Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 123, Issue 7, Pages 3923-3934Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.8b10876
Keywords
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Funding
- U.S. Department of Energy (DOE) [DE-AC36-08G028308]
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences
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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.
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