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Related Experiment Video

Updated: Jul 12, 2025

Single Molecule Analysis of Laser Localized Psoralen Adducts
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Singlet Fission in Lycopene H-Aggregates.

William Barford1

  • 1Department of Chemistry, Physical and Theoretical Chemistry Laboratory,University of Oxford, Oxford, OX1 3QZ, United Kingdom.

The Journal of Physical Chemistry Letters
|October 27, 2023
PubMed
Summary
This summary is machine-generated.

Singlet fission (SF) in lycopene H-aggregates is explained by a theory involving excited state relaxation and localization. This process leads to the formation of free single triplets within 50 nanoseconds.

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Area of Science:

  • Photochemistry
  • Physical Chemistry
  • Materials Science

Background:

  • Singlet fission (SF) is a crucial process for enhancing solar cell efficiency.
  • Carotenoids are promising organic chromophores for SF applications.
  • Understanding SF mechanisms in aggregates is key to optimizing energy conversion.

Purpose of the Study:

  • To explain the observed singlet fission in lycopene H-aggregates.
  • To elucidate the role of excited states and their dynamics in lycopene SF.
  • To provide a theoretical framework for SF in carotenoid systems.

Main Methods:

  • Application of a theoretical model for singlet fission in carotenoid dimers.
  • Analysis of high-energy photoexcitation dynamics in lycopene H-aggregates.
  • Computational simulation of excited-state relaxation, internal conversion, and triplet-pair formation.

Main Results:

  • A high-energy bright state (1B+) localizes onto a single lycopene monomer.
  • Internal conversion leads to the 11B- state, enabling exothermic SF.
  • Simulations predict near-complete population transfer to singlet-pair states within 100 ps, followed by triplet-pair formation and equilibration.

Conclusions:

  • The proposed theory successfully explains SF in lycopene H-aggregates.
  • The dynamics involve excited-state localization, internal conversion, and bimolecular SF.
  • Free single triplets are formed within 50 ns, with intermediate quintet states populated via ZFS interactions.