Unencapsulated Perovskite Solar Cells Research Articles

Lattice Strain Regulation and Halogen Vacancies Passivation Enable High-Performance Formamidine-Based Perovskite Solar Cells.

Formamidinium lead iodide (FAPbI3) perovskite has lately surfaced as the preferred contender for highly proficient and robust perovskite solar cells (PSCs), owing to its favorable bandgap and superior thermal stability. Nevertheless, volatilization and migration of iodide ions (I-) result in non-radiating recombination centers, and the presence of large formamidine (FA) cations tends to cause lattice strain, thereby reducing the power conversion efficiency (PCE) and stability of PSCs. To solve these problems, the lead formate (PbFa) is added into the perovskite solution, which effectively mitigates the halogen vacancy and provides tensile strain outside the perovskite lattice, thereby enhancing its properties. The strong coordination between the C═O of HCOO- and Pb-I backbones effectively immobilizes anions, significantly increases the energy barrier for anion vacancy formation and migration, and reduces the risk of lead ion (Pb2+) leakage, thereby improving the operation and environmental safety of the device. Consequently, the champion PCE of devices with Ag electrodes can be increased from 22.15% to 24.32%. The unencapsulated PSCs can still maintain 90% of the original PCE even be stored in an N2 atmosphere for 1440h. Moreover, the target devices have significantly improved performance in terms of light exposure, heat, or humidity.

High-Efficiency Perovskite Solar Cells with Improved Interfacial Charge Extraction by Bridging Molecules.

The interface between the perovskite layer and electron transporting layer is a critical determinate for the performance and stability of perovskite solar cells (PSCs). The heterogeneity of the interface critically affects the carrier dynamics at the buried interface. To address this, a bridging molecule, (2-aminoethyl)phosphonic acid (AEP), is introduced for the modification of SnO2/perovskite buried interface in n-i-p structure PSCs. The phosphonic acid group strongly bonds to the SnO2 surface, effectively suppressing the surface carrier traps and leakage current, and uniforming the surface potential. Meanwhile, the amino group influences the growth of perovskite film, resulting in higher crystallinity, phase purity, and fewer defects. Furthermore, the bridging molecules facilitate the charge extraction at the interface, as indicated by the femtosecond transient reflection (fs-TR) spectroscopy, leading to champion power conversion efficiency (PCE) of 26.40% (certified 25.98%) for PSCs. Additionally, the strengthened interface enables improved operational durability of ≈1400 h for the unencapsulated PSCs under ISOS-L-1I protocol.

Target therapy at buried interfaces toward efficient and stable inorganic perovskite solar cells

The enhancement of power conversion efficiency (PCE) of perovskite solar cells (PSCs) is critically affected by charge recombination induced by buried interface defects. In light of this, a simple and effective target therapy strategy has been developed by doping 4-(diphenylphosphino)benzoic acid (4DBA) molecules at the tin oxide (SnO2)/perovskite interface. The effects of 4DBA on carrier transport, perovskite growth, defect passivation, and PSCs properties were systematically investigated. It is illustrated that 4DBA molecules not only passivate oxygen vacancy (OV) defects on the SnO2 surface, enhancing the conductivity of the SnO2 film and accelerating electron transfer, but also passivate perovskite interface defects, thereby improving the quality of the perovskite film. Ultimately, the efficiency of CsPbBr3 device with 4DBA-modified buried interface increased from 8.87% to 10.78%, an improvement of 21.53%. Furthermore, the efficiency of CsPbI2Br increased from 12.83% to 14.44%, an improvement of 12.55%, further demonstrating the effectiveness and universality of this strategy. Excitingly, the unencapsulated PSCs exhibit excellent long-term stability under high relative humidity and high temperatures.

Halogenated Hole Selective Contact Enhances Interfacial Weak Bonding of Perovskite Solar Cells

AbstractWeak bonding between the perovskite and charge transport layers can lead to interfacial defects, hindering charge transfer and limiting the efficiency and stability of perovskite solar cells (PSCs). To address this issue, two halogenated spiro[fluorene‐9,9′‐xanthene]‐based molecules (SFX‐DM‐F and SFX‐DM‐Cl) are designed as an interfacial layer between perovskite and hole transport materials (HTMs). Both first‐principles simulations and experimental results are used to demonstrate that these halogenated interfacial layers improve the contact stability between perovskite's Pb(II) and HTMs, increasing the efficiency of charge transfer. The similar structure of interlayer to HTM also enhances the interfacial hole transfer integral, favoring effective hole transport. The PSCs based on SFX‐DM‐Cl achieve power conversion efficiencies of 24.8% (0.0625 cm2) and 23.1% (1 cm2). Even after 2000 h at a relative humidity of 15–20%, the unencapsulated PSC retains 94% of its initial efficiency. This work proposes the halogenated homologous HTMs as interfacial molecular bridges to optimize weak chemical bonds and hole transfer, thereby enabling efficient and stable PSCs.

Perovskite solar cells with self-disintegrating seeds deliver an 83.64 % fill factor

Large-seed-induced regulation significantly impacts perovskite film grain growth; however, it inadequately addresses stress and defect issues at the perovskite interface. To counter this, we introduce an innovative self-disintegrating seed approach, employing 2D (4-FBZA)2PbI4 perovskite to enhance the crystallization process. During perovskite crystal growth, (4-FBZA)2PbI4 could disintegrate and release 4-FBZA+ ions. These ions effectively anchor the perovskite interface and interact with FA+ and [PbI6]4- within the lattice, passivating defects and releasing detrimental stress. This strategy results in reduced nonradiative recombination and residual stress, culminating in perovskite solar cells (PSCs) achieving a champion power conversion efficiency (PCE) of 23.73 % and a remarkable fill factor of 83.64 %. Crucially, unencapsulated PSCs retain over 90 % of their initial PCE following 2000 h of exposure in ambient conditions at 25±5 °C and 60 % relative humidity.

Improving Buried Interface Contact by Bidentate Anchoring for Inverted Perovskite Solar Cells.

Nickel oxide (NiOx) is a promising hole transport layer (HTL) to fabricate efficient and large-scale inverted perovskite solar cells (PSCs) due to its low cost and superior chemical stability. However, inverted PSCs based on NiOx are still lagging behind that of other HTL because of the poor quality of buried interface contact. Herein, a bidentate ligand, 4,6-bis (diphenylphosphino) phenoxazine (2DPP), is used to regulate the NiOx surface and perovskite buried interface. The diphosphine Lewis base in the 2DPP molecule can coordinate both with NiOx and lead ions at NiOx/perovskite interface, leading to high-quality perovskite films with minimized defects. It is found that the inverted PSCs with 2DPP-modified buried interface exhibit double advantages of being both fast charge extraction and reduced nonradiative recombination, which is a combination of multiple factors including favorable energetic alignment, improved interface contact and strong binding between NiOx/2DPP and perovskite. The optimal PSC based on 2DPP modification yields a champion power conversion efficiency (PCE) of 21.9%. The unencapsulated PSC maintains above 75% of its initial PCE in the air with a relative humidity (RH) of 30-40% for 1000h.

In-situ defect passivation assisted three-step printing of efficient and stable formamidine-lead bromide solar cells

Perovskite solar cells (PSCs) emerge as the most promising photovoltaics (PV) for their high performance and potential convenient cost-effective production routes comparing to the sophomore PV technologies. The printed PSCs with simplified device architecture and fabrication procedures could further enhance the competitive strength of PSC technology. In this work, we present an in-situ defect passivation (ISDP) assisted full-printing of high performance formamidine-lead bromide (FAPbBr3) PSCs. Only three rapid printing steps are involved for electron transporting layer (ETL), perovskite and carbon to form a complete solar cell on the low-cost fluorine-doped tin oxide (FTO) substrate. Long-chain polymer monomethyl ether polyethylene glycol is particularly utilized as the ISDP passivator, leading to conformal coating on the rough FTO and defect passivation for both ETL and perovskite during printing. A high efficiency of 10.85% (certified 10.14%) and a high Voc up to 1.57 V are achieved for the printed device. The unencapsulated PSCs maintain above 90% of the initial efficiency after continuously heating at 85 °C for 1000 h and over 80% of the efficiency after the maximum power point tracking for 3500 h. The fully printed semitransparent PSCs with carbon grids (CGs) show average visible light transmittance over 33% and an efficiency of 8.81%.

Synergetic Exterior and Interfacial Approaches by Colloidal Carbon Quantum Dots for More Stable Perovskite Solar Cells Against UV.

The achievement of both efficiency and stability in perovskite solar cells (PSCs) remains a challenging and actively researched topic. In particular, among different environmental factors, ultraviolet (UV) photons play a pivotal role in contributing to device degradation. In this work, by harvesting simultaneously both the optical and the structural properties of bottom-up-synthesized colloidal carbon quantum dots (CQDs), a cost-effective means is provided to circumvent the UV-induced degradation in PSCs without scarification on their power conversion efficiencies (PCEs). By exploring and optimizing the number of CQDs and the different locations/interfaces of the solar cells where CQDs are applied, a synergetic configuration is achieved where the photovoltaic performance drop due to optical loss is completely compensated by the increased perovskite crystallinity due to interfacial modification. As a result, on the optimized configurations where CQDs are applied both on the exterior front side as an optical layer and at the interface between the electron transport layer and the perovskite absorber, unencapsulated PSCs with PCEs >20% are fabricated which can maintain up to ≈94% of their initial PCE after 100h of degradation in ambient air under continuous UV illumination (5mWcm-2).

Minimizing Voltage Losses via Synergistically Reducing Hetero-Interface Energy Offset for High Efficiency Perovskite Solar Cells.

The open circuit voltage (VOC) losses at multiple interfaces within perovskite solar cells (PSCs) limit the improvements in power conversion efficiency (PCE). Herein, a tailored strategy is proposed to reduce the energy offset at both hetero-interfaces within PSCs to decrease the VOC losses. For the interface of perovskite and electron transport layer where exists a mass of defects, it uses the pyromellitic acid to serve as a molecular bridge, which reduces non-radiative recombination and energy level offset. For the interface of perovskite and hole transport layer, which includes a passivator of PEAI, the detrimental effect (negative shift of work function) of PEAI passivation and optimizing the interface energy level alignment are neutralized by incorporating (2-(4-(bis(4-methoxyphenyl)amino)phenyl)-1-cyanovinyl)phosphonic acid. Owing to synergistically reduced hetero-interface energy offset, the PSCs achieve a PCE of 25.13%, and the VOC is increased from 1.134 to 1.174V. In addition, the resulting PSCs possess enhanced stability, the unencapsulated PSCs can maintain ≈96% and ≈97% of their initial PCE after 2000h of aging under ambient conditions and 210h under operation conditions.

Zn–Porphyrin Antisolvent Engineering‐Enhanced Grain Boundary Passivation for High‐Performance Perovskite Solar Cell

Perovskite solar cells (PSCs) represent a promising and rapidly evolving technology in the field of photovoltaics due to their easy fabrication, low‐cost materials, and remarkable efficiency improvements over a relatively short period. However, the grain boundaries in the polycrystalline films exhibit a high density of defects, resulting in not only heightened reactivity to oxygen and water but also hampered charge transport and long‐term stability. Herein, an approach involving Zn‐porphyrin (Zn‐PP)‐upgraded antisolvent treatment to enhance the grain size and meanwhile passivate grain boundary defects in FA0.95MA0.05PbI2.85Br0.15 perovskites is presented. The Zn‐PP molecules significantly improve structural and optical properties, effectively mitigating defects and promoting carrier transport at the perovskite/hole transport layer interface. The density functional theory simulation confirms that Zn‐PP forms a strong chemical bonding with the perovskite surface. With Zn‐PP passivation, the total density of state shifts to higher‐energy regions with molecular adsorption, especially near the valence and conduction band edges, indicating that there is an increase in conducting properties of the surface with molecular adsorption. The power conversion efficiency (PCE) of PSCs increases significantly as a result of this improvement, rising from 15.38% to 19.11%. Moreover, unencapsulated PSCs treated with Zn‐PP exhibit outstanding stability, retaining over 91% of their initial PCE.

A Universal and Versatile Hole Transport Layer “Activator” Enables Stable Perovskite Solar Cells with Efficiency Near 25%

AbstractOrganic small molecules have been proven to be the most efficient and predominantly employed hole transport layers (HTLs) in perovskite solar cells (PSCs), the reliance of HTLs on additives like Li‐TFSI has been unavoidable, particularly in terms of the well‐known Spiro‐OMeTAD. However, Li‐TFSI aggregation in HTL results in the decreased performance and stability of PSCs with serious hysteresis. It is an urgent need to explore a universal strategy to solve Li‐TFSI‐induced issues. Herein, a pyrene‐based organic semiconductor (PC) as an effective and universal additive for HTL application is developed. It is found that the introduction of PC can efficiently improve the hot carriers extraction/transfer and reduce the charge recombination in the device. Consequently, PSCs based on Spiro‐OMeTAD+PC as a HTL exhibit an excellent PCE of 24.80% with a negligible hysteresis, much higher than the control device (22.14%). Additionally, the efficiency of the PC incorporated into another well‐known X60 HTL‐treated device is enhanced to 24.12% from the control device (22.04%), confirming its universal application in PSCs. Moreover, PC can effectively suppress the Li+ aggregation in HTL, and the unencapsulated PSCs exhibit high stability. The findings in this work provide an effective and universal avenue to construct highly efficient and stable PSCs.

Fine optimized cation immobilization strategy for enhancing stability and efficiency of perovskite solar cells

The migration and volatilization of cations within organic–inorganic hybrid perovskite (OIPs) materials has been identified as a major issue for irreversibly degrading perovskite solar cells (PSCs), severely limiting their performance and impeding progress toward large-scale applications. To mitigate these problems, an adjustable cation immobilization strategy was proposed for the first time, in which a series of fluorobenzenesulfonamide (FBSA) molecules was introduced into perovskite precursor, a strong coordination bond was formed between the sulfonamide group with the octahedral imperfection caused by iodine vacancy, along with a hydrogen bond formed between the cation and F atom. As a result, the A-site cations were tightly immobilized in the octahedral of perovskite crystal lattice and the uncoordinated Pb2+ defects were effectively eliminated. Besides, the immobilization distance of cation was finely optimized by changing the substitution position of F atoms. Based on the cation-immobilized perovskite film, the efficiency of PSCs was significantly increased from 19.88 % to 22.30 %. Moreover, the unencapsulated PSCs exhibited impressive light and thermal stability, retaining 82 % of the initial efficiency after 720 h illumination at 1-sun, and maintaining nearly 80 % of the initial PCE after heating at 85 °C for 240 h. Thus, the present study offers a promising approach for advancing the commercialization of stable and high-efficiency perovskite solar cells.

Reinforced SnO2 tensile‐strength and “buffer‐spring” interfaces for efficient inorganic perovskite solar cells

AbstractSuppressing nonradiative recombination and releasing residual strain are prerequisites to improving the efficiency and stability of perovskite solar cells (PSCs). Here, long‐chain polyacrylic acid (PAA) is used to reinforce SnO2 film and passivate SnO2 defects, forming a structure similar to “reinforced concrete” with high tensile strength and fewer microcracks. Simultaneously, PAA is also introduced to the SnO2/perovskite interface as a “buffer spring” to release residual strain, which also acts as a “dual‐side passivation interlayer” to passivate the oxygen vacancies of SnO2 and Pb dangling bonds in halide perovskites. As a result, the best inorganic CsPbBr3 PSC achieves a champion power conversion efficiency of 10.83% with an ultrahigh open‐circuit voltage of 1.674 V. The unencapsulated PSC shows excellent stability under 80% relative humidity and 80°C over 120 days.

Enhanced Efficiency and Stability of Quasi Two-dimensional Perovskite Solar Cells via Dual Additives

Quasi two-dimensional alternating cation (ACI)-type perovskites have drawn extensive research interest owing to better stability than their 3D counterparts. However, the poor charge-transfer characteristics of quasi two-dimensional perovskite film significantly impact the efficiency and stability of the devices. Herein, we propose a dual additives strategy utilizing urea and methylammonium chloride to manage the growth of (GA)(MA)5Pb5I16 perovskite films. The morphology and photoelectric characteristics manifest that the dual additives not only significantly enlarge the crystal size of the film, but also optimize the distribution of the quantum well thickness. Therefore, the solar cell based on dual additives-treated perovskite film achieves an optimal efficiency of 20.86%, far higher than 17.11% for that without additive. Moreover, the environmental stability of the quasi two-dimensional perovskite solar cells (PSCs) is raised. The unencapsulated PSCs hold 93% of the initial efficiency after being placed under environmental conditions for 1500hours. These results demonstrate that using dual additives is a promising strategy to obtain high-performance PSCs.

One‐Step Construction of a Perovskite/TiO2 Heterojunction toward Highly Stable Inverted All‐Layer‐Inorganic CsPbI2Br Perovskite Solar Cells with 17.1% Efficiency

AbstractAll‐layer‐inorganic perovskite solar cells (PSCs) are prized for their remarkable thermal stability and low cost. However, “imperfect contact” at the perovskite heterojunction hinders charge transport and causes photochemical deterioration, restricting photovoltaic performance, and operational stability. Herein, an efficient perovskite/TiO2 heterojunction is constructed, produced by adding TiO2 to an antisolvent to concurrently form a CsPbI2Br perovskite layer and a top TiO2 electron transport layer in one step, which significantly improves the interfacial contact and thus facilitates charge transport at the heterojunction. The resultant inverted all‐layer‐inorganic PSCs exhibit a superior efficiency of 17.1%. Moreover, given the high‐quality perovskite/TiO2 heterojunction and low interface defects, the encapsulated PSCs retain 91% or 92% of their initial efficiency for 1000 h under maximum power point tracking or damp‐heat conditions (85 °C and 85% relative humidity), respectively. Surprisingly, the unencapsulated PSCs maintain an initial efficiency of 86% during aging, even at 200 °C for 200 h.

Thick film high-performance carbon-based CsPbIBr2 perovskite solar cells vis nano-perovskite modified hot casting method

All-inorganic carbon-based CsPbIBr2 perovskite solar cells (PSCs) have attracted attention due to their more balanced performance and stability. The performance of the PSCs is highly dependent on the quality of the absorber films. Unfortunately, most high-performance films are prepared in a glove box and conventional preparation methods often produce perovskite films within 400 nm of thickness, which is detrimental to large area device fabrication and limits their commercial application. Here we had demonstrated a short chain ligands nano-CsPbIBr2 particles modified hot-casting method to deposit a perovskite film with thickness up to 800 nm. It was carried out by spin-coating a hot CsPbIBr2 precursor solution onto nano-CsPbIBr2 particles film on an electron transport layer (ETL), and then depositing nano-CsPbIBr2 particles on the precursor film again before annealing. The nano-CsPbIBr2 particles on the ETL promotes precursor solution crystallization and increased film thickness, and the nano-CsPbIBr2 particles on the precursor film promoted grain growth and reduced defects due to compositional deviations from stoichiometric ratios. The power conversion efficiency (PCE) of the PSCs fabricated by this method is up to 10.66 %. The unencapsulated PSCs still retain more than 85 % of the initial PCE when stored at ambient atmosphere (RH 50–60 %) for 10 days.

Regulating molecular stacking to construct a superior interfacial contact for highly efficient and stable perovskite solar cells

The non-radiative charge carrier recombination loss at the surface and interface of the perovskite layers in perovskite solar cells (PSCs) is the main cause of their limited power conversion efficiency (PCE). Here we propose an efficient strategy to minimize the non-radiative recombination by introducing symmetric molecules with regular arrangement at the interface between the perovskite layer and hole transport layer (HTL). One end of the symmetric molecule gets in a close contact with the terminal groups of the molecules in the HTL, while the other end promotes connection with the perovskite, resulting in an enhanced interfacial electrical contact and a better valence band energy-level alignment for efficient hole extraction. In contrast, introducing similar but asymmetrical molecules forms a dimer structure and mismatched energy levels at the interface region, which is detrimental to the carrier transport. The best-performing planar PSC with the symmetric molecular modification exhibited an increase in the PCE from 21.05% to 24.02% with a substantially enhanced fill factor of 84.0%, which can be ascribed to the synergistic effects of surface defect passivation and reduction in the interfacial energy barrier. Furthermore, the corresponding unencapsulated PSC retained 80% of the original PCE after 4,000 h of aging in dry air.

Regulating the Crystallization Growth of Sn-Pb Mixed Perovskites Using the 2D Perovskite (4-AMP)PbI4 Substrate for High-Efficiency and Stable Solar Cells.

Sn-Pb mixed perovskite solar cells (PSCs) are developing rapidly and making great progress due to their environmentally friendly advantages. High-crystalline quality perovskite films are essential for obtaining high-efficiency and -stability PSCs. Here, the DJ-phase two-dimensional (2D) perovskite (4-AMP)PbI4 (4-AMP is 4-(aminomethyl) piperidine) was used as a substrate to regulate the crystallization growth of the Sn-Pb mixed perovskite for preparing high-quality perovskite films, and the regulation mechanism was analyzed in detail. The results indicate that the suitable amount of the 2D perovskite substrate is favorable for the formation of PbI2/SnI2 films with wide intergranular gaps and vertical distribution grain boundaries. Moreover, the suitable hydrophobicity of the PbI2/SnI2 film made on the 2D perovskite substrate also provides a better template for regulating the formation and dissolution of prophase perovskite capping. In addition, the 4-AMP cations from the collapsed 2D perovskite substrate can diffuse into PbI2/SnI2 films and interact with PbI2 to form the intermediate (4-AMP)-PbI2-(4-AMP) and with SnI2 to form the 2D perovskite (4-AMP)SnI4. All of these promote the diffusion of FAI/MAI molecules and decrease the crystallization growth rate of the Sn-Pb perovskite and thus increase the conversion levels of the perovskite phase and improve the crystallization orientation and quality of the perovskite, which helps mitigate the erosion of water and oxygen. In addition, the 2D perovskite used as a substrate can passivate the buried interface defects and improve the interfacial contact. Moreover, the diffusion behavior of 4-AMP cations regulates the perovskite energy levels, which match more with those of the electron transport layer. As a result, the champion device made on the (4-AMP)PbI4 substrate acquires a power conversion efficiency (PCE) of 17.7% with an open-circuit voltage (Voc) of 0.806 V, a short-circuit current density (Jsc) of 28.97 mA cm-2, and a fill factor (FF) of 75.86%, far exceeding those of the control device. Meanwhile, the unencapsulated PSCs modified with 4-AH retain above 70% of the initial efficiency value after storage for 1200 h in N2 at room temperature and about 25% of its initial efficiency after exposure to air for nearly 300 h with RH = 30 ± 10% at room temperature, while the control device has only 30% of the initial efficiency and near-zero efficiency at the same conditions.

Laser Derived Electron Transport Layers with Embedded p-n Heterointerfaces Enabling Planar Perovskite Solar Cells with Efficiency over 25.

Electron transport layers (ETLs) with pronounced electron conducting capability are essential for high performance planar perovskite photovoltaics, with the great challenge being that the most widely used metal oxide ETLs unfortunately have intrinsically low carrier mobility. Herein is demonstrated that by simply addressing the carrier loss at particle boundaries of TiO2 ETLs, through embedding in ETL p-n heterointerfaces, the electron mobility of the ETLs can be boosted by three orders of magnitude. Such embedding is encouragingly favorable for both inhibiting the formation of rutile phase TiO2 in ETL, and initiating the growth of high-quality perovskite films with less defect states. By virtue of these merits, creation of formamidinium lead iodide perovskite solar cells (PSCs) with a champion efficiency of 25.05% is achieved, setting a new benchmark for planar PSCs employing TiO2 ETLs. Unencapsulated PSCs deliver much-improved environmental stability, i.e., more than 80% of their initial efficiency after 9000 h of air storage under RH of 40%, and over 90% of their initial efficiency at maximum power point under continuous illumination for 500 h. Further work exploring other p-type nanocrystals for embedding warrants the proposed strategy as a universal alternative for addressing the low-carrier mobility of metal oxide based ETLs.

In-situ compensation for thermal strain by phase transformation strain in all-inorganic perovskite solar cells

The presence of defects and residual tensile strain in perovskites has a significant and deleterious impact on the efficiency and stability of all-inorganic perovskite solar cells (PSCs). Here, dimethyl sulfoxide (DMSO) with strong polarity and high boiling point is introduced into the PbBr2 precursor to delay the crystallization of PbBr2, leading to the formation of high-quality PbBr2 films by delaying the solution reaching supersaturation. The formation of PbBr2(DMSO) adduct facilitates the complete reaction of PbBr2 with CsBr via intramolecular exchange, thus preventing the formation of impurity phases such as CsPb2Br5. As a result, the defect density of CsPbBr3 films decreased by 33% due to the improved phase purity, thicker films, larger grain sizes, and reduced grain boundaries. The small porosity of PbBr2 film combined with a more complete phase-conversion process results in an expanded perovskite film that experiences compressive strain, effectively compensating for the tensile strain generated during annealing and thereby achieving the goal of strain relaxation. The optimized DMSO-based device, which exhibits compressive strain and minimal defects, achieves a remarkable efficiency of 10.11% with an open-circuit voltage of up to 1.611 V. Additionally, the unencapsulated PSC demonstrates excellent stability under 80% relative humidity and 80 °C over 30 days.