Novel Polymeric Materials for the Additive Manufacturing of Microwave Devices
O'Keefe, Shamus Emmett
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The past decade has seen a rapid increase in the deployment of additive manufacturing (AM) due to the perceived benefits of lower cost, higher quality, and a smaller environmental footprint. And while the hardware behind most of AM processes is mature, the study and development of material feedstock(s) are in their infancy, particularly so for niche areas. In this dissertation, we look at novel polymeric materials to support AM for microwave devices. Chapter 1 provides an overview of the benefits of AM, followed by the specific motivation for this work, and finally a scope defining the core objectives. Chapter 2 delves into a higher-level background of dielectric theory and includes a brief overview of the two common dielectric spectroscopy techniques used in this work. The remaining chapters, summarized below, describe experiments in which novel polymeric materials were developed and their microwave dielectric properties measured. Chapter 3 describes the successful synthesis of polytetrafluroethylene (PTFE)/polyacrylate (PA) core-shell nanoparticles and their measured microwave dielectric properties. PTFE/PA core-shell nanoparticles with spherical morphology were successfully made by aersol deposition followed by a brief annealing. The annealing temperature is closely controlled to exceed the glass transition (Tg) of the PA shell yet not exceed the Tg of the PTFE core. Furthermore, the annealing promotes coalescence amongst the PA shells of neighboring nanoparticles and results in the formation of a contiguous PA matrix that has excellent dispersion of PTFE cores. The measured dielectric properties agree well with theoretical predictions and suggest the potential of this material as a feedstock for AM microwave devices. Chapter 4 delves into the exploration of various polyimide systems with the aim of replacing the PA in the previously studied PTFE/PA core-shell nanoparticles. Fundamental relationships between polymer attributes (flexibility/rigidity and functional groups) and dielectric properties were explored. The results indicate that backbone rigidity and the inclusion of fluorine lead to excellent dielectric properties, however, often at the expense of mechanical properties. Chapter 5 explores the optimization of PTFE core-shell nanoparticles via a novel PTFE/polyimide (PI) core-shell nanoparticle. PTFE/PI core-shell nanoparticles were synthesized via electrostatic interaction between the PTFE cores and a PI precursor, poly(amic) acid salt (PAAS). The PAAS is converted to PI by thermal imidization. The PI has properties superior to those of PA for microwave applications and the results suggest the promise of PTFE/PI core-shell nanoparticles for use in AM of microwave devices. Chapter 6 describes the first report of on actively-tunable microwave substrate made possible by a semiconducting polymer composite blend. The composite blend is comprised of poly(3-hexylthiophene) (P3HT) as the semiconducting polymer and [6,6]-Phenyl C61 butyric acid methyl ester (PCBM) while the remainder of the composite is comprised of a low dielectric constant polymer polydimethylsiloxane (PDMS). When subjected to photo excitation (white light, spectrum centered at 532 nm), the composite exhibits a tunability of the permittivity up to 20%. The results suggest strong promise for the use of semiconducting polymers in actively-tunable microwave devices. Finally, Chapter 7 presents a summary of the salient conclusions of the reported studies. The chapter concludes with a few brief remarks of my personal experience as a non-traditional student and the challenges therein.