Chiral Rotaxane-Branched Dendrimers as Relays in Artificial Light-Harvesting Systems with Boosted Circularly Polarized Luminescence

Angew Chem Int Ed Engl. 2024 Nov 22:e202419434. doi: 10.1002/anie.202419434. Online ahead of print.

Abstract

Starting from AIEgen-functionalized chiral [2]rotaxane building block, we have successfully synthesized a new class of chiral rotaxane-branched dendrimers through controllable divergent strategy for the first time, based on which novel chiral artificial light-harvesting systems (LHSs) were successfully constructed in aqueous phase by sequentially introducing achiral donor and acceptor. More importantly, accompanied by the two-step Förster resonance energy transfer (FRET) process in the resultant artificial LHSs, the sequentially amplified circularly polarized luminescence (CPL) performances were achieved, highlighting that the chiral rotaxane-branched dendrimers could serve as excellent relay for both energy transfer and chirality transmission. Impressively, compared with the sole chiral rotaxane-branched dendrimers, the dissymmetry factors (glum) values of the resultant artificial LHSs were amplified by one order of magnitude up to 0.038, enabling their further applications in information storage and encryption. The proof-of concept study provides not only a feasible approach for the efficient amplification of CPL performances but also a novel platform for the construction of novel chiral luminescent materials.

Keywords: Chiral Rotaxane Dendrimers; Förster Resonance Energy Transfer; Information Storage and Encryption; Mechanically Interlocked Molecules; aggregation-induced emission.