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Published online by Cambridge University Press: 16 February 2011
This paper describes an approach to crystal engineering based on designing and analyzing hierarchical levels of crystalline architecture. The system under study consists of 1:1 co-crystals of melamines and barbituric acids that self-assemble into crystallographically infinite hydrogen-bonded tapes. The formation of structural elements can be rationalized and controlled using familiar molecular concepts such as steric repulsion.