-35R, respectively. Differences of up to +/-45% in the activity determination were observed between values obtained with the manufacturers recommended setting and the settings obtained experimentally for each specific geometry. Calibration factors were also determined for a Vinten 671 Radionuclide Calibrator, giving values of 0.226+/-0.009 pA x MBq(-1) and 0.231+/-0.004 pA x MBq(-1) (expanded uncertainties), respectively, for the 1 and 2 g dispensings. This study demonstrates that experimentally determined calibration factors for the exact measurement geometry are necessary when measuring radionuclides in configurations other than the manufacturers standard geometry, especially when nuclides that emit low-energy radiations are involved.

The Standardization of 188W/188Re by 4πβ Liquid Scintillation Spectrometry with the CIEMAT/NIST 3H-standard Efficiency Tracing Method

The massic activity of a solution containing 188W in equilibrium with its daughter, 188Re, has been standardized by the National Institute of Standards and Technology using 4pi beta liquid scintillation counting with efficiency tracing using the CIEMAT NIST method. Confirmatory measurements were carried out with gamma-ray spectrometry using high purity germanium detectors and a 4pi gamma NaI(Tl) system. A calibration factor of 1.68 MBq pA(-1) +/-0.03 MBq pA(-1) (expanded, k = 2, uncertainty) for the 188W in the solution was determined, along with correction factors for activity determinations using Capintec dose calibrators. A half-life value of 69.78 d +/- 0.05 d (standard uncertainty) was determined by measurement in the NIST 4pi gamma ionization chamber and is consistent with currently recommended values.