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Organic-based scintillators are indispensable materials for radiation detection owing to their high sensitivity to fast neutrons, low cost, and tailorable properties. There has been a recent resurgence of interest in organic scintillators due to exciting discoveries related to neutron discrimination and gamma-ray spectroscopy, which represent capabilities previously thought not possible in these materials. I will discuss our development of crystalline and polymer-based scintillators for these applications. Structure-property relationships related to intermolecular interactions and host-guest electronic exchange will be discussed in the context of energy-transfer pathways relevant to scintillation. An emphasis will be placed on the rational design of these materials, as guided by first principles and DFT calculations.
Two related topics will be discussed:
1) Incorporation of organometallic triplet-harvesting additives to plastic scintillator matrices to confer a 'two-state' (singlet and triplet) luminescence signature to different types of ionizing radiation. This approach relies upon energetic and spatial overlap between the donor and acceptor excited states for efficient electronic exchange. Key considerations also include synthetic modification of the luminescence spectra and kinetics, as well as the addition of secondary additives to increase the recombination efficiency.
2) Design of organotin-containing plastic scintillators as a route towards gamma-ray spectroscopy. Organometallic compounds were selected on the basis of distance-dependent quenching relationships, phase compatibility with the polymer matrix, and the gamma-ray cross sections. This approach is guided by molecular modeling and radiation transport modeling to achieve the highest possible detection sensitivity luminescence intensity.
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