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[en] Experiments have been carried out to investigate the feasibility and utility of using neutron interrogation and small-scale, portable prompt gamma-ray neutron activation analysis (PGNAA) instruments for assaying uranium for safeguards applications. Prior work has shown the potential of the PGNAA technique for assaying uranium using reactor-based neutron sources and high-yield electronic neutron generators (ENGs). In this project we adapted Idaho National Laboratory's portable isotopic neutron spectroscopy (PINS) PGNAA system for measuring natural-enrichment uranium yellowcake and metallic depleted uranium and highly enriched uranium. This work used 252Cf as well as deuterium-deuterium (DD) and deuterium-tritium (DT) ENGs. For PGNAA measurements a limiting factor when assaying large objects is the detector dead time due to fast-neutron scattering off of the uranium; this limits the maximum useable neutron source strength to O(107) neutrons per second. Under these conditions the low PGNAA reaction cross sections for uranium prohibited the collection of useful uranium PGNAA signatures from either the yellowcake or metallic uranium samples. Measurement of the decay product activation in these materials following irradiation in the PGNAA geometry similarly did not produce useful uranium activation product - fission product signatures. A customized irradiation geometry tailored to optimally thermalize the interrogation neutron source, intended only for generating long-lived activation products - fission products and not intended for PGNAA measurements, might be possible using small scale ENGs but an application need and a modeling simulation exercise would be recommended before advancing to experiments. Neutron interrogation PGNAA using a DT-ENG was found to be a quick and useful qualitative method for detecting the presence of oxygen in natural-enrichment uranium yellowcake. With a low effort of development work it would be reasonable to expect this measurement could be transitioned to a qualitative technique for assaying oxides as well as other common uranium matrices including nitrides, fluorides, carbides, and sodium-bonded metals. Inert-matrix fuel material confirmation would also be well-served through this technique. This may be of interest for nuclear Material Protection, Accounting, and Control for Transmutation (MPACT) safeguards applications as a method for confirming material-form declarations in advanced fuel cycle material inventories and for quality control during fuel fabrication.