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Phys Rev Lett. 2015 Dec 31;115(26):267401. doi: 10.1103/PhysRevLett.115.267401. Epub 2015 Dec 30.

Theory of Primary Photoexcitations in Donor-Acceptor Copolymers.

Physical review letters

Karan Aryanpour, Tirthankar Dutta, Uyen N V Huynh, Zeev Valy Vardeny, Sumit Mazumdar

Affiliations

  1. Department of Physics, University of Arizona, Tucson, Arizona 85721, USA.
  2. Department of Physics, University of Utah, Salt Lake City, Utah 84112, USA.
  3. Departments of Physics and Chemistry, University of Arizona, Tucson, Arizona 85721, USA.
  4. College of Optical Sciences, University of Arizona, Tucson, Arizona 85721, USA.

PMID: 26765027 DOI: 10.1103/PhysRevLett.115.267401

Abstract

We present a generic theory of primary photoexcitations in low band gap donor-acceptor conjugated copolymers. Because of the combined effects of strong electron correlations and broken symmetry, there is considerable mixing between a charge-transfer exciton and an energetically proximate triplet-triplet state with an overall spin singlet. The triplet-triplet state, optically forbidden in homopolymers, is allowed in donor-acceptor copolymers. For an intermediate difference in electron affinities of the donor and the acceptor, the triplet-triplet state can have a stronger oscillator strength than the charge-transfer exciton. We discuss the possibility of intramolecular singlet fission from the triplet-triplet state, and how such fission can be detected experimentally.

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