POLYMER-NANOPARTICLE COMPOSITES FOR APPLICATIONS IN FLEXIBLE ELECTRONICS

The aim of this dissertation was to investigate flexible polymer-nanoparticle composites with unique magnetic and electrical properties. Toward this goal, two distinct projects were carried out. The first project explored the magneto-dielectric properties and morphology of flexible polymer-nanoparticle composites that possess high permeability (µ), high permittivity (ε) and minimal dielectric, and magnetic loss (tan δε, tan δµ). The main materials challenges were the synthesis of magnetic nanoparticle fillers displaying high saturation magnetization (Ms), limited coercivity, and their homogeneous dispersion in a polymeric matrix. Nanostructured magnetic fillers including polycrystalline iron core-shell nanoparticles, and constructively assembled superparamagnetic iron oxide nanoparticles were synthesized, and dispersed uniformly in an elastomer matrix to minimize conductive losses. The resulting composites have demonstrated promising permittivity (22.3), permeability (3), and sustained low dielectric (0.1), magnetic (0.4) loss for frequencies below 2 GHz. This study demonstrated nanocomposites with tunable magnetic resonance frequency, which can be used to develop compact and flexible radio frequency devices with high efficiency. The second project focused on fundamental research regarding methods for the design of highly conductive polymer-nanoparticle composites that can maintain high electrical conductivity under tensile strain exceeding 100%. We investigated a simple solution spraying method to fabricate stretchable conductors based on elastomeric block copolymer fibers and silver nanoparticles. Silver nanoparticles were assembled both in and around block copolymer fibers forming interconnected dual nanoparticle networks, resulting in both in-fiber conductive pathways and additional conductive pathways on the outer surface of the fibers. Stretchable composites with conductivity values reaching 9000 S/cm maintained 56% of their initial conductivity after 500 cycles at 100% strain. The developed manufacturing method in this research could pave the way towards direct deposition of flexible electronic devices on any shaped substrate. The electrical and electromechanical properties of these dual silver nanoparticle network composites make them promising materials for the future construction of stretchable circuitry for displays, solar cells, antennas, and strain and tactility sensors.

Characterization of Copper Covetic Bulk and Films: Copper with High Carbon Content

Incorporation of carbon nanostructures in metals is desirable to combine the strongly bonded electrons in the metal and the free electrons in carbon nanostructures that give rise to high ampacity and high conductivity, respectively. Carbon in copper has the potential to impact industries such as: building construction, power generation and transmission, and microelectronics. This thesis focuses on the structure and properties of bulk and thin films of a new material, Cu covetic, that contains carbon in concentrations up to 16 at.%. X-ray photoelectron spectroscopy (XPS) shows C 1s peak with both sp2 and sp3 bonded C measuring up to 3.5 wt.% (16 at.%). High resolution transmission electron microscopy and electron diffraction of bulk covetic samples show a modulated structure of ≈ 1.6 nm along several crystallographic directions in regions that have high C content suggesting that the carbon incorporates into the copper lattice forming a network. Electron energy loss spectra (EELS) from covetics reveal that the level of graphitization from the source material, activated carbon, is maintained in the covetic structure. Bulk Cu covetics have a slight increase in the lattice constant, as well as <111> texturing, or possibly a different structure, compared to pure Cu. Density functional theory calculations predict bonding between C and Cu at the edges and defects of graphene sheets. The electrical resistivity of bulk covetics first increases and then decreases with increasing C content. Cu covetic films were deposited using e-beam and pulsed laser deposition (PLD) at different temperatures. No copper oxide or any allotropes of carbon are present in the films. The e-beam films show enhanced electrical and optical properties when compared to pure Cu films of the same thickness even though no carbon was detected by XPS or EELS. They also have slightly higher ampacity than Cu metal films. EELS analysis of the C-K-edge in the PLD films indicate that graphitic carbon is transferred from the bulk into the films with uniform carbon distribution. PLD films exhibit flatter and higher transmittance curves and sheet resistance two orders of magnitude lower than e-beam films leading to a high figure of merit as transparent conductors.