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
The purpose of this paper is to synthesize a micrometric inorganic perovskite CsPbCl_(3):Nd^(3+)and investigate the impact of doping with rare-earth ions on structural and optical properties,as well as energy transfer...The purpose of this paper is to synthesize a micrometric inorganic perovskite CsPbCl_(3):Nd^(3+)and investigate the impact of doping with rare-earth ions on structural and optical properties,as well as energy transfer pathways between the host and dopant.Herein,we report the solid-state reaction synthesis of a concentration series of CsPbCl_(3):x%Nd^(3+)annealed under a nitrogen atmosphere.Additional doping of a material that already exhibits luminescence with an optically active ion increases its application potential.Structural features were determined using X-ray powder diffraction and Raman spectroscopy.Morphology studies performed with scanning electron microscopy revealed micrometric,well-separated cubic-like crystallites with a good distribution of individual elements.Surprisingly,a photoluminescence(PL)study showed that only blue emission appears when the material is excited with a diode operating in the UV range.Apparently,the emission of Nd^(3+)ions can only be obtained with direct excitation of the lanthanide.The photoluminescence excitation(PLE)spectrum monitored for Nd^(3+)emission confirmed the lack of energy transfer between the host and dopant.Possible explanations for this behavior have been put forth and substantiated by the first-principles electronic structure calculations in the framework of hybrid density functional theory.展开更多
In the present work,an improved hot injection technique,namely microwave-assisted hot injection,for mass production of Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3))perovskite nanocrystals(NCs)was reported.This strategy...In the present work,an improved hot injection technique,namely microwave-assisted hot injection,for mass production of Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3))perovskite nanocrystals(NCs)was reported.This strategy combines the advantages of both microwave irradiation and hot injection,which represents characteristics such as homogeneous heating and rapid production of Mn^(2+):CsPbCl_(3)NCs with a homogeneous size distribution.Meanwhile,it exhibits the capacity for gram-scale synthesis of Mn^(2+):CsPbCl_(3)NCs.The Mn^(2+)doping concentrations can be facilely tailored by controlling the reaction temperatures and feed ratios of the MnCl_(2)precursor,resulting in their enhanced optical properties with a PL QY up to 65%,which is the highest among the Mn^(2+)-doped perovskite NCs ever reported.The as-constructed light emitting diodes(LEDs)based on Mn^(2+):CsPbCl_(3)NCs emit highly bright white light,suggesting their potential applications in optoelectronic devices.展开更多
In this study,we employed a luminescenct agent CsPbCl_(3) perovskite nanocrystal for Cu^(2+) detection,and achieved a prominent enhancement in sensitivity by the introduction of ytterbium acetate(Yb(OAc)_(3)).The intr...In this study,we employed a luminescenct agent CsPbCl_(3) perovskite nanocrystal for Cu^(2+) detection,and achieved a prominent enhancement in sensitivity by the introduction of ytterbium acetate(Yb(OAc)_(3)).The introduced Yb(OAc)_(3) is capable of causing a morphology transformation of CsPbCl_(3) nanocrystals from initial nanocubes into one-dimensional(1D)nanowires(NWs).The formed 1D CsPbCl_(3) NWs paved a direct charge transport path and exhibited low defect density as well as superior conductivity,which were beneficial to accelerating the rapid electron transport from the luminescent agent to Cu^(2+),and to give rise to an efficient inhibition of undesired charge trap,respectively.Besides,AcO−rendered a reduced steric hindrance during the formation of a copper-based counter-ion pair,thus improving the adsorption capacity of Cu^(2+) on the surface of the luminescent agent,CsPbCl_(3) nanocrystals.As results,the 1D Yb(OAc)_(3) passivated CsPbCl_(3) NWs exhibited efficient luminescence quenching for enhanced detection sensitivity.This Yb(OAc)_(3)-involved system exhibited a detection limit as low as 0.06 nM in the Cu^(2+) detection window range from 0 to 1000 nM,and such value is optimal in the documented works for Cu^(2+)detection based on luminescent perovskite materials.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
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
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funded by the National Science Center,Poland,grant no.NCN-2021/43/D/ST5/01865the support from the National Natural Science Foundation of China(Grant No.52161135110 and 12274048)the support from the Scientific and Technological Research Program of the Chongqing Municipal Education Commission(Grant No.KJQN202200629).
文摘The purpose of this paper is to synthesize a micrometric inorganic perovskite CsPbCl_(3):Nd^(3+)and investigate the impact of doping with rare-earth ions on structural and optical properties,as well as energy transfer pathways between the host and dopant.Herein,we report the solid-state reaction synthesis of a concentration series of CsPbCl_(3):x%Nd^(3+)annealed under a nitrogen atmosphere.Additional doping of a material that already exhibits luminescence with an optically active ion increases its application potential.Structural features were determined using X-ray powder diffraction and Raman spectroscopy.Morphology studies performed with scanning electron microscopy revealed micrometric,well-separated cubic-like crystallites with a good distribution of individual elements.Surprisingly,a photoluminescence(PL)study showed that only blue emission appears when the material is excited with a diode operating in the UV range.Apparently,the emission of Nd^(3+)ions can only be obtained with direct excitation of the lanthanide.The photoluminescence excitation(PLE)spectrum monitored for Nd^(3+)emission confirmed the lack of energy transfer between the host and dopant.Possible explanations for this behavior have been put forth and substantiated by the first-principles electronic structure calculations in the framework of hybrid density functional theory.
基金supported by the National Natural Science Foundation for Excellent Young Scholars of China(Grant No.51522402)the National Natural Science Foundation of China(NSFC,Grant No.51572133,51672137 and 51702175)+1 种基金the Zhejiang Provincial Nature Science Foundation(Grant No.LQ17E020002)the and Natural Science Foundation of Ningbo Municipal Government(Grant No.2017A610002).
文摘In the present work,an improved hot injection technique,namely microwave-assisted hot injection,for mass production of Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3))perovskite nanocrystals(NCs)was reported.This strategy combines the advantages of both microwave irradiation and hot injection,which represents characteristics such as homogeneous heating and rapid production of Mn^(2+):CsPbCl_(3)NCs with a homogeneous size distribution.Meanwhile,it exhibits the capacity for gram-scale synthesis of Mn^(2+):CsPbCl_(3)NCs.The Mn^(2+)doping concentrations can be facilely tailored by controlling the reaction temperatures and feed ratios of the MnCl_(2)precursor,resulting in their enhanced optical properties with a PL QY up to 65%,which is the highest among the Mn^(2+)-doped perovskite NCs ever reported.The as-constructed light emitting diodes(LEDs)based on Mn^(2+):CsPbCl_(3)NCs emit highly bright white light,suggesting their potential applications in optoelectronic devices.
基金supported by the National Natural Science Foundation of China(Grant No.61822506,11974142,11874181,12174151)the Fundamental Research Funds for the Central Universities.
文摘In this study,we employed a luminescenct agent CsPbCl_(3) perovskite nanocrystal for Cu^(2+) detection,and achieved a prominent enhancement in sensitivity by the introduction of ytterbium acetate(Yb(OAc)_(3)).The introduced Yb(OAc)_(3) is capable of causing a morphology transformation of CsPbCl_(3) nanocrystals from initial nanocubes into one-dimensional(1D)nanowires(NWs).The formed 1D CsPbCl_(3) NWs paved a direct charge transport path and exhibited low defect density as well as superior conductivity,which were beneficial to accelerating the rapid electron transport from the luminescent agent to Cu^(2+),and to give rise to an efficient inhibition of undesired charge trap,respectively.Besides,AcO−rendered a reduced steric hindrance during the formation of a copper-based counter-ion pair,thus improving the adsorption capacity of Cu^(2+) on the surface of the luminescent agent,CsPbCl_(3) nanocrystals.As results,the 1D Yb(OAc)_(3) passivated CsPbCl_(3) NWs exhibited efficient luminescence quenching for enhanced detection sensitivity.This Yb(OAc)_(3)-involved system exhibited a detection limit as low as 0.06 nM in the Cu^(2+) detection window range from 0 to 1000 nM,and such value is optimal in the documented works for Cu^(2+)detection based on luminescent perovskite materials.
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.
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.
