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<p>Singlet exciton fission (SF), in which one singlet exciton (S<sub>1</sub>) generates two triplet excitons (T<sub>1</sub>), is one of the few available options for exceeding the theoretical limit of solar energy use, the so-called Shockley–Queisser limit. Although most SF systems applicable to Si solar cells exhibit a thermodynamically unfavourable endothermic process, a few approaches exist for overcoming the endothermic SF process. Here we discovered that combining SF molecules with quantum dots (QDs) is an alternative for improving the endothermic SF efficiency. Inter-material orbital hybridization between SF molecules and QDs harnesses the endothermic SF. Theoretical calculations and transient-absorption measurements of tetracene–CdX (X = Te, Se or S) QD composites showed that several orbital hybrid levels that formed due to orbital hybridization act as intermediate levels to facilitate SF. This result highlights alternative factors affecting SF efficiency beyond the molecular packing of SF molecules on the QD surface.</p>

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Molecular quantum-dot orbital hybridization supports efficient endothermic singlet exciton fission

  • 期刊论文

  • 发表日期：

    2026年5月4日

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  • Jie Zhang,
  • Hayato Sakai,
  • Katsuaki Suzuki,
  • Ramsha Khan,
  • Taku Hasobe,
  • I-Ya Chang,
  • Kim Hyeon-Deuk,
  • Hironori Kaji,
  • Masanori Sakamoto

摘要

Singlet exciton fission (SF), in which one singlet exciton (S1) generates two triplet excitons (T1), is one of the few available options for exceeding the theoretical limit of solar energy use, the so-called Shockley–Queisser limit. Although most SF systems applicable to Si solar cells exhibit a thermodynamically unfavourable endothermic process, a few approaches exist for overcoming the endothermic SF process. Here we discovered that combining SF molecules with quantum dots (QDs) is an alternative for improving the endothermic SF efficiency. Inter-material orbital hybridization between SF molecules and QDs harnesses the endothermic SF. Theoretical calculations and transient-absorption measurements of tetracene–CdX (X = Te, Se or S) QD composites showed that several orbital hybrid levels that formed due to orbital hybridization act as intermediate levels to facilitate SF. This result highlights alternative factors affecting SF efficiency beyond the molecular packing of SF molecules on the QD surface.