Proceedings of the National Academy of Sciences · 2021 · 70 citations · 37 references
Natural SciencesMaterials SciencePhysicsChemical KineticsComputational Materials SciencePhysical ChemistryMolecular DynamicsReaction DynamicsSelf-assembled MaterialsSelf-assembled NanostructuresSelf-assemblyStatistical MechanicsAutomatic DifferentiationCrystallizationDifferentiationEmergent PropertiesEmergent StructureKinetic Control In Self-assemblySelf-assembly KineticsSelf-assembly Modeling
The inverse problem of designing component interactions to target emergent structure is fundamental to numerous applications in biotechnology, materials science, and statistical physics. Equally important is the inverse problem of designing emergent kinetics, but this has received considerably less attention. Using recent advances in automatic differentiation, we show how kinetic pathways can be precisely designed by directly differentiating through statistical physics models, namely free energy calculations and molecular dynamics simulations. We consider two systems that are crucial to our understanding of structural self-assembly: bulk crystallization and small nanoclusters. In each case, we are able to assemble precise dynamical features. Using gradient information, we manipulate interactions among constituent particles to tune the rate at which these systems yield specific structures of interest. Moreover, we use this approach to learn nontrivial features about the high-dimensional design space, allowing us to accurately predict when multiple kinetic features can be simultaneously and independently controlled. These results provide a concrete and generalizable foundation for studying nonstructural self-assembly, including kinetic properties as well as other complex emergent properties, in a vast array of systems.
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Natural Sciences, Chemistry, Physics +16