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

Yixuan Dou; Catherine Demangeat; Miaosheng Wang; Hengxing Xu; Bogdan Dryzhakov; Eunkyoung Kim; Tangui Le Bahers; Kwang Sup Lee; André Jean Attias; Bin Hu

doi:10.1038/s41467-021-23791-9

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

Yixuan Dou, Catherine Demangeat, Miaosheng Wang, Hengxing Xu, Bogdan Dryzhakov, Eunkyoung Kim, Tangui Le Bahers, Kwang Sup Lee, André Jean Attias, Bin Hu

Department of Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

4 Citations (Scopus)

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.

Original language	English
Article number	3485
Journal	Nature communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-23791-9
Publication status	Published - 2021 Dec 1

Bibliographical note

Funding Information:
This research was supported by Air Force Office of Scientific Research (AFOSR) under the grant number AOARD (FA2386-17-1-4060; FA2386-15-1-4104), and National Science Foundation (NSF-1911659). This research was partially conducted at the Center for Nanophase Materials Sciences based on user projects (CNMS2019-245), which is sponsored by Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. The author (Y.D.) acknowledges the financial support from the China Scholarship Council through university agreement for her Ph.D. study at the University of Tennessee. The UTK authors thank the Center for Materials Processing, a Center of Excellence at the University of Tennessee at Knoxville, funded by the Tennessee Higher Education Commission, for financial support (M.W.). We also thank Professor Frank Loeffler, Dr. Gao Chen, and Yanchen Sun for the help on the HPLC test at the University of Tennessee at Knoxville.

Publisher Copyright:
© 2021, The Author(s).

All Science Journal Classification (ASJC) codes

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

Access to Document

10.1038/s41467-021-23791-9

Cite this

@article{c914e2a9995c4592a654e56f15fb13d2,

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.",

author = "Yixuan Dou and Catherine Demangeat and Miaosheng Wang and Hengxing Xu and Bogdan Dryzhakov and Eunkyoung Kim and {Le Bahers}, Tangui and Lee, {Kwang Sup} and Attias, {Andr{\'e} Jean} and Bin Hu",

note = "Funding Information: This research was supported by Air Force Office of Scientific Research (AFOSR) under the grant number AOARD (FA2386-17-1-4060; FA2386-15-1-4104), and National Science Foundation (NSF-1911659). This research was partially conducted at the Center for Nanophase Materials Sciences based on user projects (CNMS2019-245), which is sponsored by Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. The author (Y.D.) acknowledges the financial support from the China Scholarship Council through university agreement for her Ph.D. study at the University of Tennessee. The UTK authors thank the Center for Materials Processing, a Center of Excellence at the University of Tennessee at Knoxville, funded by the Tennessee Higher Education Commission, for financial support (M.W.). We also thank Professor Frank Loeffler, Dr. Gao Chen, and Yanchen Sun for the help on the HPLC test at the University of Tennessee at Knoxville. Publisher Copyright: {\textcopyright} 2021, The Author(s).",

year = "2021",

month = dec,

day = "1",

doi = "10.1038/s41467-021-23791-9",

language = "English",

volume = "12",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

number = "1",

}

TY - JOUR

T1 - Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping

AU - Dou, Yixuan

AU - Demangeat, Catherine

AU - Wang, Miaosheng

AU - Xu, Hengxing

AU - Dryzhakov, Bogdan

AU - Kim, Eunkyoung

AU - Le Bahers, Tangui

AU - Lee, Kwang Sup

AU - Attias, André Jean

AU - Hu, Bin

N1 - Funding Information: This research was supported by Air Force Office of Scientific Research (AFOSR) under the grant number AOARD (FA2386-17-1-4060; FA2386-15-1-4104), and National Science Foundation (NSF-1911659). This research was partially conducted at the Center for Nanophase Materials Sciences based on user projects (CNMS2019-245), which is sponsored by Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. The author (Y.D.) acknowledges the financial support from the China Scholarship Council through university agreement for her Ph.D. study at the University of Tennessee. The UTK authors thank the Center for Materials Processing, a Center of Excellence at the University of Tennessee at Knoxville, funded by the Tennessee Higher Education Commission, for financial support (M.W.). We also thank Professor Frank Loeffler, Dr. Gao Chen, and Yanchen Sun for the help on the HPLC test at the University of Tennessee at Knoxville. Publisher Copyright: © 2021, The Author(s).

PY - 2021/12/1

Y1 - 2021/12/1

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85107475079&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85107475079&partnerID=8YFLogxK

U2 - 10.1038/s41467-021-23791-9

DO - 10.1038/s41467-021-23791-9

M3 - Article

C2 - 34108487

AN - SCOPUS:85107475079

SN - 2041-1723

VL - 12

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 3485

ER -

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

Abstract

Bibliographical note

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this