Maximizing singlet fission in organic dimers: Theoretical investigation of triplet yield in the regime of localized excitation and fast coherent electron transfer

Eric C. Greyson, Josh Vura-Weis, Josef Michl, Mark A Ratner

Research output: Contribution to journalArticle

162 Citations (Scopus)

Abstract

In traditional solar cells one photon absorbed can lead to at most one electron of current. Singlet fission, a process in which one singlet exciton is converted to two triplet excitons, provides a potential improvement by producing two electrons from each photon of sufficient energy. The literature contains several reports of singlet fission in various systems, but the mechanism of this process is poorly understood. In this paper we examine a two-step mechanism with a charge transfer state intermediate, applicable when the initial excited state is localized. Density matrix theory is used to examine how various molecular properties such as orbital energies and electronic couplings affect singlet fission yield in the regime of fast, coherent electron transfer. Several promising chromophores are discussed and density functional theory is used to predict fission yield for each in the context of this mechanism. Finally, implications for chromophore design are discussed, and future experiments are suggested.

Original languageEnglish
Pages (from-to)14168-14177
Number of pages10
JournalJournal of Physical Chemistry B
Volume114
Issue number45
DOIs
Publication statusPublished - Dec 8 2010

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Dimers
fission
electron transfer
dimers
Chromophores
Excitons
Electrons
Photons
chromophores
excitation
excitons
Excited states
Density functional theory
Charge transfer
molecular properties
Solar cells
matrix theory
photons
electrons
solar cells

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Surfaces, Coatings and Films

Cite this

Maximizing singlet fission in organic dimers : Theoretical investigation of triplet yield in the regime of localized excitation and fast coherent electron transfer. / Greyson, Eric C.; Vura-Weis, Josh; Michl, Josef; Ratner, Mark A.

In: Journal of Physical Chemistry B, Vol. 114, No. 45, 08.12.2010, p. 14168-14177.

Research output: Contribution to journalArticle

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