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An activity standard for

Interest in targeted cancer therapy with alpha-emitting radionuclides is growing. To evaluate emerging radiotherapeutic agents requires precise activity measurements for consistent dose-response relationships and patient-specific dosimetry. National metrology institutes around the world have reported on the development and comparison of activity standards for medically important alpha emitters. This review describes the relevant methods and models underpinning these standards, the generation of new nuclear decay data, and the impacts on preclinical and clinical activity assays using radionuclide calibrators and γ-ray spectrometry.

Main text Since 1976, 30 laboratories have submitted 85 samples of 60Co to the International Reference System (SIR) for activity comparison at the Bureau International des Poids et Mesures (BIPM), with comparison identifier BIPM.RI(II)- K1.Co-60. Recently, the PTB (Germany), the NIST (United States), the SMU (Slovakia), the BARC (India), the LNE-LNHB (France), the POLATOM (Poland), the ENEA-INMRI (Italy), the NPL (United Kingdom), the LNMRI-IRD (Brazil), the NMISA (South Africa) and the ANSTO (Australia) participated in the comparison and the key comparison reference value (KCRV) has been updated. The degrees of equivalence between each equivalent activity measured in the SIR and the updated KCRV have been calculated and the results are given in the form of a table. A graphical representation is also given. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database https://www.bipm.org/kcdb/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

If dark matter has mass lower than around 1 GeV, it will not impart enough energy to cause detectable nuclear recoils in many direct-detection experiments. However, if dark matter is upscattered to high energy by collisions with cosmic rays, it may be detectable in both direct-detection experiments and neutrino experiments. We report the results of a dedicated search for boosted dark matter upscattered by cosmic rays using the PROSPECT reactor antineutrino experiment. We show that such a flux of upscattered dark matter would display characteristic diurnal sidereal modulation, and use this to set new experimental constraints on sub-GeV dark matter exhibiting large interaction cross-sections., 11 pages, 8 figures

We describe our progress toward a system to calibrate electrometers that measure currents from ionization chambers. The calibration system uses a $1\ \mathrm{G}\Omega$ standard resistor in series with a stable voltage source to generate calibration currents from 1 pA to 20 nA, traceable to quantum voltage and resistance standards through an 8-1/2 digit digital multimeter and the standard resistor. Expanded uncertainties ( $k=2$ ) of $100\times 10^{-6}$ or better for the calibration of the electrometer are needed for the ionization chamber measurements. We show our preliminary results including our initial calibration correction.

Reactor neutrino experiments have seen major improvements in precision in recent years. With the experimental uncertainties becoming lower than those from theory, carefully considering all sources of ν ¯ e is important when making theoretical predictions. One source of ν ¯ e that is often neglected arises from the irradiation of the nonfuel materials in reactors. The ν ¯ e rates and energies from these sources vary widely based on the reactor type, configuration, and sampling stage during the reactor cycle and have to be carefully considered for each experiment independently. In this article, we present a formalism for selecting the possible ν ¯ e sources arising from the neutron captures on reactor and target materials. We apply this formalism to the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory, the ν ¯ e source for the the Precision Reactor Oscillation and Spectrum Measurement (PROSPECT) experiment. Overall, we observe that the nonfuel ν ¯ e contributions from HFIR to PROSPECT amount to 1% above the inverse beta decay threshold with a maximum contribution of 9% in the 1.8-2.0 MeV range. Nonfuel contributions can be particularly high for research reactors like HFIR because of the choice of structural and reflector material in addition to the intentional irradiation of target material for isotope production. We show that typical commercial pressurized water reactors fueled with low-enriched uranium will have significantly smaller nonfuel ν ¯ e contribution.

A suspension of (224)Ra adsorbed onto CaCO(3) microparticles shows promise for α-therapy of intracavitary micro-metastatic diseases. To facilitate accurate activity administrations, geometry-specific calibration factors for commercially available reentrant ionization chambers (ICs) have been developed for (224)RaCl(2) solutions and (224)Ra adsorbed onto CaCO(3) microparticles in suspension in ampoules, vials, and syringes. Ampoules and vials give IC responses consistent with each other to < 1%. Microparticles attenuation leads to a ≈ 1% to ≈ 2.5% reduction in response in the geometries studied.

A suspension of 224Ra adsorbed onto CaCO3 microparticles shows promise for α-therapy of intracavitary micro-metastatic diseases. To facilitate accurate activity administrations, geometry-specific calibration factors for commercially available reentrant ionization chambers (ICs) have been developed for 224RaCl2 solutions and 224Ra adsorbed onto CaCO3 microparticles in suspension in ampoules, vials, and syringes. Ampoules and vials give IC responses consistent with each other to

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 4πβ(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 β+/- branching probabilities and a better treatment of β+/- spectra.

Background Most clinical measurements of radioactivity, whether for therapeutic or imaging nuclides, rely on commercial re-entrant ionization chambers ('dose calibrators'). The National Institute of Standards and Technology (NIST) maintains a battery of representative calibrators and works to link calibration settings ('dial settings') to primary radioactivity standards. Here, we provide a summary of NIST-determined dial settings for 22 radionuclides. Methods We collected previously published dial settings and determined some new ones using either the calibration curve method or the dialing-in approach. Results The dial settings with their uncertainties are collected in a comprehensive table. Conclusion In general, current manufacturer-provided calibration settings give activities that agree with National Institute of Standards and Technology standards to within a few percent.

The radionuclide copper-64 is a promising candidate for nuclear medicine, but its complex decay creates challenges in the primary standardization of its activity. Monte Carlo simulations of live-timed anticoincidence (LTAC) counting of (64)Cu were used to calculate corrections to extrapolation intercepts, resulting in improved activity determinations. A small correction (−0.33 %) to the linear extrapolation of LTAC data acquired with a γ-gate over the 1346 keV gamma peak was determined. We discuss the physical origin of the correction. We also use experimental data to demonstrate a Monte Carlo scaling that allows for inclusion of data acquired with a γ-gate set over the annihilation photon peak(s).

In nuclear medicine, (68)Ge is used to generate (68)Ga for imaging by positron emission tomography (PET) and sealed sources containing (68)Ge/(68)Ga in equilibrium have been adopted as long-lived calibration surrogates for the more common PET nuclide, (18)F. We prepared several (68)Ge sources for measurement on a NaI(Tl) well counter and a pressurized ionization chamber, following their decay for 110 weeks (≈ 2.8 half-lives). We determined values for the (68)Ge half-life of T(1/2) = 271.14(15) d and T(1/2) = 271.07(12) d from the NaI(Tl) well counter and ionization chamber measurements, respectively. These are in accord with the current Decay Data Evaluation Project (DDEP) recommended value of T(1/2) = 270.95(26) d and we discuss the expected impact of our measurements on this value.

With the recent redefinition of the SI base units in terms of constants of nature, the race is on to maximize achievable precision by developing primary standards based on quantum metrology, thereby to realize the Quantum SI. For the becquerel (Bq) and gray (Gy), the derived SI units for activity and absorbed dose, respectively, this is especially challenging because production and detection of ionizing radiation is difficult to manage at the atomic scale, and quantum coherences are easily lost in the cascade of inelastic processes that accompany the slowing of energetic particles in matter. This would not preclude a secondary role for quantum metrology in the pursuit of single-event detection and resolution of radiation effects at microscopic scales, where we are beginning to apply new transition-edge sensors, silicon photonics, and link to quantum electrical standards. Here we summarize recent results for microcalorimetry in activity and dosimetry measurements and discuss their potential as next-generation standards.

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.

This Letter reports the first measurement of the ^{235}U ν[over ¯]_{e} energy spectrum by PROSPECT, the Precision Reactor Oscillation and Spectrum experiment, operating 7.9 m from the 85 MW_{th} highly enriched uranium (HEU) High Flux Isotope Reactor. With a surface-based, segmented detector, PROSPECT has observed 31678±304(stat) ν[over ¯]_{e}-induced inverse beta decays, the largest sample from HEU fission to date, 99% of which are attributed to ^{235}U. Despite broad agreement, comparison of the Huber ^{235}U model to the measured spectrum produces a χ^{2}/ndf=51.4/31, driven primarily by deviations in two localized energy regions. The measured ^{235}U spectrum shape is consistent with a deviation relative to prediction equal in size to that observed at low-enriched uranium power reactors in the ν[over ¯]_{e} energy region of 5-7 MeV.

A standard for activity of (224)Ra in secular equilibrium with its progeny has been developed, based on triple-to-double coincidence ratio (TDCR) liquid scintillation (LS) counting. The standard was confirmed by efficiency tracing and 4παβ(LS)-γ(NaI(Tl)) anticoincidence counting, as well as by 4πγ ionization chamber and NaI(Tl) measurements. Secondary standard ionization chambers were calibrated with an expanded uncertainty of 0.62 % (k = 2). Calibration settings were also determined for a 5 mL flame-sealed ampoule on several commercial reentrant ionization chambers (dose calibrators).

The Precision Reactor Oscillation and Spectrum (PROSPECT) Experiment is a reactor neutrino experiment designed to search for sterile neutrinos with a mass on the order of 1 eV/c$^2$ and to measure the spectrum of electron antineutrinos from a highly-enriched $^{235}$U nuclear reactor. The PROSPECT detector consists of an 11 by 14 array of optical segments in $^{6}$Li-loaded liquid scintillator at the High Flux Isotope Reactor in Oak Ridge National Laboratory. Antineutrino events are identified via inverse beta decay and read out by photomultiplier tubes located at the ends of each segment. The detector response is characterized using a radioactive source calibration system. This paper describes the design, operation, and performance of the PROSPECT source calibration system.

Re-entrant ionization chambers (ICs) are essential to radionuclide metrology and nuclear medicine for maintaining standards and measuring half-lives. The requirements of top-level metrology demand that systems must be precise and stable to 0.1 % over many years, and linear from 10−14 A to 10−8 A. Thus, laboratories depend on bespoke current measurement systems and often rely on sealed sources to generate reference currents. To maintain and improve present capabilities, metrologists need to overcome two looming challenges: ageing electronics and decreasing availability of sealed sources. Possible solutions using Ultrastable Low-Noise Current Amplifiers (ULCAs), resistive-feedback electrometers, and (quantum) single-electron pumps are reviewed. Broader discussions of IC design and methodology are discussed. ULCAs show promise and resistive-feedback systems which take advantage of standard resistor calibrations offer an alternative.

A solution of 124I was standardized for activity by 4πβ(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.

Main text Since 1988, 3 laboratories have submitted 5 samples of 153Gd to the International Reference System (SIR) for activity comparison at the Bureau International des Poids et Mesures (BIPM), with comparison identifier BIPM.RI(II)-K1.Gd-153. Recently, the NIST (United States) participated in the comparison and the key comparison reference value (KCRV) has been updated. The degrees of equivalence between each equivalent activity measured in the SIR and the updated KCRV have been calculated and the results are given in the form of a table. A graphical presentation is also given. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database https://www.bipm.org/kcdb/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

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.

A new National Institute of Standards and Technology (NIST) tritiated-water ((3)H-labeled oxidane) standard was prepared and calibrated. It is the 17th in a series of linked standards since 1954 and will be disseminated as Standard Reference Material® SRM 4927G, having a massic activity of 544.2kBqg(-1), with an expanded (k=2) relative standard uncertainty of 0.96%, at a Reference Time of 1200 EST, 1 May 2015. The calibration is based on relative liquid scintillation (LS) measurements using quench-varied efficiency tracing with two previous 1999 issues, viz., SRM 4927F and 4926E. Measurement comparisons were also made with respect to a 1994 tritiated-water French national standard and to a tritiated-water solution measured by 19 laboratories as part of an international measurement comparison organized by the Bureau International des Poids et Mesures (BIPM) in 2009. Confirmatory measurements for the massic activity of both SRM 4927F and 4927G by a triple-to-double coincidence ratio (TDCR) technique were also made.

The Compton spectrum quenching technique is used to monitor the effect of ethyl alcohol (EtOH) additions on phase boundaries in two systems. In toluenic solutions of the nonionic surfactant, Triton X-100, EtOH shifts the boundary separating the first clear phase from the first turbid phase to higher water:surfactant ratios. In a commonly used scintillant, Ultima Gold AB, the critical micelle concentration is not shifted. The molecular interactions behind the observations and implications for liquid scintillation counting are discussed.

Using NIST-calibrated solutions of (131)Ba and (131)I in the 5mL NIST ampoule geometry, measurements were made in three NIST-maintained Capintec activity calibrators and the NIST Vinten 671 ionization chamber to evaluate the suitability of using (133)Ba as a calibration surrogate for (131)I. For the Capintec calibrators, the (133)Ba response was a factor of about 300% higher than that of the same amount of (131)I. For the Vinten 671, the Ba-133 response was about 7% higher than that of (131)I. These results demonstrate that (133)Ba is a poor surrogate for (131)I. New calibration factors for these radionuclides in the ampoule geometry for the Vinten 671 and Capintec activity calibrators were also determined.

Neutral particle detection in high-background environments is greatly aided by the ability to easily load 6Li into liquid scintillators. We describe a readily available and inexpensive liquid scintillation cocktail stably loaded with a Li mass fraction up to 1 %. Compositions that give thermodynamically stable microemulsions (reverse-micellar systems) were explored, using a Compton spectrum quenching technique to distinguish these from unstable emulsions. Scintillation light yield and transmittance were characterized. Pulse shape discrimination (PSD) was measured using a 252Cf source, showing that electron-like and proton-like recoil events are well-resolved even for Li loading up to 1 %, providing a means of background suppression in neutron/neutrino detectors. While samples in this work were prepared with nat Li (7.59 % 6Li), the neutron capture peak was clearly visible in the PSD spectrum; this implies that while extremely high capture efficiency could be achieved with 6Li-enriched material, a very inexpensive neutron-sensitive detector can be prepared with nat Li.

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 ± 1.5) × 10−6 (k = 1), agrees within 1 standard uncertainty with the recommended value of (32.6 ± 0.7) × 10−6 (k = 1) from the DDEP database.

A standard for activity of 224Ra in secular equilibrium with its progeny has been developed, based on triple-to-double coincidence ratio (TDCR) liquid scintillation (LS) counting. The standard was confirmed by efficiency tracing and 4παβ(LS)-γ(NaI(Tl)) anticoincidence counting, as well as by 4πγ ionization chamber and NaI(Tl) measurements. Secondary standard ionization chambers were calibrated with an expanded uncertainty of 0.62% (k = 2). Calibration settings were also determined for a 5 mL flame-sealed ampoule on several commercial reentrant ionization chambers (dose calibrators).

This report summarises the results for the new BIPM.RI(II)-K1.Ge-68 comparison. Six metrology institutes have participated, enabling the first value of the key comparison reference value(KCRV) to be determined. The KCRV was calculated using the power-moderated weighted mean and the results. A link has been made to the CCRI(II)-K2.Ge-68 comparison held in 2015 through the NIST, NIM,IRA-METAS and the LNE-LNHB who participated in both comparisons. One NMI used the K2 comparison to update their degree of equivalence. The degrees of equivalence between each equivalent activity measured in the International Reference System (SIR) and the KCRV have been calculated and the results are given in the form of a table for the remaining five NMIs in the BIPM.RI(II)-K1.Ge-68 comparison and the 12 other participants in the CCRI(II)-K2.Ge-68 comparison. A graphical presentation is also given. Main text To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Proceedings of the 21st International Conference on Radionuclide Metrology and its Applications (ICRM), May 15-19, 2017, Buenos Aires, Argentina. Organizer: Argentinian National Atomic Energy Commission; International audience; 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 $^{68}$Ge/$^{68}$Ga solution. Results for the activity concentration, CA, of $^{68}$Ge 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)β-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) kBq g$^{−1}$, based on 14 results. The degrees of equivalence and their associated uncertainties are evaluated for each participant. Several participants submitted 3.6 mL 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.

This paper describes the design and performance of a 50 liter, two-segment $^{6}$Li-loaded liquid scintillator detector that was designed and operated as prototype for the PROSPECT (Precision Reactor Oscillation and Spectrum) Experiment. The two-segment detector was constructed according to the design specifications of the experiment. It features low-mass optical separators, an integrated source and optical calibration system, and materials that are compatible with the $^{6}$Li-doped scintillator developed by PROSPECT. We demonstrate a high light collection of 850$\pm$20 PE/MeV, an energy resolution of $\sigma$ = 4.0$\pm$0.2% at 1 MeV, and efficient pulse-shape discrimination of low $dE/dx$ (electronic recoil) and high $dE/dx$ (nuclear recoil) energy depositions. An effective scintillation attenuation length of 85$\pm$3 cm is measured in each segment. The 0.1% by mass concentration of $^{6}$Li in the scintillator results in a measured neutron capture time of $\tau$ = 42.8$\pm$0.2 $\mu s$. The long-term stability of the scintillator is also discussed. The detector response meets the criteria necessary for achieving the PROSPECT physics goals and demonstrates features that may find application in fast neutron detection., Comment: 16 pages, 13 figures; minor edits to design detail and references

This Letter reports the first scientific results from the observation of antineutrinos emitted by fission products of $^{235}$U at the High Flux Isotope Reactor. PROSPECT, the Precision Reactor Oscillation and Spectrum Experiment, consists of a segmented 4 ton $^6$Li-doped liquid scintillator detector covering a baseline range of 7-9 m from the reactor and operating under less than 1 meter water equivalent overburden. Data collected during 33 live-days of reactor operation at a nominal power of 85 MW yields a detection of 25461 $\pm$ 283 (stat.) inverse beta decays. Observation of reactor antineutrinos can be achieved in PROSPECT at 5$\sigma$ statistical significance within two hours of on-surface reactor-on data-taking. A reactor-model independent analysis of the inverse beta decay prompt energy spectrum as a function of baseline constrains significant portions of the previously allowed sterile neutrino oscillation parameter space at 95% confidence level and disfavors the best fit of the Reactor Antineutrino Anomaly at 2.2$\sigma$ confidence level., Comment: 7 pages, 5 figures; v3: Added additional supplemental files

The Precision Reactor Oscillation and Spectrum Experiment, PROSPECT, is designed to make both a precise measurement of the antineutrino spectrum from a highly-enriched uranium reactor and to probe eV-scale sterile neutrinos by searching for neutrino oscillations over meter-long baselines. PROSPECT utilizes a segmented $^6$Li-doped liquid scintillator detector for both efficient detection of reactor antineutrinos through the inverse beta decay reaction and excellent background discrimination. PROSPECT is a movable 4-ton antineutrino detector covering distances of 7m to 13m from the High Flux Isotope Reactor core. It will probe the best-fit point of the $\bar\nu_e$ disappearance experiments at 4$\sigma$ in 1 year and the favored regions of the sterile neutrino parameter space at more than 3$\sigma$ in 3 years. PROSPECT will test the origin of spectral deviations observed in recent $\theta_{13}$ experiments, search for sterile neutrinos, and address the hypothesis of sterile neutrinos as an explanation of the reactor anomaly. This paper describes the design, construction, and commissioning of PROSPECT and reports first data characterizing the performance of the PROSPECT antineutrino detector., Comment: 30 pages, 33 figures; updated with journal revision and reference

Ra-223 is an alpha-emitter that is being used as a bone-seeking radiotherapeutic agent. The relatively large uncertainty on its evaluated half-life (0.26%, Be et al., 2011 ) is an impediment to precision activity assays, which often involve measurements by various methods over time spans of days or weeks. We have performed two series of measurements using an ionization chamber (IC) and a NaI(Tl) well counter (γ-wc) to determine new, precise values for the 223Ra half-life. We have endeavored to realistically assess the uncertainties on the derived half-lives, looking beyond the fit uncertainties to identify uncertainty components acting on multiple timescales. We recovered respective values of 11.447(6) d and 11.445(13) d from the IC and γ-wc measurements. Our values are in accord with the evaluated value of 11.43(3) d, but with smaller combined uncertainties.

As a result of a recent change in the National Institute of Standards and Technology (NIST) activity standard for 18F, we have determined new relative response ratios for a 68Ge solid epoxy mock syringe source used in activity calibrators as a long-lived substitute for 18F. New standardized solutions of each radionuclide were used to determine the response ratios while maintaining traceability to national standards. This work updates our previously published data from 2010. Methods: Following our previously published methodology, solution-filled mock syringe sources, identical in geometry to the solid 68Ge epoxy calibration source currently on the market, were prepared using NIST-calibrated solutions of 68GeCl4 and 18F-FDG and directly compared in several models of activity calibrators to determine empirically the relative response ratios for these 2 radionuclides. Results: The new relative response ratios measured in this study reflect the change in 18F activity measurements that arise from the recent −4% change in the NIST activity standard. The results allow the 68Ge activity of the mock syringe source to be expressed in terms of equivalent 18F activity, with a relative combined standard uncertainty of about 0.8% for the activity calibrators used in this study. Conclusion: This work revises our previously derived relative response ratios for 18F and 68Ge by −3.7%, allowing users of the commercial mock syringe surrogate source to calibrate their activity calibrators in a way that is consistent with the recent change in the NIST 18F standard.

Dose calibrator dial settings reported by NIST in 2010 (ARI, v. 68, p. 1367) are now known to give erroneously low (by 10%) activity readings. The original determinations were based on a chain of calibrations; a broken link in this chain was recently discovered. New calibration factors (i.e., dial settings), directly linked to updated NIST primary standards, are reported here. In addition, the raw data used to derive the factors reported in 2010 are revisited. The validity of the reevaluation is established via comparison with the new experiments and revised calibration factors for numerous clinical geometries are reported. The main conclusions of the 2010 report regarding geometry effects remain valid.

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.

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.

Source self-attenuation for solutions of (57)Co of varying density and carrier concentration was measured in nine re-entrant ionization chambers maintained at NIST. The magnitude of the attenuation must be investigated to determine whether a correction is necessary in the determination of the activity of a source that differs in composition from the source used to calibrate the ionization chamber. At our institute, corrections are currently made in the measurement of (144)Ce, (109)Cd, (67)Ga, (195)Au, (166)Ho, (177)Lu, and (153)Sm. This work presents the methods used as recently applied to (57)Co. A range of corrections up to 1% were calculated for dilute to concentrated HCl at routinely used carrier concentrations.

Using uniform cylindrical phantoms containing calibrated solutions of 18F and 64Cu, we evaluated for the first time the accuracy with which the activity concentration of 64Cu can be quantified on an absolute basis using Positron Emission Tomography (with X-ray Computed Tomography, PET-CT). The scanner was first calibrated for 18F using the manufacturer's calibration protocol and a phantom with an activity concentration value traceable to the U.S. National standard. By using a similarly calibrated 18F solution phantom, we were able to determine a correction factor that can be applied to the 64Cu imaging data that gave a result that is consistent with 100% recovery with a combined standard uncertainty of 2%. We also demonstrate how a calibrated, solid phantom containing 68Ge as a long-lived 18F surrogate can be used to monitor and transfer the correction factor to other studies.

Calibration factors for commercial ionization chambers (i.e. dose calibrators) were determined for a solution of 123I; the activity was based on the 1976 NBS standard. A link between the NIST standard and the International Reference System (SIR) was established. The two major U.S. dose calibrator manufacturers recommend oppositely biased calibration factors, giving a spread of 11.3% in measured activities. With modern quantitative imaging techniques capable of ≤10% accuracy, this bias for a SPECT nuclide is highly significant.

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.

A new primary standardization of 18 F by NIST is reported. The standard is based on live-timed beta-gamma anticoincidence counting with confirmatory measurements by three other methods: ( i ) liquid scintillation (LS) counting using CIEMAT/NIST 3 H efficiency tracing; ( ii ) triple-to-double coincidence ratio (TDCR) counting; and ( iii ) NaI integral counting and HPGe γ-ray spectrometry. The results are reported as calibration factors for NIST-maintained ionization chambers (including some “dose calibrators”). The LS-based methods reveal evidence for cocktail instability for one LS cocktail. Using an ionization chamber to link this work with previous NIST results, the new value differs from the previous reports by about 4%, but appears to be in good agreement with the key comparison reference value (KCRV) of 2005.

PROSPECT, the Precision Reactor Oscillation and SPECTrum experiment, is a short-baseline reactor antineutrino experiment designed to provide precision measurements of the $^{235}$U product $\overline{\nu}_e$ spectrum of utilizing an optically segmented 4-ton liquid scintillator detector. PROSPECT's segmentation system, the optical grid, plays a central role in reconstructing the position and energy of $\overline{\nu}_e$ interactions in the detector. This paper is the technical reference for this PROSPECT subsystem, describing its design, fabrication, quality assurance, transportation and assembly in detail. In addition, the dimensional, optical and mechanical characterizations of optical grid components and the assembled PROSPECT target are also presented. The technical information and characterizations detailed here will inform geometry-related inputs for PROSPECT physics analysis, and can guide a variety of future particle detection development efforts, such as those using optically reflecting materials or filament-based 3D printing., Comment: 31 pages, 28 figures

This work reports the production and characterization of lithium-loaded liquid scintillator (LiLS) for the Precision Reactor Oscillation and Spectrum Experiment (PROSPECT). Fifty-nine 90 liter batches of LiLS (${}^6{\rm Li}$ mass fraction 0.082%$\pm$0.001%) were produced and samples from all batches were characterized by measuring their optical absorbance relative to air, light yield relative to a pure liquid scintillator reference, and pulse shape discrimination capability. Fifty-seven batches passed the quality assurance criteria and were used for the PROSPECT experiment., 16 pages, 15 figures

International audience; The hypothesis that proximity to the Sun causes variation of decay constants at permille level has been tested and disproved. Repeated activity measurements of mono-radionuclide sources were performed over periods from 200 days up to four decades at 14 laboratories across the globe. Residuals from the exponential nuclear decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ from one data set to another and are attributable to instabilities in the instrumentation and measurement conditions. The most stable activity measurements of alpha, beta-minus, electron capture, and beta-plus decaying sources set an upper limit of 0.0006% to 0.008% to the amplitude of annual oscillations in the decay rate. Oscillations in phase with Earth's orbital distance to the Sun could not be observed within a 10−6 to 10−5 range of precision. There are also no apparent modulations over periods of weeks or months. Consequently, there is no indication of a natural impediment against sub-permille accuracy in half-life determinations, renormalisation of activity to a distant reference date, application of nuclear dating for archaeology, geo- and cosmochronology, nor in establishing the SI unit becquerel and seeking international equivalence of activity standards.

Ligand exchange reactions important in the formation of L3- and L5-protected gold clusters (L3 = 1,3-bis(diphenylphosphino)propane; L5 = 1,5-bis(diphenylphosphino)pentane) are investigated at the molecular level. We establish that molecular complexes, [Au(PPh3)xL2-xn]+, in which Au+ is bound to at least one triphenylphosphine ligand (PPh3) act as precursors to cluster formation, while complexes in which Au+ is bound only to the diphosphine ligands do not. Ligand exchange reactions and ion equilibria were studied via electrospray ionization mass spectrometry, and a critical reaction was studied with ab initio molecular dynamics simulations. The displacement of one PPh3 by L3 on [Au(PPh3)2]+ was studied with transition path sampling calculations with Car−Parrinello molecular dynamics simulations. The experiments and simulations are in excellent agreement, and we demonstrate the applicability of these tools to chemical reactions involving ligand exchange.