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Exploring Spin-State Selective Harvesting Pathways from Singlet Fission Dimers to a Near-Infrared-Emissive Spin-Flip
Percy Gonzalo Sifuentes-Samanamud1, Adrian Sauer2, Aki Masaoka1
1Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
Journal of the American Chemical Society
|March 25, 2026
Summary
Singlet fission (SF) generates two triplets from one singlet, boosting solar cell efficiency. Researchers used a molybdenum complex to efficiently capture these triplets, overcoming energy transfer limitations and advancing SF applications.
Area of Science:
- Photophysical processes
- Materials science
- Organic electronics
Background:
- Singlet fission (SF) generates two triplet excitons from one singlet exciton, offering potential for enhanced photovoltaic and organic light-emitting diode efficiencies.
- Controlling energy levels and intermolecular interactions are crucial for maximizing SF efficiency.
- Isothermic/endothermic SF systems, like tetracene derivatives, face challenges with competing Förster resonance energy transfer (FRET), reducing sensitization efficiency.
Purpose of the Study:
- To demonstrate a molybdenum-based near-infrared light-emitting spin-flip emitter as a triplet-selective energy acceptor.
- To overcome FRET limitations in tetracene-based SF systems by utilizing efficient triplet energy transfer (TET).
- To advance the development of exciton/photon amplification materials by combining SF with transition-metal complexes.
Main Methods:
- Utilized tetracene-based dimers with phenylene, 2,5-methylphenylene, and p-terphenylene bridging units.
- Employed a molybdenum-based spin-flip emitter as a near-infrared light-emitting acceptor.
- Quantified quantum yields of doublet state formation and analyzed fluorescence lifetimes.
Main Results:
- Achieved efficient exothermic triplet energy transfer (TET) to the molybdenum complex's spin-flip excited doublet state.
- Circumvented FRET from the tetracene singlet state due to a large energy gap in the molybdenum complex.
- Quantified quantum yields for doublet state formation: 112 ± 6% (phenylene), 132 ± 2% (2,5-methylphenylene), and 128 ± 4% (p-terphenylene).
- Observed a drop in SF dimer fluorescence lifetimes with increasing molybdenum complex concentration, indicating energy transfer from exchange-coupled triplet pairs.
Conclusions:
- Demonstrated efficient triplet-selective energy acceptance by a molybdenum complex, overcoming FRET limitations.
- Highlighted the importance of controlling exchange interactions and triplet pair recombination for efficient energy transfer.
- Paved the way for developing advanced exciton/photon amplification materials by integrating SF with transition-metal complexes.
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