Perovskite-based Optoelectronic Devices Research Articles

Evolution of Defects, Morphology, and Strain during FAMAPbI3 Perovskite Vacuum Deposition: Insights from In Situ Photoluminescence and X-ray Scattering.

At present, the power conversion efficiency of single-junction perovskite-based solar cells reaches over 26%. The further efficiency increase of perovskite-based optoelectronic devices is limited mainly by defects, causing the nonradiative recombination of charge carriers. To improve efficiency and ensure reproducible fabrication of high-quality layers, it is crucial to understand the perovskite nucleation and growth mechanism along with associated process control to reduce the defect density. In this study, we investigate the growth kinetics of a promising narrow bandgap perovskite, formamidinium methylammonium lead iodide (FAMAPbI3), for high-performance single-junction solar cells. The temporal evolution of structural and optoelectronic properties during FAMAPbI3 vacuum codeposition was inspected in real time by grazing-incidence wide-angle X-ray scattering and photoluminescence. Such a combination of analytical techniques unravels the evolution of intrinsic defect density and layer morphology correlated with lattice strain from the early stages of the perovskite deposition.

High-performance CsPbBr3-silicon heterojunction photodetectors fabricated by chemical vapor deposition

Inorganic perovskite cesium lead halide (CsPbBr3) has attracted extensive research attention due to its excellent photoelectric properties and long-term stability to water, oxygen, light and heat. In this work, high crystallinity CsPbBr3 microcrystals with different morphologies and grain sizes were synthesized by one-step chemical vapor deposition (CVD) on silicon (Si) wafers and silicon nanowires (SiNWs), respectively. Characterization results show that the CsPbBr3 microcrystals grown on SiNWs (CsPbBr3-SiNWs) display more compact and uniform morphologies than those grown on Si wafer (CsPbBr3-Si). Moreover, CsPbBr3-SiNWs exhibits higher detectivity and larger on/off ratio than CsPbBr3-Si, which are 5.1 × 1012 Jones over 3.4 × 1012 Jones, and 51.3 over 14.7, respectively. Furthermore, CsPbBr3-SiNWs shows a faster photo response with a rise/fall time of 0.22 s/0.28 s than 0.26 s/0.32 s in CsPbBr3-Si. In addition, the CsPbBr3-SiNWs photodetector maintained 90% of its original photocurrent after 60 days of exposure to air, showing excellent stability. These results strongly suggest a promising fabrication approach for constructing perovskite-based heterojunction optoelectronic devices with high performance and excellent stability.

Defect Engineering and Emission Tuning of Wide-Bandgap MAPbCl3 Perovskite.

Lead-chloride perovskites are promising candidates for optoelectronic applications, such as visible-blind UV photodetection. It remains unclear how the deep defects in this wide-bandgap material impact the carrier recombination dynamics. In this work, we study the defect properties of MAPbCl3 (MA = CH3NH3) based on photoluminescence (PL) measurements. Our investigations show that apart from the intrinsic emission, four sub-bandgap emissions emerge, which are very likely to originate from the radiative recombination of excitons bound to several intrinsic vacancy and interstitial defects. The intensity of various emission features can be tuned by adjusting the type and ratio of precursors used during synthesis. Our study not only provides important insights into the defect property and carrier recombination mechanism in this class of material but also demonstrates efficient strategies for defect passivation and engineering, paving the way for further development of lead-chloride perovskite-based optoelectronic devices.

Computational synthesis of a new generation of 2D-based perovskite quantum materials

Perovskite-based optoelectronic devices have emerged as a promising energy source due to their potential for scalable production. This study introduces “perovskene,” a novel class of 2D materials derived from the ABC3-like perovskites, synthesized via a data-driven, high-throughput computational strategy. We harness machine learning and multitarget deep neural networks to systematically investigate the structure–property relations, paving the way for targeted material design and optimization in fields such as renewable energy, electronics, and catalysis. The characterization of over 1500 synthesized structures shows that more than 500 structures are stable, revealing properties such as ultra-low work function and large magnetic moment, underscoring the potential for advanced technological applications.

Photocurrent Enhancement by Copper Incorporation in Chemical-Solution-Synthesized Inorganic Lead Perovskite Thin Films.

Perovskite thin films are at the forefront of highly promising photovoltaic technologies due to their remarkable optoelectronic properties. Herein, we explore a low-cost, reproducible, and industry-scalable methodology to synthesize an all-inorganic CsPbI1.5Br1.5 perovskite thin film with additional incorporation of copper and chloride ions into the lattice structure. The synthesis process involves chemical bath deposition of PbS, followed by a gas-solid iodination reaction to yield PbI2. Subsequently, dip-coating incorporates Cs+, Cu2+, Br-, and Cl- ions into PbI2, and annealing at 270 °C produces perovskite thin films. The results show a large coverage area and a uniform thickness of each perovskite thin film. Comprehensive characterization, including X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, and photoluminescence, provides the structural, chemical, and optical properties of the synthesized thin films. To evaluate the practical implications of our methodology, we fabricated photodetectors employing CsPbI1.5Br1.5 and (Cs0.95:Cu0.01)PbI1.5Br1.3Cl0.1 perovskite films. A comparative analysis unequivocally demonstrates a significant increase in photodetector performance when utilizing (Cs0.95:Cu0.01)PbI1.5Br1.3Cl0.1 perovskite films. While our findings quantitatively assess the tangible enhancement in photocurrent, we acknowledge the potential for improvement in device fabrication to enhance the overall performance. This study not only affirms the successful low-cost synthesis of perovskite thin films but also emphasizes the pivotal role of Cu2+ and Cl- ions in enhancing the performance of perovskite-based optoelectronic devices.

Understanding Defects in Perovskite Solar Cells through Computation: Current Knowledge and Future Challenge.

Lead halide perovskites with superior optoelectrical properties are emerging as a class of excellent materials for applications in solar cells and light-emitting devices. However, perovskite films often exhibit abundant intrinsic defects, which can limit the efficiency of perovskite-based optoelectronic devices by acting as carrier recombination centers. Thus, an understanding of defect chemistry in lead halide perovskites assumes a prominent role in further advancing the exploitation of perovskites, which, to a large extent, is performed by relying on first-principles calculations. However, the complex defect structure, strong anharmonicity, and soft lattice of lead halide perovskites pose challenges to defect studies. In this perspective, on the basis of briefly reviewing the current knowledge concerning computational studies on defects, this work concentrates on addressing the unsolved problems and proposing possible research directions in future. This perspective particularly emphasizes the indispensability of developing advanced approaches for deeply understanding the nature of defects and conducting data-driven defect research for designing reasonable strategies to further improve the performance of perovskite applications. Finally, this work highlights that theoretical studies should pay more attention to establishing close and clear links with experimental investigations to provide useful insights to the scientific and industrial communities.

Unveiling heterogeneity of hysteresis in perovskite thin films

The phenomenon of current–voltage hysteresis observed in perovskite-based optoelectronic devices is a critical issue that complicates the accurate assessment of device parameters, thereby impacting performance and applicability. Despite extensive research efforts aimed at deciphering the origins of hysteresis, its underlying causes remain a subject of considerable debate. By employing nanoscale investigations to elucidate the relationship between hysteresis and morphological characteristics, this study offers a detailed exploration of photocurrent–voltage hysteresis at the nanoscale within perovskite optoelectronic devices. Through the meticulous analysis of localized I–V curve arrays, our research identifies two principal hysteresis descriptors, uncovering a predominantly inverted hysteresis pattern in 87% of the locations examined. This pattern is primarily attributed to the energetic barrier encountered at the interface between the probe and the perovskite material. Our findings underscore the pronounced heterogeneity and grain-dependent variability inherent in hysteresis behavior, evidenced by an average Hysteresis Index value of 0.24. The investigation suggests that the localized hysteresis phenomena cannot be exclusively attributed to either photocharge collection processes or organic cation migration at grain boundaries. Instead, it appears significantly influenced by localized surface trap states, which play a pivotal role in modulating electron and hole current dynamics. By identifying the key factors contributing to hysteresis, such as localized surface trap states and their influence on electron and hole current dynamics, our findings pave the way for targeted strategies to mitigate these effects. This includes the development of novel materials and device architectures designed to minimize energy barriers and enhance charge carrier mobility, thereby improving device performance and longevity. This breakthrough in understanding the microscale mechanisms of hysteresis underscores the critical importance of surface/interface defect trap passivation in mitigating hysteretic effects, offering new pathways for enhancing the performance of perovskite solar cells.

Exciton dynamics in two-dimensional metal halide perovskite: The impact of film processing.

We investigate the hot carrier and exciton dynamics in two-dimensional (2D) metal halide perovskites using time-resolved spectroscopy. 2D perovskite films were prepared with and without dimethyl sulfoxide treatment to elucidate the effect of film processing techniques on optoelectronic properties. Femtosecond transient absorption measurements reveal that the charge carrier dynamics are different in the two samples, and excitons survive for a longer time in the treated sample than the untreated one. While the early-time carrier dynamics in the untreated sample are dominated by charges trapped by defect states, the hot free carriers govern the dynamics in the treated sample due to fewer defects in it. Morphological and other spectroscopic studies, including time-resolved photoluminescence, further suggest the formation of more defects in the untreated sample. These results can guide the future development of efficient 2D perovskite-based optoelectronic devices.

ETL/perovskite interface engineering using cadmium and lead chalcogenide quantum dots

Photovoltaic (PV) technology plays a significant role in renewable energy research, while devices based on hybrid perovskite materials have reached efficiencies which exceed 26 %. Nevertheless, perovskite solar cells (PSCs) are facing chemical, thermal and humidity stability issues, which prevent their commercialization. Thus, the use of quantum dots (QDs) has been proposed as an innovative strategy to tackle with device performance issues. This work investigates the effect of PbS and CdS chalcogenide QDs on the interface modification of CsFAMAPbI3-xBrx PSCs. The successive ionic layer adsorption and reaction (SILAR) method was employed as an innovative engineering approach to adjust effectively the perovskite interface energetics and optimize the solar cell's characteristics. By tuning the deposition conditions of QDs and adding TiCl4 to the electron transport layer (ETL), an efficiency improvement from 15.52 to 18.83 % was recorded. These results highlight the use of a facile and fast method to integrate chalcogenide quantum dots into perovskite-based optoelectronic devices, thus improving the surface crystallinity and overall device performance.

Accelerated design of stable halide perovskite heterostructure film in hostile condition via surface modifier

The bulk halide perovskite heterostructure has been adopted for perovskite-based optoelectronic devices owing to their interesting interfacial phenomena; however, most of them are unstable in hostile condition and the extremely large virtual design space causes problems for traditional trial-and-error methods to optimize them. In this study, we combine photoelectrochemical experiments, machine learning and first-principles calculations (Exp + ML + DFT) to accelerate the design of halide perovskite heterostructures in aqueous solution, in an effort to improve stability of halide perovskite materials in hostile condition (prototypical CH3NH3PbI3 quickly deactivates in water within seconds). The optimization of halide perovskite heterojunction with surface modifier is speeded up via machine learning using extra tree algorithm, and a large virtual design space consisting of halide perovskite heterostructure composites is predicted. Five new water-stable perovskite heterostructure candidates predicted via machine learning are experimentally validated, and the first-principles calculations reveal the detailed atomic and electronic structures of an exemplar stable heterostructure candidate. This study demonstrates the effectiveness of machine learning to accelerate the design of stable halide perovskite heterostructure materials in hostile condition.

Experimental analysis of methylammonium and Formamidinium-based halide perovskite properties for optoelectronic applications

Nowadays, the toxicity of lead in metal-halide perovskites is the most precarious obstruction in the commercialization of perovskite-based optoelectronic devices. However, Pb-free metal halide perovskites as environment-friendly materials because of their exceptional properties, such as band-gap tunability, narrow emission spectra, low toxicity and easy solution-processability, are potential candidates for optoelectronic applications. Recently, literature reported the poor structural stability and low-emission intensity of Bi-based perovskite NCs. Still, this paper focuses on the fabrication of Formamidinium (FA)-based Bi mixed halide and Methylammonium(MA)-based Bi-pure halide perovskites using Ligand-Assisted Reprecipitation Technique (LARP) technique. XRD diffraction patterns of FA-based perovskites were slightly broad, signifying the nanocrystalline form and limited size of perovskite nanocrystals. While the XRD diffraction patterns of MA3Bi2X9 (X = Cl/Br/I) perovskites were narrow, signifying the amorphous nature and larger size of perovskite nanocrystals. The peak positions were varied in MA-based bismuth halide perovskites with respect to the halide variation from Br to Cl to I ions. The optical study shows the variation in band gap and average lifetime with respect to halide variation leading to enhanced optical properties for device applications. The band-gap of FA3Bi2BrxCl1-x & FA3Bi2IxCl1-x perovskites was calculated to be around 3.7 & 3.8 eV, respectively, while in MA-halide perovskites the band-gap was calculated to be 2.8 eV, 3.1 eV & 3.4 eV with respect to halide variation from I to Cl to Br in perovskite samples using Tauc's plot respectively. Moreover, simulation is carried out using the SCAPS-1D software to study the various parameters in MA & FA-based Bi-pure or mixed halide perovskites. Here, we discussed the variation in efficiency with respect to the thickness variation from 100 to 500 nm for MA3Bi2I9 halide perovskites. These MA3Bi2I9 halide perovskites show minimum efficiency of 4.65 % at 100 nm thickness, while the perovskite sample exhibits maximum efficiency of 10.32 % at 500 nm thickness. Thus, the results stated that the thickness of absorber layers directly affects the device characteristics for optoelectronic applications.

Boosting the Self-Trapped Exciton Emission in Cs4SnBr6 Zero-Dimensional Perovskite via Rapid Heat Treatment.

Zero-dimensional (0D) tin halide perovskites feature extraordinary properties, such as broadband emission, high photoluminescence quantum yield, and self-absorption-free characteristics. The innovation of synthesis approaches for high-quality 0D tin halide perovskites has facilitated the flourishing development of perovskite-based optoelectronic devices in recent years. However, discovering an effective strategy to further enhance their emission efficiency remains a considerable challenge. Herein, we report a unique strategy employing rapid heat treatment to attain efficient self-trapped exciton (STE) emission in Cs4SnBr6 zero-dimensional perovskite. Compared to the pristine Cs4SnBr6, rapid thermal treatment (RTT) at 200 °C for a duration of 120 s results in an augmented STE emission with the photoluminescence (PL) quantum yield rising from an initial 50.1% to a substantial 64.7%. Temperature-dependent PL spectra analysis, Raman spectra, and PL decay traces reveal that the PL improvement is attributed to the appropriate electron-phonon coupling as well as the increased binding energies of STEs induced by the RTT. Our findings open up a new avenue for efficient luminescent 0D tin-halide perovskites toward the development of efficient optoelectronic devices based on 0D perovskites.

A Multifunctional Liquid Crystal as Hole Transport Layer Additive Enhances Efficiency and Stability of Perovskite Solar Cells.

Lithium bis(trifluoromethanesulfonyl)imide (Li-TFSI) has been identified as the most used and effective p-dopant for hole transport layer (HTL) in perovskite solar cells (PSCs). However, the migration and agglomeration of Li-TFSI in HTL negatively impact PSCs performance and stability. Herein, we report an effective strategy for adding a liquid crystal organic small molecule (LQ) into Li-TFSI doped (2,2',7,7'-tetrakis(N,N-di-p-methoxyphenylamine)-9,9'- spirobifluorene (Spiro-OMeTAD) HTL. It was found that the introduction of LQ into Spiro-OMeTAD HTL can efficiently enhance the charge carrier extraction and transportation in device, which can strongly retard the charge-carrier recombination in device. Consequently, the PSCs efficiency is significantly enhanced to 24.42% (Spiro-OMeTAD+LQ) from 21.03% (Spiro-OMeTAD). The chemical coordination between LQ and Li-TFSI can strongly confine Li+ ions migration and agglomeration of Li-TFSI, thus, achieving the enhanced device stability. Only a 9% efficiency degradation is observed for un-encapsulated device prepared with Spiro-OMeTAD and LQ after 1700 h under air environment, while the efficiency drops by 30% for the reference device. This work provides an effective strategy for improving the efficiency and stability of PSCs, and gives some important insights for understanding intrinsic HCs dynamics for HCs-enhanced perovskite-based optoelectronic devices.

Quantification of strain and its impact on the phase stabilization of all-inorganic cesium lead iodide perovskites

•CsPbI3 nanoplates are epitaxially grown on muscovite mica single-crystal substrates •Lattice strain is present and found to increase with decreasing nanoplate thickness •The strained epitaxy enhances the metastable perovskite high-T phase stability The high-temperature perovskite γ-phase of CsPbI3 readily undergoes phase transition at ambient conditions to a low-temperature non-perovskite δ-phase with a poorer optoelectronic performance, thus hindering commercialization of these materials in photovoltaics. Here, we present the epitaxial growth of CsPbI3 nanoplates on muscovite mica single-crystal substrates and demonstrate that the high-temperature phase stability of these nanoplates is enhanced by a strained interface. Strain is measured as a function of nanoplate thickness on a single-particle level through spatially resolved structural and optical characterizations and is found to increase with decreasing thickness. From quantitatively tracking the CsPbI3 phase transition for thin (<400 nm) and thick (>400 nm) nanoplates, we observe a larger fraction of thin nanoplates still maintaining their high-temperature phase after 1 month compared with their thick counterparts. These findings establish a relationship between strain and phase transition kinetics, which is critical for rational design of stable perovskite-based optoelectronic devices. The high-temperature perovskite γ-phase of CsPbI3 readily undergoes phase transition at ambient conditions to a low-temperature non-perovskite δ-phase with a poorer optoelectronic performance, thus hindering commercialization of these materials in photovoltaics. Here, we present the epitaxial growth of CsPbI3 nanoplates on muscovite mica single-crystal substrates and demonstrate that the high-temperature phase stability of these nanoplates is enhanced by a strained interface. Strain is measured as a function of nanoplate thickness on a single-particle level through spatially resolved structural and optical characterizations and is found to increase with decreasing thickness. From quantitatively tracking the CsPbI3 phase transition for thin (<400 nm) and thick (>400 nm) nanoplates, we observe a larger fraction of thin nanoplates still maintaining their high-temperature phase after 1 month compared with their thick counterparts. These findings establish a relationship between strain and phase transition kinetics, which is critical for rational design of stable perovskite-based optoelectronic devices.

Zero Threshold for Water Adsorption on MAPbBr3

Hybrid organic-inorganic perovskites (HOIPs) have shown great promise in a wide range of optoelectronic applications. However, this performance is inhibited by the sensitivity of HOIPs to various environmental factors, particularly high levels of relative humidity. This study uses X-ray photoelectron spectroscopy (XPS)to determine that there is essentially no threshold to water adsorption on the in situ cleaved MAPbBr3 (001) single crystal surface. Using scanning tunneling microscopy (STM), it shows that the initial surface restructuring upon exposure to water vapor occurs in isolated regions, which grow in area with increasing exposure, providing insight into the initial degradation mechanism of HOIPs. The electronic structure evolution of the surface wasalso monitored via ultraviolet photoemission spectroscopy (UPS), evidencing an increased bandgap state density following water vapor exposure, which is attributed to surface defect formation due to lattice swelling. This study will help to inform the surface engineering and designs of future perovskite-based optoelectronic devices.

Mixed Organic Cations Promote Ambient Light-Induced Formation of Metallic Lead in Lead Halide Perovskite Crystals.

One major concern toward the performance and stability of halide perovskite-based optoelectronic devices is the formation of metallic lead that promotes nonradiative recombination of charge carriers. The origin of metallic lead formation is being disputed whether it occurs during the perovskite synthesis or only after light, electron, or X-ray beam irradiation or thermal annealing. Here, we show that the quantity of metallic lead detected in perovskite crystals depends on the concentration and composition of the precursor solution. Through a controlled crystallization process, we grew black-colored mixed dimethylammonium (DMA)/methylammonium (MA) lead tribromide crystals. The black color is suggested to be due to the presence of small lead clusters. Despite the unexpected black coloring, the crystals show higher crystallinity and less defect density with respect to the standard yellow-colored DMA/MAPbBr3 crystals, as indicated by X-ray rocking curve and dark current measurements, respectively. While the formation of metallic lead could still be induced by external factors, the precursor solution composition and concentration can facilitate the formation of metallic lead during the crystallization process. Our results indicate that additional research is required to fully understand the perovskite precursor solution chemistry.

Influence of Halides on Elastic and Vibrational Properties of Mixed-Halide Perovskite Systems Studied by Brillouin and Raman Scattering.

The relationship between halogen content and the elastic/vibrational properties of MAPbBr3-xClx mixed crystals (x = 1.5, 2, 2.5, and 3) with MA = CH3NH3+ has been studied using Brillouin and Raman spectroscopy at room temperature. The longitudinal and transverse sound velocities, the absorption coefficients and the two elastic constants C11 and C44 could be obtained and compared for the four mixed-halide perovskites. In particular, the elastic constants of the mixed crystals have been determined for the first time. A quasi-linear increase in the sound velocity and the elastic constant C11 with increasing chlorine content was observed for the longitudinal acoustic waves. C44 was insensitive to the Cl content and very low, indicating a low elasticity to shear stress in mixed perovskites regardless of the Cl content. The acoustic absorption of the LA mode increased with increasing heterogeneity in the mixed system, especially for the intermediate composition where the Br and Cl ratio was 1:1. In addition, a significant decrease in the Raman-mode frequency of the low-frequency lattice modes and the rotational and torsional modes of the MA cations was observed with decreasing Cl content. It clearly showed that the changes in the elastic properties as the halide composition changes were correlated with the lattice vibrations. The present findings may facilitate a deeper understanding of the complex interplay between halogen substitution, vibrational spectra and elastic properties, and may also pave the way for optimizing the operation of perovskite-based photovoltaic and optoelectronic devices by tailoring their chemical composition.

Femtosecond Laser-Processed Perovskite Thin Films with Reduced Nonradiative Recombination and Improved Photodetecting Performance

Carrier recombination plays a key role in determining the performance of perovskite devices, wherein nonradiative recombination hinders carrier extraction and limits the performance of perovskite-based optoelectronic devices (e.g., solar cells and photodetectors). To reduce nonradiative recombination, passivating the surface and grain boundary defects with chemicals has been extensively studied. However, this method has limitations such as pollution, complicated procedures, etc. Here, we provide a physical approach to reduce the nonradiative recombination loss of MAPbI3 perovskite thin films using femtosecond (fs) laser processing. Perovskite thin films processed by fs laser show an enhanced photoluminescence (PL) intensity, extended lifetime, smaller grain size, smooth surface, and improved photodetector performance. The effect of laser processing is attributed to a decrease in the number of trap centers per grain and polished perovskite surface, which act as nonradiative recombination centers in the perovskite thin films. This research provides a promising way to improve the performance of perovskite optoelectronic devices.

Kinetic Control of Solvate Intermediate Evolution for High-Performance Perovskite Solar Cells by the Facial Mask Incubation Technique

The growth of high-quality perovskite films is complicated by the fact of uncontrollable crystallization pathways from perovskite precursors. During solution processing, extensive undesired nonperovskite products including residual solvate intermediates are produced due to quick solvent evaporation, which will adversely affect the efficiency and stability of perovskite solar cells (PSCs). Herein, we developed a highly efficient phase-transition pathway using a polydimethylsiloxane (PDMS)-based facial mask (FM) incubation technique, which enables significant reduction of the perovskite crystallization rate and depression of perovskite aggregation behavior. A surprising finding reveals that this technique induces complete phase transition from solvate intermediates to the perovskite phase, thereby obtaining phase-pure perovskite film. Meanwhile, a high-quality perovskite film with a shiny smooth surface, decreased defect states, and alleviated lattice strain is achieved after utilizing the FM strategy. Consequently, the target-inverted PSCs deliver a respectable efficiency of ∼21% and superior stability in both shelf storage (over 3700 h with 90% of initial efficiency) and light soaking (over 1000 h with 80% of initial efficiency) conditions. Our work highlights the importance of eliminating residual solvate intermediates to construct high-quality perovskites with excellent phase purity for ongoing production of high-performance perovskite-based optoelectronic devices.

Enhanced performance in perovskites films by defect engineering and charge carrier transportation via pulsed laser doping of 2D MoS2

High-performance perovskite-based optoelectronic devices require low defect density and efficient charge carrier extraction. In this paper, pulsed laser annealing was combined with two-dimensional MoS2 doping to develop an efficient strategy for the extraction of charge carriers from perovskite films with low defect density. In pulse laser annealing of perovskite films with 2D MoS2 dopant, due to their localized temperature gradients caused by fast laser annealing, the grains are much larger, and the film quality is much better than that of traditional thermal annealing perovskite films. As a result, the films absorb light better. After doping of 2D MoS2, the carrier transport in perovskite films can be increased significantly by passivating Pb-related defects through PbS coordination bonds. Additionally, the shift of the conduction band minimum (CBM) from the perovskite layer to the Au layer provides a well-matched alignment in energy levels between the perovskite and Au layers, which encourages charge carrier extraction. Moreover, the interfacial perovskite lattice moves freely during the annealing and chilling processes due to laser-induced thermomechanical momentum and weak interactions between 2D MoS2 and, thereby reducing the tensile strain in perovskite films. In addition, by improving surface hydrophobicity and relieving residual stresses, perovskite films are more humidity and thermal stable.