Coincidence Counting Technique Research Articles

Practical Method for Achieving Single-Photon Femtosecond Time-Resolved Spectroscopy: Transient Stimulated Emission.

Recent advances in single-photon femtosecond spectroscopy have highlighted the power of entangled photons in probing the properties of materials, previously inaccessible through semiclassical spectroscopic approaches. In this study, we theoretically propose a new single-photon-based femtosecond time-resolved spectroscopy technique termed single-photon transient stimulated emission (SP-TSE). SP-TSE not only enables the selective investigation of singly excited superposition states but also harnesses the quantum mechanical nature of photons for the efficient data acquisition of transient responses, thereby supporting the feasibility of experimental realization of SP-TSE. The key aspect of SP-TSE is the selective detection of two-photon states produced through stimulated emission using coincidence counting techniques. Our theoretical framework, supported by numerical simulations, demonstrates the efficacy in capturing the pure decoherence dynamics of a model molecular cavity, highlighting its potential to reveal quantum mechanical properties that are difficult to observe with semiclassical femtosecond time-resolved experiments.

Monte Carlo simulations of correlation between anisotropic emission characteristics of prompt fission neutrons and sample multiplication

In the present study, the correlation between prompt neutron angular distributions and sample multiplication for three spontaneously fissionable nuclides (252Cf, 244Cm, and 240Pu) was quantitatively determined by Monte Carlo simulations with MCNP6.2 and Geant4.10. To this end, various parameters (i.e., point, area, gradient, and net-area-based parameters) were investigated to analyze the asymmetry of the angular distribution. It was confirmed that the asymmetry decreases as leakage multiplication increases, and that the extent of this variation depends on the given nuclear isotopes. After comparing the sensitivity of the asymmetry values to leakage multiplication, the net-area-based parameter was determined to be the optimal asymmetry parameter. Finally, fitting equations were determined in order to determine, by regression analysis, leakage multiplication as a function of the asymmetry parameter for each isotope of interest. The results presented here could contribute to the development of a fast-neutron-based coincidence counting technique for nuclear material accountancy in safeguards applications.

A Direct Nondestructive Assay for the Pu of U/TRU Ingot in Pyroprocessing Using 244Cm Neutron Albedo Reactivity Technique and Its Error

The transuranic (TRU) ingot is considered to be the most prominent target material of pyroprocessing in terms of safeguards since it contains almost all of the Pu of the feed spent fuel. Due to the high density, excessively high neutron emission rates, and high neutron multiplication of the U/TRU ingot, it is impractical to apply gamma-ray spectroscopy or neutron coincidence counting techniques to the quantification of the Pu content of the U/TRU ingot. Since the passive neutron albedo reactivity (PNAR) technique is known to be sensitive to the total fissile mass of target material and the uncertainty of its singles Cd ratio is independent of the accidental coincidence coming from the high neutron emission rate, the capability of the PNAR technique for the quantification of the Pu content of the U/TRU ingot has been investigated using the MCNPX code with a spent fuel library with 81 different cases of various kinds of initial enrichment, burnup, and cooling time. The MCNPX simulation results for the Cd ratio versus Pu content of the U/TRU ingot show the maximum error in the Pu mass between the linear fit and the real Pu content in the U/TRU ingot is 2.14% for 4.5 wt% initial enrichment cases. The results of this study show that the PNAR technique can be one possible method for the direct nondestructive assay for the Pu of the U/TRU ingot.

Primary activity standardization of 177Lu for calibrating commercial dose calibrator

Primary activity standardization of 177Lu has been conducted at the Center for Technology of Radiation Safety and Metrology-National Nuclear Energy Agency (PTKMR-BATAN) to establish a national reference standard for 177Lu measurements. The standardization was performed using a 47i(3(LS)-y coincidence counting system with digital coincidence counting (DCC) technique. The activity standardization of 177Lu gave a result of 148 kBq/g + 1.78 kBq/g at a reference time with uncertainty value evaluated at k = 2. The result was then used to establish a secondary standard by calibrating the reference ionization chamber using the ‘dialing-in’ method. A dial setting value of 024 was obtained on the standard reference IC. The new dial setting will be used in the routine calibration services of commercial dose calibrator to ensure all measurements of 177Lu are traceable to the national standards.

Measurement of the tensor analyzing power for the reaction γd → pnπ0

The paper discusses the results of measurement for three components of tensor analyzing power for the reaction of incoherent [Formula: see text]-meson photoproduction on a deuteron within the proton energy range of 15–200[Formula: see text]MeV and the neutron energy range of 15–150[Formula: see text]MeV. The experiment was performed on the deuterium internal gas target of VEPP-3 electron accelerator using the protons and neutrons coincidence counting technique. The results of measurements of the tensor analyzing power’s components are compared with the results of statistical modeling performed within the frameworks of a theoretical model.

ASNC upgrade for nuclear material accountancy of ACPF

A safeguards neutron coincidence counter for nuclear material accountancy of the Advanced spent-fuel Conditioning Process Facility (ACPF), known as the ACP Safeguards Neutron Counter (ASNC), was upgraded to improve its remote-handling and maintenance capabilities. Based on the results of the previous design study, the neutron counter was completely rebuilt, and various detector parameters for neutron coincidence counting (i.e., high-voltage plateau, efficiency profile, dead time, die-away time, gate length, doubles gate fraction, and stability) were experimentally determined. The measurement data showed good agreement with the MCNP simulation results. To the best of the authors’ knowledge, the ASNC is the only safeguards neutron coincidence counter in the world that is installed and operated in a hot-cell. The final goals to be achieved were (1) to evaluate the uncertainty level of the ASNC in nuclear material accountancy of the process materials of the oxide-reduction process for spent fuels and (2) to evaluate the applicability of the neutron coincidence counting technique within a strong radiation field (e.g., in a hot-cell environment).

Activity determination of 67Ga using 4πβ‒γ coincidence counting

The activity of a 67Ga solution was measured by means of the 4πβ–γ coincidence counting technique. A setup with a proportional counter and non-extending dead-time modules in the two detector channels was used. The influence of the delayed state affecting the measured count rates was taken into account by using appropriate correction formulae. The analysis requires a variation of the dead time and a subsequent extrapolation to infinite dead time. An uncertainty of about 0.5% was obtained and the result was used to make an intercomparison with the SIR of the BIPM.

Activity determination of 88Y by means of 4πβ(LS)-γ coincidence counting

The activity concentration of an 88Y solution was measured by means of a new custom-built 4πβ(LS)-γ coincidence counting system. Efficiency variation was carried out using chemical quenching and neutral density filters. A relative uncertainty of 0.57% was obtained for the activity concentration. Details of the measurements and of the analysis, as well as possibilities to reduce the uncertainty are discussed. Additional validation measurements were carried out by means of the well-established coincidence counting technique using a proportional counter (PC) in the β channel. The results of both coincidence methods were found to be in excellent agreement.

A fast-neutron coincidence collar using liquid scintillators for fresh fuel verification

The IAEA has developed a liquid scintillator-based system for the non-destructive assay of 235U in fresh fuel assemblies. The fast neutron coincidence collar (FNCL) addresses current limitations in existing neutron coincidence counting techniques when measuring fuel containing burnable neutron poisons. Detection of fast neutrons rather than thermal neutrons allows the minimisation of measurement time and biases (due to effects of burnable poisons). The FNCL hardware, software and instrument optimisation are discussed. Experimental results from measurements of mock-up uranium fuel assemblies at the institute for transuranium elements, Karlsruhe, Germany with varying 235U enrichment and burnable neutron poison content are presented.

Activity determination of 60Co and the importance of its beta spectrum

The activity concentration of a 60Co solution was measured by means of two 4πβ-γ coincidence counting systems using a liquid scintillation counter and a proportional counter (PC) in the beta channel, respectively. Additional liquid scintillation measurements were carried out and CIEMAT/NIST efficiency tracing as well as the triple-to-double coincidence ratio (TDCR) methods were applied to analyse the data. The last two methods require computed beta spectra to determine the counting efficiencies.The results of both 4πβ-γ coincidence counting techniques are in very good agreement and yield a robust reference value. The initial activity concentration determined with liquid scintillation counting was found to be significantly lower than the results from 4πβ-γ coincidence counting. In addition, the results from TDCR and CIEMAT/NIST show some inconsistency.The discrepancies were resolved by applying new beta spectrum calculations for the dominant allowed beta transition of 60Co. The use of calculations which take screening effects as well as the atomic exchange effect into account leads to good agreement between all four methods; the combination of these techniques delivers an important validation of beta spectra.

Standardization of 106Ru/Rh by live-timed anticoincidence counting and gamma emission determination

The absolute activity standardization measurement system of radionuclide by live-timed anticoincidence counting was implemented at LNMRI in 2008 to reduce the effects of some correction factors on the determination of activity with coincidence counting technique used for decades in the laboratory, for example, the corrections of dead time and resolution.With the live-timed anticoincidence system, the variety of radionuclides that can be calibrated by LNMRI was increased in relation to the type of decay. The objective of this study was to standardize the 106Ru activity, determine gamma emission probabilities by spectrometric method for some energies, and estimate measurement uncertainties.

Absolute intensities of the γ-ray emissions originating from the electron capture decay of 153Gd

153 Gd has widespread use, in non-destructive testing, as a line source in SPECT imaging and has been recently proposed as an in-vitro interstitial rotating shield brachytherapy (I-RSBT) source. In this work, the six most intense emissions in the de-excitation of the daughter nucleus 153 Eu have been measured, with an improved accuracy and precision to γ-ray emission intensities reported previously, via two characterised HPGe spectrometers. A specific absolute activity of 512.5 (25) kBq g−1 was determined using the 4π (LS)-γ digital coincidence counting technique. This absolute activity was used to determine an absolute intensity for the 97.4 keV γ-ray emission of 30.15 (20) per 100 decays. The reported absolute emission intensity of this transition in this work has a relative difference of 4% from the currently recommended value.

Application of the coincidence counting technique to DD neutron spectrometry data at the NIF, OMEGA, and Z.

A compact neutron spectrometer, based on a CH foil for the production of recoil protons and CR-39 detection, is being developed for the measurements of the DD-neutron spectrum at the NIF, OMEGA, and Z facilities. As a CR-39 detector will be used in the spectrometer, the principal sources of background are neutron-induced tracks and intrinsic tracks (defects in the CR-39). To reject the background to the required level for measurements of the down-scattered and primary DD-neutron components in the spectrum, the Coincidence Counting Technique (CCT) must be applied to the data. Using a piece of CR-39 exposed to 2.5-MeV protons at the MIT HEDP accelerator facility and DD-neutrons at Z, a significant improvement of a DD-neutron signal-to-background level has been demonstrated for the first time using the CCT. These results are in excellent agreement with previous work applied to DT neutrons.

Standardization of the radionuclides 60Co and 59Fe by digital 4πβ(PC)-γ(NaI) coincidence counting

The digital coincidence counting (DCC) technique has been developed at NIM, China to replace the classical analog coincidence units in the 4πβ-γ counting system. The detector system comprises two NaI (Tl) γ-ray detectors and a 4πβ proportional counter (PC) operated with a mixture of argon and methane at atmospheric pressure in a gas flow arrangement. To update the activity results of radionuclide 60Co in the KCDB and contribute to the APMP.RI(II)-K2.Fe-59 comparison, 60Co and 59Fe dry sources were prepared and measured using the digital 4πβ(PC)-γ(NaI) coincidence system by applying the efficiency extrapolation method. For 60Co nuclide, the activity concentration value equal to 290.6kBqg−1 with a relative standard uncertainty of 0.26%, is consistent with the result given by the calibrated ionization chamber. For the nuclide 59Fe, the activity concentration value at the reference date was 471.7kBqg−1 with a relative standard uncertainty of 0.34%. This value is in good agreement with the result obtained with the HPGe γ spectrometry, which was calibrated by using a series of standard point sources from PTB.

Experimental investigation of the influence of laser intensity on the quality of Einstein-Podolsky-Rosen entangled photons

Using spontaneous parametric down conversion, polarization post selection and coincidence counting technique, the polarization Einstein-Podolsky-Rosen (EPR) entangled states are prepared. Experimental studies on the efficiency, contrast and fidelity with different pump laser intensities are performed systematically. The results show that the pump laser intensity distinctly influences the quality of entangled photons, especially the contrast and the fidelity. On the other hand, the pump efficiency of entangled photons is almost invariable, namely the entangled source brightness increases linearly with the increase of pump laser power.

Precise measurements of the absolute γ-ray emission probabilities of 223Ra and decay progeny in equilibrium

Precise measurements of the absolute γ-ray emission probabilities have been made of radiochemically pure solutions of 223Ra in equilibrium with its decay progeny, which had been previously standardised by 4π(liquid scintillation)-γ digital coincidence counting techniques. Two high-purity germanium γ-ray spectrometers were used which had been accurately calibrated using a suite of primary and secondary radioactive standards. Comparison of the activity concentration determined by the primary technique against γ-ray spectrometry measurements using the nuclear data evaluations of the Decay Data Evaluation Project exhibited a range of ~18% in the most intense γ-ray emissions (>1% probability) of the 223Ra decay series. Absolute γ-ray emission probabilities and standard uncertainties have been determined for the decay of 223Ra, 219Rn, 215Po, 211Pb, 211Bi and 207Tl in equilibrium. The standard uncertainties of the measured γ-ray emission probabilities quoted in this work show a significant improvement over previously reported γ-ray emission probabilities. Correlation coefficients for pairs of the measured γ-ray emission probabilities from the decays of the radionuclides 223Ra, 219Rn and 211Pb have been determined and are presented. The α-transition probabilities of the 223Ra have been deduced from P(γ+ce) balance using the γ-ray emission probabilities determined in this work with some agreement observed with the published experimental values of the α-emission probabilities.

Standardisation of 223Ra by liquid scintillation counting techniques and comparison with secondary measurements

An aqueous solution of 223Ra chloride in equilibrium with its decay progeny was standardised by liquid scintillation counting techniques. Since secular equilibrium with the decay progeny of 223Ra had been established by the time of measurement, the apparent detection efficiency of 223Ra was approximately 6 and was determined by both the CIEMAT/NIST efficiency tracing technique and the 4π(LS)-γ digital coincidence counting techniques. The results obtained were compared with γ-spectrometry and ionisation chamber measurements. Whilst the γ-spectrometry measurements were in agreement (albeit exhibiting a large spread (18%) in the individual activity estimations using the main γ-emissions), a significant discrepancy of the order of 9% was identified between the liquid scintillation counting results and those obtained using published calibration factors for a variety of radionuclide calibrators.

First principle active neutron coincidence counting measurements of uranium oxide

Uranium is present in most nuclear fuel cycle facilities ranging from uranium mines, enrichment plants, fuel fabrication facilities, nuclear reactors, and reprocessing plants. The isotopic, chemical, and geometric composition of uranium can vary significantly between these facilities, depending on the application and type of facility. Examples of this variation are: enrichments varying from depleted (~0.2wt% 235U) to high enriched (>20wt% 235U); compositions consisting of U3O8, UO2, UF6, metallic, and ceramic forms; geometries ranging from plates, cans, and rods; and masses which can range from a 500kg fuel assembly down to a few grams fuel pellet. Since 235U is a fissile material, it is routinely safeguarded in these facilities. Current techniques for quantifying the 235U mass in a sample include neutron coincidence counting. One of the main disadvantages of this technique is that it requires a known standard of representative geometry and composition for calibration, which opens up a pathway for potential erroneous declarations by the State and reduces the effectiveness of safeguards. In order to address this weakness, the authors have developed a neutron coincidence counting technique which uses the first principle point-model developed by Boehnel instead of the “known standard” method. This technique was primarily tested through simulations of 1000g U3O8 samples using the Monte Carlo N-Particle eXtended (MCNPX) code. The results of these simulations showed good agreement between the simulated and exact 235U sample masses.

New concepts for radiometric measurements of environmental samples

The Radiation Detection and Nuclear Sciences Group at Pacific Northwest National Laboratory has a long history in conducting measurements of radioisotopes for various applications. This experience includes ultra-low background measurements, arrays of germanium detectors, automated sampling and measurement systems and coincidence measurement systems. A recent lab-supported effort has been studying how these capabilities, both in terms of hardware and experience, can be leveraged to enable environmental sampling measurements. One area of interest is the release of fission products and actinides into the environment from a reactor incident. While the initial survey of this area is still under way, one isotope of interest that surfaced early in the study is 238Pu. Existing techniques to assay this isotope suffer from measurement challenges. In alpha counting, there can be significant interference with 241Am, while in mass spectrometry, there can be interference with 238U. The authors are developing the concept for a detector that through coincidence counting techniques can distinguish 238Pu and 241Am. In addition, we will design the system to conduct radiometric measurements of other plutonium isotopes to enable a direct comparison of those isotopes. We will present our concept of the detector system for 238Pu, as well as discuss other radiometric measurements of fission products and actinides with which we intend to advance the state of the art for environmental measurements.

Standardization of 18F by digital coincidence counting

The radioactivity of 18F has been measured by a digital coincidence counting (DCC) system. The main advantages of the digital coincidence counting technique are a shortening of the measurement time as compared with conventional coincidence counting and an ability to obtain activities with various experimental parameters through off-line analysis. The measurement results of radioactivity for 18F solution were compared with those of a conventional coincidence counting technique and a reference ion chamber method.