Lawrence Berkeley National Laboratory

In nuclear resonance fluorescence (NRF) measurements, resonances are excited by an external photon beam leading to the emission of gamma rays with specific energies that are characteristic of the emitting isotope. NRF promises the unique capability of directly quantifying a specific isotope without the need for unfolding the combined responses of several fissile isotopes as is required in other measurement techniques. We have analyzed the potential of NRF as a non-destructive analysis technique for quantitative measurements of Pu isotopes in spent nuclear fuel (SNF). Given the low concentrations of 239Pu in SNF and its small integrated NRF cross sections, the main challenge in achieving precise and accurate measurements lies in accruing sufficient counting statistics in a reasonable measurement time. Using analytical modeling, and simulations with the radiation transport code MCNPX that has been experimentally tested recently, the backscatter and transmission methods were quantitatively studied for differing photon sources and radiation detector types. Resonant photon count rates and measurement times were estimated for a range of photon source and detection parameters, which were used to determine photon source and gamma-ray detector requirements. The results indicate that systems based on a bremsstrahlung source and present detector technology are not practical for high-precision measurements of 239Pu in SNF. Measurements that achieve the desired uncertainties within hour-long measurements will either require stronger resonances, which may be expressed by other Pu isotopes, or require quasi-monoenergetic photon sources with intensities that are approximately two orders of magnitude higher than those currently being designed or proposed. This work is part of a larger effort sponsored by the Next Generation Safeguards Initiative to develop an integrated instrument, comprised of individual NDA techniques with complementary features, that is fully capable of determining Pu mass in spent fuel assemblies.