Magnetic dipolar interaction between correlated triplets created by singlet fission in tetracene crystals

@article{Wang2015MagneticDI,
  title={Magnetic dipolar interaction between correlated triplets created by singlet fission in tetracene crystals},
  author={Rui Wang and Chunfeng Zhang and Bo Zhang and Yunlong Liu and Xiaoyong Wang and Min Xiao},
  journal={Nature Communications},
  year={2015},
  volume={6}
}
Singlet fission can potentially break the Shockley–Queisser efficiency limit in single-junction solar cells by splitting one photoexcited singlet exciton (S1) into two triplets (2T1) in organic semiconductors. A dark multiexciton state has been proposed as the intermediate connecting S1 to 2T1. However, the exact nature of this multiexciton state, especially how the doubly excited triplets interact, remains elusive. Here we report a quantitative study on the magnetic dipolar interaction between… 

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References

SHOWING 1-10 OF 52 REFERENCES

Mechanism for singlet fission in pentacene and tetracene: from single exciton to two triplets.

This ab initio study characterizes the low-lying excited states in acene molecular crystals in order to describe how SF occurs in a realistic crystal environment and shows how intermolecular interactions are shown to localize the initially delocalized bright state onto a pair of monomers.

Temperature-independent singlet exciton fission in tetracene.

Together, these results require that singlets and triplet pairs in tetracene are effectively degenerate in energy, and begin to reconcile the temperature dependence of many macroscopic observables with a fission process which does not require thermal activation.

Quantum beats in crystalline tetracene delayed fluorescence due to triplet pair coherences produced by direct singlet fission.

The model provides good overall agreement with the data, supporting the conclusion that singlet fission in tetracene proceeds through the "direct" mechanism without strong electronic coupling between the singlet and triplet pair states.

A transferable model for singlet-fission kinetics.

This work lays the foundation for tailoring molecular properties like solubility and energy level alignment while maintaining the high fission yield required for photovoltaic applications.

Singlet fission in pentacene through multi-exciton quantum states.

It is shown that singlet fission to produce a pair of triplet excitons must involve an intermediate state that has a multi-exciton character, is energetically accessible from the optically allowed excited state, and efficiently dissociates into multiple electron-hole pairs.

The energy barrier in singlet fission can be overcome through coherent coupling and entropic gain.

This work attributes entropic gain in crystalline tetracene as the driving force for the subsequent decay of S(1) ⇔ ME into 2 × T(1), which leads to a high singlet-fission yield.

Singlet Fission: From Coherences to Kinetics.

A full understanding of singlet fission requires consideration of a sequence of photophysical events (decoherence, relaxation, and diffusion) occurring on different time scales.

Exciton fission and fusion in bis(tetracene) molecules with different covalent linker structures.

A detailed study of exciton fission in three novel phenylene-linked bis(tetracene) molecules is presented, showing that it is important to consider the effects of the linker structure on both energy relaxation and electronic coupling in bichromophoric molecules.

Theory of Singlet Fission in Polyenes, Acene Crystals and Covalently Linked Acene Dimers

We report quadruple configuration interaction calculations within the extended Pariser$-$Parr$-$Pople Hamiltonian on the excited states of aggregates of polyenes, crystalline acenes, and covalently

Nonlinear Density Dependence of Singlet Fission Rate in Tetracene Films.

It is experimentally show that the rate of singlet fission has a nonlinear dependence on the density of photoexcited singlet excitons in tetracene films with small crystalline grains.
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