We describe a chemical robotic assistant equipped with a curiosity algorithm (CA) that can efficiently explore the states a complex chemical system can exhibit. The CA-robot is designed to explore formulations in an open-ended way with no explicit optimization target. By applying the CA-robot to the study of self-propelling multicomponent oil-in-water protocell droplets, we are able to observe an order of magnitude more variety in droplet behaviors than possible with a random parameter search and given the same budget. We demonstrate that the CA-robot enabled the observation of a sudden and highly specific response of droplets to slight temperature changes. Six modes of self-propelled droplet motion were identified and classified using a time-temperature phase diagram and probed using a variety of techniques including NMR. This work illustrates how CAs can make better use of a limited experimental budget and significantly increase the rate of unpredictable observations, leading to new discoveries with potential applications in formulation chemistry.
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