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PURPOSE: To develop and implement an efficient and accurate commissioning procedure for small field static beam animal irradiation studies on an MV research linear accelerator (Linatron-M9) using radiochromic gel dosimetry. MATERIALS: The research linear accelerator (Linatron-M9) is a 9 MV linac with a static fixed collimator opening of 5.08 cm diameter. Lead collimators were manually placed to create smaller fields of 2x2 cm(2), 1x1 cm(2) and 0.5x0.5 cm(2). Relative dosimetry measurements were performed, including profiles, percent depth dose (PDD) curves, beam divergence, and relative output factors using various dosimetry tools, including a small volume ionization chamber (A14), GAFCHROMIC™ EBT3 film, and Clearview gel dosimeters. The gel dosimeter was used to provide a 3D volumetric reference of the irradiated fields. The Linatron profiles and relative output factors were extracted at a reference depth of 2 cm with the output factor measured relative to the 2x2 cm(2) reference field. Absolute dosimetry was performed using A-14 ionization chamber measurements, which were verified using a national standards laboratory remote dosimetry service. RESULTS: Absolute dosimetry measurements were confirmed within 1.4% (k = 2, 95% confidence = 5%). The relative output factor of the small fields measured with films and gels agreed with a maximum relative percent error difference between the two methods of 1.1 % for the 1x1 cm(2) field and 4.3 % for the 0.5x0.5 cm(2) field. These relative errors were primarily due to the variability in the collimator positioning. The measured beam profiles demonstrated excellent agreement for beam size (measured as FWHM), within approximately 0.8 mm (or less). Film measurements were more accurate in the penumbra region due to the film’s finer resolution compared with the gel dosimeter. Following the van Dyk criteria, the PDD values of the film and gel measurements agree within 11% in the buildup region starting from 0.5 cm depth and within 2.6 % beyond maximum dose and into the fall-off region for depths up to 5 cm. The 2D beam profile isodose lines agree within 0.5 mm in all regions for the 0.5x0.5 cm(2) and the 1x1 cm(2) fields and within 1 mm for the larger field of 2x2 cm(2). The 2D PDD curves agree within approximately 2% of the maximum in the typical therapy region (1–4 cm) for the 1x1 cm(2) and 2x2 cm(2) and within 5% for the 0.5x0.5 cm(2) field. CONCLUSION: This work provides a commissioning process to measure the beam characteristics of a fixed beam MV accelerator with detailed dosimetric evaluation for its implementation in megavoltage small animal irradiation studies. Radiochromic gel dosimeters are efficient small field relative dosimetry tools providing 3D dose measurements allowing for full representation of dose, dosimeter misalignment corrections and high reproducibility with low inter-dosimeter variability. Overall, radiochromic gels are valuable for fast, full relative dosimetry commissioning in comparison to films for application in high energy small-field animal irradiation studies.

A compact radiation imaging system capable of detecting, localizing, and characterizing special nuclear material (e.g. highly-enriched uranium, plutonium…) would be useful for national security missions involving inspection, emergency response, or war-fighters. Previously-designed radiation imaging systems have been large and bulky with significant portions of volume occupied by photomultiplier tubes (PMTs). The prototype imaging system presented here uses silicon photomultipliers (SiPMs) in place of PMTs because SiPMs are much more compact and operate at low power and voltage. The SiPMs are coupled to the ends of eight stilbene organic scintillators, which have an overall volume of 5.74 × 5.74 × 7.11 cm3. The prototype dual-particle imager’s capabilities were evaluated by performing measurements with a 252Cf source, a sphere of 4.5 kg of alpha-phase weapons-grade plutonium known as the BeRP ball, a 6 kg sphere of neptunium, and a canister of 3.4 kg of plutonium oxide (7% 240Pu and 93% 239Pu). These measurements demonstrate neutron spectroscopic capabilities, a neutron image resolution for a Watt spectrum of 9.65 ± 0.94° in the azimuthal direction and 22.59 ± 5.81° in the altitude direction, imaging of gamma rays using organic scintillators, and imaging of multiple sources in the same field of view.

PURPOSE: Electron-based ultra-high dose rate radiation therapy (UHDR-RT), also known as Flash-RT, has shown the ability to improve the therapeutic index in comparison to conventional radiotherapy (CONV-RT) through increased sparing of normal tissue. However, the extremely high-dose rates in UHDR-RT have raised the need for accurate real-time dosimetry tools. This work aims to demonstrate the potential of the emerging technology of Ionized Radiation Acoustic Imaging (iRAI) through simulation studies and investigate its characteristics as a promising relative in vivo dosimetric tool for UHDR-RT. METHODS: The detection of induced acoustic waves following a single UHDR pulse of a modified 6 MeV 21EX Varian Clinac in a uniform porcine gelatin phantom that is brain-tissue equivalent was simulated for an ideal ultrasound transducer. The full 3D dose distributions in the phantom for a 1x1 cm(2) field were simulated using EGSnrc (BEAMnrc\DOSXYZnrc) Monte Carlo (MC) codes. The relative dosimetry simulations were verified with dose experimental measurements using Gafchromic films. The spatial dose distribution was converted into an initial pressure source spatial distribution using the medium dependent dose-pressure relation. The MATLAB based toolbox k-Wave was then used to model the propagation of acoustic waves through the phantom and perform time-reversal (TR) based imaging reconstruction. The effect of the various linear accelerator (linac) operating parameters, including linac pulse duration and pulse repetition rate (frequency), were investigated as well. RESULTS: The Monte Carlo dose simulation results agreed with the film measurement results, specifically at the central beam region up to 80% dose within approximately 5% relative error for the central profile region and a local relative error of < 6 % for percentage dose depth. IRAI-based FWHM of the radiation beam was within approximately 3 mm relative to the MC simulated beam FWHM at the beam entrance. The real time pressure signal change agreed with the dose changes proving the capability of the iRAI for predicting the beam position. IRAI was tested through 3D simulations of its response to be based on the temporal changes in the linac operating parameters on a dose per pulse basis as expected theoretically from the pressure-dose proportionality. The pressure signal amplitude obtained through 2D simulations was proportional to the dose per pulse. The instantaneous pressure signal amplitude decreases as the linac pulse duration increases, as predicted from the pressure wave generation equations, such that the shorter the linac pulse the higher the signal and the better the temporal (spatial) resolutions of iRAI. The effect of the longer linac pulse duration on the spatial resolution of the 3D constructed iRAI images was corrected for through linac pulse deconvolution. This correction has improved the passing rate of the 1%/1mm gamma test criteria, between the pressure-constructed and dosimetric beam characteristic, to as high as 98%. CONCLUSIONS: A full simulation workflow was developed for testing the effectiveness of iRAI as a promising relative dosimetry tool for UHDR-RT radiation therapy. IRAI has shown the advantage of 3D dose mapping through the dose signal linearity and hence has the potential to be a useful dosimeter at depth dose measurement and beam localization and hence potentially for in vivo dosimetry in UHDR-RT.

The emission of neutrons and $\ensuremath{\gamma}$ rays by fission fragments reveal important information about the properties of fragments immediately following scission. The initial fragment properties, correlations between fragments, and emission competition give rise to correlations in neutron-$\ensuremath{\gamma}$ emission. Recent theoretical and experimental advances have been proposed to explain the mechanism of angular momentum generation in fission, which would result in observable signature in neutron-$\ensuremath{\gamma}$ emission correlations. In this paper, we present a novel analysis method of neutrons and $\ensuremath{\gamma}$ rays emitted by fission fragments that allows us to discern structure in the observed correlations. We have analyzed data collected on $^{252}\mathrm{Cf}$(sf) at the Chi-Nu array at the Los Alamos Neutron Science Center. Through our analysis of the energy-differential neutron-$\ensuremath{\gamma}$ multiplicity covariance, we have observed enhanced neutron-$\ensuremath{\gamma}$ correlations, corresponding to rotational band $\ensuremath{\gamma}$-ray transitions, at $\ensuremath{\gamma}$-ray energies of 0.7 and 1.2 MeV. To shed light on the origin of this structure, we compare the experimental data with the predictions of three model calculations. The origin of the observed correlation structure is understood in terms of a positive spin-energy correlation in the generation of angular momentum in fission.

In this work, an epithermal neutron multiplicity counter (ENMC) and an organic scintillator multiplicity counter (OSMC) are compared in the assay of 237Np, a potentially weapons-usable isot...

Rossi-alpha measurements of fissionable assemblies are used to estimate the prompt neutron decay constant α. Reactivity can be inferred from α if the values of the neutron generation time a...

The neutron light-output response from quasi-monoenergetic neutrons was measured for a O5.08 × 5.08 cm trans-stilbene and a O5.08 × 5.08 cm small-molecule organic glass scintillator . Quasi-monoenergetic neutrons were isolated from a time-of-flight measurement of a Cf-252 spontaneous fission source with a flight distance of 200 cm. Two different methods of waveform analysis were implemented, where the neutron light output response proportional to the detected pulse height distribution (PHD) and pulse integral distribution (PID) were extracted for both types of scintillators. The light output response proportional to the pulse integral was determined by integrating the digitized waveform with an integration window length of 150 ns, which contained > 90% and > 95% of the scintillation light for an averaged neutron and photon waveform above 0.5 MeVee. The extracted light-output data were fitted with a semi-empirical function based on the Birks’ formula. The results show that the small-molecule organic glass scintillator produced more light than the trans-stilbene scintillator for a range of neutron energies of 0.79 ± 0.04 MeV to 3.65 ± 0.38 MeV. The fitted semi-empirical function was used in MCNPX-PoliMi with MPPost to simulate the detector response from an independent measurement of a Cf-252 spontaneous fission source to test the fidelity of the extracted light output response functions. The simulated and measured total neutron count rate agreed to within ± 3 % and ± 1% for the trans-stilbene and small-molecule organic glass scintillators. Due to the different light-output response of the two scintillators, the intrinsic neutron detection efficiency was calculated for equal observable ranges in light output and neutron-equivalent energy units. The intrinsic neutron detection efficiency in the observable light-output range of 0.06 MeVee to 2.4 MeVee was calculated to be 28.66 ± 1.43 % and 34.66 ± 1.73 % for pulse height and pulse integral analysis, respectively. For the same observable light-output range, the intrinsic efficiency of small-molecule organic glass was calculated to be 32.54 ± 1.63 % and 37.39 ± 1.87 % for pulse height and pulse integral analysis, respectively. When observing equal light-output ranges, the small-molecule organic glass was 11.92 ± 6.23% and 7.88 ± 7.35% more efficient than the trans-stilbene using pulse height and pulse integral analysis, respectively. When observing equal neutron-equivalent energy ranges, the trans”–stilbene scintillator was 8.4 ± 6.46% and 11.95 ± 6.23% more efficient than the small-molecule organic glass for pulse height and pulse integral analysis, respectively.

A prototype stilbene beta cell has been designed, manufactured, tested, and compared to a plastic scintillator beta cell used for nuclear explosion monitoring of radioxenon. Measurements of the four isotopes of interest show similar responses for both the plastic scintillator and stilbene cell. However, we show that the stilbene cell exhibits 100-times smaller memory effect than the plastic cell, a capability that is of interest in nuclear explosion monitoring because it improves detection sensitivity, allowing for decreased time between measurements. The resolution of the stilbene cell is improved slightly (decreased by 2.2 keV at 129 keV) when compared to the plastic scintillator cell. The efficiency of the stilbene cell is lower than that of the plastic by an average 15%. These results suggest that the light-collection efficiency of the stilbene cell could be improved in future designs. Pulse shape discrimination analysis decreases the minimum detectable concentration by 1%. The use of this geometry allows for a simple replacement of the plastic cells currently used in the field versus a complete overhaul of the existing radioxenon monitoring stations.

Fission neutron anisotropy, due to the kinematics of the fission process, has been studied for non-multiplying sources and highly multiplying subcritical plutonium metal assemblies (i.e. relatively long fission chains). The studies on highly multiplying assemblies show that the observed neutron–neutron angular distribution appear isotropic, while the studies on non-multiplying sources show that the neutron–neutronangular distribution appear anisotropic. No measured data exists, however, that investigates the dependence of neutron anisotropy on multiplication for low-multiplying assemblies. We have experimentally characterized the dependence of fission neutron anisotropy on multiplication for low-multiplying plutonium metal assemblies. Here, an array of 16 organic scintillators was used to measure plutonium metal assemblies (95% 239 Pu, by mass) exhibiting a leakage multiplication of 1.0722(3) to 1.6006(4). Full neutron–neutron angular distributions were measured, and the fission neutron anisotropy was quantified with the ratio of neutron–neutron coincidences observed at 180°and 90°. The results show that the neutron–neutron angular distribution becomes more isotropic as the multiplication increases. Additionally, energy–angle correlations were also characterized showing that the angular distributions are more anisotropic when observing neutrons of higher energy.

The light output, time resolution, pulse shape discrimination (PSD), neutron light output, and interaction position reconstruction of melt-cast small-molecule organic glass bar scintillators were measured. The trans-stilbene organic scintillator detects fast neutrons and gamma rays with high efficiency and exhibits excellent PSD, but the manufacturing process is slow and expensive and its light output in response to neutrons is anisotropic. Small-molecule organic glass bars offer an easy-to-implement and cost-effective solution to these problems. These properties were characterized to evaluate the efficacy of constructing a compact, low-voltage neutron and gamma-ray imaging system using organic glass bars coupled to silicon photomultiplier arrays. A complete facility for melt-casting organic glass scintillators was setup at the University of Michigan. 6 × 6 × 50 mm3glass bars were produced and the properties listed above were characterized. The first neutron image using organic glass was produced in simple backprojection.

Effective detection and characterization of special nuclear materials (SNMs) require state-of-the-art detectors and classification methods. The stilbene organic scintillator is an emerging radiation detector with the ability to simultaneously detect photons and neutrons. Dual-particle sensitivity presents a challenge in photon-induced active interrogation, where the photon flux is significantly higher than the neutron flux. Accurately detecting neutrons with minimum misclassification is crucial in these intense photon environments when looking for SNM, and the desired accuracy cannot be easily achieved using traditional charge integration (CI) methods. To address this need, an artificial neural network (ANN) system is developed to identify photon, neutron, and piled-up pulses; where possible, the piled-up pulses are recovered and classified accordingly. The developed ANN system is tested on time-of-flight (TOF) data collected at a variety of photomultiplier tube (PMT) gain settings. Across all gain settings, the ANN system produced similar classifications as the traditional CI method. The ANN performance is then evaluated in the presence of an intense photon field from a 9 MeV linear accelerator (linac). A 252Cf spontaneous fission source is measured in the presence of an intense photon environment. The ANN system demonstrated its robustness in an intense photon field by estimating the true particle count rates. However, the traditional CI method vastly overestimated neutron count rates in such intense photon field due to misclassification of pile-ups as neutrons.

This work details an optimization process for incorporating inorganic scintillators into a stilbene-based handheld dual particle imager (H2DPI). A prototype H2DPI composed of eight stilbene pillars with dimensions of 6 x 6 x 50.5 mm3 coupled to silicon photomultipliers has been built and is capable of imaging both neutrons and gamma rays emitted by special nuclear material. Gamma-ray imaging with the prototype was performed using an approximate Compton imaging method due to lack of photoelectric absorption of gamma rays in stilbene. Incorporation of inorganic scintillators significantly increases the probability of photoelectric absorption, allowing for Compton imaging. Simulations were made for several geometries where the placement of CeBr3 scintillators was varied to analyze how the system geometry impacts the image quality of simulated measurements. These were compared to a step function using a structural similarity index to determine which system geometry produced the optimal images. It was found that placing the CeBr3 scintillators in the corners of the system produced the best gamma-ray images while maintaining high neutron double-scatter efficiency.

Radioxenon detection is an important component of the verification regime for the Comprehensive Nuclear-Test-Ban Treaty. We developed and validated a new model in MCNPX-PoliMi to simulate the decay of various radioxenon isotopes and the detector response of a variety of detector types. The model was validated using calibration data from a plastic and NaI(Tl) beta–gamma coincidence detector and the results are presented. The results of this validation show that this model can also be used as a tool to produce training spectra and as a method to calibrate radioxenon detection systems.

An algorithm was developed to improve the quantification of metastable isotopes in the presence of 133Xe. Radioxenon emissions are commonly used to monitor for nuclear explosions. When 133Xe is present in these samples it causes interference in the activity calculation of the metastable isotopes. The alternative analysis method analyzes the anticoincidence spectrum of the plastic detector to decrease interference from 133Xe. Simulation results show that the anticoincidence analysis accurately quantifies the activity of 131mXe. For the data analyzed here, the anticoincidence method identifies 83% more samples above the minimum detectable activity than the traditional method.

We present the first measurements of energy-dependent light output from carbon recoils in the liquid organic scintillator EJ-309. For this measurement, neutrons were produced by an associated particle deuterium–tritium generator and scattered by a volume of EJ-309 scintillator into stop detectors positioned at four fixed angles. Carbon recoils in the scintillator were isolated using triple coincidence among the associated particle detector , scatter detector, and stop detectors. The kinematics of elastic and inelastic scatter allowed data collection at eight specific carbon recoil energies between 2.86 and 3.95 MeV. We found the light output caused by carbon recoils in this energy range to be approximately 1.14% of that caused by electrons of the same energy, which is comparable to the values reported for other liquid organic scintillators. A comparison of the number of scattered neutrons at each angle to a Monte Carlo N-Particle eXtended simulation indicates that the ENDF/B-VII.1 evaluation of differential cross sections for 14.1 MeV neutrons on carbon has discrepancies with the experiment as large as 55%, whereas those reported in the JENDL-4.0u evaluation agree with experiment.

Organic glass scintillator (OGS) bars (6 × 6 × 50 mm 3 ) were melt-cast and characterized with dual-ended readout by silicon photomultiplier arrays. The results were compared to trans-stilbene bars of the same size. Energy resolution was measured via a 137Cs Compton-coincidence experiment. Time resolution was determined via a 22Na coincidence-timing experiment. Depth-of-interaction resolution was measured by moving a gamma-ray fan beam along the major axis of the bars. Pulse shape discrimination capability and neutron light output were determined via a time-of-flight measurement of a 252Cf source. The OGS bars exhibited better energy resolution at 478 keV ( 10 . 3 ± 0 . 5 % vs. 11 . 2 ± 0 . 5 %), better time resolution from 200–341 keVee ( 270 ps vs. 340 ps FWHM), slightly poorer depth-of-interaction resolution, poorer PSD performance, and higher neutron light output than the stilbene bars. The low cost, ease of manufacturing, brightness, and excellent time resolution make OGS a strong candidate for use in compact radiation imaging systems.

This manuscript details measurements of the anisotropic light-output response of trans-stilbene, henceforth referred to as stilbene, along the three primary crystal planes and analyzes how this anisotropic response impacts neutron image reconstruction in a handheld dual particle imager (H2DPI). A prototype H2DPI composed of stilbene pillars ( 6 × 6 × 50 mm 3 ) coupled to silicon photomultipliers was built and is capable of imaging both fast neutrons and gamma rays from kilogram quantities of special nuclear material. Stilbene was chosen as the scintillating medium for the imager because of its pulse shape discrimination capability, time resolution and relatively high light output. A drawback to using stilbene, however, is the anisotropic response. A recoiling proton from a neutron elastic-scattering event in stilbene will yield different amounts of scintillation light depending on the direction of the recoiling proton with respect to the crystal lattice. This manuscript analyzes how this anisotropic response impacts neutron image reconstruction in 4 π . The light output in the three primary crystal planes of stilbene were independently measured 6–7 times for proton recoil energies ranging from 0.5–5.0 MeV using a quasi-monoenergetic time-of-flight neutron source. The measured light-output data in the three crystal planes were fit with a semi-empirical function based on Birks’ formula. These fits were used to reconstruct the location of a 252Cf source in front of the imager (0°, −0.8°), to the left of the imager (−90°, −0.8°) and directly above the imager (0°, 90°) to determine if it is necessary to apply the directionally-dependent response of stilbene to accurately reconstruct source locations. A bootstrapping technique was applied to the measured data sets to produce 1000 images composed of 2000 cone projections for each source location and each measured light-output curve. List-mode maximum likelihood expectation maximization was applied to each image; the highest pixel location and the full width at half maximum (FWHM) were then recorded. The average and standard deviations of these parameters were taken for each set of images. The maximum difference in the average azimuthal pixel location when varying between the appropriate and incorrect light-output curves for the source locations at (0°, −0.8°) and (−90°, −0.8°) were respectively found to be 1 . 85 ± 1 . 3 9 ° and 2 . 03 ± 1 . 7 8 ° . All other pixel locations and FWHMs were within a single standard deviation of uncertainty. Taken together, the anisotropic response of stilbene has negligible impact on the neutron image reconstruction capability of the H2DPI.

The Feynman-alpha method is a neutron noise technique that is used to estimate the prompt neutron period of fissile assemblies. The method and quantity are of widespread interest including in applications such as nuclear criticality safety, safeguards and nonproliferation, and stockpile stewardship; the prompt neutron period may also be used to infer the k eff multiplication factor. The Feynman-alpha method is predicated on time-correlated neutron detections that deviate from a Poisson random variable due to multiplication. Traditionally, such measurements are diagnosed with one-region point kinetics, but two-region models are required when the fissile assembly is reflected. This paper presents a derivation of the two-region point kinetics Feynman-alpha equations based on a double integration of the Rossi-alpha equations, develops novel propagation of measurement uncertainty, and validates the theory. Validation is achieved with organic scintillator measurements of weapons-grade plutonium reflected by various amounts of copper to achieve k eff values of 0.83–0.94 and prompt periods of 5–75 ns. The results demonstrate that Feynman-alpha measurements should use the two-region model instead of the one-region model. The simplified one-region model deviates from the validated two-region models by as much as 10% in the estimate of the prompt neutron period, and the two-region model reduces to the one-region model for small amounts of reflector. The Feynman-alpha estimates of the prompt neutron period are compared to those of the Rossi-alpha approach. The comparative results demonstrate that the Feynman-alpha method is more precise than the Rossi-alpha method and more accurate for k eff 0.92 , whereas the Rossi-alpha method is generally more accurate for higher multiplications. The uncertainty propagation developed in this work should be used for all Feynman-alpha measurements and will therein improve fitting accuracy and appropriate precision estimates.

Characterization of special nuclear material may be performed using energy spectroscopy of either the neutron or gamma-ray emissions from the sample. Gamma-ray spectroscopy can be performed relatively easily using high-resolution semiconductors such as high-purity germanium. Neutron spectroscopy, by contrast, is a complex inverse problem. Here, results are presented for 252 Cf and PuBe energy spectra unfolded using a single EJ309 organic scintillator; excellent agreement is observed with the reference spectra. Neutron energy spectroscopy is also possible using a two-plane detector array, whereby time-of-flight kinematics can be used. With this system, energy spectra can also be obtained as a function of position. Spatial-dependent energy spectra are presented for neutron and gamma-ray sources that are in excellent agreement with expectations.

Neutron multiplicity counting (NMC) techniques are widely used for nuclear materials accountability and international safeguards applications to quantitatively evaluate characteristic properties pertaining to fissile material. Mathematical models for NMC moments have been previously derived for systems that use capture-based detectors; however, these models are not applicable when scatter-based detectors are used because of "neutron cross talk." Neutron cross talk occurs when a single neutron scatters and deposits energy above threshold into multiple detectors causing spurious increase in multiplicity counts; this, in turn, has caused fissile mass to be overestimated when not treated. In this paper, we propose new mathematical models derived from point kinetics to correct for neutron cross-talk effects up to any arbitrary order N, where N denotes the maximum number of counts a single neutron can cause. The new models were used to estimate the fissile mass of plutonium metal and oxide samples with effective 240Pu mass ranging from 2.5 to 250 g. The adequacy of the models was confirmed using simulations of a conceptual scatter-based neutron multiplicity counter (e.g., organic scintillators) using MCNPX v2.7e with the PoliMi fission event generating extension. The fissile mass estimates with no correction for neutron cross-talk events yielded an average relative deviation from the true 240Pueff mass of 55.94% and 84.56% for metal and oxide samples, respectively. When neutron cross-talk events of order N = 2 are included in the model, the fissile mass estimates yielded an average relative deviation of 11.89% for metal and 13.21% for oxide samples. Accounting for neutron cross-talk events of order N = 3 resulted in fissile mass estimates with an average relative deviation of 9.58% and 10.51% for metal and oxide samples, respectively. These mass estimates were compared to a reference case (i.e., no neutron crosstalk effects) that yielded an average relative deviation of 6.81% and 4.77% for metal and oxide samples, respectively. The discrepancy between the estimates from the proposed model and the reference case is attributed to the assumed value of N, which sets a finite upper bound on the order of cross-talk events the model treats (i.e., the model for N = 3 assumes that a neutron will never cause more than three counts).

We developed a fast-neutron multiplicity counter based on organic scintillators (EJ-309 liquid and stilbene). The system detects correlated photon and neutron multiplets emitted by fission reactions, within a gate time of tens of nanoseconds. The system was used at Idaho National Laboratory to assay a variety of plutonium metal plates. A coincidence counting strategy was used to quantify the 240Pu effective mass of the samples. Coincident neutrons, detected within a 40-ns coincidence window, show a monotonic trend, increasing with the 240Pu-effective mass (in this work, we tested the 0.005–0.5 kg range). After calibration, the system estimated the 240Pu effective mass of an unknown sample (240Pueff >50 g) with an uncertainty lower than 1% in a 4-min assay time.

An accurate model of the nonlinear detector response of organic scintillators to neutrons is required to correctly simulate fast neutron detection, as well as interpret measured pulse height data. Several empirical and semi-empirical models are available to fit measured scintillator light output data. In this work, EJ-309 light output data from neutrons depositing 1.15–5.15 MeV on hydrogen were analyzed using empirical models as well as semi-empirical models based on the work of Birks and Voltz. Although all tested models fit the experimental light output data well in the measured range, the models were observed to diverge in low-energy extrapolation. The models were then tested by comparing a measurement and MCNPX-PoliMi simulation of an EJ-309 detector response to fast neutrons from a 252 Cf spontaneous fission source. The agreement between the measured and simulated pulse height distributions varied significantly depending on the light output model used. The best agreement between simulated and measured neutron pulse height distributions was achieved by using the Birks model. The bin-by-bin agreement was better than 5% over the range 0.08–2.18 MeVee, and better than 10% from 2.18 to 3.13 MeVee. The integral count rate over the range 0.08–3.14 MeVee differed by less than 1% in absolute units.

In this work we present a technique for isolating the gamma-ray and neutron energy spectra from multiple radioactive sources localized in an image. Image reconstruction algorithms for radiation scatter cameras typically focus on improving image quality. However, with scatter cameras being developed for non-proliferation applications, there is a need for not only source localization but also source identification. This work outlines a modified stochastic origin ensembles algorithm that provides localized spectra for all pixels in the image. We demonstrated the technique by performing three experiments with a dual-particle imager that measured various gamma-ray and neutron sources simultaneously. We showed that we could isolate the peaks from 22 Na and 137 Cs and that the energy resolution is maintained in the isolated spectra. To evaluate the spectral isolation of neutrons, a 252 Cf source and a PuBe source were measured simultaneously and the reconstruction showed that the isolated PuBe spectrum had a higher average energy and a greater fraction of neutrons at higher energies than the 252 Cf. Finally, spectrum isolation was used for an experiment with weapons grade plutonium, 252 Cf, and AmBe. The resulting neutron and gamma-ray spectra showed the expected characteristics that could then be used to identify the sources.

In recent years, solution grown trans-stilbene crystals have become widely used for gamma ray and fast neutron detection in many applications, including nuclear safeguards and nonproliferation. These crystals exhibit excellent pulse shape discrimination (PSD), enabling simultaneous detection and identification of gamma rays and fast neutrons. Stilbene crystals have been made widely available in 5 cm by 5 cm cylinders by Inrad Optics; production of cylinders up to 10 cm long have been demonstrated. Time-of-flight experiments using a 252Cf source have been performed to characterize 5 cm diameter stilbene crystals with 2.5 cm, 5 cm, 7.6 cm, and 10 cm lengths: all four crystals were coupled to photomultiplier tubes and symmetrically placed around the source, 1 m away. These data have been analyzed to obtain detector response functions (scintillation light output as a function of neutron energy deposited) for each of the four crystals. These functions can be used in Monte Carlo simulations to model the absolute detector response. Results will compare the performance of these stilbene cylinders as a function of length using the following quantities: neutron detection efficiency, gamma-ray detection efficiency, PSD figure of merit, and the total detector response function. Additionally, the measured detector response will be compared to Monte Carlo simulations using the MCNPX-PoliMi code.

A prototype handheld dual particle imager composed of stilbene bars coupled to silicon photomultipliers was used to measure a 4.5 kg sphere of alpha-phase weapons-grade plutonium and a canister containing 3.4 kg of plutonium oxide (7% 240P u and 93% 239P u). Each object was measured independently and both objects were measured in the same field of view separated by 50 cm. Experimental results of the measurements conducted are presented. These results demonstrate the ability of the handheld dual particle imager to image and obtain neutron spectroscopic information for sources that would be of great interest for nuclear safeguards and emergency response applications.

Nuclear safeguards applications require accurate fission models that exhibit prompt neutron anisotropy. In the laboratory reference frame, an anisotropic neutron angular distribution is observed because prompt fission neutrons carry momentum from fully accelerated fission fragments. A liquid organic scintillation detector array was used with pulse shape discrimination techniques to produce neutron-neutron cross-correlation time distributions and angular distributions from spontaneous fission in a 252 Cf, a 0.84 g 240 Pu eff metal, and a 1.63 g 240 Pu eff metal sample. The effect of cross-talk, estimated with MCNPX-PoliMi simulations, is removed from neutron-neutron coincidences as a function of the angle between detector pairs. Fewer coincidences were observed at detector angles near 90°, relative to higher and lower detector angles. As light output threshold increases, the observed anisotropy increases due to spectral effects arising from fission fragment momentum transfer to emitted neutrons. Stronger anisotropy was observed in Cf-252 spontaneous fission prompt neutrons than in Pu-240 neutrons.

We have developed and tested a radiation portal monitor using organic liquid scintillation detectors. In order to optimize our system designs, neutron measurements were carried out with three organic liquid scintillation detectors of different shapes and sizes, along with a 3 He radiation portal monitor (RPM) as a reference. The three liquids tested were a 7.62 cm diameter by 7.62 cm length cylindrical active volume organic liquid scintillation detector, a 12.7 cm diameter by 12.7 cm length cylindrical active volume organic liquid scintillation detector, and a 25 cm by 25 cm by 10 cm “paddle” shaped organic liquid scintillation detector. Background and Cf-252 neutron measurements were recorded to allow for a comparison of neutron intrinsic efficiencies as well as receiver operating characteristics (ROC) curves between detectors. The 12.7 cm diameter cylindrical active volume organic liquid scintillation detector exhibited the highest intrinsic neutron efficiency (54%) of all three liquid scintillators. An ROC curve analysis for a heavily moderated Cf-252 measurement showed that using the 12.7 cm diameter by 12.7 cm length cylindrical active volume Eljen EJ309 organic liquid scintillation detector would result in the fewest needed detector units in order to achieve a near 100% positive neutron alarm rate while maintaining a better than 1 in 10,000 false alarm rate on natural neutron background. A small number of organic liquid scintillation detectors could therefore be a valid alternative to 3 He in some RPM applications.

A solution-based technique for growing large-volume stilbene scintillators was developed in 2013; crystals up to diameters of 10 cm, or larger, have been grown while preserving excellent pulse shape discrimination (PSD) properties. The goal of this study is to evaluate the PSD capabilities of 5.08 by 5.08-cm stilbene crystals grown by Lawrence Livermore National Laboratory and Inrad Optics when exposed to a 1000 to 1 gamma ray-neutron ratio and operating at a 100-kHz count rate. Results were compared to an equivalent EJ-309 liquid scintillation detector. 252 Cf neutron pulses were recorded in two experiments where 60 Co and 137 Cs sources created the high-gamma field. The high count rate created numerous double pulses that were cleaned using fractional and template approaches designed to remove double pulses while preserving neutron counts. PSD was performed at a threshold of 42 keVee (440-keV proton) for stilbene and 60 keVee (610-keV proton) for EJ-309 liquid. The lower threshold in stilbene resulted in a neutron intrinsic efficiency of approximately 14.5%, 10% higher than EJ-309 liquid, for bare 252 Cf and 13% for 252 Cf in the high-gamma field. Despite the lower threshold, the gamma misclassification rate in stilbene was approximately 3×10 −6 , nearly a factor-of-five lower than what we found with the EJ-309 liquid.

We report the results of experimental and numerical-simulation studies of shielded radiography using narrowband MeV-energy X-rays from a compact all-laser-driven inverse-Compton-scattering X-ray light source. This recently developed X-ray light source is based on a laser-wakefield accelerator with ultra-high-field gradient (GeV/cm). We demonstrate experimentally high-quality radiographic imaging (image contrast of 0.4 and signal-to-noise ratio of 2:1) of a target composed of 8-mm thick depleted uranium shielded by 80-mm thick steel, using a 6-MeV X-ray beam with a spread of 45% (FWHM) and 107 photons in a single shot. The corresponding dose of the X-ray pulse measured in front of the target is ∼100 nGy/pulse. Simulations performed using the Monte-Carlo code MCNPX accurately reproduce the experimental results. These simulations also demonstrate that the narrow bandwidth of the Compton X-ray source operating at 6 and 9 MeV leads to a reduction of deposited dose as compared to broadband bremsstrahlung sources with the same end-point energy. The X-ray beam’s inherently low-divergence angle (∼mrad) is advantageous and effective for interrogation at standoff distance. These results demonstrate significant benefits of all-laser driven Compton X-rays for shielded radiography.

Rossi-alpha neutron experiments are used to estimate the prompt neutron decay constant of a fissile assembly, a quantity of widespread interest in applications including in nuclear nonproliferation and criticality safety. This work develops a mathematical model to efficiently estimate measurement uncertainty of Rossi-alpha neutron experiments inferred from a two-exponential fit model with histogram binning. The derived uncertainty estimates were validated using repeated Rossi-alpha measurements of a subcritical, 4.5-kg sphere of weapons-grade, alpha-phase plutonium with nickel, copper, tungsten, and polyethylene reflectors. The estimates of uncertainty for the histogram data produced by the model were conservative and agree with the reference uncertainties within noise. The estimates of the prompt neutron decay constant uncertainty agreed with the reference uncertainties within one standard deviation. The proposed model will reduce total measurement times, ultimately reducing operational and procedural costs in application.

Excited nuclear fragments are emitted during nuclear fission. The de-excitation of these fission fragments takes place as sequential emission of neutrons followed by photons. Correlations between neutron and photon multiplicities accompanying fission is thus expected. Fission event generators based on established statistical nuclear physics models predict negative event-by-event correlations in neutron–photon multiplicity. A survey of published experimental results of an event-by-event covariance between the neutron and photon multiplicities emitted following the spontaneous fission of 252Cf is presented. Analytic unfolding expressions are developed in this work to determine the bias introduced by background sources, particle misclassification, pulse pileup, and inelastic photon production. The published experimental data are re-analyzed using these unfolding techniques and are found to be in qualitative agreement with the predictions of model-based calculations. In particular, we have concluded that there exists a significant event-by-event neutron–photon emission competition following the spontaneous fission of 252Cf.

The reactivity and the k-effective multiplication factor ( k eff ) of a fissionable assembly are quantities of widespread interest. These values can be inferred from Rossi-alpha measurements of the prompt neutron decay constant (or the inverse: α − 1 ). It has been shown that 3 He-gas proportional counter-based detection systems are insensitive to α − 1 of fast assemblies (much faster than tens of microseconds). Therefore, it is of interest to investigate fast detection systems such as those based on organic scintillation detectors. In this work, an array of 12 cylindrical, 5.08 cm × 5.08 cm diameter trans-stilbene organic scintillators was used to measure five subcritical assemblies. One assembly was a sphere of approximately 4.5 kg of alpha-phase, weapons-grade plutonium ( k eff = 0 . 773 , α − 1 = 11 . 84 ns ) known as the BeRP ball encased in a thin stainless-steel clad. The other assemblies used the same encased sphere and 7.62 cm of iron, nickel, copper, or tungsten reflectors ( k eff = 0 . 884 , 0 . 916 , 0 . 924 , 0 . 939 , respectively and α − 1 = 36 . 60 , 41 . 56 , 49 . 60 , 70 . 32 ns , respectively). This work (1) validates Rossi-alpha measurements with organic scintillators by demonstrating good agreement between measurements and simulations; and (2), demonstrates that organic scintillator-based systems are sensitive to α − 1 on the order of 10–100 ns.

Safeguarding the contents of spent nuclear fuel dry storage casks requires the verification of cask contents, especially if continuity of knowledge has been lost. The high attenuation of the cask’s thick shielding and stored fuel assemblies makes verification difficult using conventional photon radiography. Thomson-scattering quasi-monoenergetic photon sources offer narrow angular and energy spread for increased penetration. This paper demonstrates the advantages of such a source by examining effects of source properties on transmission through thick, highly attenuating objects. This information is then applied to calculations and simulations of transmission for a variety of photon sources and cask configurations. The performance of the source is compared to traditional bremsstrahlung sources and other advanced methods, in the context of typical nuclear fuel dry storage casks. It is shown that the use of a Thomson scattering based quasi-monoenergetic photon source enables determination of fuel assembly occupancies faster and more accurately than other methods.

Traditionally, capture-based neutron multiplicity counters (i.e. He-3 based systems) are used for non-destructive assay of special nuclear material. Using capture-based detectors for non-destructive assay requires intervening moderating material that inhibits the ability to observe characteristic energy and angular signatures. Therefore, these systems rely on observing only the emitted neutron multiplicity to infer physical properties such as fissile mass, leakage multiplication, and contribution from non-fission neutrons (α-ratio). We have developed a fast neutron multiplicity counter using 24 – 5.08 cm x 5.08 cm stilbene detectors coupled to ETL 9214B photomultiplier tubes, and demonstrate that the system is sensitive to the emitted neutron energy and angular distributions, in addition to the multiplicity distribution. The system was used for passive assay of Pu-metal and Pu-oxide samples, and the detected neutron multiplicity, energy, and angular distributions are used to demonstrate that new correlated signatures exist related to the physical properties of the item. We also demonstrate the neutron cross-talk effects can be considered in order to yield more accurate estimates of the aforementioned physical properties. The final paper will present correlated signatures in energy, angle, and multiplicity that can potentially provide new quantities for characterizing special nuclear material when traditional techniques become unreliable.

The detection and characterization of highly enriched uranium (HEU) presents a large challenge in the non-proliferation field. HEU has a low neutron emission rate and most gamma rays are low energy and easily shielded. To address this challenge, an instrument known as the dual-particle imager (DPI) was used with a portable deuterium-tritium (DT) neutron generator to detect neutrons and gamma rays from induced fission in HEU. We evaluated system response using a 13.7-kg HEU sphere in several configurations with no moderation, high-density polyethylene (HDPE) moderation, and tungsten moderation. A hollow tungsten sphere was interrogated to evaluate the response to a possible hoax item. First, localization capabilities were demonstrated by reconstructing neutron and gamma-ray images. Once localized, additional properties such as fast neutron energy spectra and time-dependent neutron count rates were attributed to the items. For the interrogated configurations containing HEU, the reconstructed neutron spectra resembled Watt spectra, which gave confidence that the interrogated items were undergoing induced fission. The time-dependent neutron count rate was also compared for each configuration and shown to be dependent on the neutron multiplication of the item. This result showed that the DPI is a viable tool for localizing and confirming fissile mass and multiplication.

Accurate and timely characterization of physical properties pertinent to plutonium bearing materials is important for fulfilling nuclear nonproliferation and safeguards goals. Physical properties include the fissile mass, leakage multiplication, and the α -ratio, defined as the ratio of ( α ,n) neutrons to spontaneous fission neutrons. Traditionally, these properties can be inferred by relating the measured neutron multiplicity count rates to the well-established point kinetics moments equations; the current state-of-the-art utilizes 3 He-based detection systems. Organic scintillators have been used extensively to study and measure characteristic signatures in the neutron angular and energy distributions. Previous work has proposed techniques that independently leverage the energy and angle sensitivity of organic scintillators to estimate the α -ratio of plutonium bearing material; however, it is expected that the energy and angular distributions are correlated to one another due to the underlying physics of fission and ( α ,n) neutron emissions. This work presents experimental results that characterize neutron-neutron angular distribution and subsequently the neutron-neutron energy-angle correlations for plutonium samples of similar mass and multiplication, but varying α -ratio due to the type of low-Z impurity. Full neutron-neutron angular distributions are presented using a low-energy detection threshold of 0.10, 0.15, and 0.20 MeVee (0.73, 0.96, 1.16 MeV neutron-equivalent energy). Neutron anisotropy was quantified by taking the ratio of neutron-neutron coincidences at 180°to those at 90°, where a value of unity indicates a purely isotropic source. The results show that the observed neutron-neutron correlations transition away from fission-induced signal to the cross-talk signal associated with single ( α ,n) neutrons with increasing α -ratio. Energy-angle correlations are characterized by calculating the neutron anisotropy at various detection thresholds and show positive correlation between the observed anisotropy and the energy of the neutrons.

A dual-particle imaging (DPI) system, capable of simultaneously imaging fast neutrons and gamma rays, has been operated in the presence of mixed-oxide (MOX) fuel to assess the system׳s angular resolution and material-characterization capabilities. The detection principle is based on the scattering physics of neutrons (elastic scattering) and gamma rays (Compton scattering) in organic and inorganic scintillators. The detection system is designed as a combination of a two-plane Compton camera and a neutron-scatter camera. The front plane consists of EJ-309 liquid scintillators and the back plane consists of interleaved EJ-309 and NaI(Tl) scintillators. MCNPX-PoliMi was used to optimize the geometry of the system and the resulting prototype was built and tested using a Cf-252 source as an SNM surrogate. A software package was developed to acquire and process data in real time. The software was used for a measurement campaign to assess the angular resolution of the imaging system with MOX samples. Measurements of two MOX canisters of similar isotopics and intensity were performed for 6 different canister separations (from 5° to 30°, corresponding to distances of 21 cm and 131 cm, respectively). The measurements yielded a minimum separation of 20° at 2.5 m (86-cm separation) required to see 2 separate hot spots. Additionally, the results displayed good agreement with MCNPX-PoliMi simulations. These results indicate an angular resolution between 15° and 20°, given the 5° step. Coupled with its large field of view, and its capability to differentiate between spontaneous fission and (α,n) sources, the DPI system shows its potential for nuclear-nonproliferation applications.