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Charge transfer-mediated singlet fission.

N Monahan1, X-Y Zhu

  • 1Department of Chemistry, Columbia University, New York, New York 10027;

Annual Review of Physical Chemistry
|February 5, 2015
PubMed
Summary
This summary is machine-generated.

Singlet fission splits one high-energy singlet exciton into two lower-energy triplet excitons. This process, crucial for solar energy, requires understanding charge transfer excitons in organic semiconductors.

Keywords:
Mott-Wannier excitondynamicspentacenequantum coherencesolar energy conversion

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Organic Electronics

Background:

  • Singlet fission is a process where one singlet exciton splits into two triplet excitons.
  • It holds significant promise for enhancing solar energy conversion efficiency.
  • Conventional models struggle to fully explain singlet fission in crystalline organic semiconductors.

Purpose of the Study:

  • To address limitations in current models of singlet fission.
  • To highlight the importance of electronic delocalization and charge transfer (CT) excitons.
  • To explore design principles for intramolecular singlet fission.

Main Methods:

  • Analysis of crystalline organic semiconductors (pentacene, tetracene).
  • Focus on Mott-Wannier (charge transfer) excitons.
  • Presentation of experimental evidence for quantum superposition states.

Main Results:

  • The conventional four-electron and dimer models are insufficient for describing singlet fission.
  • Electronic delocalization and CT excitons play a critical role.
  • Experimental data supports a quantum superposition of singlet, CT, and triplet-pair states.

Conclusions:

  • A deeper understanding of electronic delocalization is essential for singlet fission.
  • CT excitons are key mediators in this process.
  • Mechanistic insights are guiding the design of new materials for improved solar energy applications.