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Synthesis and metrology of conducting carbon nanotube assemblies


Since its discovery, the carbon nanotube (CNT) has been proposed as one of the ultimate materials for its electrical, thermal and mechanical properties due to its incredibly strong sp2 bonds, low defect density, and large aspect ratio. Many experimental results on individual CNTs have confirmed these outstanding theoretically predicted properties. However, scaling these properties to the macroscopic regime has proved to be challenging. This work focused on the synthesis and measurement of highly conducting, macroscopic, CNT assemblies. Scaling up the synthesis of vertically aligned multiwalled CNT (MWNT) forests was investigated through the development of a large, 100mm, wafer scale, cold wall chemical vapor deposition chamber. In addition to the synthesis, two distinct CNT assemblies have been investigated. A linear morphology where CNTs are strung in series for electrical transport (CNT wires) and a massively parallel 2D array of vertically aligned CNTs for Thermal Interface Material (TIM) applications.

Poymer-CNT wire composites have been fabricated by developing a coaxial CNT core-polymer shell electrospinning technique. The core-shell interactions in this system have been studied by way of Hansen's solubility parameters. The most well defined CNT core was achieved using a core solvent that is semi-immiscible with the shell solution, yet still a solvent of the shell polymer. Electrical characterization of the resulting CNT core has shown a two orders of magnitude increase in conductivity over traditional, homogeneously mixed, electrospun CNT wires.

A number of vertically aligned MWNT assemblies were studied for their thermal interface properties. Double-sided Silicon substrate (MWNT-Si-MWNT) TIM assemblies were characterized using a DC, 1D reference bar, thermal measurement technique. While attempts to control MWNT density via a micelle template technique produced only 'spaghetti like' CNTs, sputter deposited catalyst provided stark variations in array density. Relevant array morphologies such as density, height, and crystallinity were studied in conjunction with their thermal performance. A Euler buckling model was used to identify the transition between increasing and decreasing resistance with density over array height, these two regimes are explained by way of contact analysis.

Self catalyzing Fecralloy substrate MWNT TIMs were studied in a similar vein to the Silicon based assemblies. This substrate was investigated because of its malleability, ease of CNT synthesis and increased CNT adhesion. The growth behavior was studied with respect to the array morphologies, i.e. array height, density, crystallinity, and diameter, while the contact resistance was evaluated using a DC, 1D reference bar technique. The best performing samples were found to have a factor of two increase over their Si counterparts. Temperature dependent thermal measurements offer insight into the interfacial phonon conduction physics and are found to agree with other temperature dependent studies, suggesting inelastic scattering at the MWNT-Cu interface. Due to the challenges associated with deliberately controlling a single array morphology, a statistical approach was used for identifying the influences of the multivariate array morphology on contact resistance. Showing the strongest correlation with array height, following a R ~ L-0.5. Several models were investigated to help explain this behavior, although little insight is gained over the empirical relations.

To better characterize these MWNT TIM assemblies two experimental techniques were developed. A transient 3ω thermal measurement technique was adapted to characterize the thermal performance of CNT TIMs, offering insight into the limiting resistance in a mulilayer material stack. The MWNT-growth substrate interface was found to dominate in the Si samples while the MWNT-opposing substrate interface dominated in the Fecralloy samples. These measurements strongly supported the DC thermal measurements and the qualitative observations of substrate adhesion. Additionally, a new technique for observing nano sized contacts was established by viewing contact loading through an electron transparent membrane, imaged under an SEM. The contrast mechanism is explained by a voltage contrast phenomenon developed by trapped charges at the interface. The resolution limits have been studied by way of electron beam interactions and the use of Monte Carlo simulations, showing nanometer resolution with appropriate experimental conditions. The real MWNT contact area was found to be less than 1/100th the apparent contact area even at moderate pressures and the number of contacting CNTs is approximately 1/10th the total number of CNTs. These results confirm experimental measurement values for van der Waals adhesion strengths and thermal interface resistance.

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