Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers
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.
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 2006886
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 14 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
Citation Formats
He, Guiying, Churchill, Emily M., Parenti, Kaia R., Zhang, Jocelyn, Narayanan, Pournima, Namata, Faridah, Malkoch, Michael, Congreve, Daniel N., Cacciuto, Angelo, Sfeir, Matthew Y., and Campos, Luis M. Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers. United Kingdom: N. p., 2023.
Web. doi:10.1038/s41467-023-41818-1.
He, Guiying, Churchill, Emily M., Parenti, Kaia R., Zhang, Jocelyn, Narayanan, Pournima, Namata, Faridah, Malkoch, Michael, Congreve, Daniel N., Cacciuto, Angelo, Sfeir, Matthew Y., & Campos, Luis M. Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers. United Kingdom. https://doi.org/10.1038/s41467-023-41818-1
He, Guiying, Churchill, Emily M., Parenti, Kaia R., Zhang, Jocelyn, Narayanan, Pournima, Namata, Faridah, Malkoch, Michael, Congreve, Daniel N., Cacciuto, Angelo, Sfeir, Matthew Y., and Campos, Luis M. Thu .
"Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers". United Kingdom. https://doi.org/10.1038/s41467-023-41818-1.
@article{osti_2006886,
title = {Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers},
author = {He, Guiying and Churchill, Emily M. and Parenti, Kaia R. and Zhang, Jocelyn and Narayanan, Pournima and Namata, Faridah and Malkoch, Michael and Congreve, Daniel N. and Cacciuto, Angelo and Sfeir, Matthew Y. and Campos, Luis M.},
abstractNote = {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.},
doi = {10.1038/s41467-023-41818-1},
journal = {Nature Communications},
number = 1,
volume = 14,
place = {United Kingdom},
year = {Thu Sep 28 00:00:00 EDT 2023},
month = {Thu Sep 28 00:00:00 EDT 2023}
}
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