<p>This dissertation addresses a key 21st Century Grand Challenge – "Combatting Nuclear Terrorism”. A principal component associated with addressing this challenge pertains to timely and near real-time detection and tracking of small quantities of special nuclear materials (SNMs); the isotopes of uranium (U-235), and Plutonium (Pu) which constitute the key components of nuclear warheads. Such detection and tracking, especially for shielded U-235 using passive means is virtually impossible due to the extremely faint neutron-photon emission signals from radioactive decay which can be readily masked. Active photon and/or neutron interrogation methods are the only viable means for HEU detection but the field suffers from detector saturation in extreme 10⁴ R h^-1 radiation fields. Pu isotopes in multi-kg levels emanate neutrons from spontaneous fission that offer a means for passive interrogation with directionality, even at low levels assuming novel, high-efficiency detectors are available. Both U-235 and Pu isotopes also emit Rn gas (an alpha radiation emitter) at trace levels, during decay - which offers a possible novel means for identifying the presence of SNMs – from the faint multi Bq m^-3(pCi L^-1) alpha emitting gas and progeny in air - if only a real time sensitive enough detector were available. </p> <p> </p> <p>This thesis work was aimed at filling critical technology gaps, via researching and advancing the field of metastable fluid detector (TMFD) technology pertaining to novel/transformational passive and active (photoneutron) interrogation of SNMs. The results of R&D from this dissertation provide evidence for rapidly and conclusively monitoring for the presence of Rn-222 and progeny in air at ultra-trace (pCi L^-1) levels – even below the action levels mandated by the U.S. EPA by the development of protocols for sampling and detection using centrifugally tensioned metastable fluid detectors (CTMFD). </p> <p> </p> <p>For SNM neutron emission (either spontaneous or induced) based active and passive interrogation this dissertation presents evidence for advancing into novel designs, and schemes resulting in 100-1000x enhancements in detection efficiency for the acoustically driven ATMFD architecture in single and array forms. Novel drive modes: a direct (fixed and sweep) resonance mode, and radically novel indirect traveling wave mode were used to expand ATMFD capabilities and efficiencies beyond previous iterations of ATMFD technology. The experimentation work has been coupled with multi-physics theoretical modeling and simulations benchmarked against experimental data. ATMFDs in single and array-based architectures are being investigated for offering a novel, high-efficiency means for passive interrogation of SNMs. Coupled together with the Rn-alpha sensing approach, the ATMFD sensors for neutron monitoring enable a first-of-a-kind transformational dual mode architecture for monitoring both HEU (U-235) and Pu based SNMs.</p> <p> </p> <p>Successful results were also demonstrated for rapid and convincing 9 MeV (end point x-ray) photoneutron based active interrogation of 4.5 kg of depleted uranium in ultra-high gamma background of ~10⁴ R h^-1 using a single CTMFD or ATMFD sensor. Under such intense gamma backgrounds, conventional detectors are known to get saturated and have presented a major challenge. The research from this thesis offers a novel solution for both passive and active SNM interrogation. </p>