Tangential flow interfacial self-assembly (TaFISA) is a promising scalable technique enabling uniformly aligned carbon nanotubes for high-performance semiconductor electronics. In this process, flow is utilized to induce global alignment in two-dimensional nematic carbon nanotube assemblies trapped at a liquid/liquid interface, and these assemblies are subsequently deposited on target substrates. Here, we present an observational study of experimental parameters that affect the interfacial assembly and subsequent aligned nanotube deposition. We specifically study the water contact angle (WCA) of the substrate, nanotube ink composition, and water subphase and examine their effects on liquid crystal defects, overall and local alignment, and nanotube bunching or crowding. By varying the substrate chemical functionalization, we determine that highly aligned, densely packed, individualized nanotubes deposit only at relatively small WCA between 35 and 65°. At WCA (< 10°), high nanotube bunching or crowding occurs, and the film is nonuniform, while aligned deposition ceases to occur at higher WCA (>65°). We find that the best alignment, with minimal liquid crystal defects, occurs when the polymer-wrapped nanotubes are dispersed in chloroform at a low (0.6:1) wrapper polymer to nanotube ratio. We also demonstrate that modifying the water subphase through the addition of glycerol not only improves overall alignment and reduces liquid crystal defects but also increases local nanotube bunching. These observations provide important guidance for the implementation of TaFISA and its use toward creating technologies based on aligned semiconducting carbon nanotubes.
more »
« less
Substrate‐Wide Confined Shear Alignment of Carbon Nanotubes for Thin Film Transistors
To exploit their charge transport properties in transistors, semiconducting carbon nanotubes must be assembled into aligned arrays comprised of individualized nanotubes at optimal packing densities. However, achieving this control on the wafer‐scale is challenging. Here, solution‐based shear in substrate‐wide, confined channels is investigated to deposit continuous films of well‐aligned, individualized, semiconducting nanotubes. Polymer‐wrapped nanotubes in organic ink are forced through sub‐mm tall channels, generating shear up to 10 000 s−1uniformly aligning nanotubes across substrates. The ink volume and concentration, channel height, and shear rate dependencies are elucidated. Optimized conditions enable alignment within a ±32° window, at 50 nanotubes µm−1, on 10 × 10 cm2substrates. Transistors (channel length of 1–5 µm) are fabricated parallel and perpendicular to the alignment. The parallel transistors perform with 7× faster charge carrier mobility (101 and 49 cm2V−1s−1assuming array and parallel‐plate capacitances, respectively) with high on/off ratio of 105. The spatial uniformity varies ±10% in density, ±2° in alignment, and ±7% in mobility. Deposition occurs within seconds per wafer, and further substrate scaling is viable. Compared to random networks, aligned nanotube films promise to be a superior platform for applications including sensors, flexible/stretchable electronics, and light emitting and harvesting devices.
more » « less- Award ID(s):
- 1727523
- PAR ID:
- 10462905
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Electronic Materials
- Volume:
- 5
- Issue:
- 2
- ISSN:
- 2199-160X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
The multiscale morphology and device performance of printed semiconducting polymers are highly sensitive to the substrate/ink interfacial properties during solution coating. There is an urgent need for general design rules correlating the substrate properties and conjugated polymer (CP) morphology, which do not yet exist. Dynamic surfaces are particularly promising for templating highly crystalline and highly aligned conjugated polymer thin films and have been shown in recent studies. Herein, we implement the dynamic-templating method using a series of liquid-infused nanoporous substrates as a tool to study the impact of template reconfigurability and chemistry on the multiscale morphology of conjugated polymer thin films, using a high performing donor–acceptor polymer (DPP-BTz) as a model compound. By quantifying the enthalpy of adsorption, we demonstrate that the strength of template–CP interactions directly measures the effectiveness of dynamic surfaces in promoting conjugated polymer crystallization and alignment. We further show that the enthalpy of interactions increases by enhancing the template dynamics and is sensitively modulated by template chemistry. Specifically, increasing the template–CP interactions leads to a larger domain size and higher degree of crystallinity in templated conjugated polymer thin films prepared by meniscus-guided solution coating. This observation validates our hypothesis that dynamic templates function by promoting the nucleation of conjugated polymers. We also demonstrate that such dynamic-template-dependent morphology is independent of coating speed. Notably, the enhanced morphological properties modulate the charge carrier mobility in field-effect transistors (FETs) over an order of magnitude reaching a hole mobility of 2.8 cm 2 V −1 s −1 . This work is a significant step towards establishing general guidelines on how the substrate–ink interfacial properties influence morphology and performance of solution coated CP thin films.more » « less
-
more » « less
Abstract The large‐scale growth of semiconducting thin films on insulating substrates enables batch fabrication of atomically thin electronic and optoelectronic devices and circuits without film transfer. Here an efficient method to achieve rapid growth of large‐area monolayer MoSe2films based on spin coating of Mo precursor and assisted by NaCl is reported. Uniform monolayer MoSe2films up to a few inches in size are obtained within a short growth time of 5 min. The as‐grown monolayer MoSe2films are of high quality with large grain size (up to 120 µm). Arrays of field‐effect transistors are fabricated from the MoSe2films through a photolithographic process; the devices exhibit high carrier mobility of ≈27.6 cm2V–1s–1and on/off ratios of ≈105. The findings provide insight into the batch production of uniform thin transition metal dichalcogenide films and promote their large‐scale applications.
-
Semiconducting carbon nanotubes promise faster performance and lower power consumption than Si in field-effect transistors (FETs) if they can be aligned in dense arrays. Here, we demonstrate that nanotubes collected at a liquid/liquid interface self-organize to form two-dimensional (2D) nematic liquid crystals that globally align with flow. The 2D liquid crystals are transferred onto substrates in a continuous process generating dense arrays of nanotubes aligned within ±6°, ideal for electronics. Nanotube ordering improves with increasing concentration and decreasing temperature due to the underlying liquid crystal phenomena. The excellent alignment and uniformity of the transferred assemblies enable FETs with exceptional on-state current density averaging 520 μA μm −1 at only −0.6 V, and variation of only 19%. FETs with ion gel top gates demonstrate subthreshold swing as low as 60 mV decade −1 . Deposition across a 10-cm substrate is achieved, evidencing the promise of 2D nanotube liquid crystals for commercial semiconductor electronics.more » « less
-
more » « less
Abstract Single‐walled carbon nanotubes (SWCNTs) are a class of 1D nanomaterials that exhibit extraordinary electrical and optical properties. However, many of their fundamental studies and practical applications are stymied by sample polydispersity. SWCNTs are synthesized in bulk with broad structural (chirality) and geometrical (length and diameter) distributions; problematically, all known post‐synthetic sorting methods rely on ultrasonication, which cuts SWCNTs into short segments (typically <1 µm). It is demonstrated that ultralong (>10 µm) SWCNTs can be efficiently separated from shorter ones through a solution‐phase “self‐sorting”. It is shown that thin‐film transistors fabricated from long semiconducting SWCNTs exhibit a carrier mobility as high as ≈90 cm2V−1s−1, which is ≈10 times higher than those which use shorter counterparts and well exceeds other known materials such as organic semiconducting polymers (<1 cm2V−1s−1), amorphous silicon (≈1 cm2V−1s−1), and nanocrystalline silicon (≈50 cm2V−1s−1). Mechanistic studies suggest that this self‐sorting is driven by the length‐dependent solution phase behavior of rigid rods. This length sorting technique shows a path to attain long‐sought ultralong, electronically pure carbon nanotube materials through scalable solution processing.
