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Throughout the physical sciences, entropy stands out as a pivotal butenigmatic concept that, in materials design, often takes a backseat to energy.Here, we demonstrate how to precisely engineer entropy to achieve desiredcolloidal crystals. We demonstrate the inverse design of hard particles thatassemble six different target colloidal crystals due solely to entropymaximization. Our approach efficiently samples $10^8$ particle shapes from 88-and 192-dimensional design spaces to discover thermodynamically optimal shapes.We design particle shapes that self assemble known crystals with optimizedthermodynamic stability, as well as new crystal structures with no known atomicor other equivalent.

Engineering Entropy for the Inverse Design of Colloidal Crystals from Hard Shapes