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Creators/Authors contains: "Dou, Yixuan"

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  1. 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.

     
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  2. Abstract

    The ultralong‐lived upconversion luminescence with the lifetime of 0.48 s in a broad spectral range (530–650 nm) is observed in CD49 (9‐(3‐(5‐bromopyridin‐3‐yl)prop‐2‐yn‐1‐yl)‐9H‐carbazole) crystal designed with donor–acceptor (carbazole–pyridine) structures under infrared excitation, simultaneously accompanied with second harmonic generation (SHG). This phenomenon indicates orderly packing donor–acceptor structures form a nonlinearly polarizable ferroelectric‐like lattice with ultralong‐lived light‐emitting states, leading to much prolonged nonlinear optical behaviors. The persistent upconversion luminescence together with SHG is largely reduced when lowering crystallinity. This implies that nonlinearly polarizable ferroelectric‐like lattice provides the necessary condition to generate persistent upconversion luminescence. Evidently, persistent upconversion luminescence becomes completely lacking when only using ultralong‐lived light‐emitting states without nonlinearly polarizable ferroelectric‐like lattice, exampled by 4‐(dimethylamino)benzonitrile dispersed in polyvinyl alcohol matrix. Magneto‐photoluminescence shows that persistent upconversion luminescence is essentially a super‐delayed fluorescence from crystalline intermolecular charge‐transfer excitons formed in the nonlinearly polarizable ferroelectric‐like lattice. Magnetodielectrics indicate crystalline intermolecular charge‐transfer excitons are coupled with nonlinearly polarizable ferroelectric‐like lattice, leading to prolonged nonlinear optical behaviors shown as persistent upconversion luminescence through super delayed fluorescence. Therefore, crystalline intermolecular charge‐transfer excitons formed in nonlinearly polarizable ferroelectric‐like lattice provide an interesting platform to generate prolonged nonlinear optical behaviors toward developing persistent upconversion luminescence under multiphoton excitation.

     
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  3. Abstract

    Photoinduced polarization and orbit–orbit interaction are important issues in hybrid perovskites toward developing optoelectronic functionalities. This paper identifies that photoinduced polarization occurs in hybrid perovskites with mixed‐cation methylammonium (MA)/formamidinium (FA) (MAxFA(1−x)PbI3) by measuring bulk polarization at 1 MHz in a magnetic field. Interestingly, when the internal dipole moment is increased upon increasing the MA:FA ratio, the photoinduced dipolar polarization can be substantially enhanced, clarifying the controversial issue of whether photoexcitation can induce a dielectric polarization within dipolar polarization regime in hybrid perovskites. Furthermore, upon increasing photoinduced dipolar polarization, it is found that the intrinsic orbit–orbit interaction between excitons can be increased, revealed by monitoring photocurrent change (ΔJsc) upon switching the photoexcitation between linear and circular polarizations. This presents that organic cations are directly involved in the orbit–orbit interaction within band structures. Clearly, the studies provide an insightful understanding of the dipole moment effects on photoinduced dipolar polarization and orbit–orbit interaction between excitons in hybrid perovskites toward controlling the optoelectronic properties.

     
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