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Most synthetic building blocks self-assemble into one- or three-dimensional architectures. However, fewer examples have been reported on the aggregation of amphiphiles to form optically-active two-dimensional (2D) structures. Herein, we report the self-assembly of tetraphenylethylene (TPE)-containing hydrophilic dendrons into 2D sheet structures in aqueous methanol solution. TEM and AFM investigations showed that the self-assembly of disubstituted TPE generates helical nanofibers as an intermediate structure which, in turn, laterally as
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