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Stochastic analog neutron transport with TRIPOLI-4 and FREYA: Bayesian uncertainty quantification for neutron multiplicity counting

From nuclear safeguards to homeland security applications, the need for the better modeling of nuclear interactions has grown over the past decades. Current Monte Carlo radiation transport codes compute average quantities with great accuracy and performance; however, performance and averaging come at the price of limited interaction-by-interaction modeling. These codes often lack the capability of modeling interactions exactly: for a given collision, energy is not conserved, energies of emitted particles are uncorrelated, and multiplicities of prompt fission neutrons and photons are uncorrelated. Many modern applications require more exclusive quantities than averages, such as the fluctuations in certain observables (e.g., the neutron multiplicity) and correlations between neutrons and photons. In an effort to meet this need, the radiation transport Monte Carlo code TRIPOLI-4® was modified to provide a specific mode that models nuclear interactions in a full analog way, replicating as much as possible the underlying physical process. Furthermore, the computational model FREYA (Fission Reaction Event Yield Algorithm) was coupled with TRIPOLI-4 to model complete fission events. As a result, FREYA automatically includes fluctuations as well as correlations resulting from conservation of energy and momentum.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterizing Shielded Special Nuclear Material by Neutron Capture Gamma-Ray Multiplicity Counting

We present a new neutron multiplicity counting analysis and measurement method for neutron-shielded fissile material using neutron-capture gamma rays. Neutrons absorbed in shielding produce characteristic gamma rays that preserve the otherwise lost neutron multiplicity signature. Neutron multiplicity counting provides estimates of fission parameters, such as neutron leakage multiplication, spontaneous fissioner (e.g. Pu-240) mass, and (α,n) ratio. Standard neutron multiplicity counting can incorporate the new neutron-capture gamma-ray multiplicity counting technique to characterize previously degenerate or intractable source configurations by maximizing the multiplicity signature. The new method decouples neutron source-detector interferences, such as reflection and thermalization time in the detector, that could improve measurements of the mean neutron lifetime. We also develop a detector prototype for the multiplicity counting of neutron-capture gamma rays and present detector design considerations, such as detection material and shielding, to optimize the detection of the 2.2 MeV hydrogen capture gamma ray. We simulate the prototype neutron- capture gamma-ray multiplicity counter against the BeRP ball in polyethylene shells to inform future measurements.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Neutron multiplicity ,easurements With 3 He alternative: Straw neutron detectors

Counting neutrons emitted by special nuclear material (SNM) and differentiating them from the background neutrons of various origins is the most effective passive means of detecting SNM. Unfortunately, neutron detection, counting, and partitioning in a maritime environment are complex due to the presence of high-multiplicity spallation neutrons (commonly known as “ship effect”) and to the complicated nature of the neutron scattering in that environment. In this study, a prototype neutron detector was built using 10 B as the converter in a special form factor called “straws” that would address the above problems by looking into the details of multiplicity distributions of neutrons originating from a fissioning source. This paper describes the straw neutron multiplicity counter (NMC) and assesses the performance with those of a commercially available fission meter. The prototype straw neutron detector provides a large-area, efficient, lightweight, more granular (than fission meter) neutron-responsive detection surface (to facilitate imaging) to enhance the ease of application of fission meters. Presented here are the results of preliminary investigations, modeling, and engineering considerations leading to the construction of this prototype. This design is capable of multiplicity and Feynman variance measurements. This prototype may lead to a near-term solution to the crisis that has arisen from the global scarcity of 3 He by offering a viable alternative to fission meters. This paper describes the work performed during a 2-year site-directed research and development (SDRD) project that incorporated straw detectors for neutron multiplicity counting. The NMC is a two-panel detector system. We used 10 B (in the form of enriched boron carbide: 10 B 4 C) for neutron detection instead of 3 He. In the first year, the project worked with a panel of straw neutron detectors, investigated its characteristics, and developed a data acquisition (DAQ) system to collect neutron multiplicity information from spontaneous fission sources using a single panel consisting of 60 straws equally distributed over three rows in high-density polyethylene moderator. In the following year, we developed the field-programmable gate array and associated DAQ software. Finally, this SDRD effort successfully produced a prototype NMC with ~33% detection efficiency compared to a commercial fission meter.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Validation of the Fast-Neutron Multiplicity Expressions for Fissile Mass Estimation

Neutron multiplicity analysis is a non-destructive assay technique that involves measurement of the multiplets of neutrons that are emitted from fission of fissile material. Typically, multiplicity analysis is conducted by means of a neutron multiplicity counting (NMC) system that uses capture-based thermal-neutron detectors (e.g., 3He-gas detectors). To relieve the reliance on such detectors, we have developed a fast-neutron multiplicity counting (FNMC) system that uses scatter-based, organic scintillators to directly detect the fast fission neutrons emitted from the sample. One challenge with FNMC systems, however, is that they are prone to effects of neutron cross-talk, where a single neutron may scatter and cause more than one detection event. This leads to an overestimate of the fission rate (F) and inaccurate estimation of other sample parameters such as the leakage multiplication (M) and the alpha-ratio (a) when using the traditional capture-based NMC equations. We have formulated fully generalized multiplicity expressions that account for cross-talk effects for any arbitrary order N. The validity of these expressions were verified with MCNPX-PoliMi simulations and experimental measurements; this paper will present the validation of the proposed generalized multiplicity expressions. Californium-252 and Pu metal plates were measured using the FNMC system and the data was used for neutron multiplicity analysis to estimate sample parameters F, M, and a. We demonstrate that accounting for neutron cross-talk effects of order N = 2 and 3 improves the accuracy of the estimated sample parameters.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The Impact of Gate Width Setting and Gate Utilization Factors on Plutonium Assay in Passive Correlated Neutron Counting

In the field of nuclear safeguards, passive neutron multiplicity counting (PNMC) is a method typically employed in non-destructive assay (NDA) of special nuclear material (SNM) for nonproliferation, verification and accountability purposes. PNMC is generally performed using a well-type thermal neutron counter and relies on the detection of correlated pairs or higher order multiplets of neutrons emitted by an assayed item. To assay SNM, a set of parameters for a given well-counter is required to link the measured multiplicity rates to the assayed item properties. Detection efficiency, die-away time, gate utilization factors (tightly connected to die-away time) as well as optimum gate width setting are among the key parameters. These parameters along with the underlying model assumptions directly affect the accuracy of the SNM assay. In this paper we examine the role of gate utilization factors and the single exponential die-away time assumption and their impact on the measurements for a range of plutonium materials. In addition, we examine the importance of item-optimized coincidence gate width setting as opposed to using a universal gate width value. Finally, the traditional PNMC based on multiplicity shift register electronics is extended to Feynman-type analysis and application of this approach to Pu mass assay is demonstrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Characterizations of double pulsing in neutron multiplicity and coincidence counting systems

Passive neutron coincidence/multiplicity counters are subject to non-ideal behavior, such as double pulsing and dead time. It has been shown in the past that double-pulsing exhibits a distinct signature in a Rossi-alpha distribution, which is not readily noticed using traditional Multiplicity Shift Register analysis. But, it has been assumed that the use of a pre-delay in shift register analysis removes any effects of double pulsing. Here, we use high-fidelity simulations accompanied by experimental measurements to study the effects of double pulsing on multiplicity rates. By exploiting the information from the double pulsing signature peak observable in the Rossi-alpha distribution, the double pulsing fraction can be determined. Algebraic correction factors for the multiplicity rates in terms of the double pulsing fraction have been developed. We also discuss the role of these corrections across a range of scenarios.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fundamentals of Nondestructive Assay [Slides]

NDA measurements play an important role in managing nuclear material through their ability to detect, identify, locate, and often quantify the composition and/or mass of material within a relatively short amount of time. The three main passive NDA measurement techniques that are utilized in managing nuclear material are (1) Gamma-ray spectroscopy (composition); (2) Neutron Multiplicity counting (fission rate of Pu items); and (3) Calorimetry (heat production from decay of Pu bearing items). Through combination of Gamma-ray spectroscopy and either neutron multiplicity counting or calorimetry, mass of Pu bearing items can be measured.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Gamma and Neutron Measurement and Modeling of Irradiated TRISO Fuel

Given the unique characteristics of the PBR fuel cycle, both gamma and neutron measurements are expected to play important roles in performing and maintaining nuclear material control and accounting for spent pebbles to safeguard the fuel cycle. Given the lack of irradiated pebbles in the US, a variety of irradiated TRISO fuel samples with wide ranges of burnups and cooling times available at ORNL were used in this work. A large number of gamma and neutron measurements have been performed on these samples to collect data to test the various detectors and to benchmark the computer models to simulate the depletion and decay of the fuel and the measurements themselves. Two neutron detectors, including a custom-made detector and the Very High-Performance Neutron Multiplicity Counting, were used to measure the neutrons emitted by these TRISO samples. Three gamma spectrometry detectors, including an HPGe and the M400 CZT detector, were used to measure gamma-ray emissions from these samples. The M400 was recently adopted by the IAEA for fresh uranium measurements, but it was tested for spent fuel measurements prior to this project. Detailed MCNP models were developed to simulate these neutron and gamma measurements. Some GADRAS models were also developed to cross check the MCNP models for the gamma measurements. It was found challenging to perform neutron measurements in the hot cell due to the high background counts. Close agreements were observed between the simulated and measured neutron count rates in both detectors’ measurements of californium calibration sources. Both the HPGe and M400 detectors were able to measure the 604 and 662 keV peaks from these samples, which are the two most important peaks used to infer fuel burnup. Although the M400 detector did not have nearly good energy resolution and did not detect some of the minor peaks as the HPGe detector, it was found to be capable of handling significantly higher dose rates than HPGe. Given the complexities in the TRISO samples (e.g., different samples sizes) and uncertainties in the alignments between the detector and the TRISO fuel inside the containers, large scatters were found between the peak area rates and the samples’ burnups. However, the 604/662 peak ratios were found to trend well with the samples’ burnups among most samples in both measured and simulated results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Implementation and Initial Testing of Advanced Processing and Analysis Algorithms for Correlated Neutron Counting

In order to improve the accuracy and capabilities of neutron multiplicity counting, additional quantifiable information is needed in order to address the assumptions that are present in the point model. Extracting and utilizing higher order moments (Quads and Pents) from the neutron pulse train represents the most direct way of extracting additional information from the measurement data to allow for an improved determination of the physical properties of the item of interest. The extraction of higher order moments from a neutron pulse train required the development of advanced dead time correction algorithms which could correct for dead time effects in all of the measurement moments in a self-consistent manner. In addition, advanced analysis algorithms have been developed to address specific assumptions that are made within the current analysis model, namely that all neutrons are created at a single point within the item of interest, and that all neutrons that are produced within an item are created with the same energy distribution. This report will discuss the current status of implementation and initial testing of the advanced dead time correction and analysis algorithms that have been developed in an attempt to utilize higher order moments to improve the capabilities of correlated neutron measurement techniques.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A Note on the Nomenclature in Neutron Multiplicity Mathematics

The purpose of this technical note is to consolidate the notations used for describing parameters that pertain to neutron multiplicity mathematics relevant to various applications including nonproliferation, international safeguards, and criticality safety among others. The nomenclatures used in these techniques vary widely depending on the origin of the work and their applications. We aim here to consolidate many of the previously used notations in a single document to enhance past, present, and future technical exchanges pertaining to neutron multiplicity. This will help avoid confusion in future publications and will facilitate wider application-independent advancements and utility of peer-reviewed findings. A brief introduction and history of neutron multiplicity counting is presented, followed by a summary of commonly used techniques in a variety of different applications. In each section, we present the notations used in previous publications for the reader’s reference.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Comparison of NMC estimates with trans-stilbene, EJ-309, and He-3 detection systems

Neutron multiplicity counting (NMC) is a technique for the assay of fissile material. In this work, three detection systems are utilized for active interrogation assay of shells of the Rocky Flats shells (highly enriched uranium, 93% 235U) stacked from 13.25-54.92 kg assemblies. The singles ($R_1$) and doubles ($R_2$) rates are calculated with each system to estimate two sample parameters: $M_L$- the leakage multiplication and F - the sample fission rate. The estimated mass, m, is found by dividing F by a constant activity per unit mass. Since we are interrogating HEU, the α ratio of (α; n) to fission neutrons is taken to be zero. The system of equations to calculate these quantities was originally derived. The Neutron Multiplicity 3 He Array Detector (NOMAD) consists of 15 3 He tubes inside polyethylene and is the traditional, capture-based detection system for NMC. The polyethylene moderates incoming neutrons for thermal capture in individual tubes. The low gamma background, discrete capture signals, and high efficiency of the NOMAD are beneficial for NMC. However, the time to slow down neutrons to thermal energies leads to a system die away time on the scale of microseconds. Comparatively, the Rossi-alpha Measurements – Rapid Organic (n, γ) Discrimination Detector (RAMRODD) and the Organic Scintillator Array (OSCAR) are scatter-based detection systems. RAMRODD consists of 8, 5.08 by 5.08 cm EJ-309 liquid scintillators in 4 pairs, evenly-spaced with 90 degrees separation about the center of each assembly. OSCAR consists of a single array of 12, 5.08 by 5.08 cm trans-stilbene crystals aligned with the center of the assembly. Scatter-based systems detect fast neutrons without any moderation, leading to system die away times on the scale of tens of nanoseconds. This allows much shorter timing gate widths compared to thermal systems, thus increasing counting statistics of true correlated fission events. However, scatter-based systems are susceptible to neutron cross-talk when an incident neutron scatters off one detector and interacts in an adjacent detector, causing two seemingly correlated detection signals. The equations developed adjust for cross-talk to conduct NMC with scatter-based systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗