Center for Nanochemistry, Beijing Science and Engineering Center for Nanocarbons, Beijing National Laboratory for Molecular Sciences, Key Laboratory for the Physics and Chemistry of Nanodevices, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
Suzhou Institute of Nanotech and Nanobionics, Chinese Academy of Sciences, Suzhou 215123, China.
Nature. 2017 Mar 9;543(7644):234-238. doi: 10.1038/nature21051. Epub 2017 Feb 15.
The semiconductor industry is increasingly of the view that Moore's law-which predicts the biennial doubling of the number of transistors per microprocessor chip-is nearing its end. Consequently, the pursuit of alternative semiconducting materials for nanoelectronic devices, including single-walled carbon nanotubes (SWNTs), continues. Arrays of horizontal nanotubes are particularly appealing for technological applications because they optimize current output. However, the direct growth of horizontal SWNT arrays with controlled chirality, that would enable the arrays to be adapted for a wider range of applications and ensure the uniformity of the fabricated devices, has not yet been achieved. Here we show that horizontal SWNT arrays with predicted chirality can be grown from the surfaces of solid carbide catalysts by controlling the symmetries of the active catalyst surface. We obtained horizontally aligned metallic SWNT arrays with an average density of more than 20 tubes per micrometre in which 90 per cent of the tubes had chiral indices of (12, 6), and semiconducting SWNT arrays with an average density of more than 10 tubes per micrometre in which 80 per cent of the nanotubes had chiral indices of (8, 4). The nanotubes were grown using uniform size MoC and WC solid catalysts. Thermodynamically, the SWNT was selectively nucleated by matching its structural symmetry and diameter with those of the catalyst. We grew nanotubes with chiral indices of (2m, m) (where m is a positive integer), the yield of which could be increased by raising the concentration of carbon to maximize the kinetic growth rate in the chemical vapour deposition process. Compared to previously reported methods, such as cloning, seeding and specific-structure-matching growth, our strategy of controlling the thermodynamics and kinetics offers more degrees of freedom, enabling the chirality of as-grown SWNTs in an array to be tuned, and can also be used to predict the growth conditions required to achieve the desired chiralities.
半导体行业越来越认为,摩尔定律——预测每个微处理器芯片上的晶体管数量每两年翻一番——即将结束。因此,人们继续寻求用于纳米电子器件的替代半导体材料,包括单壁碳纳米管(SWNTs)。水平纳米管阵列特别吸引人,因为它们优化了电流输出。然而,具有可控手性的水平 SWNT 阵列的直接生长,这将使阵列能够适应更广泛的应用,并确保制造器件的均匀性,尚未实现。在这里,我们通过控制活性催化剂表面的对称性,表明可以从固体碳化物催化剂的表面生长出具有预测手性的水平 SWNT 阵列。我们获得了具有超过 20 根/微米平均密度的水平排列金属 SWNT 阵列,其中 90%的管具有(12,6)的手性指数,以及具有超过 10 根/微米平均密度的半导体 SWNT 阵列,其中 80%的纳米管具有(8,4)的手性指数。使用均匀尺寸的 MoC 和 WC 固体催化剂生长纳米管。从热力学角度来看,SWNT 通过与其结构对称性和直径相匹配来选择性地成核。我们生长出具有(2m,m)手性指数的纳米管(其中 m 是正整数),通过提高碳浓度来最大化化学气相沉积过程中的动力学生长速率,可以增加其产率。与之前报道的方法,如克隆、播种和特定结构匹配生长相比,我们控制热力学和动力学的策略提供了更多的自由度,使阵列中生长的 SWNT 的手性能够被调谐,并且还可以用于预测实现所需手性所需的生长条件。