Infiltrated 2D/3D Heterojunction with Tunable Electric Field Landscape for Robust Inverted Perovskite Solar Cells with over 24% Efficiency.

In inverted perovskite solar cells, conventional planar 2D/3D perovskite heterojunctions typically exhibit a type-II band alignment, where the electric field tends to drive the electron motion in the opposite direction to the direction of electron transfer. Here, a 2D/3D gradient heterojunction is developed by allowing the 2D perovskite to infiltrate the 3D perovskite surface along the grain boundaries using the interaction between the organic cation of the 2D perovskite and the pseudohalogen thiocyanate ion (SCN-), which has the ability to diffuse downward. The infiltrated 2D perovskite not only fills the gaps of grain boundaries with improved structural stability, but it also reconstructs the original landscape of the electric field toward the n-doped surface to enable more rapid electron transfer and weaken the adverse type-II band alignment effect. Since 2D perovskite seals the GBs, the nonvolatile SCN- can accumulate at the top and bottom dual interfaces, releasing residual stress and significantly inhibiting nonradiative recombination. The device exhibits an excellent efficiency of 24.76% (certified 24.29%) and long-term stability that is >90% of the original PCE value after 800 h of heating at 85 °C or in high humidity (≈65%).

Lead Iodide Redistribution Enables In Situ Passivation for Blading Inverted Perovskite Solar Cells with 24.5% Efficiency.

Blade-coating stands out as an alternative for fabricating scalable perovskite solar cells. However, it demands special control of the precursor composition regarding nucleation and crystallization and currently exhibits lower performance than the spin-coating process. It is mainly the resulting film morphology and excess lead iodide (PbI2) distribution that influences the optoelectronic properties. Here, the effectiveness of introducing N-Methyl-2-pyrrolidone (NMP) to regulate the structure of the perovskite layer and the redistribution of PbI2 is found. The introduction of NMP leads to the accumulation of excess PbI2, mainly on the top surface, reducing residual PbI2 at the perovskite buried interface. This not only facilitates the passivation of perovskite grain boundaries but also eliminates the potential degradation of the PbI2 triggered by light illumination in the perovskite buried interface. The optimized NMP-modified inverted perovskite solar cell achieves a champion efficiency of 24.5%, among the highest reported blade-coated perovskite solar cells. Furthermore, 13.68 cm2 blading perovskite solar modules are fabricated and demonstrate an efficiency of up to 20.4%. These findings underscore that with proper modulation of precursor composition, blade-coating can be a feasible and superior alternative for manufacturing high-quality perovskite films, paving the way for their large-scale applications in photovoltaic technology.

Amphoteric Ion Bridged Buried Interface for Efficient and Stable Inverted Perovskite Solar Cells.

Synergistic morphology and defects management at the buried perovskite interface are challenging but crucial for the further improvement of inverted perovskite solar cells (PerSCs). Herein, an amphoteric organic salt, 2-(4-fluorophenyl)ethylammonium-4-methyl benzenesulfonate (4FPEAPSA), is designed to optimize the film morphology and energy level alignment at the perovskite buried interface. 4FPEAPSA treatment promotes the growth of a void-free, coarse-grained, and hydrophobic film by inducing the crystal orientation. Besides, the dual-functional 4FPEAPSA can chemically interact with the perovskite film, and passivate the defects of iodine and formamidine vacancies, tending to revert the fermi level of perovskite to its defect-free state. Meanwhile, the formation of a p-type doping buried interface can facilitate the interfacial charge extraction and transport of PerSCs for reduced carrier recombination loss. Consequently, 4FPEAPSA treatment improves the efficiency of the perovskite devices to 25.03% with better storage, heat, and humidity stability. This work contributes to strengthening the systematic understanding of the perovskite buried interface, providing a synergetic approach to realize precise morphology control, effective defect suppression, and energy level alignment for efficient PerSCs.

23.81%-Efficiency Flexible Inverted Perovskite Solar Cells with Enhanced Stability and Flexibility via a Lewis Base Passivation.

Lewis base molecules bind the undercoordinated lead atoms at interfaces and grain boundaries, leading to the high efficiency and stability of flexible perovskite solar cells (PSCs). We demonstrated a highly efficient, stable, and flexible PSC via interface passivation using a Lewis base of tri(o-tolyl)phosphine (TTP). It not only induced an intimate interface contact and a complete deposition of the perovskite thin layers on hole transport layers (HTLs) but also led to a better perovskite with a raised crystallinity, fewer defects, and a better morphology, including fewer gullies, high uniformity, and low roughness. Furthermore, the TTP treatments induced a good alignment of energy levels among the perovskites, HTLs, and C60. The resultant flexible inverted PSCs exhibited a high power conversion efficiency (PCE) of 23.81%, which is one of the highest PCEs among these flexible inverted PSCs. Moreover, the optimized flexible PSCs exhibited high storage stability, superior operation stability, and enhanced mechanical flexibility. This study presents an effective method to substantially raise the PCE, stability, and mechanical flexibility of the flexible inverted perovskite photovoltaics.

Ion-Exchange Polymer Network Enhanced Interfacial Compatibility for Stable and Efficient Inverted Perovskite Solar Cells.

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as a low-cost and water-processable hole transport material has been widely used in various optoelectronic devices. Although the incorporation of anionic polyelectrolyte PSS in PEDOT contributes to superior water solubility, the trade-off between efficiency and stability remains a challenging issue, limiting its reliable application in perovskite solar cells (PSCs). Herein, we proposed an ion-exchange (IE) strategy to effectively control the doping degree, interfacial charge dynamics, and reliability of PEDOT:PSS in PSCs. This IE approach based on hard cation-soft anion rules enabled effective anion exchange between PEDOT:PSS and lithium bis(trifluoromethylsulfonyl)imide (LiTFSI), which favored enhancing the film conductivity, regulating the perovskite crystallization, and reducing the carrier losses at the interfaces. Consequently, a notable increase of the open-circuit voltage from 0.88 to 1.02 V was realized, resulting in a champion efficiency of 18.7% compared to the control (15.4%) in inverted PSCs. More encouragingly, this IE strategy significantly promoted the thermal and environmental stability of unsealed devices by maintaining over 80% of initial efficiencies after 2000 h. This work provides an effective way to regulate the doping state of the PEDOT-based hole transport material and guides the development of robust polymeric conducting materials for efficient perovskite photovoltaics.

Inorganic-Derived 0D Perovskite Induced Surface Lattice Arrangement for Efficient and Stable All-Inorganic Perovskite Solar Cells.

The inverted inorganic CsPbI3 perovskite solar cells (PSCs) are prospective candidates for next-generation photovoltaics owing to inherent robust thermal/photo-stability and compatibility for tandems. However, the performance and stability of the inverted CsPbI3 PSCs fall behind the n-i-p counterparts due to poor energetic alignment and abundant interfacial defect states. Here, an inorganic 0D Cs4PbBr6 with a good lattice strain arrangement is implemented as the surface anchoring capping layer on CsPbI3. The Cs4PbBr6 perovskite induces enhanced electron-selective junction and thus facilitates efficient charge extraction and effectively inhibits non-radiative recombination. Consequently, the CsPbI3 PSCs with Cs4PbBr6 demonstrate the highest power conversion efficiency (PCE) of CsPbI3-based inverted PSCs, reaching 21.03% PCE from a unit cell and 17.39% PCE from a module with a 64 cm2 aperture area. Furthermore, the resulting devices retain 92.48% after 1000 h under simultaneous 1-sun and damp heat (85 °C / 85% relative humidity) environment.

Graphene-Like Conjugated Molecule as Hole-Selective Contact for Operationally Stable Inverted Perovskite Solar Cells and Modules.

Further enhancing the operational lifetime of inverted-structure perovskite solar cells (PSCs) is crucial for their commercialization, and the design of hole-selective contacts at the illumination side plays a key role in operational stability. In this work, the self-anchoring benzo[rst]pentaphene (SA-BPP) is developed as a new type of hole-selective contact toward long-term operationally stable inverted PSCs. The SA-BPP molecule with a graphene-like conjugated structure shows a higher photostability and mobility than that of the frequently-used triphenylamine and carbazole-based hole-selective molecules. Besides, the anchoring groups of SA-BPP promote the formation of a large-scale uniform hole contact on ITO substrate and efficiently passivate the perovskite absorbers. Benefiting from these merits, the champion efficiencies of 22.03% for the small-sized cells and 17.08% for 5 × 5 cm2 solar modules on an aperture area of 22.4 cm2 are achieved based on this SA-BPP contact. Also, the SA-BPP-based device exhibits promising operational stability, with an efficiency retention of 87.4% after 2000 h continuous operation at the maximum power point under simulated 1-sun illumination, which indicates an estimated T80 lifetime of 3175 h. This novel design concept of hole-selective contacts provides a promising strategy for further improving the PSC stability.

Opportunities and challenges of hole transport materials for high-performance inverted hybrid-perovskite solar cells.

Inverted perovskite solar cells (inverted-PSCs) have exhibited advantages of longer stability, less hysteresis, and lower fabrication temperature when compared to their regular counterparts, which are important for industry commercialization. Because of the great efforts that have been conducted in the past several years, the obtained efficiency of inverted-PSCs has almost caught up with that of the regular ones, 25.0% versus 25.7%. In this perspective, the recent studies on the design of high-performance inverted-PSCs based on diverse hole transport materials, as well as device fabrication and characterization are first reviewed. After that, the authors moved on to the interface and additive engineering that were exploited to suppress the nonradiative recombination. Finally, the challenges and possible research pathways for facilitating the industrialization of inverted-PSCs were envisaged.

Reduction of Nonradiative Loss in Inverted Perovskite Solar Cells by Donor-π-Acceptor Dipoles.

Inverted perovskite solar cells (IPSCs) attract growing interest because of their simple configuration, reliable stability, and compatibility with tandem applications. However, the power conversion efficiency (PCE) of IPSCs still lags behind their regular counterparts, mainly due to the more serious nonradiative loss. Here, we design three donor-π-acceptor (D-π-A) dipoles with various dipole moments to introduce extra electric fields at the interface of perovskites and electron transport materials via the binding between the carboxylate end group and under-coordinated divalent Pb. The chemical binding reduces the recombination centers, while the superposition of the built-in electric field facilitates the electron collection and the hole blocking. As a result, the nonradiative loss is diminished as the dipole moments of D-π-A dipoles increase, which contributes to a PCE of 21.4% with enhancement in both the open-circuit voltage and fill factor. The stability for an unencapsulated device is also improved due to the hydrophobic property of D-π-A dipoles.

Suppressing the Phase Segregation with Potassium for Highly Efficient and Photostable Inverted Wide-Band Gap Halide Perovskite Solar Cells.

Wide-band gap (WBG) mixed-halide perovskites have drawn much attention because of their excellent optoelectronic properties and the potential to be deployed in tandem solar cells. Nevertheless, the bromine incorporation inevitably leads to photoinduced phase segregation in WBG mixed-halide perovskites. Herein, potassium is used to effectively suppress photoinduced phase segregation, which is visualized with confocal photoluminescence microscopy imaging. Strikingly, the potassium passivation not only inhibits the formation of the narrow-band gap subphase but also enhances the crystallinity of the WBG mixed-halide perovskite. In addition, the potassium-passivated WBG perovskite exhibits lower defect density, longer charge carrier lifetime, and better photostability. As a result, the optimized KI (2 mol %)-passivated WBG perovskite solar cells (PSCs) deliver a champion power conversion efficiency of 18.3% with negligible hysteresis. They maintain 98% of their initial efficiency after 400 h under 100 mW·cm-2 white light illumination in nitrogen.

Bifunctional Ultrathin PCBM Enables Passivated Trap States and Cascaded Energy Level toward Efficient Inverted Perovskite Solar Cells.

Inverted perovskite solar cells (PSCs) with a C60 framework are known for their common drawback of low power conversion efficiency (PCE) of <20% because of nonradiative recombination and inefficient charge transport at their perovskite interfaces. Here, we report an ultrathin [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) as a cap layer on perovskite films to overcome this issue. Such a functional cap layer efficiently passivates trap states and establishes a gradient energy level alignment onto perovskite, facilitating the efficient charge transfer and extraction. The as-fabricated inverted PSCs capped with such ultrathin PCBM exhibit a record PCE of 20.07%. After the storage under a N2 atmosphere for more than 500 h, the PCE of PSCs retains over 85% of its initial level. Our work provides an effective method to upgrade inverted PSCs with the C60 framework with improved efficiency and stability.

The Role of Lanthanum in a Nickel Oxide-Based Inverted Perovskite Solar Cell for Efficiency and Stability Improvement.

A high-performing inverted perovskite solar cell (PSC) always relies on the hole transporting layer (HTL) quality and its interfaces. This work investigates the impact of La incorporation within the NiOx matrix for defects passivation, thus leading to high charge extraction ability and stability without compromising its power conversion efficiency. In the presence of La, the La-NiOx quality is clearly improved; without the formation of pinholes. In addition, the inclusion of La alters the energy band alignment; consequently, enhancing the hole transportation and widening the Voc (>1 V), as compared to the pristine NiOx . The beneficial effect of La was further revealed through the photoluminescence measurement and density of states (DOS) analysis, in which trap states are passivated by La. More importantly, the perovskite solar cell, with La-NiOx as the HTL, exhibits 21 % enhancement in efficiency and a remarkable stability that is greater than that of pristine NiOx . This also unlocks an opportunity for commercialization.

Enhanced Efficiencies of Perovskite Solar Cells by Incorporating Silver Nanowires into the Hole Transport Layer.

In this study, we incorporated silver nanowires (AgNWs) into poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) as a hole transport layer (HTL) for inverted perovskite solar cells (PVSCs). The effect of AgNW incorporation on the perovskite crystallization, charge transfer, and power conversion efficiency (PCE) of PVSCs were analyzed and discussed. Compared with neat PEDOT:PSS HTL, incorporation of few AgNWs into PEDOT:PSS can significantly enhance the PCE by 25%. However, the AgNW incorporation may result in performance overestimation due to the lateral charge transfer. The corrosion of AgNWs with a perovskite layer was discussed. Too much AgNW incorporation may lead to defects on the interface between the HTL and the perovskite layer. An extra PEDOT:PSS layer over the pristine PEDOT:PSS-AgNW layer can prevent AgNWs from corrosion by iodide ions.

Power Conversion Efficiency and Device Stability Improvement of Inverted Perovskite Solar Cells by Using a ZnO:PFN Composite Cathode Buffer Layer.

We have demonstrated in this article that both power conversion efficiency (PCE) and performance stability of inverted planar heterojunction perovskite solar cells can be improved by using a ZnO:PFN nanocomposite (PFN: poly[(9,9-bis(3'-(N,N-dimethylamion)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctyl)-fluorene]) as the cathode buffer layer (CBL). This nanocomposite could form a compact and defect-less CBL film on the perovskite/PC61BM surface (PC61BM: phenyl-C61-butyric acid methyl ester). In addition, the high conductivity of the nanocomposite layer makes it works well at a layer thickness of 150 nm. Both advantages of the composite layer are helpful in reducing interface charge recombination and improving device performance. The power conversion efficiency (PCE) of the best ZnO:PFN CBL based device was measured to be 12.76%, which is higher than that of device without CBL (9.00%), or device with ZnO (7.93%) or PFN (11.30%) as the cathode buffer layer. In addition, the long-term stability is improved by using ZnO:PFN composite cathode buffer layer when compare to that of the reference cells. Almost no degradation of open circuit voltage (VOC) and fill factor (FF) was found for the device having ZnO:PFN, suggesting that ZnO:PFN is able to stabilize the interface property and consequently improve the solar cell performance stability.