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 Bahers, Kwang-Sup Lee, André-Jean Attias () and Bin Hu ()
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Yixuan Dou: University of Tennessee
Catherine Demangeat: CNRS - Sorbonne Université -Yonsei University
Miaosheng Wang: University of Tennessee
Hengxing Xu: University of Tennessee
Bogdan Dryzhakov: University of Tennessee
Eunkyoung Kim: CNRS - Sorbonne Université -Yonsei University
Tangui Bahers: CNRS - Sorbonne Université -Yonsei University
Kwang-Sup Lee: Hannam University
André-Jean Attias: CNRS - Sorbonne Université -Yonsei University
Bin Hu: University of Tennessee

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-23791-9

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