Nuclear Resonance Fluorescence to Measure Plutonium Mass in Spent Nuclear Fuel

The Next Generation Safeguard Initiative (NGSI) of the U.S Department of Energy is supporting a multi-lab/university collaboration to quantify the plutonium (Pu) mass in spent nuclear fuel (SNF) assemblies and to detect the diversion of pins with non-destructive assay (NDA) methods. The following 14 NDA techniques are being studied: Delayed Neutrons, Differential Die-Away, Differential Die-Away Self-Interrogation, Lead Slowing Down Spectrometer, Neutron Multiplicity, Passive Neutron Albedo Reactivity, Total Neutron (Gross Neutron), X-Ray Fluorescence, {sup 252}Cf Interrogation with Prompt Neutron Detection, Delayed Gamma, Nuclear Resonance Fluorescence, Passive Prompt Gamma, Self-integration Neutron Resonance Densitometry, and Neutron Resonance Transmission Analysis. Understanding and maturity of the techniques vary greatly, ranging from decades old, well-understood methods to new approaches. Nuclear Resonance Fluorescence (NRF) is a technique that had not previously been studied for SNF assay or similar applications. Since NRF generates isotope-specific signals, the promise and appeal of the technique lies in its potential to directly measure the amount of a specific isotope in an SNF assay target. The objectives of this study were to design and model suitable NRF measurement methods, to quantify capabilities and corresponding instrumentation requirements, and to evaluate prospects and the potential of NRF for SNF assay. The main challenge of the technique is to achieve the sensitivity and precision, i.e., to accumulate sufficient counting statistics, required for quantifying the mass of Pu isotopes in SNF assemblies. Systematic errors, considered a lesser problem for a direct measurement and only briefly discussed in this report, need to be evaluated for specific instrument designs in the future. Also, since the technical capability of using NRF to measure Pu in SNF has not been established, this report does not directly address issues such as cost, size, development time, nor concerns related to the use of Pu in measurement systems. This report discusses basic NRF measurement concepts, i.e., backscatter and transmission methods, and photon source and {gamma}-ray detector options in Section 2. An analytical model for calculating NRF signal strengths is presented in Section 3 together with enhancements to the MCNPX code and descriptions of modeling techniques that were drawn upon in the following sections. Making extensive use of the model and MCNPX simulations, the capabilities of the backscatter and transmission methods based on bremsstrahlung or quasi-monoenergetic photon sources were analyzed as described in Sections 4 and 5. A recent transmission experiment is reported on in Appendix A. While this experiment was not directly part of this project, its results provide an important reference point for our analytical estimates and MCNPX simulations. Used fuel radioactivity calculations, the enhancements to the MCNPX code, and details of the MCNPX simulations are documented in the other appendices