Mirka Brendan, Rice Nicole A, Williams Phillip, Tousignant Mathieu N, Boileau Nicholas T, Bodnaryk William J, Fong Darryl, Adronov Alex, Lessard Benoît H
Department of Chemical and Biological Engineering, University of Ottawa, 161 Louis Pasteur, Ottawa, Ontario, Canada K1N 6N5.
Department of Chemistry and Chemical Biology, McMaster University, 1280 Main Street W, Hamilton, Ontario, Canada L8S 4M1.
ACS Nano. 2021 May 25;15(5):8252-8266. doi: 10.1021/acsnano.0c08584. Epub 2021 Apr 8.
Ultrapure semiconducting single-walled carbon nanotube (sc-SWNT) dispersions produced through conjugated polymer sorting are ideal candidates for the fabrication of solution-processed organic electronic devices on a commercial scale. 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-performance TFTs. However, this is time-consuming, wasteful, and resource-intensive. In this report, we challenge this paradigm and demonstrate that excess unbound polymer during semiconductor film fabrication is not necessarily detrimental to device performance. Over 1200 TFT devices were fabricated from 30 unique polymer-sorted SWNT dispersions, prepared using two different alternating copolymers. Detailed Raman spectroscopy, x-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM) studies of the random-network semiconductor films demonstrated that a simple solvent rinse during TFT fabrication was sufficient to remove unbound polymer from the sc-SWNT films, thus eliminating laborious polymer removal before TFT fabrication. Furthermore, below a threshold polymer concentration, the presence of excess polymer during fabrication did not significantly impede TFT performance. Preeminent performance was achieved for devices prepared from native polymer-sorted SWNT dispersions containing the "original" amount of excess unbound polymer (immediately following enrichment). Lastly, we developed an open-source Machine Learning algorithm to quantitatively analyze AFM images of SWNT films for surface coverage, number of tubes, and tube alignment.
通过共轭聚合物分选制备的超纯半导体单壁碳纳米管(sc-SWNT)分散体是大规模制备溶液处理有机电子器件的理想选择。用于薄膜晶体管(TFT)应用的用共轭聚合物分选和分散超纯sc-SWNT的方案已经得到了很好的完善。传统观念认为,通过过滤或离心去除过量的未结合聚合物对于制备高性能TFT是必要的。然而,这既耗时、浪费又耗费资源。在本报告中,我们对这一范式提出挑战,并证明在半导体薄膜制造过程中过量的未结合聚合物不一定会对器件性能产生不利影响。我们用两种不同的交替共聚物制备了30种独特的聚合物分选SWNT分散体,并从中制造了1200多个TFT器件。对随机网络半导体薄膜进行的详细拉曼光谱、X射线光电子能谱(XPS)和原子力显微镜(AFM)研究表明,在TFT制造过程中简单的溶剂冲洗足以从sc-SWNT薄膜中去除未结合的聚合物,从而省去了在TFT制造之前费力的聚合物去除步骤。此外,在低于阈值聚合物浓度时,制造过程中过量聚合物的存在并不会显著阻碍TFT性能。对于由含有“原始”量过量未结合聚合物(富集后立即)的天然聚合物分选SWNT分散体制备的器件,实现了卓越的性能。最后,我们开发了一种开源机器学习算法,用于定量分析SWNT薄膜的AFM图像,以确定表面覆盖率、管数量和管排列情况。