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Quantum master equation approach to singlet fission dynamics in pentacene ring-shaped aggregate models
1Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan; Center for Spintronics Research Network (CSRN), Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan; Quantum Information and Quantum Biology Division, Institute for Open and Transdisciplinary Research Initiatives, Osaka University, Toyonaka, Osaka 560-8531, Japan; and Institute for Molecular Science, 38 Nishigo-Naka, Myodaiji, Okazaki 444-8585, Japan.
Singlet fission (SF) in pentacene aggregates shows complex dynamics influenced by structure and size. Frenkel excitonic coupling significantly impacts SF rates and triplet yields, offering insights for designing efficient materials.
Area of Science:
- Physical Chemistry
- Materials Science
- Quantum Dynamics
Background:
- Singlet fission (SF) is a crucial process for enhancing solar cell efficiency.
- Understanding exciton dynamics in molecular aggregates is key to optimizing SF.
Purpose of the Study:
- To investigate the effects of Frenkel excitonic (FE) coupling on SF dynamics in ring-shaped pentacene aggregates.
- To clarify the influence of aggregate structure and size on SF rate and triplet-triplet (TT) pair yield.
Main Methods:
- Quantum master equation approach applied to pentacene ring-shaped aggregate models.
- Analysis of SF rate and TT yield dependencies on aggregate size and FE coupling strength.
Main Results:
- The smallest ring model (trimer) shows reduced SF rate and TT yield compared to a dimer.
- SF rate increases with aggregate size, peaking at 17-mer, then decreases.
- TT yield shows a stationary decrease with increasing aggregate size.
Conclusions:
- Aggregate structure and size significantly modulate SF dynamics.
- FE coupling plays a critical role in dictating SF efficiency.
- Results provide guidelines for designing high-efficiency SF aggregates.
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