The performance of conjugated polymer devices is largely dictated by charge transport processes. However, it is difficult to obtain a clear relationship between conjugated polymer structures and charge transport properties, due to the complexity of the structure and the dispersive nature of charge transport in conjugated polymers. Here, we develop a method to map the energy landscape for charge transport in conjugated polymers based on simultaneous, correlated charge carrier tracking and single-particle fluorescence spectroscopy. In nanoparticles of the conjugated polymer poly[9,9-dioctylfluorenyl-2,7-diyl)-
Population dynamics of multiple triplet excitons revealed from time-dependent fluorescence quenching of single conjugated polymer chains
The advent of multiple exciton harvesting schemes and prolonging exciton lifetimes to improve performance attributes of solar cells based on conjugated organic materials presents some interesting challenges that must be overcome in order to realize the full potential of these strategies. This is especially important for applications involving multi-chromophoric conjugated polymers where interactions between multiple spin-forbidden triplet excitons can be significant and are mediated by chain conformation. We use single molecule spectroscopic techniques to investigate interactions between multiple triplet excitons and emissive singlets by monitoring time-dependent fluorescence quenching on time scales commensurate with the triplet lifetime. Structurally related conjugated polymers differing by heteroatom substitution were targeted and we use a stochastic photodynamic model to numerically simulate the evolution of multi-exciton populations following photoexcitation. Single chains of poly(3-hexylthiophene) (P3HT) exhibit longer-lived triplet dynamics and larger steady-state triplet occupancies compared to those of poly(3-hexylselenophene) (P3HS), which has a larger reported triplet yield. Triplet populations evolve and relax much faster in P3HS which only becomes evident when considering all kinetic factors governing exciton population dynamics. Overall, we uncover new guidelines for effectively managing multi-exciton populations and interactions in conjugated polymers and improving their light harvesting efficiency.
- Publication Date:
- NSF-PAR ID:
- 10153348
- Journal Name:
- Scientific Reports
- Volume:
- 9
- Issue:
- 1
- ISSN:
- 2045-2322
- Publisher:
- Nature Publishing Group
- Sponsoring Org:
- National Science Foundation
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