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A transferable model for singlet-fission kinetics.

Shane R Yost1, Jiye Lee2, Mark W B Wilson3

  • 11] Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachussetts 02139, USA [2].

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Exciton fission, a process where one singlet exciton splits into two triplets, boosts solar cell efficiency. Optimizing fission yield is key for photovoltaic applications.

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Area of Science:

  • Materials Science
  • Photovoltaics
  • Physical Chemistry

Background:

  • Exciton fission is a photophysical process where a singlet exciton splits into two triplet excitons.
  • This process holds potential for enhancing photovoltaic device efficiencies beyond the Shockley-Queisser limit.
  • Achieving high exciton fission yields is crucial for realizing efficient solar energy conversion.

Purpose of the Study:

  • To investigate the dynamics of exciton fission in organic materials.
  • To develop a first-principles model for predicting exciton fission rates.
  • To understand the relationship between molecular structure, intermolecular interactions, and fission efficiency in neat films.

Main Methods:

  • Ultrafast photoinduced absorption spectroscopy was employed to measure exciton fission dynamics.
  • A first-principles theoretical expression was derived to model the fission rate.
  • Studies were conducted on neat films to assess fission yields at various monomer separations.

Main Results:

  • Exciton fission dynamics were found to be non-adiabatic and Marcus-like in weakly interacting systems, transitioning to adiabatic and coupling-independent behavior at higher interaction strengths.
  • Near-unity fission yields were observed in neat films, even with monomer separations exceeding 5 Å.
  • The derived first-principles expression accurately reproduced fission rates across materials with diverse structures.
  • For efficient solar cells, exciton fission must compete effectively with direct charge generation from singlet excitons.

Conclusions:

  • This study provides a fundamental understanding of exciton fission mechanisms and their dependence on electronic coupling.
  • The findings establish a framework for designing organic materials with tailored properties (e.g., solubility, energy levels) for high photovoltaic performance.
  • Optimizing the balance between exciton fission and charge generation is critical for developing next-generation solar cells.