Abstract
Rapid validation of newly predicted materials through autonomous synthesis requires real-time adaptive control methods that exploit physics knowledge, a capability that is lacking in most systems. Here, we demonstrate an approach to enable real-time control of thin film synthesis by combining in situ optical diagnostics with a Bayesian state estimation method. We developed a physical model for film growth and applied the direct filter (DF) method for real-time estimation of nucleation and growth rates during pulsed laser deposition (PLD). We validated the approach using simulated and experimental reflectivity data for WSe2 growth and ultimately deployed the algorithm on an autonomous PLD system during the growth of 1T′-MoTe2. The DF robustly estimates growth parameters in real time at early stages of growth, down to 15% monolayer area coverage. This fusion of in situ diagnostics, data assimilation, and physical modeling opens new opportunities in adaptive control of synthesis trajectories toward desired material states.
