Pluperfect Nanocrystal Architectures aims to create, characterize, and control the architectures of nanocrystal-based materials that transcend the structure and function of translationally periodic nanocrystal assemblies that have dominated the research landscape to date. In creating synthetic materials, we typically aim for perfection, preparing pure and periodic materials that are easy to model and measure. However, an opportunity exists for the self- and directed-assembly of nanocrystals that break from perfection by exploiting additional degrees of design freedom that are unavailable in atomic systems. The team will explore combinations of surface chemistry and geometrical cues that trigger and direct the formation of compositional defects, aperiodicity, and heterogeneity in nanocrystal assemblies in “hard” fabricated and “soft” liquid crystal templates. Targeted imperfection will unlock a palette of conﬁgurable and reconﬁgurable architectures with new functions that are not possible in traditionally “perfect” assemblies. In this way we aspire to create pluperfect nanocrystal architectures, i.e., complex, beyond-perfect, or literally “more than perfect” nanocrystal assemblies, that impart novel optical and magnetic responses.