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Two-dimensional radial-π-stacks in solution

Highly organized π-aggregate architectures can strongly affect electronic couplings, leading to important photophysical behaviors. With the escalating interest in two-dimensional (2D) materials attributed to their exceptional electronic and optical characteristics, there is growing anticipation that...

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Published in:Chemical science (Cambridge) 2024-04, Vol.15 (15), p.564-5611
Main Authors: Su, Feng, Hong, Yongseok, Zhang, Guilan, Wu, Kongchuan, Kim, Juno, Chen, Zhi, Zhang, Hui-Jun, Kim, Dongho, Lin, Jianbin
Format: Article
Language:English
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Summary:Highly organized π-aggregate architectures can strongly affect electronic couplings, leading to important photophysical behaviors. With the escalating interest in two-dimensional (2D) materials attributed to their exceptional electronic and optical characteristics, there is growing anticipation that 2D radial-π-stacks built upon radial π-conjugation nanorings, incorporating intra- and inter-ring electronic couplings within the confines of a 2D plane, will exhibit superior topological attributes and distinct properties. Despite their immense potential, the design and synthesis of 2D π-stacks have proven to be a formidable challenge due to the insufficient π-π interactions necessary for stable stacking. In this study, we present the successful preparation of single-layer 2D radial-π-stacks in a solution. Pillar-shaped radially π-conjugated [4]cyclo-naphthodithiophene diimide ( [4]C-NDTIs ) molecules were tetragonally arranged via in-plane intermolecular π-π interactions. These 2D π-stacks have a unique topology that differs from that of conventional 1D π-stacks and exhibit notable properties, such as acting as a 2D template capable of absorbing C 60 guest molecules and facilitating the formation of 2D radial-π-stacks comprising [4]C-NDTI -C 60 complexes, rapid exciton delocalization across the 2D plane, and efficient excitation energy funneling towards a trap. We present the formation of 2D radial-π-stacks, consisting of radial π-conjugation nanorings in solution, characterized by their distinctive structure and remarkable properties.
ISSN:2041-6520
2041-6539
DOI:10.1039/d4sc00195h