Even a little delocalization produces large kinetic enhancements of charge-separation efficiency in organic photovoltaics

@article{Balzer2022EvenAL,
  title={Even a little delocalization produces large kinetic enhancements of charge-separation efficiency in organic photovoltaics},
  author={Daniel Balzer and Ivan Kassal},
  journal={Science Advances},
  year={2022},
  volume={8}
}
In organic photovoltaics, charges can separate efficiently even if their Coulomb attraction is an order of magnitude greater than the available thermal energy. Delocalization has been suggested to explain this fact, because it could increase the initial separation of charges in the charge-transfer (CT) state, reducing their attraction. However, understanding the mechanism requires a kinetic model of delocalized charge separation, which has proven difficult because it involves tracking the… 

References

SHOWING 1-10 OF 120 REFERENCES

Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport.

TLDR
In both the hopping and band-like transport regimes, it is demonstrated that at low temperature, the zero-point fluctuations of the bath lead to non-zero transport rates and hence a finite diffusion constant.

Noise-induced quantum coherence drives photo-carrier generation dynamics at polymeric semiconductor heterojunctions.

TLDR
An exciton/lattice model of the electronic dynamics of primary photo excitations in a polymeric semiconductor heterojunction that includes both polymer π-stacking, energetic disorder and phonon relaxation indicates that resonant tunnelling processes brought about by environmental fluctuations couple photo excitation directly to photocurrent producing charge-transfer states on <100 fs time scales.

Phys

  • 142, 164103
  • 2015

Delocalised kinetic Monte Carlo for simulating delocalisation-enhanced charge and exciton transport in disordered materials

TLDR
This work presents the first three-dimensional model of partially delocalised charge and exciton transport in materials in the intermediate disorder regime, based on polaron-transformed Redfield theory but overcomes several computational roadblocks by mapping the quantum-mechanical techniques onto kinetic Monte Carlo.

Polaron States in Fullerene Adducts Modeled by Coarse-Grained Molecular Dynamics and Tight Binding.

TLDR
A simple and efficient model to determine the energy and spatial extent of polaron states within a coarse-grained representation of a disordered molecular film is proposed and helps to establish the conditions under which a hopping transport model is justified.

Phys

  • 24, 966
  • 1956

Partially polaron-transformed quantum master equation for exciton and charge transport dynamics.

Polaron-transformed quantum master equation (PQME) offers a unified framework to describe the dynamics of quantum systems in both limits of weak and strong couplings to environmental degrees of

Impact of Nanoscale Morphology on Charge Carrier Delocalization and Mobility in an Organic Semiconductor

TLDR
A novel computational methodology is presented that shows that amorphous pentacene spontaneously self-assembles to nanocrystalline structures that, at long quench times, form the characteristic herringbone layer of the single crystal.

Formally exact simulations of mesoscale exciton dynamics in molecular materials†

TLDR
It is demonstrated that the adaptive HOPS (adHOPS) methodology provides a formally exact and size-invariant scaling algorithm for simulating mesoscale quantum dynamics.

Exciton transport in amorphous polymers and the role of morphology and thermalisation

Understanding the transport mechanism of electronic excitations in conjugated polymers is key to advancing organic optoelectronic applications, such as solar cells, organic light-emitting diodes and
...