Stable α‐CsPbI3 Perovskite Nanowire Arrays with Preferential Crystallographic Orientation for Highly Sensitive Photodetectors

All‐inorganic metal‐halide perovskites CsPbX₃ (X = Cl, Br, I) exhibit higher stability than their organic–inorganic hybrid counterparts, but the thermodynamically instable perovskite α phase at room temperature of CsPbI₃ restricts the practical optoelectronic applications. Although the stabilization of α‐CsPbI₃ polycrystalline thin films is extensively studied, the creation of highly crystalline micro/nanostructures of α‐CsPbI₃ with large grain size and suppressed grain boundary remains challenging, which impedes the implementations of α‐CsPbI₃ for lateral devices, such as photoconductor‐type photodetectors. In this work, stable α‐CsPbI₃ perovskite nanowire arrays are demonstrated with large grain size, high crystallinity, regulated alignment, and position by controlling the dewetting dynamics of precursor solution on an asymmetric‐wettability topographical template. The correlation between the higher photoluminescence (PL) intensity and longer PL lifetime indicates the nanowires exhibit stable α phase and suppressed trap density. The preferential (100) orientation is characterized by discrete diffraction spots in grazing incidence wide‐angle scattering patterns, suggesting the long‐range crystallographic order of these nanowires. Based on these high‐quality nanowire arrays, highly sensitive photodetectors are realized with a responsivity of 1294 A W^?1 and long‐term stability with 90% performance retention after 30‐day ambient storage.     

FAPbI3‐Based Perovskite Solar Cells Employing Hexyl‐Based Ionic Liquid with an Efficiency Over 20% and Excellent Long‐Term Stability

Formamidinium lead triiodide (FAPbI₃)‐based perovskite materials are of interest for photovoltaics in view of their close‐to‐ideal bandgap, allowing absorption of photons over a broad solar spectrum. However, FAPbI₃‐based materials suffer from a notorious phase transition from the photoactive black phase (α‐FAPbI₃) to nonperovskite yellow phase (δ‐FAPbI₃) under ambient conditions. This transition dramatically reduces light absorbtion, thus, degrading the photovoltaic performance and stability of ensuring solar cells. In this study, 1‐hexyl‐3‐methylimidazolium iodide (HMII) ionic liquid (IL) is employed as an additive for the first time in FAPbI₃ perovskite to overcome the above‐mentioned issues. HMII incorporation facilitates the grain coarsening of FAPbI₃ crystal owing to its high‐polarity and high‐boiling point, which yields liquid domains between neighboring grains to reduce the activation energy of the grain‐boundary migration. As a result, the FAPbI₃ active layer exhibits micron‐sized grains with substantially suppressed parasitic traps with an Urbach energy reduced by 2 meV. Hence, the resulting perovskite solar cell achieves an efficiency of 20.6% with notable increase in open circuit voltage (V_OC) of 80 mV compared with HMII‐free cells (17.1%). More importantly, the HMII‐doped FAPbI₃‐based cells show a striking enhancement in shelf‐stability under high humidity and thermal stress, retaining >80% of their initial efficiencies at 60 ± 10% relative humidity and ≈95% at 65 °C.     

Room‐Temperature Partial Conversion of α‐FAPbI3 Perovskite Phase via PbI2 Solvation Enables High‐Performance Solar Cells

The two‐step conversion process consisting of metal halide deposition followed by conversion to hybrid perovskite has been successfully applied toward producing high‐quality solar cells of the archetypal MAPbI₃ hybrid perovskite, but the conversion of other halide perovskites, such as the lower bandgap FAPbI₃, is more challenging and tends to be hampered by the formation of hexagonal nonperovskite polymorph of FAPbI₃, requiring Cs addition and/or extensive thermal annealing. Here, an efficient room‐temperature conversion route of PbI₂ into the α‐FAPbI₃ perovskite phase without the use of cesium is demonstrated. Using in situ grazing incidence wide‐angle X‐ray scattering (GIWAXS) and quartz crystal microbalance with dissipation (QCM‐D), the conversion behaviors of the PbI₂ precursor from its different states are compared. α‐FAPbI₃ forms spontaneously and efficiently at room temperature from P₂ (ordered solvated polymorphs with DMF) without hexagonal phase formation and leads to complete conversion after thermal annealing. The average power conversion efficiency (PCE) of the fabricated solar cells is greatly improved from 16.0(±0.32)% (conversion from annealed PbI₂) to 17.23(±0.28)% (from solvated PbI₂) with a champion device PCE > 18% due to reduction of carrier recombination rate. This work provides new design rules toward the room‐temperature phase transformation and processing of hybrid perovskite films based on FA⁺ cation without the need for Cs⁺ or mixed halide formulation.     

High-performance formamidinium-based perovskite photodetectors fabricated via doctor-blading deposition in ambient condition

High-purity black α-phase formamidinium lead iodide (FAPbI₃, FA is NH₂CHNH⁺) perovskite polycrystalline film was prepared using low-cost, high-output doctor-blading deposition technique in ambient condition without further annealing process and any additives. The resulting α-phase FAPbI₃ perovskite has a large domain size over 200 μm with (00l) preferential crystallographic orientation. The photodetectors with an extremely simple structure were fabricated via doctor-blading, resulting in a responsivity as high as 11.46 AW⁻¹, a ratio of photocurrent/dark current (I_light/I_dark) as large as 10⁵ and a response speed as fast as 5.4 ms. The results suggest that low-cost doctor-blading technique in ambient condition potentially pave a way to eliminate the yellow δ-phase FAPbI₃ and get a high-quality black α-FAPbI₃ perovskite film, as well as fabricate efficient FAPbI₃ perovskite optoelectronic devices.     

Short‐Chain Ligand‐Passivated Stable α‐CsPbI3 Quantum Dot for All‐Inorganic Perovskite Solar Cells

Cubic phase CsPbI₃ (α‐CsPbI₃) perovskite quantum dots (QDs) have received extensive attention due to their all‐inorganic composition and suitable band gap (1.73 eV). However, α‐CsPbI₃ QDs might convert to δ‐CsPbI₃ (orthorhombic phase with indirect band gap of 2.82 eV) due to easy loss of surface ligands. In addition, commonly used long‐chain ligands (oleic acid, OA, and oleylamine, OLA) hinder efficient charge transport in optoelectronic devices. In order to relieve these drawbacks, OA, OLA, octanoic acid, and octylamine are used as capping ligands for synthesizing high‐quality α‐CsPbI₃ QDs. The results indicate that these QDs exhibit excellent optical properties and long‐term stability compared to QDs capped only with OA and OLA. Moreover, QDs with shorter ligands exhibit an enhanced charge transport rate, which improves the power conversion efficiency of photovoltaic devices from 7.76% to 11.87%.     

Solution-Mediated Hybrid FAPbI3 Perovskite Quantum Dots for Over 15% Efficient Solar Cell

Organic–inorganic formamidinium lead triiodide (FAPbI₃) hybrid perovskite quantum dot (QD) is of great interest to photovoltaic (PV) community due to its narrow band gap, higher ambient stability, and long carrier lifetime. However, the surface ligand management of FAPbI₃ QD is still a key hurdle that impedes the design of high-efficiency solar cells. Herein, this study first develops a solution-mediated ligand exchange (SMLE) for preparing FAPbI₃ QD film with enhanced electronic coupling. By dissolving optimal methylammonium iodide (MAI) into antisolvent to treat the FAPbI₃ QD solution, the SMLE can not only effectively replace the long-chain ligands, but also passivate the A- and X-site vacancies. By combining experimental and theoretical results, this study demonstrates that the SMLE engineered FAPbI₃ QD exhibits lower defect density, which is beneficial for fabricating high-quality QD arrays with desired morphology and carrier transport. Consequently, the SMLE FAPbI₃ QD based solar cell outputs a champion efficiency of 15.10% together with improved long-term ambient storage stability, which is currently the highest reported value for hybrid perovskite QD solar cells. These results would provide new design principle of hybrid perovskite QDs toward high-performance optoelectronic application.     

HPbI3: A New Precursor Compound for Highly Efficient Solution‐Processed Perovskite Solar Cells

Recently, there have been extensive research efforts on developing high performance organolead halide based perovskite solar cells. While most studies focused on optimizing the deposition processes of the perovskite films, the selection of the precursors has been rather limited to the lead halide/methylammonium (or formamidium) halide combination. In this work, we developed a new precursor, HPbI₃, to replace lead halide. The new precursor enables formation of highly uniform formamidium lead iodide (FAPbI₃) films through a one‐step spin‐coating process. Furthermore, the FAPbI₃ perovskite films exhibit a highly crystalline phase with strong (110) preferred orientation and excellent thermal stability. The planar heterojunction solar cells based on these perovskite films exhibit an average efficiency of 15.4% and champion efficiency of 17.5% under AM 1.5 G illumination. By comparing the morphology and formation process of the perovskite films fabricated from the formamidium iodide (FAI)/HPbI₃, FAI/PbI₂, and FAI/PbI₂ with HI additive precursor combinations, it is shown that the superior property of the HPbI₃ based perovskite films may originate from 1) a slow crystallization process involving exchange of H⁺ and FA⁺ ions in the PbI₆ octahedral framework and 2) elimination of water in the precursor solution state.     

In Situ Observation of Crystallization Dynamics and Grain Orientation in Sequential Deposition of Metal Halide Perovskites

Metal halide perovskites have revolutionized the development of highly efficient, solution‐processable solar cells. Further advancements rely on improving perovskite film qualities through a better understanding of the underlying growth mechanism. Here, a systematic in situ grazing‐incidence X‐ray diffraction investigation is performed, facilitated by other techniques, on the sequential deposition of formamidinium lead iodide (FAPbI₃)‐based perovskite films. The active chemical reaction, composition distribution, phase transition, and crystal grain orientation are all visualized following the entire perovskite formation process. Furthermore, the influences of additive ions on the crystallization speed, grain orientation, and morphology of FAPbI₃‐based films, along with their photovoltaic performances, are fully evaluated and optimized, which leads to highly reproducible and efficient perovskite solar cells. The findings provide key insights into the perovskite growth mechanism and suggest the fabrication of high‐quality perovskite films for widespread optoelectronic applications.     

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.     

Inorganic Rubidium Cation as an Enhancer for Photovoltaic Performance and Moisture Stability of HC(NH2)2PbI3 Perovskite Solar Cells

Perovskite solar cells (PSCs) based on organic monovalent cation (methylammonium or formamidinium) have shown excellent optoelectronic properties with high efficiencies above 22%, threatening the status of silicon solar cells. However, critical issues of long‐term stability have to be solved for commercialization. The severe weakness of the state‐of‐the‐art PSCs against moisture originates mainly from the hygroscopic organic cations. Here, rubidium (Rb) is suggested as a promising candidate for an inorganic–organic mixed cation system to enhance moisture‐tolerance and photovoltaic performances of formamidinium lead iodide (FAPbI₃). Partial incorporation of Rb in FAPbI₃ tunes the tolerance factor and stabilizes the photoactive perovskite structure. Phase conversion from hexagonal yellow FAPbI₃ to trigonal black FAPbI₃ becomes favored when Rb is introduced. The authors find that the absorbance and fluorescence lifetime of 5% Rb‐incorporated FAPbI₃ (Rb_0.05FA_0.95PbI₃) are enhanced than bare FAPbI₃. Rb_0.05FA_0.95PbI₃‐based PSCs exhibit a best power conversion efficiency of 17.16%, which is much higher than that of the FAPbI₃ device (13.56%). Moreover, it is demonstrated that the Rb_0.05FA_0.95PbI₃ film shows superior stability against high humidity (85%) and the full device made with the mixed perovskite exhibits remarkable long‐term stability under ambient condition without encapsulation, retaining the high performance for 1000 h.     

Photoluminescence Enhancement in Formamidinium Lead Iodide Thin Films

Formamidinium lead iodide (FAPbI₃) has a broader absorption spectrum and better thermal stability than the most famous methylammonium lead iodide, thus exhibiting great potential for photovoltaic applications. In this report, the light‐induced photoluminescence (PL) evolution in FAPbI₃ thin films is investigated. The PL intensity evolution is found to be strongly dependent on the atmosphere surrounding the samples. When the film is exposed to air, its photoluminescence intensity is enhanced more than 140 times after continuous ultraviolet laser illumination for 2 h, and the average lifetime is prolonged from 17 to 389 ns. The enhanced photoluminescence implies that the trap density is significantly reduced. The comparative study of the photoluminescence properties in air, nitrogen, and oxygen/helium environment suggests that moisture is important for the PL enhancement. This is explained in terms of moisture‐assisted light‐healing effect in FAPbI₃ thin films. With this study, a new method is demonstrated to increase and control the quality of hybrid perovskite thin films.     

Non‐Lithographic Fabrication of All‐2D α‐MoTe2 Dual Gate Transistors

As one of the emerging new transition‐metal dichalcogenides materials, molybdenum ditelluride (α‐MoTe₂) is attracting much attention due to its optical and electrical properties. This study fabricates all‐2D MoTe₂‐based field effect transistors (FETs) on glass, using thin hexagonal boron nitride and thin graphene in consideration of good dielectric/channel interface and source/drain contacts, respectively. Distinguished from previous works, in this study, all 2D FETs with α‐MoTe₂ nanoflakes are dual‐gated for driving higher current. Moreover, for the present 2D dual gate FET fabrications on glass, all thermal annealing and lithography processes are intentionally exempted for fully non‐lithographic method using only van der Waal's forces. The dual‐gate MoTe₂ FET displays quite a high hole and electron mobility over ≈20 cm² V^?1 s^?1 along with ON/OFF ratio of ≈10⁵ in maximum as an ambipolar FET and also demonstrates high drain current of a few tens‐to‐hundred μA at a low operation voltage. It appears promising enough to drive organic light emitting diode pixels and NOR logic functions on glass.     

Remarkable Improvements in Volumetric Energy and Power of 3D MnO2 Microsupercapacitors by Tuning Crystallographic Structures

Transition‐metal oxides as faradaic charge‐storage intermediates sandwiched between conductor and electrolyte are key components to store/deliver high‐density energy in microsupercapacitors for many applications in miniaturized portable electronics and microelectromechanical systems. While the conductor facilitating their electron transports, they generally suffer from a switch of rate‐determining step to their sluggish redox reactions in pseudocapacitive energy storage, during which poor cation accessibility and diffusion leads to high internal resistances and lowers volumetric capacitance and rate performance. Here it is shown that the faradaic processes in a model system of MnO₂ can be radically boosted by tuning crystallographic structures from cryptomelane (α‐MnO₂) to birnessite (δ‐MnO₂). As a result of greatly enhanced Na⁺ accessibility and diffusion, 3D layered crystalline δ‐MnO₂ microelectrodes exhibit volumetric capacitance as high as ≈922 F cm^?3 (≈1.5‐fold higher than α‐MnO₂, ≈617 F cm^?3) and excellent rate performance. This enlists δ‐MnO₂ microsupercapacitor to deliver ultrahigh stack electrical powers (up to ≈295 W cm^?3) while maintaining volumetric energy density much higher than that of thin‐film lithium battery.     

Energy Transfer Induced by TADF Polymer Enables the Recycling of Excitons in Perovskite Solar Cells

Formamidinium lead triiodide (FAPbI₃) has been demonstrated as the most efficient perovskite system to date, due to its excellent thermal stability and an ideal bandgap approaching the Shockley-Queisser limit. Whereas, there are intrinsic quantum confinement effects in FAPbI₃, which lead to unwanted non-radiative recombination. Additionally, the black α-phase of FAPbI₃ is unstable under room temperature due to the significant residual tensile stress in the film. To simultaneously address the above issues, a thermally-activated delayed fluorescence polymer P1 is designed in the study to modify the FAPbI₃ film. Owing to the spectral overlap between the photoluminescence of P1 and absorption of the above-bandgap quantum wells of FAPbI₃, the Förster energy transfer occurs at the P1/FAPbI₃ interface, which further triggers the Dexter energy transfer within FAPbI₃. The exciton “recycling” can thus be realized, which reduces the non-radiative recombination losses in perovskite solar cells (PSCs). Moreover, P1 is found to introduce compressive stress into FAPbI₃, which relieves the tensile stress in perovskite. Consequently, the PSCs with P1 treatment achieve an outstanding power conversion efficiency (PCE) of 23.51%. Moreover, with the alleviation of stress in the perovskite film, flexible PSCs (f-PSCs) also deliver a high PCE of 21.40%.     

Ultrastable and Reversible Fluorescent Perovskite Films Used for Flexible Instantaneous Display

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.     

Preparation of Tortuous 3D γ‐CsPbI3 Films at Low Temperature by CaI2 as Dopant for Highly Efficient Perovskite Solar Cells

Inorganic cubic CsPbI₃ perovskite (α‐CsPbI₃) has been widely explored for perovskite solar cells (PSCs) due to its thermal stability and suitable bandgap of 1.73 eV. However, α‐CsPbI₃ usually requires high synthesis temperatures (>320 °C). Additionally, it usually undergoes phase transition to the nonperovskite structure phase (β‐CsPbI₃), which results in poor photoelectric performance in devices. In this study, it is first found that the tortuous 3D CsPbI₃ phase (γ‐CsPbI₃) can be prepared and used for PSCs by solution process without any additive at low temperature (60 °C). The γ‐CsPbI₃ exhibits suitable bandgap of 1.75 eV and favorable photoelectric properties. However, γ‐CsPbI₃ is a metastable phase and easily transforms into β‐CsPbI₃ in ambient moisture. In order to improve the stability of γ‐CsPbI₃, calcium ions (Ca²⁺) with a relatively small radius of 100 pm are used to partially substitute lead ions (119 pm). This research proves that Ca²⁺ can effectively improve the stability of the γ‐CsPbI₃ at room temperature. By optimizing the doping concentration of Ca²⁺ (CsPb_1?xCa_xI₃, x is from 0% to 2%), the Ca²⁺‐doped γ‐CsPbI₃ PSCs achieve a hysteresis‐free J–V curve and a maximum power conversion efficiency (PCE) of 9.20%.     

Boosting Photovoltaic Performance for Lead Halide Perovskites Solar Cells with BF4− Anion Substitutions

Composition engineering is a particularly simple and effective approach especially using mixed cations and halide anions to optimize the morphology, crystallinity, and light absorption of perovskite films. However, there are very few reports on the use of anion substitutions to develop uniform and highly crystalline perovskite films with large grain size and reduced defects. Here, the first report of employing tetrafluoroborate (BF₄^?) anion substitutions to improve the properties of (FA = formamidinium, MA = methylammonium (FAPbI₃)_0.83(MAPbBr₃)_0.17) perovskite films is demonstrated. The BF₄^? can be successfully incorporated into a mixed‐ion perovskite crystal frame, leading to lattice relaxation and a longer photoluminescence lifetime, higher recombination resistance, and 1–2 orders magnitude lower trap density in prepared perovskite films and derived solar cells. These advantages benefit the performance of perovskite solar cells (PVSCs), resulting in an improved power conversion efficiency (PCE) of 20.16% from 17.55% due to enhanced open‐circuit voltage (V_OC) and fill factor. This is the highest PCE for BF₄^? anion substituted lead halide PVSCs reported to date. This work provides insight for further exploration of anion substitutions in perovskites to enhance the performance of PVSCs and other optoelectronic devices.     

Epitaxial Growth of Branched α‐Fe2O3/SnO2 Nano‐Heterostructures with Improved Lithium‐Ion Battery Performance

We report the synthesis of a novel branched nano‐heterostructure composed of SnO₂ nanowire stem and α‐Fe₂O₃ nanorod branches by combining a vapour transport deposition and a facile hydrothermal method. The epitaxial relationship between the branch and stem is investigated by high resolution transmission electron microscopy (HRTEM). The SnO₂ nanowire is determined to grow along the [101] direction, enclosed by four side surfaces. The results indicate that distinct crystallographic planes of SnO₂ stem can induce different preferential growth directions of secondary nanorod branches, leading to six‐fold symmetry rather than four‐fold symmetry. Moreover, as a proof‐of‐concept demonstration of the function, such α‐Fe₂O₃/SnO₂ composite material is used as a lithium‐ion batteries (LIBs) anode material. Low initial irreversible loss and high reversible capacity are demonstrated, in comparison to both single components. The synergetic effect exerted by SnO₂ and α‐Fe₂O₃ as well as the unique branched structure are probably responsible for the enhanced performance.     

All‐Inorganic CsPbI3 Perovskite Phase‐Stabilized by Poly(ethylene oxide) for Red‐Light‐Emitting Diodes

Despite the excellent photoelectronic properties of the all‐inorganic cesium lead iodide (CsPbI₃) perovskite, which does not contain volatile and hygroscopic organic components, only a few CsPbI₃ devices are developed mainly owing to the frequent formation of an undesirable yellow δ‐phase at room temperature. Herein, it is demonstrated that a small quantity of poly(ethylene oxide) (PEO) added to the precursor solution effectively inhibits the formation of the yellow δ‐phase during film preparation, and promotes the development of a black α‐phase at a low crystallization temperature. A systematic study reveals that a thin, dense, pinhole‐free CsPbI₃ film is produced in the α‐phase and is stabilized with PEO that effectively reduces the grain size during crystallization. A thin α‐phase CsPbI₃ film with excellent photoluminescence is successfully employed in a light‐emitting diode with an inverted configuration of glass substrate/indium tin oxide/zinc oxide/poly(ethyleneimine)/α‐CsPbI₃/poly(4‐butylphenyl‐diphenyl‐amine)/WO₃/Al, yielding the characteristic red emission of the perovskite film at 695 nm with brightness, external quantum efficiency, and emission band width of ≈101 cd m^?2, 1.12%, and 32 nm, respectively.     

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.