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Electronic Coupling for Donor-Bridge-Acceptor Systems with a Bridge-Overlap Approach.

Alessandro Biancardi1, Seth C Martin1, Cameron Liss1,2

  • 1Department of Chemistry, University of Kansas , 1251 Wescoe Hall Drive, Lawrence, Kansas 66045, United States.

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|July 25, 2017
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Calculating electronic coupling in donor-acceptor systems is key for organic electronics. A new method accurately computes these couplings, revealing significant effects in DNA oligomers.

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Area of Science:

  • Computational Chemistry
  • Materials Science
  • Organic Electronics

Background:

  • Understanding electronic coupling in donor-acceptor systems is vital for organic electronics.
  • Aliphatic bridges play a crucial role in modulating this coupling.

Purpose of the Study:

  • To develop a first-principles method for calculating electronic coupling (transfer integrals) in donor-acceptor systems with aliphatic bridges.
  • To investigate the simultaneous contribution of through-space and through-bond couplings.

Main Methods:

  • Block-diagonalization of the Fock/Kohn-Sham matrix of the supersystem.
  • Projection onto the basis of donor and acceptor fragment orbitals.
  • Sharing the bridge in the diagonalization step for simultaneous coupling analysis.

Main Results:

  • The method achieves an average error below 10% when compared to experimental data for fused-ring bridged systems.
  • Electronic coupling in G(T)n G DNA oligomers can be significantly larger than anticipated.
  • Including the entire DNA backbone leads to a slower decay of coupling with increasing length.

Conclusions:

  • The presented first-principles approach accurately calculates electronic coupling in complex bridged systems.
  • The findings highlight the importance of the entire DNA backbone in charge transport phenomena.
  • This method offers a valuable tool for designing advanced organic electronic materials.