Controlled assembly of single-walled carbon nanotube (SWCNT) networks with high density and deposition rate is critical for many practical applications, including large-area electronics. In this regard, surfactant chemistry plays a critical role as it facilitates the substrate− nanotube interactions. Despite its importance, detailed understanding of the subject up until now has been lacking, especially toward tuning the controllability of SWCNT assembly for thin-film transistors. Here, we explore SWCNT assembly with steroid-and alkyl-based surfactants. While steroid-based surfactants yield highly dense nanotube thin films, alkyl surfactants are found to prohibit nanotube assembly. The latter is attributed to the formation of packed alkyl layers of residual surfactants on the substrate surface, which subsequently repel surfactant encapsulated SWCNTs. In addition, temperature is found to enhance the nanotube deposition rate and density. Using this knowledge, we demonstrate highly dense and rapid assembly with an effective SWCNT surface coverage of ∼99% as characterized by capacitance−voltage measurements. The scalability of the process is demonstrated through a roll-to-roll assembly of SWCNTs on plastic substrates for large-area thin-film transistors. The work presents an important process scheme for nanomanufacturing of SWCNT-based electronics. 37 printed TFTs based on SWCNT networks have also been reported, demonstrating excellent performances, surpassing that of printed organic devices by a large margin. The performance of SWCNT TFTs is largely dependent on the properties of the assembled random networks.
■ INTRODUCTION38 Specifically, high nanotube density yields high ON-state current, while bundling during assembly increases the OFF-state current. 39,40 Thus, understanding and controlling the nanotube−substrate binding as facilitated through the surfactant−surface interactions is of profound interest, with strong emphasis on enhancing density and reducing bundling. Furthermore, fast nanotube assembly on substrates is essential for practical applications as it determines the process throughput, eventually allowing roll-to-roll (R2R) assembly and processing of SWCNTs over large-areas.Significant research has focused on dispersion of SWCNTs in liquids over the past decade, 41−60 with one promising method involving the use of aqueous solutions with organic surfactants that show long-term stability over several months. 52,54,55 Thin and thick films of SWCNTs from nanotube suspensions have also been widely explored for various applications. 9,15,33,34,36,61 However, the details of the assembly process of SWCNTs for "TFT-grade" random networks have not been fully explored, which is a critical step for optimizing the deposition quality and rate. In addition, most work in literature has focused on the use of commercially available solutions of semiconductor-enriched SWCNTs for TFT fabrication. The surfactants used for these commercial solutions are often not publically known, and a change in the surfactant ...