| Abstract
| - Characterization of materials is crucial for the quantification and prediction of their physical,chemical, and mechanical properties. However, as the complexity of a system increases, so do thechallenges involved in elucidating its structure. While molecular simulation and modeling have provedinvaluable as complements to experiment, such simulations now face serious challenges: new materialsare being synthesized with ever increasing structural complexity, and it may soon prove impossible togenerate models that are sufficiently realistic to describe them adequately. Perhaps, ultimately, it will onlybe possible to generate such models by simulating the synthetic process itself. Here, we attempt such astrategy to generate full atomistic models for mesoporous molecular sieves. As in experiment, this is doneby allowing nanoparticles to self-assemble at high temperature to form an amorphous mesoporousframework. The temperature is then reduced, and the system is allowed to crystallize. Animations of atomictrajectories, available as Supporting Information, reveal the evolution of multiple seeds which propagate toform a complex framework. The products are polycrystalline mesoporous framework structures containingcavities connected by channels running along “zero”, one, two, and three perpendicular directions. Wesuggest that it is easier to generate these model structures by attempting to simulate the synthetic processrather than by using more conventional techniques. The strategy is illustrated using ZnS as a model system.Further development of the mathematics of minimal surfaces will advance our understanding of thesestructures.
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