Machine-learning-assisted fabrication: Bayesian optimization of laser-induced graphene patterning using in-situ Raman analysis

The control of the physical, chemical, and electronic properties of laser-induced graphene (LIG) is crucial in the fabrication of flexible electronic devices. However, the optimization of LIG production is time-consuming and costly. Here, we demonstrate state-of-the-art automated parameter tuning techniques using Bayesian optimization to advance rapid single-step laser patterning and structuring capabilities with a view to fabricate graphene-based electronic devices. In particular, a large search space of parameters for LIG explored efficiently. As a result, high-quality LIG patterns exhibiting high Raman G/D ratios at least a factor of four larger than those found in the literature were achieved within 50 optimization iterations in which the laser power, irradiation time, pressure and type of gas were optimized. Human-interpretable conclusions may be derived from our machine learning model to aid our understanding of the underlying mechanism for substrate-dependent LIG growth, e.g. high-quality graphene patterns are obtained at low and high gas pressures for quartz and polyimide, respectively. Our Bayesian optimization search method allows for an efficient experimental design that is independent of the experience and skills of individual researchers, while reducing experimental time and cost and accelerating materials research.