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1.
A dual‐phase all‐inorganic composite CsPbBr3‐CsPb2Br5 is developed and applied as the emitting layer in LEDs, which exhibited a maximum luminance of 3853 cd m–2, with current density (CE) of ≈8.98 cd A–1 and external quantum efficiency (EQE) of ≈2.21%, respectively. The parasite of secondary phase CsPb2Br5 nanoparticles on the cubic CsPbBr3 nanocrystals could enhance the current efficiency by reducing diffusion length of excitons on one side, and decrease the trap density in the band gap on the other side. In addition, the introduction of CsPb2Br5 nanoparticles could increase the ionic conductivity by reducing the barrier against the electronic and ionic transport, and improve emission lifetime by decreasing nonradiative energy transfer to the trap states via controlling the trap density. The dual‐phase all‐inorganic CsPbBr3‐CsPb2Br5 composite nanocrystals present a new route of perovskite material for advanced light emission applications.  相似文献   

2.
A new capacitive‐type humidity sensor is proposed using novel materials and fabrication process for practical applications in sensitive environments and cost‐effective functional devices that require ultrasensing performances. Metal halide perovskites (CsPbBr3 and CsPb2Br5) combined with diverse ceramics (Al2O3, TiO2, and BaTiO3) are selected as sensing materials for the first time, and nanocomposite powders are deposited by aerosol deposition (AD) process. A state‐of‐the‐art CsPb2Br5/BaTiO3 nanocomposite humidity sensor prepared by AD process exhibits a significant increase in humidity sensing compared with CsPbBr3/Al2O3 and CsPbBr3/TiO2 sensors. An outstanding humidity sensitivity (21426 pF RH%?1) with superior linearity (0.991), fast response/recovery time (5 s), low hysteresis of 1.7%, and excellent stability in a wide range of relative humidity is obtained owing to a highly porous structure, effective charge separation, and water‐resistant characteristics of CsPb2Br5. Notably, this unprecedented result is obtained via a simple one‐step AD process within a few minutes at room temperature without any auxiliary treatment. The synergetic combination of AD technique and perovskite‐based nanocomposite can be potentially applied toward the development of multifunctional sensing devices.  相似文献   

3.
All‐inorganic halide perovskite materials are regarded as promising materials in information display applications owing to their tunable color, narrow emission peak, and easy processability. However, the photoluminescence (PL) stability of halide perovskite films is still inferior due to their poor thermal stability and hygroscopic properties. Herein, all‐inorganic perovskite films are prepared through vacuum thermal deposition method to enhance thermal and hygroscopic stability. By intentionally adding extra bromide source, a structure of CsPbBr3 nanocrystals embedded in a CsPb2Br5 matrix (CsPbBr3/CsPb2Br5) is formed via an air exposure process, leading to impressive PL stability in ambient atmosphere. In addition, the as‐fabricated CsPbBr3/CsPb2Br5 structure shows enhanced PL intensity due to the dielectric confinement. The CsPbBr3/CsPb2Br5 structure film can almost reserve its initial PL intensity after four months, even stored in ambient atmosphere. The PL intensity for CsPbBr3/CsPb2Br5 films vanishes at elevated temperature and recovers by cooling down in a short time. The reversible PL conversion process can be repeated over hundreds of times. Based on the reversible PL property, prototype thermal‐driven information display devices are demonstrated by employing heating circuits on flexible transparent substrates. These robust perovskite films with reversible PL characteristics promise an alternative solid‐state emitting display.  相似文献   

4.
The halide perovskite CsPbBr3 belongs to the Cs-Pb-Br material system, which features two additional thermodynamically stable ternary phases, Cs4PbBr6 and CsPb2Br5. The coexistence of these phases and their reportedly similar photoluminescence (PL) have resulted in a debate on the nature of the emission in these systems. Herein, optical and microscopic characterizations are combined with an effective mass, correlated electron–hole model of excitons in confined systems, to investigate the emission properties of the ternary phases in the Cs-Pb-Br system. It is found that all Cs-Pb-Br phases exhibit green emission and the non-perovskite phases exhibit PL quantum yields orders of magnitude larger than CsPbBr3. In particular, blue- and red-shifted emission for the Cs- and Pb-rich phases, respectively, are measured, stemming from embedded CsPbBr3 nanocrystals (NCs). This model reveals that the difference in emission shift is caused by the combined effects of NC size and different band mismatch. Furthermore, the importance of including the dielectric mismatch in the calculation of the emission energy for Cs-Pb-Br composites is demonstrated. The results explain the reportedly limited blue shift in CsPbBr3@Cs4PbBr6 composites and rationalize some of its differences with CsPb2Br5.  相似文献   

5.
The disappointing stability of perovskites, especially in water, remains a key issue hindering their further commercialization. Here, CsPbBr3/CsPb2Br5@PbBr(OH) (PQDs@PbBr(OH)) nano/microspheres with superior stability and outstanding photoluminescence quantum yield (PLQY, ≈98%) are fabricated through a water-assisted process. The nano/microspheres can maintain excellent photoluminescence (PL) intensity and high PLQY (≈90%) when immersed in water for more than 18 months. By changing the water content in the reaction mixture, the phase, particle size, and PL peaks of the nano/microspheres will change. Compared with CsPbBr3/Cs4PbBr6 nanocrystals synthesized without water, PQDs@PbBr(OH) nano/microspheres exhibit better thermal stability, photostability, and superior stability in water. Based on the first-principles calculations, the enhanced stability results from PbBr(OH) with high decomposition enthalpy in water, which can effectively prevent water from contacting PQDs embedded in it. Moreover, white light-emitting diodes are fabricated by mixing green-emitting PQDs@PbBr(OH) powder and K2SiF6:Mn4+ (KSF) red phosphor on a 460 nm blue chip and the device shows a high luminous efficacy of 101.27 lm W−1 at 10 mA. This work not only provides a reliable method for the facile preparation of ultrastable perovskites, but also has great potentials for future practical applications.  相似文献   

6.
1D perovskite materials are of significant interest to build a new class of nanostructures for electronic and optoelectronic applications. However, the study of colloidal perovskite nanowires (PNWs) lags far behind those of other established perovskite materials such as perovskite quantum dots and perovskite thin films. Herein, a dual-phase passivation strategy to synthesize all-inorganic PNWs with minimized surface defects is reported. The local phase transition from CsPbBr3 to CsPb2Br5 in PNWs increases the photoluminescence quantum yield, carrier lifetime, and water-resistivity, owing to the energetic and chemical passivation effect. In addition, these dual-phase PNWs are employed as an interfacial layer in perovskite solar cells (PSCs). The enhanced surface passivation results in an efficient carrier transfer in PSCs, which is a critical enabler to increase the power conversion efficiency (PCE) to 22.87%, while the device without PNWs exhibits a PCE of 20.74%. The proposed strategy provides a surface passivation platform in 1D perovskites, which can lead to the development of novel nanostructures for future optoelectronic devices.  相似文献   

7.
Self-assembly of nanocrystals into controlled structures while uncompromising their properties is one of the key steps in optoelectronic device fabrication. Herein, zigzag CsPbBr3 perovskite nanocrystals are demonstrated with a precise number of components with nanocube morphology, these can be successfully obtained through a dipole-induced self-assembly process. The addition of a trace amount of deionized water facilitates the transfer from CsPbBr3 nanocubes to intermediates of CsPb2Br5 and Cs3In2Br9, which then fastly release reaction monomers leading to further homogenous nucleation of CsPbBr3 nanocubes, followed by the formation of zigzag CsPbBr3 nanocrystals through a dipole-induced self-assembly process. Dipole moment along <110> axis is found to be the driving force for the assembly of nanocubes into zigzag nanocrystals. The zigzag CsPbBr3 nanocrystals exhibit desirable optical properties comparable to their nanocube counterparts and offer advantages for amplified spontaneous emission and lasing applications with low pump thresholds of 3.1 and 6.02 µJ cm−2, respectively. This study not only develops a strategy for producing highly controlled zigzag perovskite nanocrystals and provides insights on the dipole-induced self-assembly mechanisms, but also opens an avenue for their application in lasing.  相似文献   

8.
Perovskites have attracted intensive attention as promising materials for the application in various optoelectronic devices due to their large light absorption coefficient, high carrier mobility, and long charge carrier diffusion length. However, the performance of the pure perovskite nanocrystals-based device is extremely restricted by the limited charge transport capability due to the existence of a large number of the grain boundary between perovskite nanocrystals. To address these issues, a high-performance photodetector based on all-inorganic CsPbBr3 perovskite nanocrystals/2D non-layered cadmium sulfide selenide heterostructure has been demonstrated through energy band engineering with designed typed-II heterostructure. The photodetector exhibits an ultra-high light-to-dark current ratio of 1.36 × 105, a high responsivity of 2.89 × 102 A W−1, a large detectivity of 1.28 × 1014 Jones, and the response/recovery time of 0.53s/0.62 s. The enhancement of the optoelectronic performance of the heterostructure photodetector is mainly attributed to the efficient charge carrier transfer ability between the all-inorganic CsPbBr3 perovskites and 2D cadmium sulfide selenide resulting from energy band alignment engineering. The charge carriers’ transfer dynamics and the mechanism of the CsPbBr3 perovskites/2D non-layered nanosheets interfaces have also been studied by state-state PL spectra, fluorescence lifetime imaging microscopy, time-resolved photoluminescence spectroscopy, and Kelvin probe force microscopy measurements.  相似文献   

9.
Cesium‐based inorganic perovskites have recently attracted great research focus due to their excellent optoelectronic properties and thermal stability. However, the operational instability of all‐inorganic perovskites is still a main hindrance for the commercialization. Herein, a facile approach is reported to simultaneously enhance both the efficiency and long‐term stability for all‐inorganic CsPbI2.5Br0.5 perovskite solar cells via inducing excess lead iodide (PbI2) into the precursors. Comprehensive film and device characterizations are conducted to study the influences of excess PbI2 on the crystal quality, passivation effect, charge dynamics, and photovoltaic performance. It is found that excess PbI2 improves the crystallization process, producing high‐quality CsPbI2.5Br0.5 films with enlarged grain sizes, enhanced crystal orientation, and unchanged phase composition. The residual PbI2 at the grain boundaries also provides a passivation effect, which improves the optoelectronic properties and charge collection property in optimized devices, leading to a power conversion efficiency up to 17.1% with a high open‐circuit voltage of 1.25 V. More importantly, a remarkable long‐term operational stability is also achieved for the optimized CsPbI2.5Br0.5 solar cells, with less than 24% degradation drop at the maximum power point under continuous illumination for 420 h.  相似文献   

10.
All‐inorganic perovskite light‐emitting diodes (LEDs) reveal efficient luminescence with high color purity, but their modest brightness and poor stability are still critical drawbacks. Here, the luminescent efficiency and the stability of perovskite LEDs (PeLEDs) are boosted by antisolvent vapor treatment of CsPbBr3 embedded in a dielectric polymer matrix of polyethylene oxide (PEO). A unique method is developed to obtain high quality CsPbBr3 emitting layers with low defects by controlling their grain sizes. CsPbBr3 in PEO matrix is post‐treated with antisolvent of chloroform (CF), leading to microcrystals with a size of ≈5 µm along the in‐plane direction with active emitting composite of 90%. A device based on CF post‐treatment (CsPbBr3‐PEO‐CF) film displays a brightness of up to 51890 cd m?2 with an external quantum efficiency of 4.76%. CsPbBr3‐PEO‐CF PeLED still maintains 82% of its initial efficiency after 80 h continuous operation in ambient air, which indicates relatively good device stability. This work highlights that film quality is not only key to promoting fluorescence in CsPbBr3, but also to achieving higher performance PeLEDs.  相似文献   

11.
2D perovskites have attracted extensive attention due to their excellent stability compared with 3D perovskites. However, the intrinsic hydrophilicity of introduced alkylammonium salts effects the humidity stability of 2D/3D perovskites. Devices based on longer chain alkylammonium salts show improvement in hydrophobicity but lower efficiency due to the poorer charge transport among various layers. To solve this issue, two hydrophobic short‐chain alkylammonium salts with halogen functional groups (2‐chloroethylamine, CEA+ and 2‐bromoethylamine, BEA+) are introduced into (Cs0.1FA0.9)Pb(I0.9Br0.1)3 3D perovskites to form 2D/3D perovskite structure, which achieve high‐quality perovskite films with better crystallization and morphology. The optimal 2D/3D perovskite solar cells (PSCs) with 5% CEA+ display a power conversion efficiency (PCE) as high as 20.08% under 1 sun irradiation. Because of the notable hydrophobicity of alkylammonium cations with halogen functional groups and the formed 2D/3D perovskite structure, the optimal PSCs exhibit superior moisture resistance and retain 92% initial PCE after aging at 50 ± 5% relative humidity for 2400 h. This work opens up a new direction for the design of new‐type 2D/3D PSCs with improved performance by employing proper alkylammonium salts with different functional groups.  相似文献   

12.
Recent years have witnessed a rapid development of all‐inorganic halide perovskite in optoelectronic devices. Ultrathin 2D CsPbBr3 nanosheets (NSs) with large lateral dimensions have demonstrated exceptional photophysical properties because of their analogous exciton electronic structure to quantum wells. Despite the incredible progress on device performance, the photophysics and carrier transportation parameters of quantum‐confined CsPbBr3 NSs are lacking, and the fundamental understanding of the exciton dissociation mechanism is far less developed. Here, a ligands rearrangement mechanism is proposed to explain why annealed NS films have an increased charge transfer rate and a decreased exciton binding energy and lifetime, prompting tunneling as a dominant way of exciton dissociation to separate photogenerated excitons between neighboring NSs. This facile but efficient method provides a new insight to manipulate perovskite nanocrystals coupling. Moreover, ultrathin 2D CsPbBr3 NS film is demonstrated to have a enhanced absorption cross section and high carrier mobility of 77.9 cm2 V?1 s?1, contributing to its high responsivity of 0.53 A W?1. The photodetector has a long‐term stability up to three months, which are responsible for reliable perovskite‐based device performance.  相似文献   

13.
Light‐emitting diodes (LEDs) based on lead halide perovskites demonstrate outstanding optoelectronic properties and are strong competitors for display and lighting applications. While previous halide perovskite LEDs are mainly produced via solution processing, here an all‐vacuum processing method is employed to construct CsPbBr3 LEDs because vacuum processing exhibits high reliability and easy integration with existing OLED facilities for mass production. The high‐throughput combinatorial strategies are further adopted to study perovskite composition, annealing temperature, and functional layer thickness, thus significantly speeding up the optimization process. The best rigid device shows a current efficiency (CE) of 4.8 cd A?1 (EQE of 1.45%) at 2358 cd m?2, and best flexible device shows a CE of 4.16 cd A?1 (EQE of 1.37%) at 2012 cd m?2 with good bending tolerance. Moreover, by choosing NiOx as the hole‐injection layer, the CE is improved to 10.15 cd A?1 and EQE is improved to a record of 3.26% for perovskite LEDs produced by vacuum deposition. The time efficient combinatorial approaches can also be applied to optimize other perovskite LEDs.  相似文献   

14.
Inorganic cesium lead halide perovskite (CsPbX3, X = Cl, Br, I) is a promising material for developing novel electronic and optoelectronic devices. Despite the substantial progress that has been made in the development of large perovskite single crystals, the fabrication of high‐quality 2D perovskite single‐crystal films, especially perovskite with a low symmetry, still remains a challenge. Herein, large‐scale orthorhombic CsPbBr3 single‐crystal thin films on zinc‐blende ZnSe crystals are synthesized via vapor‐phase epitaxy. Structural characterizations reveal a “CsPbBr3(110)//ZnSe(100), CsPbBr3[?110]//ZnSe[001] and CsPbBr3[001]//ZnSe[010]” heteroepitaxial relationship between the covering CsPbBr3 layer and the ZnSe growth substrate. It is exciting that the epitaxial film presents an in‐plane anisotropic absorption property from 350 to 535 nm and polarization‐dependent photoluminescence. Photodetectors based on the epitaxial film exhibit a high photoresponsivity of 200 A W?1, a large on/off current ratio exceeding 104, a fast photoresponse time of about 20 ms, and good repeatability at room temperature. Importantly, a strong polarization‐dependent photoresponse is also found on the device fabricated using the epitaxial CsPbBr3 film, making the orthorhombic perovskite promising building blocks for optoelectronic devices featured with anisotropy.  相似文献   

15.
As the most promising lead‐free branch, tin halide perovskites suffer from the severe oxidation from Sn2+ to Sn4+, which results in the unsatisfactory conversion efficiency far from what they deserve. In this work, by facile incorporation of methylammonium bromide in composition engineering, formamidinium and methylammonium mixed cations tin halide perovskite films with ultrahighly oriented crystallization are synthesized with the preferential facet of (001), and that oxidation is suppressed with obviously declined trap density. MA+ ions are responsible for that impressive orientation while Br ions account for their bandgap modulation. Depending on high quality of the optimal MA0.25FA0.75SnI2.75Br0.25 perovskite films, their device conversion efficiency surges to 9.31% in contrast to 5.02% of the control formamidinium tin triiodide perovskite (FASnI3) device, along with almost eliminated hysteresis. That also results in the outstanding device stability, maintaining above 80% of the initial efficiency after 300 h of light soaking while the control FASnI3 device fails within 120 h. This paper definitely paves a facile and effective way to develop high‐efficiency tin halide perovskites solar cells, optoelectronic devices, and beyond.  相似文献   

16.
Quasi‐2D (Q2D) lead halide perovskites have emerged as promising materials for light‐emitting diodes (LEDs) due to their tunable emission, slowed‐down carrier diffusion, and improved stability. However, they are primarily fabricated through solution methods, which hinders its large‐scale manufacture and practical applications. Physical‐vapor‐deposition (PVD) methods have well demonstrated the capability for reproducible, scalable, and layer‐by‐layer fabrication of high quality organic/inorganic thin films. Herein, for the first time, the full‐evaporation fabrication of organic–inorganic hybrid ((BA)2Csn?1PbnBr3n+1) Q2D–3D PeLEDs is demonstrated. The morphology and crystal phase of the perovskite are controlled from 3D to 2D by modulating material composition, annealing temperature, and film thicknesses. The confinement of carriers in 3D layers and the energy funnel effect are discovered and discussed. Importantly, a record high external quantum efficiency (EQE) of 5.3% based on evaporation method is achieved. Moreover, a centimeter‐scale PeLED (1.5 cm × 2 cm) is obtained. Furthermore, the T50 lifetime of the device with an initial brightness of 100 cd m?2 is found to be 90 min with a thin layer PMMA passivation, which is among the longest for all PVD processed PeLEDs. Overall, this work casts a solid stepping stone towards the fabrication of high‐performance PeLEDs on a large‐scale.  相似文献   

17.
Metal halide perovskites are rising as a competitive material for next‐generation light‐emitting diodes (LEDs). However, the development of perovskite LEDs is impeded by their fast carriers diffusion and poor stability in bias condition. Herein, quasi‐2D CsPbBr3 quantum wells homogeneously surrounded by inorganic crystalline Cs4PbBr6 of large bandgap are grown. The centralization of carriers in nanoregion facilitates radiative recombination and brings much enhanced luminescence quantum yield. The external quantum efficiency and luminescence intensity of the LEDs based on this nanocomposite are one order of magnitude higher than the conventional low‐dimensional perovskite. Meanwhile, the use of inorganic nanocomposite materials brings much improved device operation lifetime under constant electrical field.  相似文献   

18.
The sensitivity of organic–inorganic perovskites to environmental factors remains a major barrier for these materials to become commercially viable for photovoltaic applications. In this work, the degradation of formamidinium lead iodide (FAPbI3) perovskite in a moist environment is systematically investigated. It is shown that the level of relative humidity (RH) is important for the onset of degradation processes. Below 30% RH, the black phase of the FAPbI3 perovskite shows excellent phase stability over 90 d. Once the RH reaches 50%, degradation of the FAPbI3 perovskite occurs rapidly. Results from a Kelvin probe force microscopy study reveal that the formation of nonperovskite phases initiates at the grain boundaries and the phase transition proceeds toward the grain interiors. Also, ion migration along the grain boundaries is greatly enhanced upon degradation. A post‐thermal treatment (PTT) that removes chemical residues at the grain boundaries which effectively slows the degradation process is developed. Finally, it is demonstrated that the PTT process improves the performance and stability of the final device.  相似文献   

19.
Knowledge of the mechanism of formation, orientation, and location of phases inside thin perovskite films is essential to optimize their optoelectronic properties. Among the most promising, low toxicity, lead‐free perovskites, the tin‐based ones are receiving much attention. Here, an extensive in situ and ex situ structural study is performed on the mechanism of crystallization from solution of 3D formamidinium tin iodide (FASnI3), 2D phenylethylammonium tin iodide (PEA2SnI4), and hybrid PEA2FAn?1SnnI3n+1 Ruddlesden–Popper perovskites. Addition of small amounts of low‐dimensional component promotes oriented 3D‐like crystallite growth in the top part of the film, together with an aligned quasi‐2D bottom‐rich phase. The sporadic bulk nucleation occurring in the pure 3D system is negligible in the pure 2D and in the hybrid systems with sufficiently high PEA content, where only surface crystallization occurs. Moreover, tin‐based perovskites form through a direct conversion of a disordered precursor phase without forming ordered solvated intermediates and thus without the need of thermal annealing steps. The findings are used to explain the device performances over a wide range of composition and shed light onto the mechanism of the formation of one of the most promising Sn‐based perovskites, providing opportunities to further improve the performances of these interesting Pb‐free materials.  相似文献   

20.
Perovskite photodetectors have attracted intensive research interest due to promising applications in sensing, communication, and imaging. However, their performance is restricted by the narrow spectrum range, required power source, and instability in ambient environment. To address these issues, a self‐powered photodetector based on the inorganic CsPbBr3 perovskite nanowire array/conjugated‐polymer hybrid structure is designed. The spectra response range of the device can be extended to 950 nm, along with outstanding stability, fast response speed (111/306 µs), and large detectivity (1.2 × 1013 Jones). The performance parameters are comparable to or even better than most reported CsPbBr3 and conjugated‐polymer photodetectors. The excellent performance is mainly attributed to the efficient carrier generation, separation, and transport resulting from array structure and favorable band structure.  相似文献   

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