One-Pot Synthesis and Excited-State Dynamics of Null Exciton-Coupled Diketopyrrolopyrroles Oligo-Grids

Bo Y, Hou P, Wan J, Cao H, Liu Y, Xie L, Guldi DM (2023)


Publication Type: Journal article

Publication year: 2023

Journal

DOI: 10.1002/adma.202302664

Abstract

Exciton coupling in molecular aggregates plays a vital role in impacting and fine-tuning optoelectronic materials and their efficiencies in devices. A versatile platform to decipher aggregation-property relationships is built around multichromophoric architectures. Here, a series of cyclic diketopyrrolopyrrole (DPP) oligomers featuring nanoscale gridarene structures and rigid bifluorenyl spacers are designed and synthesized via one-pot Friedel–Crafts reaction. DPP dimer [2]Grid and trimer [3]Grid, which are cyclic rigid nanoarchitectures of rather different sizes, are further characterized via steady-state and time-resolved absorption and fluorescence spectroscopies. They exhibit monomer-like spectroscopic signatures in the steady-state measurements, from which null exciton couplings are derived. Moreover, in an apolar solvent, high fluorescence quantum yields and excited-state dynamics that resembled DPP monomer are gathered. In a polar solvent, the localized singlet excited state on a single DPP dissociates into the adjacent null coupling DPP with charge transfer characteristics. This pathway facilitates the evolution of the symmetry-broken charge-separated state (SB-CS). Notable is the fact that the SB-CS of [2]Grid is, on one hand, in equilibrium with the singlet excited state and promotes, on the other hand, the formation of the triplet excited state with a yield of 32% via charge recombination.

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How to cite

APA:

Bo, Y., Hou, P., Wan, J., Cao, H., Liu, Y., Xie, L., & Guldi, D.M. (2023). One-Pot Synthesis and Excited-State Dynamics of Null Exciton-Coupled Diketopyrrolopyrroles Oligo-Grids. Advanced Materials. https://doi.org/10.1002/adma.202302664

MLA:

Bo, Yifan, et al. "One-Pot Synthesis and Excited-State Dynamics of Null Exciton-Coupled Diketopyrrolopyrroles Oligo-Grids." Advanced Materials (2023).

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