Achieving High-Performance Polymer-Wrapper-Free Aligned Carbon Nanotube Field-Effect Transistors Through Degradable Polymer Wrapping and Efficient Removal Techniques

Semiconducting carbon nanotubes (s-CNTs) have emerged as a promising alternative to traditional silicon for ultrascaled field-effect transistors (FETs), owing to their exceptional properties. Aligned s-CNTs (A-CNTs) are particularly favored for practical applications due to their ability to provide higher driving current and lower contact resistance compared with individual s-CNTs or random networks. Achieving high-semiconducting-purity A-CNTs typically involves conjugated polymer wrapping for selective separation of s-CNTs, followed by self-assembly techniques. However, the presence of the polymer wrapper on A-CNTs can adversely impact electrical contact, gating efficiency, carrier transport, and device-to-device variations, necessitating its complete removal. While various methods have been explored for polymer removal, accurately characterizing the extent of removal remains a challenge. Traditional techniques such as absorption spectroscopy and X-ray photoelectron spectroscopy (XPS) may not accurately depict the remaining polymer content on A-CNTs due to their inherent detection limits. Consequently, the performance of FETs based on pure polymer-wrapper-free A-CNTs is unclear. In this study, we present an approach for preparing high-semiconducting-purity and polymer-wrapper-free A-CNTs using poly[(9,9-dioctylfluorenyl-2,7-dinitrilomethine)-(9,9-dioctylfluorenyl-2,7-dimethine)] (PFO-N-PFO), a degradable polymer, in conjunction with a modified dimension-limited self-alignment process (m-DLSA). Comprehensive transmission electron microscopy (TEM) characterizations, complemented by absorption and XPS characterizations, provide robust evidence of the successful near-complete removal of the polymer wrapper via a cleaning procedure involving acidic degradation, hot solvent rinsing, and vacuum annealing. Furthermore, top-gated FETs based on these high-semiconducting-purity and polymer-wrapper-free A-CNTs exhibit good performance metrics, including an on-current (I_on) of 2.2 mA/μm, peak transconductance (g_m) of 1.1 mS/μm, low contact resistance (R_c) of 191 Ω·μm, and negligible hysteresis, representing a significant advancement in the CNT-based FET technology.