Conjugated Polyelectrolyte‐Based Complex Fluids as Aqueous Exciton Transport Networks

The ability to assemble artificial systems that mimic aspects of natural light‐harvesting functions is fascinating and attractive for materials design. Given the complexity of such a system, a simple design pathway is desirable. Here, we argue that associative phase separation of oppositely charged...

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Bibliographic Details
Published in:Angewandte Chemie (International ed.) 2022-05, Vol.61 (20), p.e202117759-n/a
Main Authors: Johnston, Anna R., Minckler, Eris D., Shockley, Mia C. J., Matsushima, Levi N., Perry, Sarah L., Ayzner, Alexander L.
Format: Article
Language:English
Subjects:
chemistry
Complexity
Conjugated Polyelectrolytes
Electronics
Energy Transfer
Exciton
Excitons
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Molecular ions
Natural lighting
Phase Separation
Polyelectrolytes
Thermodynamics
Water
Wave functions
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Summary:The ability to assemble artificial systems that mimic aspects of natural light‐harvesting functions is fascinating and attractive for materials design. Given the complexity of such a system, a simple design pathway is desirable. Here, we argue that associative phase separation of oppositely charged conjugated polyelectrolytes (CPEs) can provide such a path in an environmentally benign medium: water. We find that complexation between an exciton–donor and acceptor CPE leads to formation of a complex fluid. We interrogate exciton transfer from the donor to the acceptor CPE within the complex fluid and find that transfer is highly efficient. We also find that excess molecular ions can tune the modulus of the inter‐CPE complex fluid. Even at high ion concentrations, CPEs remain complexed with significantly delocalized electronic wavefunctions. Our work lays the rational foundation for complex, tunable aqueous light‐harvesting systems via the intrinsic thermodynamics of associative phase separation. Artificial systems that mimic aspects of natural light‐harvesting functions are fascinating and attractive for materials design. Given the complexity of such a system, a simple design pathway is desirable. Associative phase separation of oppositely charged conjugated polyelectrolytes (CPEs) can provide such a path in an environmentally benign medium: water. Complexation between an exciton–donor and acceptor CPE leads to formation of a complex fluid in which energy transfer is highly efficient.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202117759