Absolute emission intensities of the gamma rays from the decay of 224Ra and 212Pb progenies and the half-life of the 212 Pb decay.

Absolute gamma-ray emission intensities for 36 characteristic gamma rays from the decay of 224Ra, 212Pb, and their progeny were determined by measuring sources calibrated for activity by means of primary methods based on well-defined high-purity germanium (HPGe) detectors at both NIST and NPL. Results from the two laboratories agree with recent data evaluations, except for gamma rays with low emission intensities. The decay schemes have been re-balanced based on the new results. In addition, the half-life for 212Pb was measured using several HPGe detectors, ionization chambers, and a well-type NaI(Tl) detector.

Determination of the half-life and the absolute photon emission intensities for the main gamma-ray energies of 124I.

The National Institute of Standards and Technology (NIST) performed new standardization measurements for 124I. As part of this work the absolute photon emission intensity for the main gamma-rays of 124I were determined using several high-purity germanium (HPGe) detectors. In addition, the half-life for 124I was also determined using an HPGe detector. Ionization chamber measurements were performed for additional sources, but it was not possible to obtain a precise half-life value.

Determination of the internal pair production branching ratio of 90Y.

The National Institute of Standards and Technology (NIST) measured the internal pair production branching ratio of 90Y using two sources and four high purity germanium (HPGe) detectors to detect the resulting annihilation radiation. The internal pair production branching ratio determined from these measurements, (32.0 ±â€¯1.5) × 10-6 (k = 1), agrees within 1 standard uncertainty with the recommended value of (32.6 ±â€¯0.7) × 10-6 (k = 1) from the DDEP database.

Standardization of I-124 by three liquid scintillation-based methods.

A solution of 124I was standardized for activity by 4πß(LS)-γ(NaI) live-timed anticoincidence (LTAC) counting, with confirmatory measurements by triple-to-double coincidence ratio (TDCR) and CIEMAT-NIST efficiency tracing (CNET) liquid scintillation counting. The LTAC-based standard was shown to be in agreement (within k = 1 uncertainties) with previous measurements at NIST and elsewhere. Calibration settings for radionuclide calibrators were determined and a discrepancy with literature values, partially due to a calibration methodology dependent upon an erroneous setting for 18F, was identified and explained.

Standardization of 64Cu activity.

The complex decay scheme that makes 64Cu promising as both an imaging and therapeutic agent in medicine also makes the absolute measurement of its activity challenging. The National Institute of Standards and Technology (NIST) has completed a primary activity standardization of a 64CuCl2 solution using the 4πß(LS)-γ(NaI) live-timed anticoincidence (LTAC) counting method with a combined standard uncertainty of 0.51 %. Two liquid scintillation (LS) counting methods were employed for confirmatory measurements. Secondary measurements were made by high-purity germanium detectors, pressurized ionization chambers (IC), and a well-type NaI(Tl) counter. Agreement between the LTAC-based standard and standards from other laboratories was established via IC calibration factors. Poor agreement between methods and with theoretical IC responses may indicate a need for improved ß+/- branching probabilities and a better treatment of ß+/- spectra.

Results of an international comparison of activity measurements of 68Ge.

An international key comparison, identifier CCRI(II)-K2.Ge-68, has been performed. The National Institute of Standards and Technology (NIST) served as the pilot laboratory, distributing aliquots of a 68Ge/68Ga solution. Results for the activity concentration, CA, of 68Ge at a reference date of 12h00 UTC 14 November 2014 were submitted by 17 laboratories, encompassing many variants of coincidence methods and liquid-scintillation counting methods. The first use of 4π(Cherenkov)ß-γ coincidence and anticoincidence methods in an international comparison is reported. One participant reported results by secondary methods only. Two results, both utilizing pure liquid-scintillation methods, were identified as outliers. Evaluation using the Power-Moderated Mean method results in a proposed Comparison Reference Value (CRV) of 621.7(11)kBqg-1, based on 14 results. The degrees of equivalence and their associated uncertainties are evaluated for each participant. Several participants submitted 3.6mL ampoules to the BIPM to link the comparison to the International Reference System (SIR) which may lead to the evaluation of a Key Comparison Reference Value and associated degrees of equivalence.

Determination of photon emission probability for the main gamma ray and half-life measurements of 64Cu.

The National Institute of Standards and Technology (NIST) performed new standardization measurements for 64Cu. As part of this work the photon emission probability for the main gamma-ray line and the half-life were determined using several high-purity germanium (HPGe) detectors. Half-life determinations were also carried out with a NaI(Tl) well counter and two pressurized ionization chambers.

Long-term stability of carrier-added (68)Ge standardized solutions.

Tests for chemical stability were carried out on carrier-added (68)Ge solutions prepared and calibrated in 2007 and 2011 to evaluate the suitability of the specific composition as a potential Standard Reference Material. Massic count rates of the stored solutions were measured using a NaI(Tl) well counter before and after gravimetric transfers. The present activity concentration of the 2007 solution was also measured using live-timed anticoincidence counting (LTAC) and compared to the 2007 calibrated value. The well counter data indicated no change in massic count rate to within uncertainties for either solution. The LTAC measurements gave a difference of -0.49% in the activity concentration 2007 solution over 7 years. However, the uncertainty in the decay correction over that time, due to the uncertainty in the (68)Ge half-life, accounted for the majority (0.67% out of 0.83%) of the standard uncertainty on the activity concentration. The results indicate that these carrier-added solutions are stable with regard to potential activity losses over several half-lives of (68)Ge.

Determination of photon emission probabilities for the main gamma-rays of ²²³Ra in equilibrium with its progeny.

The currently published (223)Ra gamma-ray emission probabilities display a wide variation in the values depending on the source of the data. The National Institute of Standards and Technology performed activity measurements on a (223)Ra solution that was used to prepare several sources that were used to determine the photon emission probabilities for the main gamma-rays of (223)Ra in equilibrium with its progeny. Several high purity germanium (HPGe) detectors were used to perform the gamma-ray spectrometry measurements.

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 (223)Ra 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 (223)Ra 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.

Development of a calibration methodology for large-volume, solid 68Ge phantoms for traceable measurements in positron emission tomography.

We have developed a methodology to calibrate the (68)Ge activity concentration in large (9L) cylindrical epoxy phantoms in a way that is traceable to national standards. The method was tested on two prototype cylindrical phantoms that are being used in a clinical trial and gave (68)Ge activity concentration values with combined standard uncertainties of about 1.1%. Imaging data from the phantoms using a calibrated PET-CT scanner gave values consistent with the calibrated activity concentrations within experimental uncertainties.

Calibration of Traceable Solid Mock (131)I Phantoms Used in an International SPECT Image Quantification Comparison.

The International Atomic Energy Agency (IAEA) has organized an international comparison to assess Single Photon Emission Computed Tomography (SPECT) image quantification capabilities in 12 countries. Iodine-131 was chosen as the radionuclide for the comparison because of its wide use around the world, but for logistical reasons solid (133)Ba sources were used as a long-lived surrogate for (131)I. For this study, we designed a set of solid cylindrical sources so that each site could have a set of phantoms (having nominal volumes of 2 mL, 4 mL, 6 mL, and 23 mL) with traceable activity calibrations so that the results could be properly compared. We also developed a technique using two different detection methods for individually calibrating the sources for (133)Ba activity based on a National standard. This methodology allows for the activity calibration of each (133)Ba source with a standard uncertainty on the activity of 1.4 % for the high-level 2-, 4-, and 6-mL sources and 1.7 % for the lower-level 23 mL cylinders. This level of uncertainty allows for these sources to be used for the intended comparison exercise, as well as in other SPECT image quantification studies.

Results of an international comparison for the activity measurement of 177Lu.

An international Key Comparison of (177)Lu has recently been carried out. Twelve laboratories performed assays for radioactivity content on aliquots of a common master solution of (177)Lu, leading to eleven results submitted for entry into the Key Comparison Database of the Mutual Recognition Arrangement. A proposed Comparison Reference Value (CRV) was calculated to be 3.288(4)MBq/g using all eleven results. Degrees of equivalence and their uncertainties were calculated for each laboratory based on the CRV. Most of the values reported by the participating laboratories were within 0.6% of the CRV.

Standardization of radium-223 by liquid scintillation counting.

Liquid scintillation (LS) counting was undertaken as part of the primary standardization of (223)Ra. Radium-223 decays with a half life of 11.43 d through a chain of shorter-lived daughter radionuclides, resulting in five alpha decays and three beta decays. The CIEMAT/NIST method of tritium efficiency tracing was employed, with the beta efficiencies being calculated using the program CN2004, developed by the Physikalisch-Technische Bundesanstalt (PTB). The total calculated LS efficiency, considering all daughter radionuclides, was approximately 598%. Separate experiments were performed to rule out loss of the 3.96 s (219)Ra daughter from the cocktail and possible counting loss of the 1.78 ms (215)Po daughter due to LS counter dead-time. No loss was observed in either experiment. In the final experiment an expanded uncertainty (k=2) of 0.55% was achieved. Results were in excellent agreement with confirmatory measurements performed by 2pialpha proportional counting. However, results are not in agreement with methods based on gamma ray measurements.

Radionuclide calibrator measurements of (18)F in a 3ml 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.

Standardization of (68)Ge/(68)Ga Using Three Liquid Scintillation Counting Based Methods.

A solution containing (68)Ge in equilibrium with its daughter, (68)Ga, has been standardized for the first time at the National Institute of Standards and Technology (NIST) using 3 liquid scintillation-based techniques: live-timed 4πß -γ anticoincidence (LTAC) counting, the Triple-to-Double Coincidence Ratio (TDCR) method, and (3)H-standard efficiency tracing with the CIEMAT(1)/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 (68)Ge/(68)Ga without the need for a primary measurement. The ability to produce standardized solutions of (68)Ge 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.

Development of activity standard for 90 Y microspheres.

(90)Y microspheres are important therapeutic radiopharmaceuticals used in the treatment of liver cancer through a process known as selective internal radiation therapy. SIR-spheres is a radiopharmaceutical product that is comprised of (90)Y microspheres suspended in sterile, pyrogen-free water for injection into patients. It is necessary to establish for the SIR-spheres production the capability of accurately measuring the activity of this product to a traceable national measurement standard. An activity standard for SIR-spheres was developed from a standard for (90)Y solution, employing a highly quantifiable chemical digestion process. Calibration factors for the manufacturer's ionisation chambers were determined for 1 and 5 ml of the SIR-spheres product placed in Wheaton vials, for both 34% and 44% of (90)Y microsphere concentration.

Construction and implementation of the NIST triple-to-double coincidence ratio (TDCR) spectrometer.

A description of the triple-to-double coincidence ratio (TDCR) spectrometer recently constructed at NIST and results of tests to assess its operating characteristics are presented. Measured activities for previously calibrated solutions of 3H (tritiated water) and 63Ni agreed with certified activity values to within 0.04% and 0.2%, respectively. Agreement between measurements of solutions containing 90Y using the TDCR and the CIEMAT/NIST efficiency tracing method was achieved to within 0.7% and within the respective experimental uncertainties. A difference of 5.3% was observed between TDCR measurements and the certified massic activity value for a calibrated solution containing 54Mn, but because of the large uncertainty on the TDCR result (3.6% relative standard uncertainty), the values agree to within the experimental uncertainties. Agreement to within experimental uncertainties (2%) for 103Pd was achieved with the TDCR and CIEMAT/NIST methods, but not between TDCR and isothermal calorimetric measurements. TDCR results for a 204Tl solution were in excellent agreement (maximum difference of 0.2% with any other method, with combined standard uncertainty of 0.45% on TDCR result) with results obtained using three other methods.

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.

Experimental determination of calibration settings for plastic syringes containing solutions of 90Y using commercial radionuclide calibrators.

Calibration factors for several makes (Capintec, AtomLab, and PTW) and models of commercially available re-entrant ionization chambers ("dose calibrators") were determined for solutions of 90Y using 10 ml plastic syringes that are used in the administration of the recently approved radioimmunotherapy drug Zevalin. Effects of filling volume on chamber response were studied for the anticipated prescription volume range of 3-9 ml in those syringes. A series of syringes were prepared over that range with accurately known volumes using a "standard" solution containing 90YCl3 in 1 moll(-1) HCl and approximately 50 microg of nonradioactive YCl3 per gram of solution. The respective calibration factors for the Capintec and AtomLab chambers required to give the correct activity reading were found to be "55+/-2 x 10" and 393+/-6, where the uncertainties are expanded (k = 2) uncertainties. The results indicated no significant effect of filling volume on the calibration setting to within the uncertainty on the activity measurement for all but the PTW chamber. In that case, a variation of about 5% was observed over the filling range. A direct comparison was also made between the actual 90Y Zevalin drug and the "standard" solution, with no differences in determined calibration settings observed within the uncertainties on the activity calibration.