Insights into Fullerene Passivation of SnO2 Electron Transport Layers in Perovskite Solar Cells

Interfaces between the photoactive and charge transport layers are crucial for the performance of perovskite solar cells. Surface passivation of SnO₂ as electron transport layer (ETL) by fullerene derivatives is known to improve the performance of n–i–p devices, yet organic passivation layers are susceptible to removal during perovskite deposition. Understanding the nature of the passivation is important for further optimization of SnO₂ ETLs. X‐ray photoelectron spectroscopy depth profiling is a convenient tool to monitor the fullerene concentration in passivation layers at a SnO₂ interface. Through a comparative study using [6,6]‐phenyl‐C₆₁‐butyric acid methyl ester (PCBM) and [6,6]‐phenyl‐C₆₁‐butyric acid (PCBA) passivation layers, a direct correlation is established between the formation of interfacial chemical bonds and the retention of passivating fullerene molecules at the SnO₂ interface that effectively reduces the number of defects and enhances electron mobility. Devices with only a PCBA‐monolayer‐passivated SnO₂ ETL exhibit significantly improved performance and reproducibility, achieving an efficiency of 18.8%. Investigating thick and solvent‐resistant C₆₀ and PCBM‐dimer layers demonstrates that the charge transport in the ETL is only improved by chemisorption of the fullerene at the SnO₂ surface.     

NbF5: A Novel α‐Phase Stabilizer for FA‐Based Perovskite Solar Cells with High Efficiency

The HC(NH₂)₂⁺(FA⁺) is a well‐known substitute to CH₃NH₃⁺(MA⁺) for its capability to extend light utilization for improved power conversion efficiency for perovskite solar cells; unfortunately, the dark cubic phase (α‐phase) can easily transition to the yellow orthorhombic phase (δ‐phase) at room temperature, an issue that prevents its commercial application. In this report, an inorganic material (NbF₅) is developed to stabilize the desired α‐phase perovskite material by incorporating NbF₅ additive into the perovskite films. It is found that the NbF₅ additive effectively suppresses the formation of the yellow δ‐phase in the perovskite synthesis and aging process, thus enhancing the humidity and light‐soaking stability of the perovskite film. As a result, the perovskite solar cells with the NbF₅ additive exhibit improved air stability by tenfold, retaining nearly 80% of their initial efficiency after aging in air for 50 d. In addition, under full‐sun AM 1.5 G illumination of a xenon lamp without any UV‐reduction, the perovskite solar cells with the NbF₅ additive also show fivefold improved illumination stability than the control devices without NbF₅.     

Dual Interfacial Modification Engineering with 2D MXene Quantum Dots and Copper Sulphide Nanocrystals Enabled High‐Performance Perovskite Solar Cells

The performance of perovskite solar cells (PSCs) strongly depends on the electron transport layer (ETL), perovskite absorber, hole transport layer (HTL), and their interfaces. Herein, the first approach to utilize ultrathin 2D titanium‐carbide MXenes (Ti₃C₂T_x quantum dots, TQD) by engineering the perovskite/TiO₂ ETL interface and perovskite absorber and introducing Cu_1.8S nanocrystals to perfect the Spiro‐OMeTAD HTL is represented. A significant hysteresis‐free power conversion efficiency improvement from 18.31% to 21.64% of PSCs is achieved after modifications with the enhanced short‐circuit current density, open‐circuit voltages, and fill factor. Various advanced characterizations, including femtosecond transient absorption spectroscopy, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectroscopy, elucidate that the TQD/Cu_1.8S significantly contribute to the improved crystalline quality of the perovskite film with its large grain size and improved electron/holes extraction efficiencies at perovskite/ETL and perovskite/HTL interfaces. Furthermore, the long‐time ambient and light stability of PSCs are largely boosted through the TQD and/or Cu_1.8S nanocrystals doping, originating from the better crystallization of perovskite, suppressing the film aggregation and crystallization of HTL, and inhibiting the ultraviolet‐induced photocatalysis of the ETL. The findings highlight the TQD and Cu_1.8S can act as a superfast electrons and holes tunnel for the optoelectronic devices.     

Core/Shell Perovskite Nanocrystals: Synthesis of Highly Efficient and Environmentally Stable FAPbBr3/CsPbBr3 for LED Applications

Lead halide perovskite nanocrystals (PeNCs) are promising materials for applications in optoelectronics. However, their environmental instability remains to be addressed to enable their advancement into industry. Here the development of a novel synthesis method is reported for monodispersed PeNCs coated with all inorganic shell of cesium lead bromide (CsPbBr₃) grown epitaxially on the surface of formamidinium lead bromide (FAPbBr₃) NCs. The formed FAPbBr₃/CsPbBr₃ NCs have photoluminescence in the visible range 460–560 nm with narrow emission linewidth (20 nm) and high optical quantum yield, photoluminescence quantum yield (PLQY) up to 93%. The core/shell perovskites have enhanced optical stability under ambient conditions (70 d) and under ultraviolet radiation (50 h). The enhanced properties are attributed to overgrowth of FAPbBr₃ with all‐inorganic CsPbBr₃ shell, which acts as a protective layer and enables effective passivation of the surface defects. The use of these green‐emitting core/shell FAPbBr₃/CsPbBr₃ NCs is demonstrated in light‐emitting diodes (LEDs) and significant enhancement of their performance is achieved compared to core only FAPbBr₃‐LEDs. The maximum current efficiency observed in core/shell NC LED is 19.75 cd A^‐1 and the external quantum efficiency of 8.1%, which are approximately four times and approximately eight times higher, respectively, compared to core‐only devices.     

Hole Transport Bilayer Structure for Quasi‐2D Perovskite Based Blue Light‐Emitting Diodes with High Brightness and Good Spectral Stability

Substantial achievements have been made in green and red perovskite light emitting diodes (PeLEDs) recently. However, blue PeLEDs still lag behind with much lower performances. One of the main reasons is the mass undesirable nonradiative recombination at interfaces and within the perovskite films. In this work, an efficient hole transport bi‐layer structure composed of PSSNa and NiO_x is demonstrated to simultaneously inhibit the nonradiative decays between NiO_x and perovskite films by reducing NiO_x surface defects and improving quasi‐2D perovskite thin film quality by minimizing its pin‐holes and reducing the film roughness. The results show that the dipole feature of PSSNa improves the hole transportation and thus PeLED performances. Moreover, by introducing KBr into the perovskite, its film quality improves and trap states reduce. Eventually, the blue PeLEDs is achieved with a very low turn‐on voltage of 3.31 V accompanied with an external quantum efficiency of 1.45% and a remarkable luminance of 4359 cd m^‐2. With further optimization of the perovskite precursor concentration, the highest luminance reaches 5737 cd m^‐2, which represents the brightest blue PeLEDs reported to date as far as it is known. Furthermore, the devices also show better spectral stability and operation lifetime as compared to other blue PeLEDs.     

Synergistic Effect of PbI2 Passivation and Chlorine Inclusion Yielding High Open‐Circuit Voltage Exceeding 1.15 V in Both Mesoscopic and Inverted Planar CH3NH3PbI3(Cl)‐Based Perovskite Solar Cells

Enhancing open‐circuit voltage in CH₃NH₃PbI₃(Cl) perovskite solar cells has become a major challenge for approaching the theoretical limit of the power conversion efficiency. Here, for the first time, it is demonstrated that the synergistic effect of PbI₂ passivation and chlorine incorporation via controlling the molar ratio of PbI₂, PbCl₂ (or MACl), and MAI in the precursor solutions, boosts the open‐circuit voltage of CH₃NH₃PbI₃(Cl) perovskite solar cells over 1.15 V in both mesoscopic and inverted planar perovskite solar cells. Such high open‐circuit voltage can be attributed to the enhanced photoluminescence emission and carrier lifetime associated with the reduced trap densities. The morphology and composition analysis using scanning electron microscopy, X‐ray diffraction measurements, and energy dispersive X‐ray spectroscopy confirm the high quality of the optimized CH₃NH₃PbI₃(Cl) perovskite film. On this basis, record‐high efficiencies of 16.6% for nonmetal‐electrode all‐solution‐processed perovskite solar cells and 18.4% for inverted planar perovskite solar cells are achieved.     

Impact of Crystal Surface on Photoexcited States in Organic–Inorganic Perovskites

Despite their outstanding photovoltaic performance, organic–inorganic perovskite solar cells still face severe stability issues and limitations in their device dimension. Further development of perovskite solar cells therefore requires a deeper understanding of loss mechanisms, in particular, concerning the origin and impact of trap states. Here, different surface properties of submicrometer sized CH₃NH₃PbI₃ particles are studied as a model system by photoluminescence spectroscopy to investigate the impact of the perovskite crystal surface on photoexcited states. Comparison of single crystals with either isolating or electron‐rich surface passivation indicates the presence of positively charged surface trap states that can be passivated in case of the latter. These surface trap states cause enhanced nonradiative recombination at room temperature, which is a loss mechanism for solar cell performance. In the orthorhombic phase, the origin of multiple emission peaks is identified as the recombination of free and bound excitons, whose population ratio critically depends on trap state properties. The dynamics of exciton trapping at 50 K are observed on a time‐scale of tens of picoseconds by a simultaneous population decrease and increase of free and bound excitons, respectively. These results emphasize the potential of surface passivation to further improve the performance of perovskite solar cells.     

Engineering of the Electron Transport Layer/Perovskite Interface in Solar Cells Designed on TiO2 Rutile Nanorods

The engineering of the electron transport layer (ETL)/light absorber interface is explored in perovskite solar cells. Single‐crystalline TiO₂ nanorod (NR) arrays are used as ETL and methylammonium lead iodide (MAPI) as light absorber. A dual ETL surface modification is investigated, namely by a TiCl₄ treatment combined with a subsequent PC₆₁BM monolayer deposition, and the effects on the device photovoltaic performance were evaluated with respect to single modifications. Under optimized conditions, for the combined treatment synergistic effects are observed that lead to remarkable enhancements in cell efficiency, from 14.2% to 19.5%, and to suppression of hysteresis. The devices show J_SC, V_OC, and fill factor as high as 23.2 mA cm^?2, 1.1 V, and 77%, respectively. These results are ascribed to a more efficient charge transfer across the ETL/perovskite interface, which originates from the passivation of defects and trap states at the ETL surface. To the best of our knowledge, this is the highest cell performance ever reported for TiO₂ NR‐based solar cells fabricated with conventional MAPI light absorber. Perspective wise, this ETL surface functionalization approach combined with more recently developed and better performing light absorbers, such as mixed cation/anion hybrid perovskite materials, is expected to provide further performance enhancements.     

Suppressing Ion Migration Enables Stable Perovskite Light‐Emitting Diodes with All‐Inorganic Strategy

Stability issue is one of the major concerns that limit emergent perovskite light‐emitting diodes (PeLEDs) techniques. Generally, ion migration is considered as the most important origin of PeLEDs degradation. In this work, an all‐inorganic device architecture, LiF/perovskite/LiF/ZnS/ZnSe, is proposed to address this imperative problem. The inorganic (Cs_1?xRb_x)_1?yK_yPbBr₃ perovskite is optimized with achieving a photoluminescence quantum yield of 67%. Depth profile analysis of X‐ray photoelectron spectroscopy indicates that the LiF/perovskite/LiF structure and the ZnS/ZnSe cascade electron transport layers significantly suppress the electric‐field‐induced ion migrations of the perovskite layers, and impede the diffusion of metallic atoms from cathode into perovskites. The as‐prepared PeLEDs display excellent shelf stability (maintaining 90% of the initial external quantum efficiency [EQE] after 264 h) and operational stability (half‐lifetime of about 255 h at an initial luminance of 120 cd m^?2). The devices also exhibit a maximum brightness of 15 6155 cd m^?2 and an EQE of 11.05%.     

Degradation Mechanism of Perovskite Light‐Emitting Diodes: An In Situ Investigation via Electroabsorption Spectroscopy and Device Modelling

The past few years have seen a significant improvement in the efficiency of organometal halide‐perovskite‐based light‐emitting diodes (PeLEDs). However, poor operation stability of the devices still hinders the commercialization of this technology for practical applications. Despite extensive studies on the degradation mechanisms of perovskite thin films, it remains unclear where and how degradation occurs in a PeLED. Electroabsorption (EA) spectroscopy is applied to study the degradation process of PeLEDs during operation and directly evaluates the stability of each functional layer (i.e., charge transporting layers and light‐emitting layer) by monitoring their unique optical signatures. The EA measurements unambiguously reveal that the degradation of the PeLEDs occurs predominantly in the perovskite layer. With finite‐element method‐based device modeling, it is further revealed that the degradation may initiate from the interface between the perovskite and hole transporting layers and that vacancy, antisite, or interstitial defects can further accelerate this degradation. Inspired by these observations, a surface‐treatment step is introduced to passivate the perovskite surface with phenethylammonium iodide. The passivation leads to a drastic enhancement of the PeLED stability, with the operation lifetime increased from 1.5 to 11.3 h under a current density of 100 mA cm^?2.     

Precisely Controlling the Grain Sizes with an Ammonium Hypophosphite Additive for High‐Performance Perovskite Solar Cells

A facile approach to precisely control the perovskite grain sizes is proposed and demonstrated for high‐performance photovoltaic (PV) solar cells. With the introduction of various amounts of NH₄H₂PO₂ (AHP) additives into the PbI₂/CH₃NH₃I precursors, the grain scale of CH₃NH₃PbI₃ films can be finely turned from hundreds of nanometer to micrometer scale, allowing evaluating the effects of crystalline grain boundary on trap densities, charge recombination, and PV device performance. The X‐ray diffraction and X‐ray photoelectron spectroscopy measurements indicate that the formation of intermediates plays a key role in assisting the perovskite crystal growth. The optimized devices show much larger open‐circuit voltages (V_OC) up to 1.10 ± 0.02 V and significantly enhance power conversion efficiencies (PCEs) of 16.5 ± 0.7%, as compared to the control devices with PCE of 9.4 ± 1.0% and V_OC of 1.00 ± 0.03 V. Further investigations confirm that the boosted PV performance origins from the decreased defect densities due to enlarged grain sizes. It is also demonstrated that the approach is general and applicable to other perovskite systems, e.g., HC(NH₂)₂PbI₃. The results suggest the promising application of AHP in achieving high‐performance perovskite PV devices, and shed light on understanding the grain boundary effects on perovskite optoelectronics.     

Double‐Sided Surface Passivation of 3D Perovskite Film for High‐Efficiency Mixed‐Dimensional Perovskite Solar Cells

Defect‐mediated carrier recombination at the interfaces between perovskite and neighboring charge transport layers limits the efficiency of most state‐of‐the‐art perovskite solar cells. Passivation of interfacial defects is thus essential for attaining cell efficiencies close to the theoretical limit. In this work, a novel double‐sided passivation of 3D perovskite films is demonstrated with thin surface layers of bulky organic cation–based halide compound forming 2D layered perovskite. Highly efficient (22.77%) mixed‐dimensional perovskite devices with a remarkable open‐circuit voltage of 1.2 V are reported for a perovskite film having an optical bandgap of ≈1.6 eV. Using a combination of experimental and numerical analyses, it is shown that the double‐sided surface layers provide effective defect passivation at both the electron and hole transport layer interfaces, suppressing surface recombination on both sides of the active layer. Despite the semi‐insulating nature of the passivation layers, an increase in the fill factor of optimized cells is observed. The efficient carrier extraction is explained by incomplete surface coverage of the 2D perovskite layer, allowing charge transport through localized unpassivated regions, similar to tunnel‐oxide passivation layers used in silicon photovoltaics. Optimization of the defect passivation properties of these films has the potential to further increase cell efficiencies.     

Combination of Hybrid CVD and Cation Exchange for Upscaling Cs‐Substituted Mixed Cation Perovskite Solar Cells with High Efficiency and Stability

Mixed cation hybrid perovskites such as Cs_xFA_1?xPbI₃ are promising materials for solar cell applications, due to their excellent photoelectronic properties and improved stability. Although power conversion efficiencies (PCEs) as high as 18.16% have been reported, devices are mostly processed by the anti‐solvent method, which is difficult for further scaling‐up. Here, a method to fabricate Cs_xFA_1?xPbI₃ by performing Cs cation exchange on hybrid chemical vapor deposition grown FAPbI₃ with the Cs⁺ ratio adjustable from 0 to 24% is reported. The champion perovskite module based on Cs_0.07FA_0.93PbI₃ with an active area of 12.0 cm² shows a module PCE of 14.6% and PCE loss/area of 0.17% cm^?2, demonstrating the significant advantage of this method toward scaling‐up. This in‐depth study shows that when the perovskite films prepared by this method contain 6.6% Cs⁺ in bulk and 15.0% at the surface, that is, Cs_0.07FA_0.93PbI₃, solar cell devices show not only significantly increased PCEs but also substantially improved stability, due to favorable energy level alignment with TiO₂ electron transport layer and spiro‐MeOTAD hole transport layer, increased grain size, and improved perovskite phase stability.     

Metal Halide Perovskite Surfaces with Mixed A-Site Cations: Atomic Structure and Device Stability

Mixing cations in the perovskite structure has been shown to improve optoelectronic device performance and stability. In particular, Cs_xMA_1-xPbBr₃ (MA = CH₃NH₃) has been used to build high-efficiency light-emitting diodes. Despite those advantages, little is known about the exact location of the cations in the mixed perovskite film, and how cation distribution affects device properties and stability. By using scanning tunneling microscopy , the exact atomic structure of the mixed cation Cs_xMA_1-xPbBr₃ perovskite interface is revealed. In addition, X-ray photoelectron spectroscopy, ultraviolet photoemission spectroscopy and inverse photoemission spectroscopy are used to study the stability and electronic properties of the Cs_xMA_1-xPbBr₃ perovskite film. Partial substitution of MA⁺ by Cs⁺ induces a modification of the perovskite surface structure, leading to improved device stability is shown. These results provide a better understanding of the key parameters involved in the stability of mixed cation perovskite solar cells.     

An Interdiffusion Method for Highly Performing Cesium/Formamidinium Double Cation Perovskites

The fabrication of high‐quality cesium (Cs)/formamidinium (FA) double‐cation perovskite films through a two‐step interdiffusion method is reported. Cs_x FA_1‐x PbI_{3‐y(1‐x )}Br_{y(1‐x )} films with different compositions are achieved by controlling the amount of CsI and formamidinium bromide (FABr) in the respective precursor solutions. The effects of incorporating Cs⁺ and Br^? on the properties of the resulting perovskite films and on the performance of the corresponding perovskite solar cells are systematically studied. Small area perovskite solar cells with a power conversion efficiency (PCE) of 19.3% and a perovskite module (4 cm²) with an aperture PCE of 16.4%, using the Cs/FA double cation perovskite made with 10 mol% CsI and 15 mol% FABr (Cs_0.1FA_0.9PbI_2.865Br_0.135) are achieved. The Cs/FA double cation perovskites show negligible degradation after annealing at 85 °C for 336 h, outperforming the perovskite materials containing methylammonium (MA).     

Constructing CsPbBr3 Cluster Passivated‐Triple Cation Perovskite for Highly Efficient and Operationally Stable Solar Cells

Ion migration and phase segregation, in mixed‐cation/anion perovskite materials, raises a bottleneck for its stability improvement in solar cells operation. Here, the synergetic effect of electric field and illumination on the phase segregation of Cs_0.05FA_0.80MA_0.15Pb(I_0.85Br_0.15)₃ (CsFAMA) perovskite is demonstrated. CsFAMA perovskite with a CsPbBr₃‐clusters passivated structure is realized, in which CsPbBr₃‐clusters are located at the surface/interface of CsFAMA grains. This structure is realized by introducing a CsPbBr₃ colloidal solution into the CsFAMA precursor. It is found that CsPbBr₃ passivation greatly suppresses phase segregation in CsFAMA perovskite. The resultant passivated CsFAMA also exhibits a longer photoluminescence lifetime due to reduced defect state densities, produces highly efficient TiO₂‐based planar solar cells with 20.6% power conversion efficiency and 1.195 V open‐circuit voltage. The optimized devices do not suffer from a fast burn‐in degradation and retain 90% of their initial performance at maximum power under one‐sun illumination at 25 °C (65 °C) exceeding 500 h (100 h) of continuous operation. This result represents the most stable output among CsFAMA solar cells in a planar structure with Spiro‐OMeTAD.     

Multi-Site Intermolecular Interaction for In Situ Formation of Vertically Orientated 2D Passivation Layer in Highly Efficient Perovskite Solar Cells

Surface passivation via 2D perovskite is critical for perovskite solar cells (PSCs) to achieve remarkable performances, in which the applied spacer cations play an important role on structural templating. However, the random orientation of 2D perovskite always hinder the carrier transport. Herein, multiple nitrogen sites containing organic spacer molecule (1H-Pyrazole-1-carboxamidine hydrochloride, PAH) is introduced to form 2D passivation layer on the surface of formamidinium based (FAPbI₃) perovskite. Deriving from the interactions between PAH and PbI₂, the defects of FAPbI₃ perovskite are effectively passivated. Interestingly, due to the multiple-site interactions, the 2D nanosheets are found to grow perpendicularly to the substrate for promotion of charge transfer. Therefore, an impressive power conversion efficiency of 24.6% and outstanding long-term stability are achieved for the 2D/3D perovskite devices. The findings further provide a perspective in structure design of novel organic halide salts for the fabrication of efficient and stable PSCs.     

Sulfate‐Assisted Interfacial Engineering for High Yield and Efficiency of Triple Cation Perovskite Solar Cells with Alkali‐Doped TiO2 Electron‐Transporting Layers

Facile electron injection and extraction are two key attributes desired in electron transporting layers to enhance the efficiency of planar perovskite solar cells. Herein it is demonstrated that the incorporation of alkali metal dopants in mesoporous TiO₂ can effectively modulate electronic conductivity and improve the charge extraction process by counterbalancing oxygen vacancies acting as nonradiative recombination centers. Moreover, sulfate bridges (SO₄^2?) grafted on the surface of K‐doped mesoporous titania provide a seamless integration of absorber and electron‐transporting layers that accelerate overall transport kinetics. Potassium doping markedly influences the nucleation of the perovskite layer to produce highly dense films with facetted crystallites. Solar cells made from K:TiO₂ electrodes exhibit power conversion efficiencies up to 21.1% with small hysteresis despite all solution coating processes conducted under ambient air conditions (controlled humidity: 25–35%). The higher device efficiencies are attributed to intrinsically tuned electronic conductivity and chemical modification of grain boundaries enabling uniform coverage of perovskite films with large grain size.     

20.7% efficient ion‐implanted large area n‐type front junction silicon solar cells with rear point contacts formed by laser opening and physical vapor deposition

In this work, we report on ion‐implanted, high‐efficiency n‐type silicon solar cells fabricated on large area pseudosquare Czochralski wafers. The sputtering of aluminum (Al) via physical vapor deposition (PVD) in combination with a laser‐patterned dielectric stack was used on the rear side to produce front junction cells with an implanted boron emitter and a phosphorus back surface field. Front and back surface passivation was achieved by thin thermally grown oxide during the implant anneal. Both front and back oxides were capped with SiN_x, followed by screen‐printed metal grid formation on the front side. An ultraviolet laser was used to selectively ablate the SiO₂/SiN_x passivation stack on the back to form the pattern for metal–Si contact. The laser pulse energy had to be optimized to fully open the SiO₂/SiN_x passivation layers, without inducing appreciable damage or defects on the surface of the n⁺ back surface field layer. It was also found that a low temperature annealing for less than 3 min after PVD Al provided an excellent charge collecting contact on the back. In order to obtain high fill factor of ~80%, an in situ plasma etching in an inert ambient prior to PVD was found to be essential for etching the native oxide formed in the rear vias during the front contact firing. Finally, through optimization of the size and pitch of the rear point contacts, an efficiency of 20.7% was achieved for the large area n‐type passivated emitter, rear totally diffused cell. Copyright © 2014 John Wiley & Sons, Ltd.     

A Large Bandgap Organic Salt Dopant for Sn-Based Perovskite Thin-Film Transistor

Metal halide perovskite optoelectronic devices have made significant progress over the past few years, but precise control of charge carrier density through doping is essential for optimizing these devices. In this study, the potential of using an organic salt, N,N-dimethylanilinium tetrakis(pentafluorophenyl)borate, as a dopant for Sn-based perovskite devices, is explored. Under optimized conditions, the thin film transistors based on the doped 2D/3D perovskite PEAFASnI₃ demonstrate remarkable improvement in hole mobility, reaching 7.45 cm²V⁻¹s⁻¹ with a low subthreshold swing and the smallest sweep hysteresis (ΔV_hysteresis = 2.27 V) and exceptional bias stability with the lowest contact resistance (2.2 kΩ cm). The bulky chemical structure of the dopant prevents it from penetrating the perovskite lattice and also surface passivation against Sn oxidation due to its hydrophobic nature surface. This improvement is attributed to the bifunctional effect of the dopant, which simultaneously passivates defects and improves crystal orientation. These findings provide new insights into potential molecular dopants that can be used in metal halide perovskite devices.