Triplet Transfer Mediates Triplet Pair Separation during Singlet Fission in 6,13-Bis(triisopropylsilylethynyl)-Pentacene

Grieco, Christopher; Doucette, Grayson S.; Munro, Jason M.; Kennehan, Eric R.; Lee, Youngmin; Rimshaw, Adam; Payne, Marcia M.; Wonderling, Nichole; Anthony, John E.; Dabo, Ismaila; Gomez, Enrique D.; Asbury, John B.

doi:10.1002/adfm.201703929

Title: Triplet Transfer Mediates Triplet Pair Separation during Singlet Fission in 6,13-Bis(triisopropylsilylethynyl)-Pentacene

Journal Article · Fri Oct 20 00:00:00 EDT 2017 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.201703929· OSTI ID:1537342

Grieco, Christopher ^[1]; Doucette, Grayson S. ^[1]; Munro, Jason M. ^[1]; Kennehan, Eric R. ^[1]; Lee, Youngmin ^[1]; Rimshaw, Adam ^[1]; Payne, Marcia M. ^[2]; Wonderling, Nichole ^[1];

^[2]; Dabo, Ismaila ^[1];

^[1];

^[1]

Pennsylvania State University, University Park, PA (United States)
University of Kentucky, Lexington, KY (United States)

Abstract Triplet population dynamics of solution cast films of isolated polymorphs of 6,13‐bis(triisopropylsilylethynyl) pentacene (TIPS‐Pn) provide quantitative experimental evidence that triplet excitation energy transfer is the dominant mechanism for correlated triplet pair (CTP) separation during singlet fission. Variations in CTP separation rates are compared for polymorphs of TIPS‐Pn with their triplet diffusion characteristics that are controlled by their crystal structures. Since triplet energy transfer is a spin‐forbidden process requiring direct wavefunction overlap, simple calculations of electron and hole transfer integrals are used to predict how molecular packing arrangements would influence triplet transfer rates. The transfer integrals reveal how differences in the packing arrangements affect electronic interactions between pairs of TIPS‐Pn molecules, which are correlated with the relative rates of CTP separation in the polymorphs. These findings suggest that relatively simple computations in conjunction with measurements of molecular packing structures may be used as screening tools to predict a priori whether new types of singlet fission sensitizers have the potential to undergo fast separation of CTP states to form multiplied triplets.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF); USDOE

Grant/Contract Number:: SC0008120; AC02-05CH11231; CMMI-1255494; DE‐SC0008120

OSTI ID:: 1537342

Alternate ID(s):: OSTI ID: 1400422

Journal Information:: Advanced Functional Materials, Vol. 27, Issue 46; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 33 works

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CCDC 1561748: Experimental Crystal Structure Determination Grieco, Christopher; Doucette, Grayson S.; Munro, Jason M. https://doi.org/10.5517/ccdc.csd.cc1pf3z6 The current record is supplemented by this dataset	dataset	January 2018
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Title: Triplet Transfer Mediates Triplet Pair Separation during Singlet Fission in 6,13-Bis(triisopropylsilylethynyl)-Pentacene

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