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Title: Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping

Abstract

When periodically packing the intramolecular donor-acceptor structures to form ferroelectric-like lattice identified by second harmonic generation, our CD49 molecular crystal shows long-wavelength persistent photoluminescence peaked at 542 nm with the lifetime of 0.43 s, in addition to the short-wavelength prompt photoluminescence peaked at 363 nm with the lifetime of 0.45 ns. Interestingly, the long-wavelength persistent photoluminescence demonstrates magnetic field effects, showing as crystalline intermolecular charge-transfer excitons with singlet spin characteristics formed within ferroelectric-like lattice based on internal minority/majority carrier-balancing mechanism activated by isomer doping effects towards increasing electron-hole pairing probability. Our photoinduced Raman spectroscopy reveals the unusual slow relaxation of photoexcited lattice vibrations, indicating slow phonon effects occurring in ferroelectric-like lattice. Here, we show that crystalline intermolecular charge-transfer excitons are interacted with ferroelectric-like lattice, leading to exciton-lattice coupling within periodically packed intramolecular donor-acceptor structures to evolve ultralong-lived crystalline light-emitting states through slow phonon effects in ferroelectric light-emitting organic crystal.

Authors:
 [1];  [2]; ORCiD logo [1];  [1];  [1]; ORCiD logo [3]; ORCiD logo [4];  [5]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  2. Sorbonne Université -Yonsei University, Seoul (Korea,Republic of). Centre National de la Recherche Scientifique (CNRS). Building Blocks for FUture Electronics Laboratory. IRL
  3. Sorbonne Université -Yonsei University, Seoul (Korea,Republic of). Centre National de la Recherche Scientifique (CNRS). Building Blocks for FUture Electronics Laboratory. IRL; Yonsei Univ., Seoul (Korea, Republic of). Dept. of Chemical and Biomolecular Engineering
  4. Sorbonne Université -Yonsei University, Seoul (Korea,Republic of). Centre National de la Recherche Scientifique (CNRS). Building Blocks for FUture Electronics Laboratory. IRL; Univ. of Lyon (France). Centre National de la Recherche Scientifique (CNRS). Laboratorie de Chimie
  5. Hannam Univ., Daejeon (Korea, Republic of). Dept. of Advanced Materials and Chemical Engineering
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
OSTI Identifier:
1816952
Grant/Contract Number:  
AC05-00OR22725; FA2386-17-1-4060; FA2386-15-1-4104; NSF-1911659; CNMS2019-245
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 42 ENGINEERING; electronic devices; synthetic chemistry methodology

Citation Formats

Dou, Yixuan, Demangeat, Catherine, Wang, Miaosheng, Xu, Hengxing, Dryzhakov, Bogdan, Kim, Eunkyoung, Le Bahers, Tangui, Lee, Kwang-Sup, Attias, André-Jean, and Hu, Bin. Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping. United States: N. p., 2021. Web. doi:10.1038/s41467-021-23791-9.
Dou, Yixuan, Demangeat, Catherine, Wang, Miaosheng, Xu, Hengxing, Dryzhakov, Bogdan, Kim, Eunkyoung, Le Bahers, Tangui, Lee, Kwang-Sup, Attias, André-Jean, & Hu, Bin. Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping. United States. https://doi.org/10.1038/s41467-021-23791-9
Dou, Yixuan, Demangeat, Catherine, Wang, Miaosheng, Xu, Hengxing, Dryzhakov, Bogdan, Kim, Eunkyoung, Le Bahers, Tangui, Lee, Kwang-Sup, Attias, André-Jean, and Hu, Bin. Wed . "Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping". United States. https://doi.org/10.1038/s41467-021-23791-9. https://www.osti.gov/servlets/purl/1816952.
@article{osti_1816952,
title = {Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping},
author = {Dou, Yixuan and Demangeat, Catherine and Wang, Miaosheng and Xu, Hengxing and Dryzhakov, Bogdan and Kim, Eunkyoung and Le Bahers, Tangui and Lee, Kwang-Sup and Attias, André-Jean and Hu, Bin},
abstractNote = {When periodically packing the intramolecular donor-acceptor structures to form ferroelectric-like lattice identified by second harmonic generation, our CD49 molecular crystal shows long-wavelength persistent photoluminescence peaked at 542 nm with the lifetime of 0.43 s, in addition to the short-wavelength prompt photoluminescence peaked at 363 nm with the lifetime of 0.45 ns. Interestingly, the long-wavelength persistent photoluminescence demonstrates magnetic field effects, showing as crystalline intermolecular charge-transfer excitons with singlet spin characteristics formed within ferroelectric-like lattice based on internal minority/majority carrier-balancing mechanism activated by isomer doping effects towards increasing electron-hole pairing probability. Our photoinduced Raman spectroscopy reveals the unusual slow relaxation of photoexcited lattice vibrations, indicating slow phonon effects occurring in ferroelectric-like lattice. Here, we show that crystalline intermolecular charge-transfer excitons are interacted with ferroelectric-like lattice, leading to exciton-lattice coupling within periodically packed intramolecular donor-acceptor structures to evolve ultralong-lived crystalline light-emitting states through slow phonon effects in ferroelectric light-emitting organic crystal.},
doi = {10.1038/s41467-021-23791-9},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United States},
year = {Wed Jun 09 00:00:00 EDT 2021},
month = {Wed Jun 09 00:00:00 EDT 2021}
}

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