Useful materials must satisfy multiple objectives, where the optimization of one objective is often at the expense of another. The Pareto front reports the optimal trade-offs between these conflicting objectives. Here we use a self-driving laboratory, Ada, to define the Pareto front of conductivities and processing temperatures for palladium films formed by combustion synthesis. Ada discovers new synthesis conditions that yield metallic films at lower processing temperatures (below 200 °C) relative to the prior art for this technique (250 °C). This temperature difference makes possible the coating of different commodity plastic materials (e.g., Nafion, polyethersulfone). These combustion synthesis conditions enable us to to spray coat uniform palladium films with moderate conductivity (1.1 × 105 S m−1) at 191 °C. Spray coating at 226 °C yields films with conductivities (2.0 × 106 S m−1) comparable to those of sputtered films (2.0 to 5.8 × 106 S m−1). This work shows how a self-driving laboratoy can discover materials that provide optimal trade-offs between conflicting objectives.

Cathode gas diffusion electrodes (GDEs) in CO 2 electrolyzers facilitate reagent transport and the reduction of CO 2 into chemicals and fuels. While GDEs are routinely leveraged to achieve high rates of product formation, design principles for highperforming cathodes have not yet been established. In this report, we demonstrate the influence of a central parameter in GDE fabrication, the catalyst ink solvent, on the properties and performance of spraycoated cathode GDEs. We show that the choice of solvent used during catalyst deposition impacts the faradaic efficiency for CO by as much as 50% at 200 mA cm −2 . Moreover, the solvent modulates the surface area, hydrophobicity, and capillarity of GDE catalyst layers. By measuring the hydrodynamic radii of catalyst inks, we conclude that solvent-mediated ionomer aggregation is a key factor that affects the microstructure and properties of GDE catalyst layers. We find that using ethanol as the ink solvent promotes moderate ionomer aggregation and yields the highest performing GDEs. This work describes the influence of electrode fabrication methodologies and demonstrates practical methods for preparing GDEs.

The sensitivity of thin-film materials and devices to defects motivates extensive research into the optimization of film morphology. This research could be accelerated by automated experiments that characterize the response of film morphology to synthesis conditions. Optical imaging can resolve morphological defects in thin films and is readily integrated into automated experiments but the large volumes of images produced by such systems require automated analysis. Existing approaches to automatically analyzing film morphologies in optical images require application-specific customization by software experts and are not robust to changes in image content or imaging conditions. Here, we present a versatile convolutional neural network (CNN) for thin-film image analysis which can identify and quantify the extent of a variety of defects and is applicable to multiple materials and imaging conditions. This CNN is readily adapted to new thin-film image analysis tasks and will facilitate the use of imaging in automated thin-film research systems.

We report a fast, reliable and non-destructive method for quantifying the homogeneity of perovskite thin films over large areas using machine vision. We adapt existing machine vision algorithms to spatially quantify multiple perovskite film properties (substrate coverage, film thickness, defect density) with pixel resolution from pictures of 25 cm2 samples. Our machine vision tool—called PerovskiteVision—can be combined with an optical model to predict photovoltaic cell and module current density from the perovskite film thickness. We use the measured film properties and predicted device current density to identify a posteriori the process conditions that simultaneously maximize the device performance and the manufacturing throughput for large-area perovskite deposition using gas-knife assisted slot-die coating. PerovskiteVision thus facilitates the transfer of a new deposition process to large-scale photovoltaic module manufacturing. This work shows how machine vision can accelerate slow characterization steps essential for the multi-objective optimization of thin film deposition processes.

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