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Title: Effect of Charge Localization on the Effective Hyperfine Interaction in Organic Semiconducting Polymers

Abstract

Hyperfine interaction (HFI), originating from the coupling between spins of charge carriers and nuclei, has been demonstrated to strongly influence the spin dynamics of localized charges in organic semiconductors. Nevertheless, the role of charge localization on the HFI strength in organic thin films has not yet been experimentally investigated. In this study, the statistical relation hypothesis that the effective HFI of holes in regioregular poly(3-hexylthiophene) (P3HT) is proportional to 1/N0.5 has been examined, where N is the number of the random nuclear spins within the envelope of the hole wave function. First, by studying magnetoconductance in hole-only devices made by isotope-labeled P3HT we verify that HFI is indeed the dominant spin interaction in P3HT. Second, assuming that holes delocalize fully over the P3HT polycrystalline domain, the strength of HFI is experimentally demonstrated to be proportional to 1/N0.52 in excellent agreement with the statistical relation. Third, the HFI of electrons in P3HT is about 3 times stronger than that of holes due to the stronger localization of the electrons. Finally, the effective HFI in organic light emitting diodes is found to be a superposition of effective electron and hole HFI. Such a statistical relation may be generally applied to other semiconductingmore » polymers. Lastly, this Letter may provide great benefits for organic optoelectronics, chemical reaction kinetics, and magnetoreception in biology.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [2]; ORCiD logo [3];  [3]; ORCiD logo [3];  [4];  [1]
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  1. Univ. of Georgia, Athens, GA (United States). Dept. of Physics and Astronomy
  2. Univ. of Science and Technology of China, Hefei (China). Hefei National Lab. for Physical Sciences at the Microscale, Dept. of Physics, and Collaborative Innovation Center of Advanced Microstructures
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  4. Univ. of Georgia, Athens, GA (United States). College of Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1494885
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 8; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Geng, Rugang, Subedi, Ram C., Luong, Hoang M., Pham, Minh T., Huang, Weichuan, Li, Xiaoguang, Hong, Kunlun, Shao, Ming, Xiao, Kai, Hornak, Lawrence A., and Nguyen, Tho D. Effect of Charge Localization on the Effective Hyperfine Interaction in Organic Semiconducting Polymers. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.086602.
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Geng, Rugang, Subedi, Ram C., Luong, Hoang M., Pham, Minh T., Huang, Weichuan, Li, Xiaoguang, Hong, Kunlun, Shao, Ming, Xiao, Kai, Hornak, Lawrence A., & Nguyen, Tho D. Effect of Charge Localization on the Effective Hyperfine Interaction in Organic Semiconducting Polymers. United States. https://doi.org/10.1103/PhysRevLett.120.086602
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Geng, Rugang, Subedi, Ram C., Luong, Hoang M., Pham, Minh T., Huang, Weichuan, Li, Xiaoguang, Hong, Kunlun, Shao, Ming, Xiao, Kai, Hornak, Lawrence A., and Nguyen, Tho D. Thu . "Effect of Charge Localization on the Effective Hyperfine Interaction in Organic Semiconducting Polymers". United States. https://doi.org/10.1103/PhysRevLett.120.086602. https://www.osti.gov/servlets/purl/1494885.
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@article{osti_1494885,
title = {Effect of Charge Localization on the Effective Hyperfine Interaction in Organic Semiconducting Polymers},
author = {Geng, Rugang and Subedi, Ram C. and Luong, Hoang M. and Pham, Minh T. and Huang, Weichuan and Li, Xiaoguang and Hong, Kunlun and Shao, Ming and Xiao, Kai and Hornak, Lawrence A. and Nguyen, Tho D.},
abstractNote = {Hyperfine interaction (HFI), originating from the coupling between spins of charge carriers and nuclei, has been demonstrated to strongly influence the spin dynamics of localized charges in organic semiconductors. Nevertheless, the role of charge localization on the HFI strength in organic thin films has not yet been experimentally investigated. In this study, the statistical relation hypothesis that the effective HFI of holes in regioregular poly(3-hexylthiophene) (P3HT) is proportional to 1/N0.5 has been examined, where N is the number of the random nuclear spins within the envelope of the hole wave function. First, by studying magnetoconductance in hole-only devices made by isotope-labeled P3HT we verify that HFI is indeed the dominant spin interaction in P3HT. Second, assuming that holes delocalize fully over the P3HT polycrystalline domain, the strength of HFI is experimentally demonstrated to be proportional to 1/N0.52 in excellent agreement with the statistical relation. Third, the HFI of electrons in P3HT is about 3 times stronger than that of holes due to the stronger localization of the electrons. Finally, the effective HFI in organic light emitting diodes is found to be a superposition of effective electron and hole HFI. Such a statistical relation may be generally applied to other semiconducting polymers. Lastly, this Letter may provide great benefits for organic optoelectronics, chemical reaction kinetics, and magnetoreception in biology.},
doi = {10.1103/PhysRevLett.120.086602},
journal = {Physical Review Letters},
number = 8,
volume = 120,
place = {United States},
year = {Thu Feb 22 00:00:00 EST 2018},
month = {Thu Feb 22 00:00:00 EST 2018}
}
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Journal Article:
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https://doi.org/10.1103/PhysRevLett.120.086602
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Cited by: 22 works
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Figures / Tables:

Figure 1 Figure 1: (a) Raman spectra of isotope-labeled P3HT. The insets show the chemical structures of hydrogenated P3HT and full-deuterated P3HT. (b) Photoluminescence of the isotopes at a low temperature of 10 K. (c) IV characteristics and (d) MC (with 0.5 G resolution) of the isotopebased hole-only devices at 10 K.
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    Tuning effective hyperfine fields in PEDOT:PSS thin films by doping
    text, January 2018

    Magnetically Tunable Organic Semiconductors with Superparamagnetic Nanoparticles
    preprint, January 2019

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