Supramolecular assembly is a promising bottom-up approach for producing materials that behave as charge transporting components in electronic devices. Although extensive advances have been made during the past two decades, formidable challenges exist in controlling the local randomness present in supramolecular assemblies. Here, a temperature-triggered supramolecular assembly strategy using heat to heal defects and disorders is reported. The central concept of the molecular design-named the "Tetris strategy" in this research-is to: i) increase the rotational freedom of the molecules through thermal perturbation, ii) induce conformation-fitting of adjacent molecules through two different kinds of intermolecular [π···π] interactions, and finally iii) lock the nearby molecules in inactive co-conformations. Experimentally, upon heating to 57 °C, amorphous solid-state films undergo spontaneous assembly, leading to the growth of uniform and highly ordered microwire arrays. Temperature-triggered supramolecular assembly provides an approach closer to the precision control of assembled structures and presents with a broad canvas to work on in approaching a new generation of supramolecular electronics. Tetris is a registered trademark of Tetris Holding, LLC, used with permission.
Keywords: [π···π] interactions; cold crystallization; noncovalent bonding interactions; organic field-effect transistors; semiconductors; solution processability.
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