Thin Film Transistors Incorporating Ultrapure Semiconducting Single-Walled Carbon Nanotubes and Green Dielectrics

Printed electronics is a burgeoning field that has received intense research interest and is beginning to experience commercial successes. Single-walled carbon nanotubes (SWNTs) are a unique and promising building block for incorporation into next generation superfast electronic devices. SWNTs have very high carrier mobilites, with band gaps compatible for integration into logic circuits. Their excellent mechanical flexibility allows for potential incorporation into flexible printed electronics, enabling fully-printed transistors and circuits with performances that support low cost, large area fabrication. Progress in incorporating SWNTs into commercial devices has been hindered by the presence of metallic SWNTs, which are produced alongside semiconducting SWNTs during synthesis, and negatively impact device performance. Fabrication of ambipolar SWNT organic thin film transistors (OTFTs) with high carrier mobilities and high on/off ratios remains particularly challenging; many examples in the literature required high temperature, expensive and energy-demanding processes. Since the initial discovery of conjugated polymer-assisted dispersion and purification of SWNTs in 2008, several polymer families have been successfully shown to selectively disperse semiconducting SWNTs. However, only a relatively small number of these supramolecular complexes have been incorporated into OTFTs. We used a novel conjugated polymer to exclusively disperse semiconducting SWNTs. The dispersal procedure requires a simple sonication and centrifugation, during which the metallic SWNTs sediment out. Solution purity was evaluated using UVVis- NIR and Raman spectroscopies. The resulting dispersions are amenable to solution processing techniques such drop casting and spin coating, allowing for the potential for large area device fabrication at room temperature. Ambipolar OTFTs were fabricated under ambient conditions using this solution and tested in both air and under inert atmosphere. The presence of excess conjugated polymer, solution deposition techniques, SWNT density, surface treatment, and post-fabrication treatment were all investigated to determine which parameters facilitated the production of OTFTs with high mobilities (>20 cm2V-1s-1), high on/off ratios (10^6-10^8), negligeble hysteresis, controlled threshold voltages, and high bias stability.[1] Protocols for sorting and dispersing ultrapure sc-SWNTs with conjugated polymers for thin-film transistor (TFT) applications have been well refined. Conventional wisdom dictates that removal of excess unbound polymer through filtration or centrifugation is necessary to produce high- erformance TFTs. However, this is time-consuming, wasteful, and resource-intensive. We challenge this paradigm and demonstrate that excess unbound polymer during semiconductor film fabrication is not necessarily detrimental to device performance.[2] With focus on further improving device performance, we look to green, compostable dielectrics to pair with SWCNTs. We report a tri-layer dielectric using poly (lactic acid) (PLA), poly(vinyl alcohol)/cellulose nanocrystals (PVAc) and toluene diisocyanate terminated poly(caprolactone) (TPCL) which we integrated into SWCNT based TFTs in a top gate bottom contact architecture. The PVA provides a high dielectric constant due to the hydroxy groups, the cellulose is used to optimize the viscosity, the TPCL layer provides a robust hydrophobic surface[3], and the PLA eliminates the interfacial charge traps present in the PVAc. This leads to a decrease in leakage currents and reduced the polarity at the dielectric/semiconductor interface. The TFTs fabricated using tri-layer dielectrics led to air stable and balanced hole and electron mobilities which was not observed for the PVAc/TPCL bilayer systems with supressed hole mobility. These TFTs were then used to study the impact of electrochemical doping on the performance of sc-SWCNT TFTs when switching from n-type, where an electrical double layer is formed, to p-type, where the TFSI anions are free to interact with the sc-SWCNTs.[4] The following presentation will focus on the engineering of sc-SWNTs based electronic devices. The choice of conjugated wrapping polymer, dielectric and processing conditions on film formation and the TFT device performance. References [1] Chem. Mater. 2019, 31, 8, 2863–2872 [2] ACS Nano., 2021, 15, 5, 8252–8266 [3] Adv. Electron. Mater.. 2021, 7, 10, 2100700. [4] Flexible and Printed Electronics, 2022, 7, 3, 034004

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