The fabrication of perovskite solar cells under ambient conditions is more compatible with industrial production and commercial applications. Nevertheless, the iodide oxidation triggered by oxygen and uncontrolled perovskite crystallization pose major challenges to achieving satisfactory performance for the air-processed perovskite solar cell. Herein, we introduce pentaerythrityl tetrakis(3-mercaptopropionate) (PETMP) into the CsPbI2Br precursor solution to simultaneously inhibit the iodide oxidation and regulate perovskite crystallization for assembling high-performance CsPbI2Br perovskite solar cells in ambient air. The coordination interaction between PETMP and CsPbI2Br precursor stabilizes the precursor and slows perovskite crystallization. Moreover, the reductive -SH groups of PETMP convert the formed molecular iodine into iodide, effectively suppressing the iodide oxidation in the precursor solution and during the perovskite crystallization process. Upon PETMP addition, we fabricate a high-quality CsPbI2Br perovskite film with enlarged grains and decreased defect density in ambient air. Consequently, the air-processed CsPbI2Br perovskite solar cell without a hole-transport layer delivers an attractive efficiency of 15.20%, on a par with those of state-of-the-art counterparts assembled under a nitrogen atmosphere. In addition, the unencapsulated air-processed cell preserves 88.7% of its original efficiency after 1200 h of storage under ambient conditions.
Inverted (p-i-n) perovskite solar cells offer advantages such as low fabrication temperatures and minimal hysteresis, but their performance is limited by energy level misalignment and non-radiative recombination at the hole transport layer/perovskite interface. Poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA), a common hole transport material, has a hydrophobic surface and poor interface contact with perovskite, limiting device efficiency and stability. To address this, we introduce 1,1'-bis(diphenylphosphino)ferrocene (DPPF), a traditional ferrocene-based complex with dual phosphine coordination sites, for interface modification between PTAA and perovskite. DPPF optimizes energy level alignment, reduces the hole extraction barrier, and forms strong coordination bonds with uncoordinated Pb2+ in the perovskite, passivating defects and suppressing carrier recombination. DPPF modification also improves perovskite film quality, enhancing crystallization, grain size, and reducing residual stress. The resulting inverted perovskite solar cell with a PTAA/DPPF hole transport layer achieves a power conversion efficiency of 24.3%, with a Voc of 1.133 V. The modified device shows excellent long-term stability, retaining over 83% of initial efficiency after 1500 h of storage in ambient air. This work highlights DPPF's potential as an effective interface modifier for perovskite solar cells.
In flexible perovskite-organic tandem solar cells (TSCs), the numerous grain boundaries (GBs) in Br-rich perovskite films are critical in determining their efficiency and mechanical durability. Exacerbated carrier recombination, photon-induced lattice expansion, and phase segregation originating from GBs substantially reduce the photovoltaic performance and reliability. In this work, we developed a conductive polymer composite by incorporating an ionic liquid into polyurethane (PU), which passivates Pb- and FA-related defects and suppresses halide segregation while mitigating residual stress. Critically, it establishes efficient lateral conductive polymer bridges (CPB) across GBs. The CPB significantly increased carrier diffusion length and suppressed nonradiative recombination. As a result, the rigid wide-bandgap (WBG) perovskite solar cells (PSCs) achieved a champion efficiency of 20.85% along with outstanding operational stability (T90 > 1000 h). In flexible configurations, CPB-mediated devices attained a high efficiency of 19.03% and exhibited excellent mechanical robustness, retaining 92% of their initial PCE after 10 000 bending cycles. Furthermore, the perovskite-organic TSCs reached notable power conversion efficiencies of 25.92% for rigid versions and 24.02% for flexible ones. Remarkably, the rigid tandem cells maintained 87% of their initial PCE after 1000 h of continuous light exposure, while the flexible counterparts retained 81% of their original PCE after 10 000 bending cycles.
The complex moisture-oxygen environment in air places stringent demands on surface passivation for air-processed perovskite solar cells. However, most conventional ammonium ligand-based passivation, which binds to the perovskite surface through a terminal site, often induces ligand intercalation, elevates interfacial resistance, and compromises environmental stability, thereby limiting efficient device fabrication under ambient conditions. In this study, we report a robust, ligand-based, intermediate-site anchoring strategy for nonlayered interfacial passivation using a series of choline derivatives. The thioacyl sulfur coordinates strongly with under-coordinated Pb2+ sites, while iodide counter-anions assist in halide vacancy healing, collectively forming a thermally robust and electronically homogeneous top interface. The surface passivation homogenizes surface potential, optimizes band alignment, relaxes residual strain, and suppresses trap-assisted recombination and halide migration. Consequently, the resulting perovskite solar cells achieve a power conversion efficiency (PCE) of 26.54%, the highest value for air-processed n-i-p PSCs reported so far. These devices also retained over 90% PCE after 2000 h at 65°C and 90% under continuous maximum power point tracking for 1000 h (AM 1.5G, 40°C ± 1°C), with projected T80 lifetimes of ∼9800 h under illumination and ∼11 000 h under thermal aging, among the most stable air-processed perovskite solar cells reported to date.
3D/2D perovskite heterojunction solar cells have attracted intensive interest, due to great advantages of both high power conversion efficiency (PCE) and superior stability. For constructing the heterojunction, transferring pure-phase 2D single crystals onto 3D perovskite effectively avoids the generation of cascaded energy barrier and promotes the carrier transport. However, the interfacial defects during the formation of 3D/2D perovskite heterojunction are scarcely noticed. To address this issue, a thin interfacial layer of octyl ammonium iodide (OAI) is introduced between 3D and 2D perovskites herein. The results show that OAI not only mitigates the erosion of 3D perovskite and passivates the residual PbI2, but also suppresses the surface vacancies defects of both 3D and 2D perovskite layers. The formation of 3D/OAI/2D heterojunction with highly interfacial lattice match induces the generation of compression strain, suppression of carrier recombination and promotion of carrier transport. The 3D/OAI/2D heterojunction devices processed in air ambient have achieved remarkable PCE of 25.07%, retaining over 90% of the initial PCEs after storing in air for 2500 h or continuous one-sun illumination for 1034 h. This work demonstrates an effective strategy of eliminating interfacial defects and lattice mismatch at transferred or epitaxial 3D/2D perovskite heterojunction for advanced optoelectronic applications.
The interface structures between dissimilar layers in perovskite solar cells (PSCs) are prone to the concurrent occurrence of lateral (in-plane) chemical aggregation and vertical (out-of-plane) mechanical delamination. This issue severely affects long-term optoelectronic processes in PSCs, and it has not been addressed holistically. Herein, we introduce an ultrathin interfacial layer of 1,3,6,8-pyrenetetrasulfonic tetrasodium salt (PTS) to stabilize the perovskite/C60 interface at the molecular level. The sulfonate groups in PTS molecules anchor to the perovskite interface, while the parallelly aligned pyrene cores establish robust π-π interactions with C60 molecules. The reconstructed interface enhances the interfacial adhesion and restricts the mobility of C60 molecules, enabling a bidirectional chemo-mechanical interface stabilization (BCIS) mechanism at the perovskite/C60 interface. The resultant PSCs deliver power conversion efficiencies (PCEs) of up to 26.53%, showing 96% PCE retention after 1,000 h maximum-power-point tracking (ISOS-L-1l), and 91% PCE retention after 300 thermal cycles (-40 to 85 °C, IEC61215 MQT11). The scalability of PTS treatment is demonstrated by the 818 cm2 (aperture area) perovskite solar modules (PSMs) with PCEs over 20% using industrial-compatible manufacturing processes under 55% relative humidity (RH). This work underscores bidirectional interface engineering as a critical strategy for advancing commercially viable perovskite photovoltaics.
Owing to their outstanding thermal resilience and appropriate bandgap, all-inorganic CsPbI2Br perovskites are increasingly recognized as attractive materials for advanced photovoltaic applications. Nevertheless, severe energy dissipation caused by interfacial nonradiative recombination, specially at the buried HTL/perovskite junction and the perovskite/ETL interface, remains a major bottleneck that constrains device efficiency. Herein, we develop a dual interface engineering strategy employing ionic liquids (ILs), 1-butyl-3-methylimidazolium hexafluorophosphate (BMIMPF6) and 1-butyl-3-methylimidazolium hexafluoroantimonate (BMIMSbF6), to simultaneously passivate defects at both interfaces in inverted CsPbI2Br perovskite solar cells (PSCs). In this work, we systematically examine the disparate roles of modification at the buried interface versus the top interface. Notably, treatment of the bottom interface with ILs primarily boosts the fill factor (FF) by virtue of enhanced hole extraction and improved perovskite crystallinity. In contrast, passivation at the upper interface significantly elevates the open-circuit voltage (Voc), owing to efficient defect neutralization at the perovskite/PCBM contact. The combined interfacial passivation affords a champion PCE of 15.08% for the BMIMPF6-based dual-surface passivation (DSP) cell and 14.52% for its BMIMSbF6-DSP counterpart, corresponding to a 24.5% relative improvement over the control device (12.11%). Comprehensive characterization reveals that BMIMPF6 outperforms BMIMSbF6 due to its superior defect passivation capability. This work establishes a comprehensive understanding of IL-mediated interface engineering and provides a rational bifacial passivation strategy for high-efficiency inverted PSCs.
Mixed tin-lead (Sn-Pb) perovskites are essential for high-efficiency tandem solar cells, typically employing a formamidinium (FA)-dominated composition with a small amount of MA. However, the regulatory role of such A-site mixing on mixed Sn-Pb perovskite properties remains underexplored. This work demonstrates that engineering the thermodynamic landscape of mixed Sn-Pb perovskite formation enables simultaneous regulation of phase homogeneity and defect chemistry. By controllably incorporating methylammonium (MA) cations, the crystallization kinetics are modulated to promote uniform nucleation, suppress Sn-Pb phase segregation, and inhibit Sn2+ oxidation, thereby mitigating non-radiative recombination losses. As a result, mix tin-lead perovskite solar cells achieved a certified power conversion efficiency (PCE) of 23.90%. By leveraging the improved compositional homogeneity and suppressed defect density, the optimized tin-lead absorber is further integrated into two-terminal monolithic all-perovskite tandem devices, delivering a PCE of 30.13% (certified 29.57%). The unencapsulated tandem devices maintained 90% of its initial PCE after 495 h of maximum power point operation under simulated one-sun illumination.
The buried interface between the hole transport layer (HTL) and the perovskite layer is critical to both the efficiency and stability of inverted perovskite solar cells (PSCs). The conventional sequential deposition approach, where the self-assembled monolayer (SAM)-based HTL is pre-deposited as a separate bottom layer prior to perovskite coating, faces inherent challenges, including insufficient interfacial wetting, high defect densities, and limited scalability. Herein, we introduce a dynamic self-assembly (DSA) approach to simultaneously fabricate the HTL and passivate the perovskite in a single step. By integrating a binary mixture of SAMs ([2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid (MeO-2PACz) and [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz)) and the monomer 2-(dimethylamino)ethyl methacrylate (DMAEMA) directly into the perovskite precursor, an in situ, uniform HTL forms during perovskite crystallization. The SAMs optimize energy alignment and interfacial contact, while the polymerized DMAEMA, localized at grain boundaries, passivates undercoordinated Pb2+ and suppresses iodide-related defects. This combined approach enhances film crystallinity, improves interfacial homogeneity, and drastically reduces non-radiative recombination. Consequently, the champion device achieves a power conversion efficiency (PCE) of 22.03% with a high open-circuit voltage (Voc) of 1.11 V, a short-circuit current density of 25.84 mA cm-2, and a fill factor of 77%. Moreover, the DSA-processed device remains operational throughout prolonged maximum power point (MPP) tracking under continuous illumination and elevated temperature. This work presents DSA as an effective strategy for simultaneous buried interface engineering and defect passivation in inverted PSCs.
Perovskite solar cells (PSCs) exhibit excellent optoelectronic properties, including a high light absorption coefficient and superior carrier mobility. However, challenges remain in their power conversion efficiency and stability. Intrinsic defects and externally introduced defects exert a key impact on their optoelectronic properties. This paper systematically reviews the core characterization techniques and the latest research progress of perovskite carrier dynamics, with a focus on the structure-property relationship and regulation strategies between bulk microstructure/interfacial properties and carrier dynamics. Research has shown that interface engineering, defect passivation, and energy level gradient design can effectively optimize carrier transport and separation processes. Optimization strategies such as additive engineering and machine learning assistance are equally crucial. Photon manipulation, low-cost carbon-based electrodes, and integrated energy storage systems are also discussed. Techniques including transient absorption spectroscopy (TAS) and time-resolved photoluminescence (TRPL) have revealed the mechanisms of carrier generation, relaxation, transport, and recombination, providing theoretical guidance for device design. We further explore the carrier dynamics in tandem perovskite devices, flexible perovskite devices, and triple-mesoporous structures-these core frontier systems are driving the commercial application of perovskite photovoltaic technology.
Driven by advances in renewable energy technologies, research on perovskite optoelectronics has advanced rapidly across material exploration, device engineering, and intelligent integrated systems. Conventional trial-and-error experiments face inherent constraints in precisely regulating perovskite chemical compositions and microstructures, as well as in mitigating degradation in perovskite solar cells (PSCs). Artificial intelligence (AI) and the Internet of Things (IoT) have emerged as powerful tools for material discovery, synthetic condition design, and the prediction of perovskite fundamental properties and device outputs. This review systematically summarizes recent advances in machine learning (ML) implementations for PSC research, covering molecular-scale material screening, synthetic parameter optimization, performance forecasting, device architecture design, and system performance evaluation. We further elaborate on key obstacles hindering ML-assisted perovskite development, including insufficient operational stability, barriers to large-scale fabrication, and limited computational efficiency. Last, we outline promising research avenues and highlight the transformative capacity of ML to advance high-performance, manufacturable perovskite optoelectronic devices.
The performance of inverted CH3NH3GeI3 (MAGeI3) perovskite solar cells incorporating both a hole transport layer (HTL) and an electron transport layer (ETL) was investigated using the Solar Cell Capacitance Simulator (SCAPS). Three candidate HTLs, including PEDOT:PSS, MoS2, and WS2, along with five ETLs including PCBM, TiO2, IGZO, ZnO, and SnO2, have been systematically evaluated. The analysis shows that WS2 and SnO2 provided the most favorable hole and electron transport, respectively. To improve device efficiency, the absorber layer thickness, defect density in MAGeI3, doping levels of WS2 and SnO2, as well as the interface defect densities and the work function of indium tin oxide (ITO), have been systematically studied. The optimal absorber layer thickness is determined to be approximately 900 nm. The optimal doping density of both WS2 and SnO2 is 1 × 1019 cm-3. The MAGeI3 layer should maintain a defect density as low as 1 × 1015 cm-3, and the defect densities at MAGeI3 interfaces should remain at 1 × 1015 cm-2. Additionally, an ITO work function of at least 5.2 eV is necessary to prevent the formation of a Schottky barrier at the ITO/WS2 interface. The simulated power conversion efficiency (PCE) can reach 22.9% under these optimized conditions. Our simulation results offer a viable route to develop high-efficiency MAGeI3 perovskite solar cells.
Realizing high-performance perovskite/silicon tandem solar cells requires precise control of wide-bandgap perovskite crystallization. Solvent engineering is the most direct lever for this task; yet, its intricate, multi-variable mechanisms defy intuition-driven design. Herein, we overcome this bottleneck by pioneering a retrieval-augmented large language model to screen > 8000 solvents, identifying γ-valerolactone (GVL) as a non-toxic, high-performance cosolvent. It is found that the GVL strongly coordinates FA+, thus precisely modulating crystallization kinetics, retarding nucleation, and promoting oriented, micrometer-scale grain growth. The resulting films exhibit not only superior crystallinity, reduced non-radiative recombination, but also improved scalability to large area and the tolerance to increased film thickness. Consequently, both the single-junction and tandem devices achieve efficiencies of 23.3% and 32.5%, respectively, along with excellent stability under moisture and illumination. This study establishes the first artificial intelligence (AI)-guided cosolvent strategy for 1-μm-thick perovskite layers in perovskite/silicon tandem architectures, underscoring the transformative role of generative AI in advancing high-performance photovoltaics.
This study presents the design of ultrathin perovskite solar cells for flexible applications with reduced toxicity. The limited thickness of the perovskite absorber layer leads to insufficient light absorption and, consequently, reduced device efficiency. To address this limitation, plasmonic Au nanowires embedded within the absorber layer are employed to enhance optical absorption through properly tuned resonance. Three-dimensional (3D) Finite-difference time-domain (FDTD) simulations are used to systematically investigate the effects of nanowire geometry, periodicity, and spatial positioning on light absorption. In addition, SiO₂ nanoparticles are incorporated as antireflection structures to further improve light trapping. The optimum structure demonstrates an overall absorption enhancement of approximately 27.8% compared to the reference device, while accounting for parasitic losses associated with Au nanowires. Quantitative analysis indicates that approximately 19.4% of the improvement arises from Au nanowires, whereas about 8.4% is attributed to the antireflective effect of SiO₂ nanoparticles. The enhancement mechanism is analyzed using extinction cross-section spectrum calculations based on Mie theory, electric field distributions, and surface reflectance. SCAPS simulations of optimum device show that the short-circuit current density increases from 15.85 mA/cm² to 19.87 mA/cm², and the power conversion efficiency rises from 14.88% to 18.40%. Furthermore, applying the proposed structures to absorber layer thicknesses of 250 nm and 400 nm results in PCE improvements of 8.7% and 4.0%, achieving efficiencies of 21.43% and 22.29% under optimum parameters. These findings demonstrate the synergistic effect of combining plasmonic nanostructures with antireflective elements, offering an effective strategy for light management in ultrathin perovskite solar cells and paving the way for high-efficiency flexible photovoltaics.
Interfacial phenomena critically influence both the performance and long-term stability of perovskite solar cells; hence, optimizing interfaces remains a key challenge for their commercialization. In this study, we investigate the chemical interactions and electronic structure of the buried interface between the FAPbI3 perovskite absorber and spiro-OMeTAD-based hole transport layer (HTL) in an ITO/SnO2/FAPbI3/HTL device using hard X-ray photoelectron spectroscopy. Our results indicate Pb and I ion incorporation in the spiro-OMeTAD HTL. The Pb 4f core level spectra show the formation of new nonperovskite Pb species, and the N 1s spectra exhibit an additional peak, indicating chemical modifications induced by the deposition of spiro-OMeTAD on the perovskite layer. Moreover, the spiro-OMeTAD N 1s peak exhibits a systematic shift toward lower binding energies with increasing HTL thickness, indicating a downward band bending in the spiro-OMeTAD HTL. Overall, these findings provide direct insight into the chemical and electronic interactions near the FAPbI3/HTL interface and emphasize the importance of optimizing transport layer thickness to achieve favorable energy level alignment and improved device performance.
Vacuum deposition of perovskite thin films offers superior conformality and precise control over solution-based methods. However, non-uniform nucleation and island-like growth produce columnar grains, voids, and trap states at the electron-transport layer (ETL)/perovskite interface, causing non-radiative recombination. In conventional co-deposition, volatile formamidinium iodide (FAI) reaches the SnO2 surface first, undergoes island-like growth in the early stages of deposition, creating pinholes and voids that act as interfacial trap sites. We present a controlled grain growth deposition (CGGD) method using FAPbI3 components. An ultrathin 3.5 nm PbI2 layer is pre-deposited on atomic layer deposited SnO2. This sacrificial nucleation template is fully converted during subsequent FAI/PbI2 co-evaporation, enabling uniform nucleation and laterally coherent grain growth without excess residual PbI2. CGGD suppresses island-like FAI growth and promotes uniform interfacial nucleation, yielding 18.6% larger grains while reducing both bulk and interfacial trap densities. The resulting FAPbI3 films exhibit a 34% reduction in trap-state density and nearly twofold longer carrier lifetimes, evidencing superior structural quality and suppressed non-radiative recombination. Implementing CGGD in perovskite solar cells delivers a stabilized power conversion efficiency (PCE) of 19.9%. This nucleation-controlled deposition route provides a general pathway to high-quality vacuum-deposited films by improving bulk crystallization and ETL/perovskite interfacial defect passivation, facilitating scalable optoelectronic devices.
Perovskite solar cells (PSCs) face significant obstacles to commercialization due to the rapid degradation of perovskite materials under non-equilibrium conditions, especially under ultraviolet (UV) radiation from sunlight. To address this critical challenge, an endogenous redox-sensitive UV absorber, 2,2″-Thiobis-(4-tert-octylphenoxy)-butylamine nickel (TTOB), was introduced into the perovskite precursor solution. The integrated TTOB enhances the efficiency and stability of PSCs through multiple synergistic functions, including superior UV shielding capability and sustained chemical passivation effects for ongoing defect repair. Ultimately, the resultant device fabricated entirely in air achieved a best-in-class power conversion efficiency (PCE) of 25.24%, accompanied by greatly improved stability under various environmental conditions, with retaining approximately 86% of initial efficiency after 1,000 h of continuous UV exposure, about 87% after 40 days of outdoor real-time storage, and over 80% after 1430 h of continuous illumination. This innovative UV protection strategy with endogenous redox-sensitive offers transformative potential for the large-scale application of perovskite photovoltaic technology during actual outdoor operation.
The ambient processing of perovskite solar cells (PSCs) is crucial for scalable industrialization; however, moisture-induced degradation and non-uniform crystallization remain significant hurdles. In this work, we demonstrate a facile, ambient-processable two-step intercalation strategy that premixes cesium iodide (CsI) directly into the PbI2 precursor to regulate the crystallization and carrier dynamics of methylammonium lead iodide (MAPbI3) PSCs. By bypassing conventional solution-processed solubility limits, this pre-intercalation approach ensures a highly uniform Cs+ distribution. Mechanistically, this kinetically promotes Ostwald ripening during crystal growth and thermodynamically relieves native lattice microstrain. Consequently, the optimal CsI concentration (2 mg mL-1) significantly enlarged the perovskite grain size (from 161 nm to 255 nm), reduced dislocation density, and suppressed deep-level trap states. These structural refinements effectively mitigated trap-assisted recombination and improved charge extraction. The optimal ambient-processed device achieved a champion power conversion efficiency (PCE) of 23.17% (average 20.57 ± 1.28%) with minimized hysteresis. Furthermore, applying this CsI-intercalated architecture in a strictly controlled environment (glovebox) validated its fundamental optoelectronic potential, yielding a true PCE of 23.78% with an excellent fill factor of 80.9%. Finally, the unencapsulated devices demonstrated remarkable durability, retaining 97.7% of their initial efficiency under continuous operational illumination and 82% after 30 days of ambient storage. These findings establish controlled CsI precursor intercalation as a scalable and mechanistically sound pathway for highly efficient and stable perovskite photovoltaics.
The long-term stability of perovskite solar cells (PSCs) is critically undermined by degradation at the buried interface, where residual tensile strain and ultraviolet (UV) irradiation act synergistically. Here, we introduce a fullerene-based photoresponsive molecule, C60-azo, to construct an adaptive SnO2/perovskite interface. Unlike static interlayers, C60-azo functions as a dynamic molecular switch. Under UV illumination, its trans-to-cis isomerization actively generates a beneficial compressive stress to counteract residual tensile strain. Simultaneously, the light-enriched cis-isomer enhances dynamic defect passivation. This mechanochemical dual mechanism effectively mitigates UV-driven lattice distortion and chemical degradation. Consequently, the modified n-i-p PSCs achieve a power conversion efficiency of 26.60% and exhibit enhanced durability. Unencapsulated devices retain 92.7% of their initial performance after 488 h of continuous UV exposure. Encapsulated cells also maintain 94.7% efficiency after 1000 h of maximum power point tracking under continuous 1-sun-equivalent LED illumination. This work establishes dynamic photoresponsive interface engineering as a pioneering strategy for durable perovskite optoelectronics.
Carbon-based perovskite solar cells (C-PSCs) offer a low-cost, stable alternative to metal electrodes; however, the high porosity of carbon electrodes leads to poor interfacial contact and weak mechanical adhesion to the underlying carrier transport layer, limiting device performance and robustness. Here, we report a solvent-free additive polishing strategy using a synergistic combination of two-dimensional (2D) graphene nanoplatelets and 3D graphite flakes to densify the hole-transport-layer (HTL)/carbon interface by creating conformal van der Waals (vdW) anchors. This graphene/graphite additive polishing process fills micro-voids on the porous carbon electrode surface, reduces carbon electrode surface roughness, and creates a graphene anchor that increases interfacial fracture energy and promotes the carbon surface heating release. Electrically, the polished interface facilitates superior charge extraction, thereby reducing charge-transfer resistance. Consequently, regular n-i-p perovskite solar devices achieve a promised power conversion efficiency (PCE) of 23.28% (0.09 cm2) and maintain a high PCE of 19.62% at a scalable 1.0 cm2 area. This work provides a high-throughput, dry-processing paradigm for more affordable, robust, and highly efficient carbon-based perovskite photovoltaics.