Direct Exciton Harvesting from a Bound Triplet Pair

He, Guiying; Parenti, Kaia R.; Campos, Luis M.; Sfeir, Matthew Y.

doi:10.1002/adma.202203974

Direct Exciton Harvesting from a Bound Triplet Pair

Journal Article · 01 September 2022 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202203974· OSTI ID:2421995

He, Guiying ^[1]; Parenti, Kaia R. ^[2]; ^[2]; ^[3]

Department of Physics Graduate Center City University of New York New York NY 10016 USA; Photonics Initiative Advanced Science Research Center City University of New York New York NY 10031 USA; OSTI
Department of Chemistry Columbia University New York NY 10027 USA
Department of Physics Graduate Center City University of New York New York NY 10016 USA; Photonics Initiative Advanced Science Research Center City University of New York New York NY 10031 USA

Abstract

Singlet fission is commonly defined as the generation of two triplet excitons from a single absorbed photon. However, ambiguities within this definition arise due to the complexity of the various double triplet states that exist in SF chromophores and the corresponding interconversion processes. To clarify this process, singlet fission is frequently depicted as sequential two‐step conversion in which a singlet exciton decays into a bound triplet‐pair biexciton state that dissociates into two “free” triplet excitons. However, this model discounts the potential for direct harvesting from the coupled biexciton state. Here, it is demonstrated that individual triplet excitons can be extracted directly from a bound triplet pair. It is demonstrated that due to the requirement for geminate triplet–triplet annihilation in intramolecular singlet fission compounds, unique spectral and kinetic signatures can be used to quantify triplet‐pair harvesting yields. An internal quantum efficiency for triplet exciton transfer from the triplet pair of >50%, limited only by the solubility of the compounds is achieved. The harvesting process is not dependent on the net multiplicity of the triplet‐pair state, suggesting that an explicit, independent dissociation step is not a requirement for using triplet pairs to do chemical or electrical work.

Research Organization:: City Univ. of New York (CUNY), NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: SC0022036; SC0012704

OSTI ID:: 2421995

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 40 Vol. 34; ISSN 0935-9648

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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