Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering

Huang, Huaxi; He, Guiying; Xu, Ke; Wu, Qin; Wu, Di; Sfeir, Matthew Y.; Xia, Jianlong

doi:10.1016/j.chempr.2019.06.007

Title: Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering

Abstract

Tuning singlet fission (SF) dynamics in the solid states in a controllable way is vitally important yet still a challenge due to the electronic coupling, which is highly sensitive to molecular packing. Here, we demonstrate a molecular engineering approach to independently optimize the triplet generation and decay process in intramolecular SF films by using terphenyl-bridged TIPS-pentacene tetramers. By controlling the degree of steric hindrance within individual tetramers, we can systematically tune the degree of intermolecular coupling in thin films. Taking advantage of both the intra- and intermolecular SF processes allows us to maintain a rapid triplet pair generation process, even in the case of weak intermolecular coupling. This approach allows us to maintain a picosecond triplet generation process while simultaneously varying the rate constants for triplet-triplet annihilation over three orders of magnitude.

Authors:

Huang, Huaxi ^[1]; He, Guiying ^[1]; Xu, Ke ^[1];

^[2]; Wu, Di ^[1]; Sfeir, Matthew Y. ^[1]; Xia, Jianlong ^[1]

Wuhan Univ., Wuhan (China); City Univ. (CUNY), NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Wed Jul 03 00:00:00 EDT 2019

Research Org.:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1543399

Report Number(s):: BNL-211849-2019-JAAM
Journal ID: ISSN 2451-9294

Grant/Contract Number:: SC0012704

Resource Type:: Accepted Manuscript

Journal Name:: Chem

Additional Journal Information:: Journal Volume: 5; Journal Issue: 9; Journal ID: ISSN 2451-9294

Publisher:: Cell Press, Elsevier

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats


                    Huang, Huaxi, He, Guiying, Xu, Ke, Wu, Qin, Wu, Di, Sfeir, Matthew Y., and Xia, Jianlong. Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering.  United States: N. p., 2019. 
Web.  doi:10.1016/j.chempr.2019.06.007.

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                    Huang, Huaxi, He, Guiying, Xu, Ke, Wu, Qin, Wu, Di, Sfeir, Matthew Y., & Xia, Jianlong. Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering.  United States.  https://doi.org/10.1016/j.chempr.2019.06.007

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                    Huang, Huaxi, He, Guiying, Xu, Ke, Wu, Qin, Wu, Di, Sfeir, Matthew Y., and Xia, Jianlong. Wed .  
"Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering".  United States.  https://doi.org/10.1016/j.chempr.2019.06.007.  https://www.osti.gov/servlets/purl/1543399.

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@article{osti_1543399,

  title        = {Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering},

  author       = {Huang, Huaxi and He, Guiying and Xu, Ke and Wu, Qin and Wu, Di and Sfeir, Matthew Y. and Xia, Jianlong},

  abstractNote = {Tuning singlet fission (SF) dynamics in the solid states in a controllable way is vitally important yet still a challenge due to the electronic coupling, which is highly sensitive to molecular packing. Here, we demonstrate a molecular engineering approach to independently optimize the triplet generation and decay process in intramolecular SF films by using terphenyl-bridged TIPS-pentacene tetramers. By controlling the degree of steric hindrance within individual tetramers, we can systematically tune the degree of intermolecular coupling in thin films. Taking advantage of both the intra- and intermolecular SF processes allows us to maintain a rapid triplet pair generation process, even in the case of weak intermolecular coupling. This approach allows us to maintain a picosecond triplet generation process while simultaneously varying the rate constants for triplet-triplet annihilation over three orders of magnitude.},

  doi          = {10.1016/j.chempr.2019.06.007},

  journal      = {Chem},

  number       = 9,

  volume       = 5,

  place        = {United States},

  year         = {Wed Jul 03 00:00:00 EDT 2019},

  month        = {Wed Jul 03 00:00:00 EDT 2019}

}

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https://doi.org/10.1016/j.chempr.2019.06.007

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Cited by: 19 works

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Figures / Tables:

Scheme 1: Summary of structure-function relations for a) typical solution phase intramolecular singlet fission dynamics, b) film dynamics for monomer and dimer materials, and c) the design strategy based on TPTPn compounds in this work. Here, the solid blue lines correspond to through bond interactions and the dashed orange linesmore »

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