Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers

Guiying He, Emily M. Churchill, Kaia R. Parenti, Jocelyn Zhang, Pournima Narayanan, Faridah Namata, Michael Malkoch, Daniel N. Congreve, Angelo Cacciuto, Matthew Y. Sfeir () and Luis M. Campos ()
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Guiying He: City University of New York
Emily M. Churchill: Columbia University
Kaia R. Parenti: Columbia University
Jocelyn Zhang: Columbia University
Pournima Narayanan: Stanford University
Faridah Namata: KTH Royal Institute of Technology, Department of Fibre and Polymer Technology
Michael Malkoch: KTH Royal Institute of Technology, Department of Fibre and Polymer Technology
Daniel N. Congreve: Stanford University
Angelo Cacciuto: Columbia University
Matthew Y. Sfeir: City University of New York
Luis M. Campos: Columbia University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Singlet fission and triplet-triplet annihilation upconversion are two multiexciton processes intimately related to the dynamic interaction between one high-lying energy singlet and two low-lying energy triplet excitons. Here, we introduce a series of dendritic macromolecules that serve as platform to study the effect of interchromophore interactions on the dynamics of multiexciton generation and decay as a function of dendrimer generation. The dendrimers (generations 1–4) consist of trimethylolpropane core and 2,2-bis(methylol)propionic acid (bis-MPA) dendrons that provide exponential growth of the branches, leading to a corona decorated with pentacenes for SF or anthracenes for TTA-UC. The findings reveal a trend where a few highly ordered sites emerge as the dendrimer generation grows, dominating the multiexciton dynamics, as deduced from optical spectra, and transient absorption spectroscopy. While the dendritic structures enhance TTA-UC at low annihilator concentrations in the largest dendrimers, the paired chromophore interactions induce a broadened and red-shifted excimer emission. In SF dendrimers of higher generations, the triplet dynamics become increasingly dominated by pairwise sites exhibiting strong coupling (Type II), which can be readily distinguished from sites with weaker coupling (Type I) by their spectral dynamics and decay kinetics.

Date: 2023
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DOI: 10.1038/s41467-023-41818-1

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