Self-Organized Co3O4-SrCO3 Percolative Composites Enabling Nanosized Hole Transport Pathways for Perovskite Solar Cells

Perovskite solar cells (PSCs) are expected to profoundly impact the photovoltaic society on account of its high-efficiency and cost-saving manufacture. As a key component in efficient PSCs, the hole transport layer (HTL) can selectively collect photogenerated carriers from perovskite absorbers and prevent the charge recombination at interfaces. However, the mainstream organic HTLs generally require multi-step synthesis and hygroscopic dopants that significantly limit the practical application of PSCs. Here, a self-organized percolative architecture composed of narrow bandgap oxides (e.g., Co₃O₄, NiO, CuO, Fe₂O₃, and MnO₂) and wide bandgap SrCO₃ oxysalt as efficient HTLs for PSCs is presented. The percolation of dual phases offers nanosized hole transport pathways and optimized interfacial band alignments, enabling significantly improved charge collection compared with the single phase HTLs. As a consequence, the power conversion efficiency boosted from 8.08% of SrCO₃ based device and 15.47% of Co₃O₄ based device to 21.84% of Co₃O₄-SrCO₃ based one without notable hysteresis. The work offers a new direction by employing percolative materials for efficient charge transport and collection in PSCs, and would be applicable to a wide range of opto-electronic thin film devices.     

Printable and Homogeneous NiOx Hole Transport Layers Prepared by a Polymer-Network Gel Method for Large-Area and Flexible Perovskite Solar Cells

As one of the most promising hole transport layers (HTLs), nickel oxide (NiO_x) has received extensive attention due to its application in flexible large-area perovskite solar cells (PSCs). However, the poor interface contact caused by inherent easy-agglomeration phenomenon of NiO_x nanoparticles (NPs) is still the bottleneck for achieving high-performance devices. Herein, a general strategy to synthesize NiO_x NPs with high crystallinity and good dispersibility via the polymer network micro-precipitation method is reported. Promisingly, this approach realizes the flow-division of precipitant and the restraint of the NPs motion, thereby effectively alleviating the coagulation phenomenon caused by excessive local concentration and secondary movement adsorption. Furthermore, the addition of ionic liquid not only inhibits the secondary aggregation of NiO_x NPs during the dispersion process, but also significantly enhances the properties of the colloidal solution. Ultimately, the 1.01 cm² PSCs based on the optimized NiO_x HTLs achieve the champion power conversion efficiency of 20.91% and 19.17% on rigid and flexible substrates, respectively. Moreover, the reproducibility and stability of PSCs are also significantly improved, especially for flexible devices. Overall, this strategy provides the possibility for flexible, large-area fabrication of high-quality NiO_x HTLs to promote the development of stable and efficient perovskite devices.     

Samarium-Doped Nickel Oxide for Superior Inverted Perovskite Solar Cells: Insight into Doping Effect for Electronic Applications

Hole transport layers (HTLs) play a key role in perovskite solar cells (PSCs), particularly in the inverted PSCs (IPSCs) that demand more in its stability. In this study, samarium-doped nickel oxide (Sm:NiO_x) nanoparticles are synthesized via a chemical precipitation method and deposited as a hole transport layer in the IPSCs. Sm³⁺ doping can reduce the formation energy of Ni vacancy and naturally increase the density of Ni vacancies, thereby rendering increased hole density. Thenceforth, the electronic conductivity is enhanced significantly, and work function enlarged in the Sm:NiO_x film in favor of extracting holes and suppressing charge recombination. Consequently, the Sm:NiO_x-based IPSCs attain outstanding power conversion efficiencies as high as 20.71%. Even when it is applied in flexible solar cells, it still outputs efficiency as high as 17.95%. More importantly, the Sm:NiO_x is compatible with large-scale processing whereby the large area IPSCs of 1.0 cm² and 40 × 40 mm² deliver high efficiencies of 18.51% and 15.27%, respectively, all are among the highest for the inorganic HTLs based IPSCs. This research demonstrates that, while revealing the doping effect in depth, Sm:NiO_x can be a promising hole transport material for fabricating efficient, large-area, and flexible IPSCs in the future.     

Enhanced Performance of Planar Perovskite Solar Cells Induced by Van Der Waals Epitaxial Growth of Mixed Perovskite Films on WS2 Flakes

Organic–inorganic metal halide perovskite solar cells (PSCs) have attracted much research interest owing to their high power conversion efficiency (PCE), solution processability, and the great potential for commercialization. However, the device performance is closely related to the quality of the perovskite film and the interface properties, which cannot be easily controlled by solution processes. Here, 2D WS₂ flakes with defect‐free surfaces are introduced as a template for van der Waals epitaxial growth of mixed perovskite films by solution process for the first time. The mixed perovskite films demonstrate a preferable growth along (001) direction on WS₂ surfaces. In addition, the WS₂/perovskite heterojunction forms a cascade energy alignment for efficient charge extraction and reduced interfacial recombination. The inverted PSCs with WS₂ interlayers show high PCEs up to 21.1%, which is among the highest efficiency of inverted planar PSCs. This work demonstrates that high‐mobility 2D materials can find important applications in PSCs as well as other perovskite‐based optoelectronic devices.     

Charge‐Carrier Dynamics,Mobilities, and Diffusion Lengths of 2D–3D Hybrid Butylammonium–Cesium–Formamidinium Lead Halide Perovskites

Perovskite solar cells (PSCs) have improved dramatically over the past decade, increasing in efficiency and gradually overcoming hurdles of temperature‐ and humidity‐induced instability. Materials that combine high charge‐carrier lifetimes and mobilities, strong absorption, and good crystallinity of 3D perovskites with the hydrophobic properties of 2D perovskites have become particularly promising candidates for use in solar cells. In order to fully understand the optoelectronic properties of these 2D–3D hybrid systems, the hybrid perovskite BA_x(FA_0.83Cs_0.17)_1‐xPb(I_0.6Br_0.4)₃ is investigated across the composition range 0 ≤ x ≤ 0.8. Small amounts of butylammonium (BA) are found that help to improve crystallinity and appear to passivate grain boundaries, thus reducing trap‐mediated charge‐carrier recombination and enhancing charge‐carrier mobilities. Excessive amounts of BA lead to poor crystallinity and inhomogeneous film formation, greatly reducing effective charge‐carrier mobility. For low amounts of BA, the benevolent effects of reduced recombination and enhanced mobilities lead to charge‐carrier diffusion lengths up to 7.7 µm for x = 0.167. These measurements pave the way for highly efficient, highly stable PSCs and other optoelectronic devices based on 2D–3D hybrid materials.     

Efficient and Stable Mesoscopic Perovskite Solar Cells Using PDTITT as a New Hole Transporting Layer

Stability is the main challenge in the field of organic–inorganic perovskite solar cells (PSCs). Finding low‐cost and stable hole transporting layer (HTL) is an effective strategy to address this issue. Here, a new donor polymer, poly(5,5‐didecyl‐5H‐1,8‐dithia‐as‐indacenone‐alt‐thieno[3,2‐b]thiophene) (PDTITT), is synthesized and employed as an HTL in PSCs, which has a suitable band alignment with respect to the double‐A cation perovskite film. Using PDTITT, the hole extraction in PSCs is greatly improved as compared to commonly used HTLs such as 2,2′,7,7′‐tetrakis[N,N‐di(4‐methoxyphenyl)amino]‐9,9′‐spirobifluorene (spiro‐OMeTAD), addressing the hysteresis issue. After careful optimization, an efficient PSC is achieved based on mesoscopic TiO₂ electron transporting layer with a maximum power conversion efficiency (PCE) of 18.42% based on PDTITT HTL, which is comparable with spiro‐OMeTAD‐based PSC (19.21%). Since spiro‐based PSCs suffer from stability issue, the operational stability in the PSC with PDTITT HTL is studied. It is found that the device with PDTITT retains 88% of its initial PCE value after 200 h under illumination, which is better than the spiro‐based PSC (54%).     

Dual Role of Cu-Chalcogenide as Hole-Transporting Layer and Interface Passivator for p–i–n Architecture Perovskite Solar Cell

Inorganic hole-transport layers (HTLs) are widely investigated in perovskite solar cells (PSCs) due to their superior stability compared to the organic HTLs. However, in p–i–n architecture when these inorganic HTLs are deposited before the perovskite, it forms a suboptimal interface quality for the crystallization of perovskite, which reduces device stability, causes recombination, and limits the power conversion efficiency of the device. The incorporation of an appropriate functional group such as sulfur-terminated surface on the HTL can enhance the interface quality due to its interaction with perovskite during the crystallization process. In this work, a bifunctional Al-doped CuS film is wet-deposited as HTL in p–i–n architecture PSC, which besides acting as an HTL also improves the crystallization of perovskite at the interface. Urbach energy and light intensity versus open-circuit voltage characterization suggest the formation of a better-quality interface in the sulfide HTL–perovskite heterojunction. The degradation behavior of the sulfide-HTL-based perovskite devices is studied, where it can be observed that after 2 weeks of storage in a controlled environment, the devices retain close to 95% of their initial efficiency.     

Tailoring Multifunctional Self-Assembled Hole Transporting Molecules for Highly Efficient and Stable Inverted Perovskite Solar Cells

The self-assembled hole transporting molecules (SAHTMs) bearing anchoring groups have been established as the hole transporting layers (HTLs) for highly efficient p–i–n perovskite solar cells (PSCs), yet their stability and engineering at the molecular level remain challenging. A topological design of highly anisotropic aligned SAHTM-based HTLs for operationally stable PSCs that exhibit exceptional solar-to-electric power conversion efficiencies (PCEs) is demonstrated. The judiciously designed multifunctional self-assembled molecules comprise the donor–acceptor subunit for hole transporting and the phosphonic acid group for anchoring, realizing face-on π-stacking parallel to the transparent conductive oxide substrate. The high affinity of SAHTMs to the multi-crystalline perovskite thin film benefits passivating the perovskite buried interface, strengthening interfacial contact while facilitating interfacial hole transfer. Consequently, highly efficient p–i–n PSC devices are obtained with a champion PCE of 23.24% and outstanding operational stability toward various environmental factors including long-term full sunlight soaking at evaluated temperatures. Perovskite solar modules with a champion efficiency approaching 20% are also fabricated for an active device area above 17 cm².     

A Self-Assembled Vertical-Gradient and Well-Dispersed MXene Structure for Flexible Large-Area Perovskite Modules

Advancing hole transport layers (HTL) to realize large-area, flexible, and high-performance perovskite solar cells (PSCs) is one of the most challenging issues for its commercialization. Here, a self-assembled gradient Ti₃C₂T_x MXene incorporated PEDOT:PSS HTL is demonstrated to achieve high-performance large-area PSCs by establishing half-caramelization-based glucose-induced MXene redistribution. Through this process, the Ti₃C₂T_x MXene nanosheets are spontaneously dispersed and redistributed at the top region of HTL to form the unique gradient distribution structure composed of MXene:Glucose:PEDOT:PSS (MG-PEDOT). These results show that the MG-PEDOT HTL not only offers favorable energy level alignment and efficient charge extraction, but also improves the film quality of perovskite layer featuring enlarged grain size, lower trap density, and longer carrier lifetime. Consequently, the power conversion efficiency (PCE) of the flexible device based on MG-PEDOT HTL is increased by 36% compared to that of pristine PEDOT:PSS HTL. Meanwhile, the flexible perovskite solar minimodule (15 cm² area) using MG-PEDOT HTL achieve a PCE of 17.06%. The encapsulated modules show remarkable long-term storage stability at 85 °C in ambient air (≈90% efficiency retention after 1200 h) and enhanced operational lifetime (≈90% efficiency retention after 200 h). This new approach shows a promising future of the self-assembled HTLs for developing optoelectronic devices.     

Functionalization of Graphene Oxide Films with Au and MoOx Nanoparticles as Efficient p‐Contact Electrodes for Inverted Planar Perovskite Solar Cells

A graphene oxide (GO) film is functionalized with metal (Au) and metal‐oxide (MoO_x) nanoparticles (NPs) as a hole‐extraction layer for high‐performance inverted planar‐heterojunction perovskite solar cells (PSCs). These NPs can increase the work function of GO, which is confirmed with X‐ray photoelectron spectra, Kelvin probe force microscopy, and ultraviolet photoelectron spectra measurements. The down‐shifts of work functions lead to a decreased level of potential energy and hence increased V_oc of the PSC devices. Although the GO‐AuNP film shows rapid hole extraction and increased V_oc, a J_sc improvement is not observed because of localization of the extracted holes inside the AuNP that leads to rapid charge recombination, which is confirmed with transient photoelectric measurements. The power conversion efficiency (PCE) of the GO‐AuNP device attains 14.6%, which is comparable with that of the GO‐based device (14.4%). In contrast, the rapid hole extraction from perovskite to the GO‐MoO_x layer does not cause trapping of holes and delocalization of holes in the GO film accelerates rapid charge transfer to the indium tin oxide substrate; charge recombination in the perovskite/GO‐MoO_x interface is hence significantly retarded. The GO‐MoO_x device consequently shows significantly enhanced V_oc and J_sc, for which its device performance attains PCE of 16.7% with great reproducibility and enduring stability.     

Improving the Performance of Perovskite Solar Cells via a Novel Additive of N,1-Fluoroformamidinium Iodide with Electron-Withdrawing Fluorine Group

Additives are widely adopted for efficient perovskite solar cells (PSCs), and proper additive design contributes a lot to PSCs’ various breakthroughs. Herein, a novel additive of N,1-fluoroformamidinium iodide (F-FAI), whose cation replaces one amino group in guanidinium (GA⁺) with electron-withdrawing fluorine group, is synthesized and applied as the additive for PSCs. The electron-withdrawing effect of fluorine promotes the molecular polarity of N,1-fluoroformamidine (F-FA), enhancing the interaction of N,1-fluoroformamidinium (F-FA⁺) with MAPbI₃. Compared with the nonpolar GA⁺, F-FA⁺ improves the crystallinity, passivates the defect, and downshifts the Fermi level of MAPbI₃ more significantly. The charge transfer and built-in field in printable triple mesoscopic PSCs are therefore enhanced. Moreover, charge transport in MAPbI₃ is also promoted by F-FAI. With these benefits, a power conversion efficiency of 17.01% for printable triple mesoscopic PSCs with improved open-circuit voltage and fill factor is obtained with the addition of F-FAI, superior to the efficiency of 15.24% for those devices with guanidinium iodide additives.     

Carbon Nanotube Based Inverted Flexible Perovskite Solar Cells with All‐Inorganic Charge Contacts

Organolead halide perovskite solar cells (PSC) are arising as promising candidates for next‐generation renewable energy conversion devices. Currently, inverted PSCs typically employ expensive organic semiconductor as electron transport material and thermally deposited metal as cathode (such as Ag, Au, or Al), which are incompatible with their large‐scale production. Moreover, the use of metal cathode also limits the long‐term device stability under normal operation conditions. Herein, a novel inverted PSC employs a SnO₂‐coated carbon nanotube (SnO₂@CSCNT) film as cathode in both rigid and flexible substrates (substrate/NiO‐perovskite/Al₂O₃‐perovskite/SnO₂@CSCNT‐perovskite). Inverted PSCs with SnO₂@CSCNT cathode exhibit considerable enhancement in photovoltaic performance in comparison with the devices without SnO₂ coating owing to the significantly reduced charge recombination. As a result, a power conversion efficiency of 14.3% can be obtained on rigid substrates while the flexible ones achieve 10.5% efficiency. More importantly, SnO₂@CSCNT‐based inverted PSCs exhibit significantly improved stability compared to the standard inverted devices made with silver cathode, retaining over 88% of their original efficiencies after 550 h of full light soaking or thermal stress. The results indicate that SnO₂@CSCNT is a promising cathode material for long‐term device operation and pave the way toward realistic commercialization of flexible PSCs.     

Pre-buried Interface Strategy for Stable Inverted Perovskite Solar Cells Based on Ordered Nucleation Crystallization

The buried interface has important effect on carrier extraction and nonradiative recombination of perovksite solar cells (PSCs). Herein, to inactivate the buried interfacial defects of perovskite and boost the crystallization quality of perovskite film, 3-amino-1-adamantanol (AAD) serves as a pre-buried interface modifier on nickel oxide (NiO_x) surface to regulate the nucleation and crystallization process of perovskite precursor. The amino and hydroxyl groups in AAD molecule can synchronously coordinate with nickel ion (Ni³⁺) in NiO_x and lead ion in perovskite, respectively. The dual action favors the ordered arrangement of AAD molecules between NiO_x and perovskite, which not only enhances hole extraction in hole transport layer, but also provides active sites for homogeneous nucleation. Furthermore, AAD modifier blocks the unfavorable reaction between Ni³⁺ and perovskite, and effectively passivates the buried interfacial defects. The optimal inverted PSCs achieve a champion power conversion efficiency of 22.21% with negligible hysteresis, favorable thermal, optical, and long-term stability. Thus, this strategy of modulating perovskite nucleation and crystallization by pre-buried modifier is feasible for achieving efficient and stable inverted perovskite solar cells.     

Boosting the Efficiency of Perovskite Solar Cells with CsBr‐Modified Mesoporous TiO2 Beads as Electron‐Selective Contact

Rapid extraction of photogenerated charge carriers is essential to achieve high efficiencies with perovskite solar cells (PSCs). Here, a new mesoscopic architecture as electron‐selective contact for PSCs featuring 40 nm sized TiO₂ beads endowed with mesopores of a few nanometer diameters is introduced. The bimodal pore distribution inherent to these films produces a very large contact area of 200 m² g^?1 whose access by the perovskite light absorber is facilitated by the interstitial voids between the particles. Modification of the TiO₂ surface by CsBr further strengthens its interaction with the perovskite. As a result, photogenerated electrons are extracted rapidly producing a very high fill factor of close to 80% a V_OC of 1.14 V and a PCE up to 21% with negligible hysteresis.     

Achieving 20% Efficiency for Low‐Temperature‐Processed Inverted Perovskite Solar Cells

Low‐temperature‐processed inverted perovskite solar cells (PVSCs) attract increasing attention because they can be fabricated on both rigid and flexible substrates. For these devices, hole‐transporting layers (HTLs) play an important role in achieving efficient and stable inverted PVSCs by adjusting the anodic work function, hole extraction, and interfacial charge recombination. Here, the use of a low‐temperature (≤150 °C) solution‐processed ultrathin film of poly[(9,9‐dioctyl‐fluorenyl‐2,7‐diyl)‐co‐(4,4′‐(N‐(4‐secbutylphenyl) diphenylamine)] (TFB) is reported as an HTL in one‐step‐processed CH₃NH₃PbI₃ (MAPbI₃)‐based inverted PVSCs. The fabricated device exhibits power conversion efficiency (PCE) as high as 20.2% when measured under AM 1.5 G illumination. This PCE makes them one of the MAPbI₃‐based inverted PVSCs that have the highest efficiency reported to date. Moreover, this inverted PVSC also shows good stability, which can retain 90% of its original efficiency after 30 days of storage in ambient air.     

FAPbI3 Flexible Solar Cells with a Record Efficiency of 19.38% Fabricated in Air via Ligand and Additive Synergetic Process

Compared with silicon‐based solar cells, organic–inorganic hybrid perovskite solar cells (PSCs) possess a distinct advantage, i.e., its application in the flexible field. However, the efficiency of the flexible device is still lower than that of the rigid one. First, it is found that the dense formamidinium (FA)‐based perovskite film can be obtained with the help of N‐methyl‐2‐pyrrolidone (NMP) via low pressure‐assisted method. In addition, CH₃NH₃Cl (MACl) as the additive can preferentially form MAPbCl_3?xI_x perovskite seeds to induce perovskite phase transition and crystal growth. Finally, by using FAI·PbI₂·NMP+x%MACl as the precursor, i.e., ligand and additive synergetic process, a FA‐based perovskite film with a large grain size, high crystallinity, and low trap density is obtained on a flexible substrate under ambient conditions due to the synergetic effect, e.g., MACl can enhance the crystallization of the intermediate phase of FAI·PbI₂·NMP. As a result, a record efficiency of 19.38% in flexible planar PSCs is achieved, and it can retain about 89% of its initial power conversion efficiency (PCE) after 230 days without encapsulation under ambient conditions. The PCE retains 92% of the initial value after 500 bending cycles with a bending radii of 10 mm. The results show a robust way to fabricate highly efficient flexible PSCs.     

Stabilization of α-phase FAPbI3 via Buffering Interfacial Region for Efficient p–i–n Perovskite Solar Cells

Formamidinium lead triiodide (FAPbI₃) with an ideal bandgap and good thermal stability has received wide attention and achieved a record efficiency of 26% in n–i–p (regular) perovskite solar cells (PSCs). However, imperfect FAPbI₃ formation on the typical hole transport layer (HTL), high interfacial trap-state density, and unfavorable energy alignment between the HTL and FAPbI₃ result in the inferior photovoltaic performance of p–i–n (inverted) PSCs with FAPbI₃ absorber. Herein, the α-phase FAPbI₃ is stabilized by constructing a buffer interface region between the NiO_x HTL and FAPbI₃, which not only diminishes NiO_x/FAPbI₃ interfacial reactions and defects but also facilitates carrier transport. Upon the construction of a buffer interface region, FAPbI₃ inverted PSC exhibits a high-power conversion efficiency of 23.56% (certified 22.58%) and excellent stability, retaining 90.7% of its initial efficiency after heating at 80 °C for 1000 h and 84.6% of the initial efficiency after operating at the maximum power point under continuous illumination for 1100 h. Besides, as a light-emitting diode device, the FAPbI₃ inverted PSC can be directly lit with an external quantum efficiency of 1.36%. This study provides a unique and efficient strategy to advance the application of α-phase FAPbI₃ in inverted PSCs.     

Advanced Characterization and Optimization of NiOx:Cu-SAM Hole-Transporting Bi-Layer for 23.4% Efficient Monolithic Cu(In,Ga)Se2-Perovskite Tandem Solar Cells

The performance of five hole-transporting layers (HTLs) is investigated in both single-junction perovskite and Cu(In, Ga)Se₂ (CIGSe)-perovskite tandem solar cells: nickel oxide (NiO_x,), copper-doped nickel oxide (NiO_x:Cu), NiO_x+SAM, NiO_x:Cu+SAM, and SAM, where SAM is the [2-(3,-6Dimethoxy-9H-carbazol-9yl)ethyl]phosphonic acid (MeO-2PACz) self-assembled monolayer. The performance of the devices is correlated to the charge-carrier dynamics at the HTL/perovskite interface and the limiting factors of these HTLs are analyzed by performing time-resolved and absolute photoluminescence ((Tr)PL), transient surface photovoltage (tr-SPV), and X-ray/UV photoemission spectroscopy (XPS/UPS) measurements on indium tin oxide (ITO)/HTL/perovskite and CIGSe/HTL/perovskite stacks. A high quasi-Fermi level splitting to open-circuit (QFLS-V_oc) deficit is detected for the NiO_x-based devices, attributed to electron trapping and poor hole extraction at the NiO_x-perovskite interface and a low carrier effective lifetime in the bulk of the perovskite. Simultaneously, doping the NiO_x with 2% Cu and passivating its surface with MeO-2PACz suppresses the electron trapping, enhances the holes extraction, reduces the non-radiative interfacial recombination, and improves the band alignment. Due to this superior interfacial charge-carrier dynamics, NiO_x:Cu+SAM is found to be the most suitable HTL for the monolithic CIGSe-perovskite tandem devices, enabling a power-conversion efficiency (PCE) of 23.4%, V_oc of 1.72V, and a fill factor (FF) of 71%, while the remaining four HTLs suffer from prominent V_oc and FF losses.     

Improving Performance of Perovskite Solar Cells Using [7]Helicenes with Stable Partial Biradical Characters as the Hole‐Extraction Layers

Organic–inorganic hybrid perovskites have realized a high power conversion efficiency (PCE) in both n–i–p and p–i–n device configurations. However, since the p–i–n structure exempts the sophisticated processing of charge‐transporting layers, it seems to possess better potential for practical applications than the n–i–p one. Currently, the inorganic NiO_x is the most prevailing hole‐transporting layer (HTL) used in p–i–n perovskite solar cells. Nevertheless, defects might exist on its surface to influence the charge transfer/extraction across the interface with perovskite and to affect the quality of the perovskite film grown on it. Herein, two novel [7]helicenes with stable open‐shell singlet biradical ground states at room temperature are demonstrated as an effective surface modifier of the NiO_x HTL. Their nonpolar feature effectively promotes the crystallinity of the perovskite film grown on them; meanwhile, their unique partial biradical character seems to provide a certain degree of defect passivation function at the perovskite interface to facilitate interfacial charge transfer/extraction. As a result, both 1ab‐ and 1bb‐modifed devices yield a PCE of >18%, exceeding the value (15.6%) of the control device using a sole NiO_x HTL, and the maximum PCE can reach 19%. Detailed characterizations are carefully conducted to understand the underlying reasons behind such enhancement.     

Tuning Hole Transport Layer Using Urea for High‐Performance Perovskite Solar Cells

Interface engineering is critical to the development of highly efficient perovskite solar cells. Here, urea treatment of hole transport layer (e.g., poly(3,4‐ethylene dioxythiophene):polystyrene sulfonate (PEDOT:PSS)) is reported to effectively tune its morphology, conductivity, and work function for improving the efficiency and stability of inverted MAPbI₃ perovskite solar cells (PSCs). This treatment has significantly increased MAPbI₃ photovoltaic performance to 18.8% for the urea treated PEDOT:PSS PSCs from 14.4% for pristine PEDOT:PSS devices. The use of urea controls phase separation between PEDOT and PSS segments, leading to the formation of a unique fiber‐shaped PEDOT:PSS film morphology with well‐organized charge transport pathways for improved conductivity from 0.2 S cm^?1 for pristine PEDOT:PSS to 12.75 S cm^?1 for 5 wt% urea treated PEDOT:PSS. The urea‐treatment also addresses a general challenge associated with the acidic nature of PEDOT:PSS, leading to a much improved ambient stability of PSCs. In addition, the device hysteresis is significantly minimized by optimizing the urea content in the treatment.