All-inorganic Lead Halide Perovskite Research Articles

On-Wire Design of Axial Periodic Halide Perovskite Superlattices for High-Performance Photodetection.

Precise synthesis of all-inorganic lead halide perovskite nanowire heterostructures and superlattices with designable modulation of chemical compositions is essential for tailoring their optoelectronic properties. Nevertheless, controllable synthesis of perovskite nanostructure heterostructures remains challenging and underexplored to date. Here, we report a rational strategy for wafer-scale synthesis of one-dimensional periodic CsPbCl3/CsPbI3 superlattices. We show that the highly parallel array of halide perovskite nanowires can be prepared roughly as horizontally guided growth on an M-plane sapphire. A periodic patterning of the sapphire substrate enables position-selective ion exchange to obtain highly periodic CsPbCl3/CsPbI3 nanowire superlattices. This patterning is further confirmed by micro-photoluminescence investigations, which show that two separate band-edge emission peaks appear at the interface of a CsPbCl3/CsPbI3 heterojunction. Additionally, compared with the pure CsPbCl3 nanowires, photodetectors fabricated using these periodic heterostructure nanowires exhibit superior photoelectric performance, namely, high ION/IOFF ratio (104), higher responsivity (49 A/W), and higher detectivity (1.51 × 1013 Jones). Moreover, a spatially resolved visible image sensor based on periodic nanowire superlattices is demonstrated with good imaging capability, suggesting promising application prospects in future photoelectronic imaging systems. All these results based on the periodic CsPbCl3/CsPbI3 nanowire superlattices provides an attractive material platform for integrated perovskite devices and circuits.

Enhanced ambient-stability and charge transport property of the CsPbBr3@Polyaniline

Although all-inorganic lead halide perovskites (CsPbX3 (X = Cl, Br, I)) have received widespread attention due to excellent optoelectronic properties, their low carrier mobility and poor stability have limited their application in photodetection. In this study, to alleviate these problems, CsPbBr3@Polyaniline composite is fabricated by passivating CsPbBr3 quantum dots (QDs) into a CSA-doped polyaniline conducting polymer. Notably, polyaniline is employed as a protective layer to block the structure damage of CsPbBr3 QDs against water, light and heat. The contact between polyaniline and CsPbBr3 QDs forms a type II heterojunction for charge transfer, which greatly reduces the recombination rate of charge carriers compared to pristine CsPbBr3 QDs. Benefiting from the high stability and enhanced charge mobility, CsPbBr3@Polyaniline-based photodetector achieves improved photocurrent signal and optical response time. The results demonstrate that the surface passivation could resolve the crucial stability problem and simultaneously facilitate the superior performance of perovskite optoelectronic devices.

Size Dependence of Ultrafast Electron Transfer from Didodecyl Dimethylammonium Bromide-Modified CsPbBr3 Nanocrystals to Electron Acceptors.

Charge transfer efficiencies in all-inorganic lead halide perovskite nanocrystals (NCs) are crucial for applications in photovoltaics and photocatalysis. Herein, CsPbBr3 NCs with different sizes are synthesized by varying the ligand contents of didodecyl dimethylammonium bromide at room temperature. Adding benzoquinone (BQ) molecules leads to a decrease in the PL intensities and PL decay times in NCs. The electron transfer (ET) efficiency (ηET) increases with NC size in complexes of CsPbBr3 NCs and BQ molecules (NC-BQ complexes), when the same concentration of BQ is maintained, as investigated by transient photobleaching and photoluminescence spectroscopies. Controlling the same number of attached BQ acceptor molecules per NC induces the same ηET in NC-BQ complexes even though with different NC sizes. Our findings provide new insights into ultrafast charge transfer behaviors in perovskite NCs, which is important for designing efficient light energy conversion devices.

Synthesis and performance optimization of CsPbBr3/CdS core/shell lead halide perovskite nanocrystals by an ion exchange method

All-inorganic lead halide perovskite nanocrystals (NCs) have excellent optoelectronic properties and promising applications. Improving the stability of inorganic halide NCs and optimizing their photoluminescence quantum yields (PLQY) has become an urgent task. Constructing core-shell structures is an effective method to improve the environmental stability and PLQY, however, realizing core-shell structured perovskite NCs with good dispersion and multiple perovskites encapsulated within the shell material remains challenging. In this work, CdS shells were grown on the surface of CsPbBr3 NCs by ion-exchange method utilizing perovskite NCs with their ionic properties, and the effectiveness of the surface shell protection is reflected in its enhancement of long-term storage stability, storage stability in water, and thermal stability of NCs. In addition, the PLQY and exciton binding energies of CsPbBr3/CdS NCs are increased. Finally, the NCs were packaged into green emitting LED devices and performed high stability. The results will facilitate the further commercialization of all-inorganic lead halide perovskite materials for optoelectronic devices.

Exceptional Stability against Water, UV Light, and Heat for CsPbBr3@Pb-MOF Composites.

All-inorganic lead halide perovskite nanocrystals (NCs) have been widely applied in optoelectronic devices owing to their excellent photoluminescence (PL) properties. However, poor stability upon exposure to water, UV light or heat strongly limits their practical application. Herein, CsPbBr3@Pb-MOF composites with exceptional stability against water, UV light, and heat are synthesized by ultrasonic processing the precursors of lead-based MOF (Pb-MOF), oleylammonium bromide (OAmBr) and cesium oleate (Cs-OA) solutions at room temperature. Pb-MOF can not only provide the lead source for the in situ growth of CsPbBr3 NCs, but also the protective layer of perovskites NCs. The formed CsPbBr3@Pb-MOF composites show a considerable PL quantum yield (PLQY) of 67.8%, and can maintain 90% of the initial PL intensity when immersed in water for 2 months. In addition, the outstanding PL stability against UV light and heat is demonstrated with CsPbBr3 NCs synthesized by the conventional method as a comparison. Finally, a green (light-emitting diode) LED is fabricated using green-emitting CsPbBr3@Pb-MOF composites and exhibits excellent stability without packaging when immersed in water for 30 days. This study provides a practical approach to improve the stability in aqueous phase, which may pave the way for future applications for various optoelectronic devices.

All-inorganic lead halide perovskites for photocatalysis: a review.

Nowadays, environmental pollution and the energy crisis are two significant concerns in the world, and photocatalysis is seen as a key solution to these issues. All-inorganic lead halide perovskites have been extensively utilized in photocatalysis and have become one of the most promising materials in recent years. The superior performance of all-inorganic lead halide perovskites distinguish them from other photocatalysts. Since pure lead halide perovskites typically have shortcomings, such as low stability, poor active sites, and ineffective carrier extraction, that restrict their use in photocatalytic reactions, it is crucial to enhance their photocatalytic activity and stability. Huge progress has been made to deal with these critical issues to enhance the effects of all-inorganic lead halide perovskites as efficient photocatalysts in a wide range of applications. In this manuscript, the synthesis methods of all-inorganic lead halide perovskites are discussed, and promising strategies are proposed for superior photocatalytic performance. Moreover, the research progress of photocatalysis applications are summarized; finally, the issues of all-inorganic lead halide perovskite photocatalytic materials at the current state and future research directions are also analyzed and discussed. We hope that this manuscript will provide novel insights to researchers to further promote the research on photocatalysis based on all-inorganic lead halide perovskites.

Enhancing the performance of PbS:CsPbBr3 bulk-heterojunction photodetectors by treating with imidazolium-based ionic liquids.

All-inorganic lead halide perovskites and quantum dots (QDs) have gained significant attention since their emergence, owing to their immense potential for applications in optoelectronic devices. Here, enhanced-performance broadband photodetectors based on the bulk-heterostructure of a CsPbBr3 perovskite and PbS colloidal quantum dots (CQDs) are presented, and 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM]BF4) ionic liquids as a dual-purpose additive were introduced in the blended film to regulate the surface of QDs by facilitating surface passivation, adjusting energy levels, and coupling with longer alkyl chains as compared to iodide ions (I-). As a result, a superior-quality bulk-heterostructure based photodetector with long-term stability was obtained, showing outstanding performance in photodetection across the visible to near-infrared wavelength range, demonstrating a high photoresponsivity of 22.4 A W-1 with a response time of 16.2 ms and a specific detectivity of 1.58 × 1014 Jones under 405 nm illumination. Thus, this work provides a novel modification strategy for PbS:CsPbBr3 as a promising material for novel optoelectronics.

Highly stable CsPbBr3 perovskite phases from new lead β-diketonate glyme adducts.

Lead is one of the key metals of the all-inorganic lead halide perovskites. This work tailors novel architectures of lead's coordination sphere using a β-diketone (H-hfa = 1,1,1,5,5,5-hexafluoro-2,4-pentanedione) and a glyme (monoglyme, diglyme, triglyme, or tetraglyme) ligand. The coordination chemistry and thermal behaviour of these "Pb(hfa)2·glyme" adducts have been analysed through FT-IR spectroscopy, 1H and 13C NMR analyses, thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). Single-crystal X-ray diffraction studies provide evidence of the formation of a monomeric Pb(hfa)2·monoglyme structure. In order to validate the potentiality of these "Pb(hfa)2·glyme" precursors for the fabrication of Pb-based halide perovskites, a facile, one-step and low-temperature solution approach has been applied to prepare CsPbBr3 microcrystals with a process carried out in air under atmospheric pressure. Pure stoichiometric CsPbBr3 powders, obtained using Cs(hfa) and Br2 as cesium and bromide sources, respectively, show excellent stability under atmospheric conditions. Better results are obtained in terms of yield and stability from the diglyme and tetraglyme lead adducts. Field emission scanning electron microscopy (FE-SEM) indicates a good uniform morphology of cubic grains, while the structure and the 1 : 1 : 3 stoichiometry of Cs : Pb : Br are confirmed by X-ray diffraction (XRD) and energy dispersive X-ray analysis (EDX), respectively. Tauc plots derived from absorption spectroscopy point to optical energy band-gaps (Eg) in the 2.21-2.27 eV range, in agreement with literature data. The present research elucidates the potential of these novel "Pb(hfa)2·glyme" adducts as promising lead precursors for CsPbBr3 perovskite synthesis, paving the way for their implementation in various technological applications.

Insight into the growth kinetics of CsPbBr3 perovskite nanocrystals using an oil-water droplet fluidic synthesis route

All-inorganic lead halide perovskite nanocrystals (PNCs) have attracted extensive attention in the optoelectronic fields owning to their exceptional photoluminescence characteristics. However, the ultra-fast growth rate of PNCs leads to challenges in controlling their size and optical properties. Here, we report a water–oil droplet fluidic synthesis method that successfully slow down the growth rate of CsPbBr3 PNCs by segregating the cation and anion precursors in the respective phases. Reaction mechanism study revealed a fast nucleation via a nanoplate-intermediate pathway upon HBr diffusion and subsequent slow growth through ripening, leading to a wide range of spectral tunability of the PNCs from 445 nm to 520 nm. The theoretical investigation into growth kinetics showed the combined effect of the ligands and temperature on the growth of the PNCs. This method provides an efficient means for producing high-performance PNCs with tunable size and wavelength while also eliminating the requirement for a Pb-rich reaction environment.

Water-stable perovskite-silica nanocomposites for encoded microbeads construction and multiplexed detection

All-inorganic lead halide perovskite nanocrystals exhibiting bright luminescence have great potential as fluorescence elements for optical encoding. However, their limited stability in water hinders the application in biosensing. In this study, novel optical encoded microbeads based on CsPbX3 (X = Cl, Br) nanocrystals are developed and applied in bead-based suspension arrays for the first time. Through the in-situ crystallization of CsPbX3 nanocrystals within mesoporous silica nano-templates (MSNs), accompanied by mesopores collapse after sintering, CsPbX3@MSNs (X3M) nanocomposites with uniform morphology and stable fluorescence intensity in aqueous solutions for up to 50 days are obtained. By assembling X3M with microspheres to form a host–guest structure, an optical encoding microbead (MX3M) library is established by varying the X3M ratio, halide composition, and the size of host microspheres, which can be easily decoded under multi-channel flow cytometer. As a result, MX3M exhibits outstanding capacity for specific target capture and negligible nonspecific absorption performance in the multiplex nucleic acid detection of respiratory viruses, with a low limit of detection (10 copies/rxn). This result highlights the tremendous potential of MX3M encoded microbeads constructed based on CsPbX3 nanocrystals for multiplexed bioassays.

Encapsulation of CsPb2Br5 in TiO2 Microcrystals to Enhance Environmental Stability.

All-inorganic lead halide perovskite has emerged as an attractive semiconducting material due to its unique optoelectronic properties. However, its poor environmental stability restricts its broad application. Here, a simple method for the fabrication of CsPb2Br5/TiO2 is investigated. The introduction of p-aminobenzoic acid, which has two functional groups, is critical for the capping of amorphous TiO2 on CsPb2Br5. After calcination at 300 °C, amorphous TiO2 crystallizes into the anatase phase. The CsPb2Br5/TiO2 NCs show high long-term stability in water and enhanced stability against ultraviolet radiation and heat treatment, owing to the chemical stability of TiO2. More importantly, photo-electrochemical characterizations indicate that the formation of TiO2 shells can increase the charge separation efficiency. Hence, CsPb2Br5/TiO2 exhibits improved photoelectric activity owing to the electrical conductivity of the TiO2 in water. This study provides a new route for the fabrication of optoelectronic devices and photocatalysts based on perovskite NCs in the aqueous phase. Furthermore, the present results demonstrate that CsPb2Br5/TiO2 NCs has considerable potential to be used as a photoelectric material in optical sensing and monitoring.

Field-Induced Transport Anisotropy in Single-Crystalline All-Inorganic Lead-Halide Perovskite Nanowires

Field-Induced Transport Anisotropy in Single-Crystalline All-Inorganic Lead-Halide Perovskite Nanowires

Study of a metal-halide perovskite CsPbBr3 thin film deposited on a 10B layer for neutron detection

Metal halide perovskite materials have received significant attention in recent years due to their promising properties and potential applications, particularly their use as scintillator detectors, which is rapidly emerging due to their promising advantages as detectors, such as low costs, fast response, high quantum yield, strong absorption, scalability, flexibility, and emission wavelength tunability. Given the effectiveness of perovskites as α particle detectors and the potential of 10B as a neutron converter, in this paper a 10B converting layer was coupled with an all-inorganic lead halide perovskite (CsPbBr3) layer aiming to create a thermal neutron detector. Specifically, a 1 µm thin film of 10B and a 1 µm thin layer of CsPbBr3 were deposited on a suitable substrate using a laser ablation process. The fabricated detector was subjected to a comprehensive characterization, including structural, morphological, and detection properties. As output, the films exhibit macroscopically uniform behavior and good adhesion to the substrate. In terms of thermal neutron efficiency, an efficiency of (7.9 ± 0.3)% was determined with respect to a commercial detector (EJ-426), which corresponds to an intrinsic efficiency of (2.5 ± 0.1)%. Also, Monte Carlo simulations were conducted, and the optimum value of the 10B layer thickness was found to be 2.5 µm.

Comprehensive Neurotoxicity of Lead Halide Perovskite Nanocrystals in Nematode Caenorhabditis elegans.

To date, all-inorganic lead halide perovskite quantum dots have emerged as promising materials for photonic, optoelectronic devices, and biological applications, especially in solar cells, raising numerous concerns about their biosafety. Most of the studies related to the toxicity of perovskite quantum dots (PeQDs) have focused on the potential risks of hybrid perovskites by using zebrafish or human cells. So far, the neurotoxic effects and fundamental mechanisms of PeQDs remain unknown. Herein, a comprehensive methodology is designed to investigate the neurotoxicity of PeQDs by using Caenorhabditis elegans as a model organism. The results show that the accumulation of PeQDs mainly focuses on the alimentary system and head region. Acute exposure to PeQDs results in a decrease in locomotor behaviors and pharyngeal pumping, whereas chronic exposure to PeQDs causes brood decline and shortens lifespan. In addition, some abnormal issues occur in the uterus during reproduction assays, such as vulva protrusion, impaired eggs left in the vulva, and egg hatching inside the mother. Excessive reactive oxygen species formation is also observed. The neurotoxicity of PeQDs is explained by gene expression. This study provides a complete insight into the neurotoxicity of PeQD and encourages the development of novel nontoxic PeQDs.

Tailoring the Electron and Hole Landé Factors in Lead Halide Perovskite Nanocrystals by Quantum Confinement and Halide Exchange.

The tunability of the optical properties of lead halide perovskite nanocrystals makes them highly appealing for applications. Halide anion exchange and quantum confinement enable tailoring of the band gap. For spintronics, the Landé g-factors of electrons and holes are essential. Using empirical tight-binding and k·p methods, we calculate them for nanocrystals of all-inorganic lead halide perovskites CsPbX3 (X = I, Br, Cl). The hole g-factor band gap dependence follows the universal law found for bulk perovskites, while for electrons, a considerable modification is predicted. Based on the k·p analysis, we conclude that this difference arises from the interaction of the bottom conduction band with the spin-orbit split electron states. These predictions are confirmed experimentally for electron and hole g-factors in CsPbI3 nanocrystals in a glass matrix, measured by time-resolved Faraday ellipticity in a magnetic field at cryogenic temperatures.

(Invited) Design of Perovskites for High-Performance Electronics and Optoelectronics

The success of lead halide perovskites as active materials in optoelectronic technologies is often associated with the unique properties of their optical excitations. Specifically, the photo-generated excitons in perovskites are responsible for the large absorption coefficients close to their band gap, reaching as high as 105 cm-1. Due to the advent of nanotechnology, perovskite materials can be readily fabricated into nanoscale configurations with different dimensionalities, and more importantly, the corresponding excitonic effects could be further enhanced. On the other hand, at length scales down to the nanoscale regime, surface features as well as quantum confinement effects, become dominant in regulating the advanced material properties of perovskite materials. [1, 2] In recent years, our group focused on the synthesis and characterization of metal halide perovskites with different forms, ranging from bulk film, microplate, and nanosheet, to nanowire. The corresponding physical properties and device applications were also systematically studied based on their widely tunable dimensionality, morphologies, and compositions.For perovskite bulk films, surface defects and bulk structural order significantly affect device performance. Through optimizing processing techniques, self-assemble quasi-2D perovskite films with graded phase distribution were successfully prepared by our group. [3] Gradient type-II band alignments along the out-of-plane direction of perovskites with spontaneous separation of photo-generated electrons and holes are obtained, which is further employed to construct self-powered vertical-structure photodetectors for the first time. Without any driving voltage, the device exhibited impressive performance with responsivity up to 444 mA/W and ultrashort response time down to 52 µs. In addition, to probe the intrinsic material properties of crystalline perovskites, freestanding MAPbI3 nanosheets, and lead-free Cs3Sb2I9 microplates were fabricated by two-step chemical vapor deposition method, in which excellent optoelectronic performance (e.g., responsively of MAPbI3 nanosheet is measured to be 40 A/W) together with ultra-fast response speed (down to 58 µs) and superior thermal stability were obtained. [4, 5]For nanostructured perovskites, understanding the dimensional features and their impact on the materials and devices is becoming increasingly important. For the first time, we reported the direct vapor-liquid-solid growth of single-crystalline all-inorganic lead halide perovskite (i.e., CsPbX3; X = Cl, Br, or I) NWs using Sn as catalyst seeds. [6] These NWs exhibited high-performance photodetection with the responsivity exceeding 4489 A/W and detectivity over 7.9 × 1012 Jones toward the visible light regime. Field-effect transistors based on individual CsPbX3 NWs were also fabricated to show the impressive carrier mobility of 3.05 cm2/Vs, being higher than other all-inorganic perovskite devices. After that, the Au catalyst seeds were used to avoid the Sn-related impurity doping, by which lower dark current and higher detectivity were achieved in Au-seeded CsPbI3 NWs. Besides, the realization of high-mobility CsPbBr3 NW devices is reported via a simple surface charge transfer doping strategy. [7] After MoO3 decoration and device fabrication, the hole mobility of CsPbBr3/MoO3 core-shell NW device is significantly enhanced to 23.3 cm2/Vs. All these results provide important guidelines for the further improvement of these perovskite nanostructures for practical utilization.

Negative Thermal Quenching in Quantum-Cutting Yb3+-Doped CsPb(Cl1-xBrx)3 Perovskite Nanocrystals.

Ytterbium-doped all-inorganic lead-halide perovskites (Yb3+:CsPb(Cl1-xBrx)3) show broadband absorption and exceptionally high near-infrared photoluminescence quantum yields, providing opportunities for solar spectral shaping to improve photovoltaic power conversion efficiencies. Here, we report that Yb3+:CsPb(Cl1-xBrx)3 NCs also show extremely strong negative thermal quenching of the Yb3+ luminescence, with intensities at room temperature >100 times those at 5 K for some compositions. Analysis of this temperature dependence as a function of x shows that it stems from thermally activated quantum cutting related to the temperature dependence of the spectral overlap between the PL of the perovskite (donor) and the simultaneous-pair absorption of two Yb3+ ions (acceptor). In the Yb3+:CsPbBr3 limit, this spectral overlap goes to zero at 5 K, such that only single-Yb3+ sensitization requiring massive phonon emission occurs. At room temperature, Yb3+ PL in this composition is enhanced ∼135-fold by thermally activated quantum cutting, highlighting the extreme efficiency of quantum cutting relative to single-Yb3+ sensitization. These results advance the fundamental mechanistic understanding of quantum cutting in doped perovskites, with potential ramifications for solar and photonics technologies.

One-step synthesis of all-inorganic high-entropy dual-phase Cs‘B’Br3/Cs‘B’2Br5 perovskite nanocrystals by high-energy ball milling

All-inorganic lead halide perovskite nanocrystals (NCs) have attracted considerable attention in field of optoelectronics due to their excellent properties such as high PLQY, tunable emission spectra in visible light region, and narrow emission peaks. However, problems existing in the research of all-inorganic lead halide perovskite materials are high lead content, low stability, and complex synthesis processes. Those problems need to be solved urgently. Therefore, dual-phase Cs‘B’Br3/Cs‘B’2Br5 perovskite material (Cs(Pb1/5Mn1/5Ni1/5Zn1/5Cd1/5)Br3/Cs(Pb1/5Mn1/5Ni1/5Zn1/5Cd1/5)2Br5) was synthesized by doping the B-site of CsPbBr3 and CsPb2Br5 using high-energy ball milling in this thesis. This dual-phase perovskite material has maximum absorption edge of 540 nm, a band gap width of 2.22 eV, the maximum emission peak at 600 nm with FWHM of 72 nm, PLQY of 24.50%, and an average fluorescence lifetime of 227.87 μs. After 21 days at room temperature, luminescent intensity of NCs increased to 156%, and still retained 109% at 120 days. After treatment at 150 °C, luminescent intensity decreased to 47%. Results show that this high-entropy dual-phase perovskite has great stability in different temperature. This proves that synthesis of high-entropy dual-phase halide perovskite by high-energy ball milling is feasible, and has great significance in solving poor stability and high lead content of all-inorganic lead halide perovskite in the future.

Multislip-enabled morphing of all-inorganic perovskites.

All-inorganic lead halide perovskites (CsPbX3, X = Cl, Br or I) are becoming increasingly important for energy conversion and optoelectronics because of their outstanding performance and enhanced environmental stability. Morphing perovskites into specific shapes and geometries without damaging their intrinsic functional properties is attractive for designing devices and manufacturing. However, inorganic semiconductors are often intrinsically brittle at room temperature, except for some recently reported layered or van der Waals semiconductors. Here, by in situ compression, we demonstrate that single-crystal CsPbX3 micropillars can be substantially morphed into distinct shapes (cubic, L and Z shapes, rectangular arches and so on) without localized cleavage or cracks. Such exceptional plasticity is enabled by successive slips of partial dislocations on multiple [Formula: see text] systems, as evidenced by atomic-resolution transmission electron microscopy and first-principles and atomistic simulations. The optoelectronic performance and bandgap of the devices were unchanged. Thus, our results suggest that CsPbX3 perovskites, as potential deformable inorganic semiconductors, may have profound implications for the manufacture of advanced optoelectronics and energy systems.

Hetero-integrated MoS2/CsPbBr3 photodetector with enhanced performance via combinational modulation of grain boundary passivation and interfacial carrier separation

The distinguished electronic and optical properties of all-inorganic lead halide perovskites (CsPbX3, X = Cl, Br, I) qualify them as ideal candidates for active layer in optoelectronic devices, especially showing more competitive development prospects in photodetection with high performance. However, superior device performance and good long-term stability is still a challenge for perovskite-based photodetectors applying in practical situation. Herein, we demonstrate a novel hetero-integrated MoS2/CsPbBr3 photodetector displaying efficient device performance, where the MoS2 nanocrystals pre-synthesized by hydrothermal route were spin-coated on the surface of CsPbBr3 films with controllable dispersion, providing effective interfacial photo-carriers separation at MoS2/CsPbBr3 van der Waals heterojunction (vdWH) and significant defect passivation for perovskite grain boundaries (GBs) simultaneously, thus boosting optoelectronic performance of our device within ultraviolet (UV)-visible wavelength range, including a higher photoresponsivity (4.79 A/W), enhanced specific detectivity (8.81 × 1012 Jones) and more durable stability than that of the pristine CsPbBr3 photodetector. Furthermore, the fast response speed (0.17/0.22 ms) is obviously more outstanding than that of most CsPbBr3-based and congeneric hybrid photodetectors. These results, combined with our experimental design strategy of the device described herein, provide an efficient approach to achieve stable, high-performance photodetection using perovskite-based hybrid nanomaterial systems, thus opening up new possibilities for two-dimensional (2D) materials/perovskites hetero-integration based photovoltaic and optoelectronic applications in the future.