Emerging design principles for enhanced solar energy utilization with singlet fission

Melissa K. Gish, Natalie A. Pace, Gary Rumbles, Justin C. Johnson

Research output: Contribution to journalArticle

Abstract

Singlet fission (SF), the generation of two triplet excitons per the absorption of one photon, is a promising strategy for increasing the efficiency of solar cells beyond the theoretical Shockley-Queisser limit of 34%. Upon photon absorption by a SF molecule, the initially created singlet excited state (S 1 ) interacts with a neighboring chromophore and is first transformed into a triplet pair (TT), which can be subsequently separated into independent triplet excitons (2T 1 ). These independent triplet excitons can be harvested through triplet charge extraction or triplet energy transfer to an acceptor. Research on SF systems has revealed rates and efficiencies of triplet formation and triplet pair decorrelation that are strongly dependent on interchromophore coupling, which is dictated by molecular structure and the resulting geometrical arrangement of chromophores adopted in covalent (e.g., dimers) and noncovalent (e.g., films and crystals) systems. Incorporation of SF materials into realistic device architectures introduces a host of new challenges to consider regarding the efficient extraction of triplets generated through SF. In this Feature Article, we review our work that has led to some degree of understanding and control of inter- and intramolecular SF rates placed in the context of solar energy harvesting architectures, including dye-sensitized solar cells, conjugated polymer films, and ligand-exchanged quantum dots. We emphasize the importance of understanding and manipulating interactions between SF molecules with each other and with the charge or energy collectors across an interface in order to strike a kinetic balance that leads to efficient utilization of triplet excitons.

Original languageEnglish
Pages (from-to)3923-3934
Number of pages12
JournalJournal of Physical Chemistry C
Volume123
Issue number7
DOIs
Publication statusPublished - Feb 21 2019

Fingerprint

solar energy
Excitons
Solar energy
fission
emerging
Energy utilization
Chromophores
excitons
Photons
Molecules
Energy harvesting
Conjugated polymers
chromophores
Polymer films
Excited states
Dimers
Energy transfer
Molecular structure
Semiconductor quantum dots
solar cells

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Emerging design principles for enhanced solar energy utilization with singlet fission. / Gish, Melissa K.; Pace, Natalie A.; Rumbles, Gary; Johnson, Justin C.

In: Journal of Physical Chemistry C, Vol. 123, No. 7, 21.02.2019, p. 3923-3934.

Research output: Contribution to journalArticle

Gish, Melissa K. ; Pace, Natalie A. ; Rumbles, Gary ; Johnson, Justin C. / Emerging design principles for enhanced solar energy utilization with singlet fission. In: Journal of Physical Chemistry C. 2019 ; Vol. 123, No. 7. pp. 3923-3934.
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