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Title: An insight into non-emissive excited states in conjugated polymers

Abstract

Conjugated polymers in the solid state usually exhibit low fluorescence quantum yields, which limit their applications in many areas such as light-emitting diodes. Despite considerable research efforts, the underlying mechanism still remains controversial and elusive. Here, the nature and properties of excited states in the archetypal polythiophene are investigated via aggregates suspended in solvents with different dielectric constants (ε). In relatively polar solvents (ε>~ 3), the aggregates exhibit a low fluorescence quantum yield (QY) of 2–5%, similar to bulk films, however, in relatively nonpolar solvents (ε<~ 3) they demonstrate much higher fluorescence QY up to 20–30%. A series of mixed quantum-classical atomistic simulations illustrate that dielectric induced stabilization of nonradiative charge-transfer (CT) type states can lead to similar drastic reduction in fluorescence QY as seen experimentally. In conclusion, fluorescence lifetime measurement reveals that the CT-type states exist as a competitive channel of the formation of emissive exciton-type states.

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
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  1. Univ. of Texas at Austin, Austin, TX (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Understanding Charge Separation and Transfer at Interfaces in Energy Materials (CST); Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1459344
Grant/Contract Number:  
SC0001091
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Hu, Zhongjian, Willard, Adam P., Ono, Robert J., Bielawski, Christopher W., Rossky, Peter J., and Vanden Bout, David A.. An insight into non-emissive excited states in conjugated polymers. United States: N. p., 2015. Web. doi:10.1038/ncomms9246.
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Hu, Zhongjian, Willard, Adam P., Ono, Robert J., Bielawski, Christopher W., Rossky, Peter J., & Vanden Bout, David A.. An insight into non-emissive excited states in conjugated polymers. United States. https://doi.org/10.1038/ncomms9246
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Hu, Zhongjian, Willard, Adam P., Ono, Robert J., Bielawski, Christopher W., Rossky, Peter J., and Vanden Bout, David A.. Tue . "An insight into non-emissive excited states in conjugated polymers". United States. https://doi.org/10.1038/ncomms9246. https://www.osti.gov/servlets/purl/1459344.
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@article{osti_1459344,
title = {An insight into non-emissive excited states in conjugated polymers},
author = {Hu, Zhongjian and Willard, Adam P. and Ono, Robert J. and Bielawski, Christopher W. and Rossky, Peter J. and Vanden Bout, David A.},
abstractNote = {Conjugated polymers in the solid state usually exhibit low fluorescence quantum yields, which limit their applications in many areas such as light-emitting diodes. Despite considerable research efforts, the underlying mechanism still remains controversial and elusive. Here, the nature and properties of excited states in the archetypal polythiophene are investigated via aggregates suspended in solvents with different dielectric constants (ε). In relatively polar solvents (ε>~ 3), the aggregates exhibit a low fluorescence quantum yield (QY) of 2–5%, similar to bulk films, however, in relatively nonpolar solvents (ε<~ 3) they demonstrate much higher fluorescence QY up to 20–30%. A series of mixed quantum-classical atomistic simulations illustrate that dielectric induced stabilization of nonradiative charge-transfer (CT) type states can lead to similar drastic reduction in fluorescence QY as seen experimentally. In conclusion, fluorescence lifetime measurement reveals that the CT-type states exist as a competitive channel of the formation of emissive exciton-type states.},
doi = {10.1038/ncomms9246},
journal = {Nature Communications},
number = 1,
volume = 6,
place = {United States},
year = {2015},
month = {9}
}
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https://doi.org/10.1038/ncomms9246
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Synthesis, Properties, and Electronic Applications of Size-Controlled Poly(3-hexylthiophene) Nanoparticles
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Fate of Excitations in Conjugated Polymers: Single-Molecule Spectroscopy Reveals Nonemissive “Dark” Regions in MEH-PPV Individual Chains
journal, December 2009

  • Lin, Hongzhen; Tian, Yuxi; Zapadka, Karolina
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A Semi‐Empirical Theory of the Electronic Spectra and Electronic Structure of Complex Unsaturated Molecules. I.
journal, March 1953

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  • The Journal of Chemical Physics, Vol. 21, Issue 3
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Modeling disorder in polymer aggregates: The optical spectroscopy of regioregular poly(3-hexylthiophene) thin films
journal, June 2005

  • Spano, Frank C.
  • The Journal of Chemical Physics, Vol. 122, Issue 23
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Interplay between intrachain and interchain interactions in semiconducting polymer assemblies: The HJ-aggregate model
journal, May 2012

  • Yamagata, H.; Spano, F. C.
  • The Journal of Chemical Physics, Vol. 136, Issue 18
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Singlet-Triplet Annihilation Limits Exciton Yield in Poly(3-Hexylthiophene)
journal, April 2014

Impedance Spectroscopy on Polymer-Fullerene Solar Cells
journal, January 2007

  • Knipper, Martin; Parisi, Jürgen; Coakley, Kevin
  • Zeitschrift für Naturforschung A, Vol. 62, Issue 9
  • DOI: 10.1515/zna-2007-0904
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