Singlet Fission in Core–Shell Micelles of End-Functionalized
Polymers
Posted on 2018-06-22 - 16:48
Singlet
fission is the process in aggregates of molecular semiconductors
where the initial product of light absorption (a singlet exciton)
is converted into two correlated spin-triplet excitons. While most
studies of singlet fission are conducted on assemblies of small molecule
singlet fission chromophores, polymer self-assembly has yet to be
explored as a means of creating nanostructures conducive for singlet
fission. In this work, we use solution self-assembly of mono- and
difunctionalized polymers to create core–shell micelles that
display efficient singlet fission. The polymers are synthesized by
copper(I)-catalyzed “click” chemistry between a 6,13-bis(triisopropylsilylethynyl)pentacene
(TIPS-Pn) alkyne precursor and the corresponding azide-terminated
poly(ethylene glycol) (PEG) polymer. Spontaneous solution self-assembly
creates starlike and flowerlike core–shell micelles that are
characterized by dynamic light scattering (DLS) and transmission electron
microscopy (TEM) experiments. Ultrafast transient absorption spectroscopy
and time-resolved fluorescence experiments evidence nearly equivalent
singlet fission dynamics in starlike and flowerlike micelles. Studies
on mixed micelles of the Pn-functionalized polymer with a C16-PEG surfactant reveal how triplet pair formation and decay rates
vary with micelle composition. The core–shell micelles developed
herein demonstrate the potential of polymer self-assembly for creating
functional singlet fission nanostructures and provide insight into
how secondary components and solubilizing blocks influence singlet
fission dynamics and triplet pair losses in self-assembled systems.
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Tilley, Andrew
J.; Pensack, Ryan D.; Kynaston, Emily L.; Scholes, Gregory D.; Seferos, Dwight S. (2018). Singlet Fission in Core–Shell Micelles of End-Functionalized
Polymers. ACS Publications. Collection. https://doi.org/10.1021/acs.chemmater.8b01814
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AUTHORS (5)
AT
Andrew
J. Tilley
RP
Ryan D. Pensack
EK
Emily L. Kynaston
GS
Gregory D. Scholes
DS
Dwight S. Seferos
KEYWORDS
Spontaneous solution self-assemblytime-resolved fluorescence experiments evidencesolubilizing blocks influence singlet fission dynamicsequivalent singlet fission dynamicstriplet pair formationsinglet fission nanostructuressinglet fissionmolecule singlet fission chromophorescoretriplet pair lossesmicelleDLSPEGTEMEnd-Functionalized Polymers Singlet fissiontransmission electron microscopypolymer self-assemblyuse solution self-assembly