Beyond Synthesis Conditions: Linking In-situ Growth Dynamics to Carbon Nanotube Forest Properties through Multimodal Machine Learning
Shun Muroga, Takashi Tsuji, Shunsuke Sakurai, Don N Futaba
Abstract
Machine learning for chemical vapor deposition (CVD) of carbon nanotubes (CNTs) has largely mapped static synthesis conditions to final properties, implicitly treating these conditions as a complete description of growth. Here, we test this assumption by integrating gas-flow conditions with in-situ time-resolve growth profiles (growth curves) of vertically aligned CNT forests. We introduce an observation-window analysis, in which prediction is evaluated as a function of observation time by providing models with the growth curve only up to progressively later times, to determine not only whether a property can be predicted, but when the necessary information becomes available during synthesis. Clustering of normalized growth curves revealed distinct growth patterns independent of final forest height. The gas conditions alone could predict the initial growth rate but not the growth lifetime and failed to capture the variation in yield (R^2<0). Adding the growth curve improved yield prediction (R^2~0.4-0.5), with the relevant information emerging during the intermediate and later stages of growth rather than at its onset. In contrast, density and G/D ratio, which forest height does not record, showed no consistent improvement. The maximum height and lifetime could be estimated with moderate accuracy midway through the 10-min growth. Permutation feature importance identified water vapor and H_2, both linked to catalyst activity, as the most informative gas variables. These results indicate that variation unexplained by synthesis conditions is not merely noise but reflects an evolving catalyst state, and they establish mid-growth decision points for autonomous synthesis, enabling early termination of unpromising batches and, ultimately, in-batch adjustment of growth conditions.