We have studied the two-and three-photon absorption(2PA and 3PA) properties of Mn-doped CsPbCl_3 twodimensional nanoplatelets(2D NPs) and cubic nanocrystals. Compared with their cubic counterparts, the Mn-doped 2D NPs...We have studied the two-and three-photon absorption(2PA and 3PA) properties of Mn-doped CsPbCl_3 twodimensional nanoplatelets(2D NPs) and cubic nanocrystals. Compared with their cubic counterparts, the Mn-doped 2D NPs exhibit stronger quantum confinement effects that can more efficiently enhance their dopantcarrier exchange interactions and multiphoton absorption. More specifically, the maximum volume-normalized 2PA and 3PA cross sections of the 2D NPs were 6.8 and 7.2 times greater than those of their cubic counterparts,respectively, reaching up to 1237 GM∕nm^3 in the visible light band and 2.24 × 10^(-78) cm^6· s^2· photon^(-2)∕nm^3 in the second biological window, respectively.展开更多
Fabricating high-quality cesium lead chloride(CsPbCl_3) perovskite nanowires(NWs) with dimension below 10 nm is not only of interests in fundamental physics, but also holds the great promise for optoelectronic applica...Fabricating high-quality cesium lead chloride(CsPbCl_3) perovskite nanowires(NWs) with dimension below 10 nm is not only of interests in fundamental physics, but also holds the great promise for optoelectronic applications. Herein, ultrathin CsPbCl_3 NWs with height of ～7 nm, have been achieved via vapor phase deposition method. Power and temperature-dependent photoluminescence(PL) spectroscopy is performed to explore the emission properties of the CsPbCl_3 NWs. Strong free exciton recombination is observed at ～3.02 eV as the temperature(T) is 78-294 K with binding energy of ～ 37.5 meV. With the decreasing of T, the PL peaks exhibit a first blueshift by 2 meV for T ～ 294-190 K and then a redshift by 4 meV for T ～ 190-78 K. The exciton–optical phonon interaction plays a major role in the linewidth broadening of the PL spectra with average optical phonon energy of ～48.0 meV and the interaction coefficient of 203.9 meV. These findings advance the fabrication of low dimensional CsPbCl_3 perovskite and provide insights into the photophysics of the CsPbCl_3 perovskite.展开更多
CsPbCl_(3) perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice ene...CsPbCl_(3) perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice energy and low polarizability result in extremely low solubility in conventional solvents, making the synthesis of CsPbCl_(3) single crystals a significant challenge. In this study, we propose a novel thermodynamically induced crystal restructuring (TICR) process that can transform microcrystalline films (MCFs) into single crystal films (SCFs) within a short period. This method, for the first time, has successfully achieved the synthesis of centimeter-sized CsPbCl_(3) SCFs and the mechanism has been explored in depth using in-situ techniques. Furthermore, we report the first instance of a CsPbCl_(3) SCF UV photodiode, which exhibits a record-breaking on/off ratio of 3.32 × 10^(7) and a detectivity of up to 1.15 × 10^(14) Jones under 0 V bias. It demonstrates excellent response even under weak light conditions of 10 nW·cm^(−2) and maintains outstanding stability with almost no performance degradation after 15 months. This study provides a novel approach for the synthesis of perovskite single crystals and holds significant potential for advancing the development of high-performance optoelectronic devices.展开更多
基金Shenzhen Basic Research Project of Science and Technology(JCYJ20150324141711581,JCYJ20170302142433007)Postgraduate Innovation Development Fund Project of Shenzhen University(PIDFPZR2018007)
文摘We have studied the two-and three-photon absorption(2PA and 3PA) properties of Mn-doped CsPbCl_3 twodimensional nanoplatelets(2D NPs) and cubic nanocrystals. Compared with their cubic counterparts, the Mn-doped 2D NPs exhibit stronger quantum confinement effects that can more efficiently enhance their dopantcarrier exchange interactions and multiphoton absorption. More specifically, the maximum volume-normalized 2PA and 3PA cross sections of the 2D NPs were 6.8 and 7.2 times greater than those of their cubic counterparts,respectively, reaching up to 1237 GM∕nm^3 in the visible light band and 2.24 × 10^(-78) cm^6· s^2· photon^(-2)∕nm^3 in the second biological window, respectively.
基金supported by National Natural Science Foundation of China(Nos.61774003,61521004,51472080)National Key Research and Development Program of China(Nos.2017YFA0205700,2017YFA0304600)+1 种基金Open Research Fund Program of the State Key Laboratory of Low-dimensional Quantum Physics(No.KF201706)Excellent Youth Foundation of Hubei Province(No.2017CFA038)
文摘Fabricating high-quality cesium lead chloride(CsPbCl_3) perovskite nanowires(NWs) with dimension below 10 nm is not only of interests in fundamental physics, but also holds the great promise for optoelectronic applications. Herein, ultrathin CsPbCl_3 NWs with height of ～7 nm, have been achieved via vapor phase deposition method. Power and temperature-dependent photoluminescence(PL) spectroscopy is performed to explore the emission properties of the CsPbCl_3 NWs. Strong free exciton recombination is observed at ～3.02 eV as the temperature(T) is 78-294 K with binding energy of ～ 37.5 meV. With the decreasing of T, the PL peaks exhibit a first blueshift by 2 meV for T ～ 294-190 K and then a redshift by 4 meV for T ～ 190-78 K. The exciton–optical phonon interaction plays a major role in the linewidth broadening of the PL spectra with average optical phonon energy of ～48.0 meV and the interaction coefficient of 203.9 meV. These findings advance the fabrication of low dimensional CsPbCl_3 perovskite and provide insights into the photophysics of the CsPbCl_3 perovskite.
基金the National Key Research and Development Program of China(Nos.2022YFB3803300 and 2023YFE0116800)Beijing Natural Science Foundation(No.IS23037).
文摘CsPbCl_(3) perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice energy and low polarizability result in extremely low solubility in conventional solvents, making the synthesis of CsPbCl_(3) single crystals a significant challenge. In this study, we propose a novel thermodynamically induced crystal restructuring (TICR) process that can transform microcrystalline films (MCFs) into single crystal films (SCFs) within a short period. This method, for the first time, has successfully achieved the synthesis of centimeter-sized CsPbCl_(3) SCFs and the mechanism has been explored in depth using in-situ techniques. Furthermore, we report the first instance of a CsPbCl_(3) SCF UV photodiode, which exhibits a record-breaking on/off ratio of 3.32 × 10^(7) and a detectivity of up to 1.15 × 10^(14) Jones under 0 V bias. It demonstrates excellent response even under weak light conditions of 10 nW·cm^(−2) and maintains outstanding stability with almost no performance degradation after 15 months. This study provides a novel approach for the synthesis of perovskite single crystals and holds significant potential for advancing the development of high-performance optoelectronic devices.
