Commercial applications of vertically aligned single-wall carbon nanotube (SWCNT) “forests” are on the horizon, with the emergence of their use in nanocomposite membranes,1 electronic interconnects, thermal interface materials, among other promising demonstrations. To realize these potential applications, we sought to not only design reproducible wafer-scale synthesis of high-density SWCNT forests but also to establish advanced metrology to enable quantitative, large-area mapping of several key forest characteristics. This detailed information will unlock better understanding of interdependent correlations among the characteristics and how these correlations inform SWCNT forest growth mechanisms toward enhanced synthetic control. We performed low-pressure chemical vapor deposition (CVD) on 4-in. Si wafers in an AIXTRON® Black Magic cold-wall furnace. The combination of a low flux of carbon precursors with sub-nm Fe/Mo catalyst films on alumina-coated Si wafers maintained small-diameter SWCNTs (mean as small at 1.87 nm) with number densities up to 2.2 x1012 cm-2. Although removing Mo resulted in categorically larger CNT diameters and lower densities (< 0.9 x1012 cm-2), the mass conversion rate from C2H2 to SWCNT product was essentially constant (~1.2 x106 % g catalyst-1) for all catalyst compositions and CNT densities. These results corroborate the notion that hydrocarbon dissociation may be thermally driven without assistance from the catalyst under these conditions, and that the role of Mo was primarily a physical one in creating smaller, denser SWCNTs. Furthermore, we leveraged a suite of advanced characterization techniques to generate area maps across a 4-in wafer to visualize and evaluate the uniformity of various forest properties, including Raman microscopy (forest height, graphitization level, diameters), synchrotron X-ray scattering (mean diameter),2 and Rutherford backscattering spectroscopy (forest density). The uniformity and coupled correlations among different structural characteristics (e.g., diameter-density, rate-density) within a single wafer were consistent with those observed for multiple wafers grown by sequential runs (up to 5 in a day). This validates the reproducibility of our process and suggests that these correlations may be more universal phenomena. Lastly, our developments in synthesis represent to our knowledge best-in-class co-optimization of small-diameter, high-density, and large-area SWCNT forest growth. We will briefly discuss growth benchmarks in context of membranes, electrochemical devices, and antireflective surfaces as examples. Bui, N.; Meshot, E. R.; Kim, S.; Peña, J.; Gibson, P. W.; Wu, K. J.; Fornasiero, F. Advanced Materials 2016, 28 (28), 5871-5877.Meshot, E.; Zwissler, D. W.; Bui, N.; Kuykendall, T. R.; Wang, C.; Hexemer, A.; Wu, K. J. J.; Fornasiero, F. ACS Nano 2017, 11 (6), 5405-5416.
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