Our studies focus on developing optoelectronically functional molecular-based materials that are facilely tractable in our hands and have a size of macroscopic length scale. Such molecular materials are designed simply from controlling a balance of intermolecular interactions in the alkyl-&#960 compounds, i.e., van der Waals and &#960-&#960 interactions among adjacent molecules (“alkyl- &#960 engineering”). Herein, novel type self-assembly techniques of alkyl-&#960 compounds are presented. One direction is using its molecular liquid state, for use as they are or for the self-assembly environment with appropriate additives. The alkyl-&#960 liquids show thermally- and optically-stable luminescent feature while resulting nanosheets and microfiber-gel by a post-assembly treatment exhibit photoconductivity. Another intriguing self-assembly strategy is at the air-water interfaces and forms into hierarchically ordered hemispherical microparticle array, like compound eye structure, in centimeter length scale. This macroscopic assembled structure is only achieved from the molecular self-assembly initiated at the water/organic solvent interface and successive organic solvent evaporation can allow the anisotropic particle growth as well as their hexagonal array formation. In the presentation, its detail formation mechanism is discussed.

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