Ultrafast Triplet Pair Separation and Triplet Trapping following Singlet Fission in Amorphous Pentacene Films

Munson, Kyle T.; Gan, Jianing; Grieco, Christopher; Doucette, Grayson S.; Anthony, John E.; Asbury, John B.

doi:10.1021/acs.jpcc.0c07920

Title: Ultrafast Triplet Pair Separation and Triplet Trapping following Singlet Fission in Amorphous Pentacene Films

Journal Article · Wed Oct 14 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c07920· OSTI ID:1839364

Munson, Kyle T. ^[1]; Gan, Jianing ^[1]; Grieco, Christopher ^[1]; Doucette, Grayson S. ^[1];

^[2];

^[1]

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

In this work, ultrafast infrared and electronic spectroscopy are used to examine the dynamics of triplet pair separation following singlet fission in amorphous and crystalline films of the model singlet fission chromophore, 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-Pn). Direct probing of correlated triplet pair intermediates through their unique vibrational frequencies, infrared electronic transitions, and indirectly through their visible triplet absorptions reveals that triplet pair separation occurs on similar picosecond timescales in both amorphous and crystalline films despite their markedly different average intermolecular coupling strengths. Although triplet pair separation occurs on similar timescales in both environments, measurements of diffusion-controlled triplet-triplet annihilation reveal that the diffusivity of triplet excited states is an order of magnitude lower in amorphous films. The data reveal the presence of sparse triplet traps in the amorphous environment that inhibit the transport of triplet excitons in comparison to crystalline films. These observations inform recent efforts to develop disordered and polymeric singlet fission sensitizers that contain amorphous regions. In particular, the data suggest that it may be possible to nanostructure amorphous or polymeric singlet fission sensitizers to allow ultrafast triplet pair separation and harvesting in photovoltaic and light emitting applications despite their low triplet exciton diffusivity.

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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); National Science Foundation (NSF)

Grant/Contract Number:: SC0019349; DGE-1255832; 1849213

OSTI ID:: 1839364

Journal Information:: Journal of Physical Chemistry. C, Vol. 124, Issue 43; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Ultrafast Triplet Pair Separation and Triplet Trapping following Singlet Fission in Amorphous Pentacene Films

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