Solvent-free preparation and thermocompression self-assembly: an exploration of performance improvement strategies for perovskite solar cells.

Perovskite solar cells (PSCs) exhibit sufficient technological efficiency and economic competitiveness. However, their poor stability and scalability are crucial factors limiting their rapid development. Therefore, achieving both high efficiency and good stability is an urgent challenge. In addition, the preparation methods for PSCs are currently limited to laboratory-scale methods, so their commercialization requires further research. Effective packaging technology is essential to protect the PSCs from degradation by external environmental factors and ensure their long-term stability. The industrialization of PSCs is also inseparable from the preparation technology of perovskite thin films. This review discusses the solvent-free preparation of PSCs, shedding light on the factors that affect PSC performance and strategies for performance enhancement. Furthermore, this review analyzes the existing simulation techniques that have contributed to a better understanding of the interfacial evolution of PSCs during the packaging process. Finally, the current challenges and possible solutions are highlighted, providing insights to facilitate the development of highly efficient and stable PSC modules to promote their widespread application.

Highly stretchable transparent bar coated Ag NW/PEDOT:PSS hybrid electrode for wearable and stretchable devices.

In this study, we demonstrated poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS) as a composite with Ag nanowire (Ag NW) to enhance the stretchability of the Ag NW network electrode. The composite Ag NW/PEDOT:PSS hybrid ink (AP ink) was prepared at a ratio of 1 : 10, 1 : 20, and 1 : 30, respectively and bar coated on polyurethane substrate. The different ink ratios were studied and optimized with a sheet resistance of 14.93 Ω sq-1. and a transmittance of 88.6% showing a high performance in mechanical stress tests such as bending, folding, rolling, twisting, and stretching. It also showed a conductive bridge effect where the PEDOT:PSS acted as an anchor or support to Ag NW during mechanical strain and PEDOT:PSS also enhanced the electrical conductivity of the Ag NW. Therefore, to prove the real time performance of the electrode as a wearable device, we fabricated transparent electroluminescence devices and thin film heater devices which are highly flexible and demonstrated excellent performance proving that the AP electrode is more suitable candidate for future wearable transparent devices.

Transparent and flexible passivation of MoS2/Ag nanowire with sputtered polytetrafluoroethylene film for high performance flexible heaters.

We demonstrated highly transparent and flexible polytetrafluoroethylene (PTFE) passivation for the MoS2/Ag nanowire (Ag NW) electrodes used in thin film heaters (TFHs). The electrical, optical, and mechanical properties of PTFE coated MoS2/Ag NW electrode were compared to the bare MoS2/Ag NW electrode to demonstrate effective passivation of the sputtered PTFE films before and after the 85 °C-85% temperature-relative humidity environment test. In addition, we investigated the performances of TFHs with PTFE/MoS2/Ag NW as a function of PTFE thickness from 50 to 200 nm. The saturation temperature (87.3 °C) of TFHs with PTFE/MoS2/Ag NW electrode is higher than that (61.3 °C) of TFHs with bare MoS2/Ag NW, even after the 85 °C-85% temperature-relative humidity environment test, due to effective passivation of the PTFE layer. This indicates that transparent PTFE film prepared by sputtering process provides effective thin film passivation for the two-dimensional (2D) MoS2 and Ag NW hybrid electrode against harsh environment condition.

Steering Interface Dipoles for Bright and Efficient All-Inorganic Quantum Dot Based Light-Emitting Diodes.

The state-of-the-art quantum dot (QD) based light-emitting diodes (QD-LEDs) reach near-unity internal quantum efficiency thanks to organic materials used for efficient hole transportation within the devices. However, toward high-current-density LEDs, such as augmented reality, virtual reality, and head-up display, thermal vulnerability of organic components often results in device instability or breakdown. The adoption of a thermally robust inorganic hole transport layer (HTL), such as NiO, becomes a promising alternative, but the large energy offset between the NiO HTL and the QD emissive layer impedes the efficient operation of QD-LEDs. Here, we demonstrate bright and stable all-inorganic QD-LEDs by steering the orientation of molecular dipoles at the surfaces of both the NiO HTL and QDs. We show that the molecular dipoles not only induce the vacuum level shift that helps alleviate the energy offset between the NiO HTL and QDs but also passivate the surface trap states of the NiO HTL that act as nonradiative recombination centers. With the facilitated hole injection into QDs and suppressed electron leakage toward trap sites in the NiO HTL, we achieve all-inorganic QD-LEDs with high external quantum efficiency (6.5% at peak) and brightness (peak luminance exceeding 77 000 cd/m2) along with prolonged operational stability. The approaches and results in the present study provide the design principles for high-performance all-inorganic QD-LEDs suited for next-generation light sources.

Room Temperature Processed Transparent Amorphous InGaTiO Cathodes for Semi-Transparent Perovskite Solar Cells.

In order to ensure high-performance semitransparent perovskite solar cells (ST-PSCs), the deposition of high-quality scalable transparent cathodes on ST-PSCs at room temperature is necessary. In this study, we designed an amorphous InGaTiO (IGTO) electrode, prepared by linear facing target sputtering (LFTS) as a transparent cathode for ST-PSCs. Even in the room temperature sputtering process, the amorphous IGTO cathode showed a low sheet resistance of 9.895 Ohm/square and a high optical transmittance of 87.53% without the occurrence of in situ or postannealing, unlike Sn-doped In2O3 (ITO) electrodes. Due to its complete amorphous structure and low energy sputtering, the amorphous IGTO electrode showed superior mechanical properties, when compared to other typical crystalline ITO films. Additionally, the LFTS process led to a low energy deposition of the amorphous IGTO cathode on ST-PSCs, and did not result in plasma damage on perovskite active layers, which is often typical in conventional situations of direct current sputtering. On the basis of these optimized plasma damage-free sputtering conditions, we examined the feasibility of LFTS-grown IGTO cathodes for ST-PSCs. In our results, we observed that a similar performance of the ST-PSC with an IGTO cathode with the opaque PSC with Ag cathode, indicated that amorphous IGTO cathode is a prospective transparent cathode for ST-PSCs on both rigid or flexible substrates.

Defect-Free Mechanical Graphene Transfer Using n-Doping Adhesive Gel Buffer.

The synthesis of uniform low-defect graphene on a catalytic metal substrate is getting closer to the industrial level. However, its practical application is still challenging due to the lack of an appropriate method for its scalable damage-free transfer to a device substrate. Here, an efficient approach for a defect-free, etchant-free, wrinkle-free, and large-area graphene transfer is demonstrated by exploiting a multifunctional viscoelastic polymer gel as a simultaneous shock-free adhesive and dopant layer. Initially, an amine-rich polymer solution in its liquid form allows for conformal coating on a graphene layer grown on a Cu substrate. The subsequent thermally cured soft gel enables the shock-free and wrinkle-free direct mechanical exfoliation of graphene from a substrate due to its strong charge-transfer interaction with graphene and excellent shock absorption. The adhesive gel with a high optical transparency works as an electron doping layer toward graphene, which exhibits significantly reduced sheet resistances without optical transmittance loss. Lastly, the transferred graphene layer shows high mechanical and chemical stabilities under the repeated bending test and exposure to various solvents. This gel-assisted mechanical transfer method can be a solution to connect the missing part between large-scale graphene synthesis and next-generation electronics and optoelectronic applications.

Transparent Molecular Adhesive Enabling Mechanically Stable ITO Thin Films.

With rapid advances in flexible electronics, transparent conductive electrodes (TCEs) have also been significantly developed as alternatives to the conventional indium tin oxide (ITO)-based material systems that exhibit low mechanical flexibility. Nanomaterial-based alternating materials, such as graphene, nanowire, and nanomesh, exhibit remarkable properties for TCE-based applications, such as high electrical conductivity, high optical transparency, and high mechanical stability. However, these nanomaterial-based systems lack scalability, which is a key requirement for practical applications, and exhibit a size-dependent property variation and inhomogeneous surface uniformity that limit reliable properties over a large area. Here, we exploited a conventional ITO-based material platform; however, we incorporated a transparent molecular adhesive, 4-aminopyridine (4-AP), to improve mechanical flexibility. While the presence of 4-AP barely affected optical transmittance and sheet resistance, it improved interfacial adhesion between the substrate and ITO as well as formed a wavy surface, which could improve the mechanical flexibility. Under various mechanical tests, ITO/4-AP/poly(ethylene terephthalate) (PET) exhibited remarkably improved mechanical flexibility as compared with that of ITO/PET. Furthermore, ITO/4-AP/PET was utilized for a flexible Joule heater application having spatial uniformity of heat generation, voltage-dependent temperature control, and mechanical flexibility under repeated bending tests. This molecular adhesive could overcome the current limitations of material systems for flexible electronics.

Thermally-evaporated C60/Ag/C60 multilayer electrodes for semi-transparent perovskite photovoltaics and thin film heaters.

We investigated the characteristics of thermally evaporated fullerene (C60)/Ag/C60 (CAC) multilayer films for use in semi-transparent perovskite solar cells (PSCs) and thin-film heaters (TFHs). The top and bottom C60 layers and Ag interlayer were prepared using multi-source thermal evaporation, and the thickness of the Ag interlayer was investigated in detail for its effects on the resistivity, optical transmittance, and mechanical properties of the CAC electrodes. We used a figure-of-merit analysis to obtain a CAC electrode with a smooth surface morphology that exhibited a sheet resistance of 5.63 Ohm/square and an optical transmittance of 66.13% at a 550 nm wavelength. We conducted mechanical deformation tests to confirm that the thermally evaporated multilayer CAC electrode has a high durability, even after 10,000 times of inner and outer bending, rolling, and twisting due to the flexibility of the amorphous C60 and Ag interlayer. We evaluated the feasibility of using CAC electrodes for semi-transparent PSCs and TFHs. The semi-transparent PSC with 1.08 cm2 active area prepared with a transparent multilayer CAC cathode showed a power conversion efficiency (PCE) of 5.1%. Furthermore, flexible TFHs (2.5 × 2.5 cm2) fabricated on a thermally evaporated CAC electrode show a high saturation temperature of 116.6 C, even at a low input voltage of 4.5 V, due to a very low sheet resistance. Based on the performance of the PSCs and TFHs, we conclude that the thermally evaporated multilayer CAC electrode is promising for use as a transparent conductive electrode (TCE) for semi-transparent PSCs and TFHs, with characteristics comparable to sputtered TCEs.

Highly transparent and flexible Ag nanowire-embedded silk fibroin electrodes for biocompatible flexible and transparent heater.

We investigated the electrical, optical and mechanical properties of silver (Ag) nanowire (NW) embedded into a silk fibroin (SF) substrate to create high performance, flexible, transparent, biocompatible, and biodegradable heaters for use in wearable electronics. The Ag NW-embedded SF showed a low sheet resistance of 15 Ω sq-1, high optical transmittance of 85.1%, and a small inner/outer critical bending radius of 1 mm. In addition, the Ag NW-embedded SF showed a constant resistance change during repeated bending, folding, and rolling because the connectivity of the Ag NW embedded into the SF substrate was well maintained. Furthermore, the biocompatible and biodegradable Ag NW-embedded SF substrate served as a flexible interconnector for wearable electronics. The high performance of the transparent and flexible heater demonstrated that an Ag NW-embedded SF-based heater can act as a biocompatible and biodegradable substrate for wearable heaters for the human body.

Comparison of NiO x thin film deposited by spin-coating or thermal evaporation for application as a hole transport layer of perovskite solar cells.

We compared nickel oxide (NiO x ) deposited by thermal evaporation and that deposited by the spin-coating process, for use in the hole transport layers of inverted planar perovskite solar cells (PSCs). Spin-coating deposition for NiO x HTL has been widely used, owing to its simplicity, low cost, and high efficiency. However, the spin-coating process has a technical limit to depositing a large-area uniformly. In contrast, thermal evaporation fabrication has a low price and is able to produce uniform and reproducible thin film. Hence, the chemical states, energy band alignment, surface morphologies, and microstructures of NiO x deposited by spin coating and thermal evaporation were analyzed. The PSC with NiO x HTL deposited by thermal evaporation showed a higher power conversion efficiency of 16.64% with open circuit voltage 1.07 V, short circuit current density of 20.68 mA cm-2, and a fill factor of 75.51% compared to that of PSC with spin-coated NiO x . We confirmed that thermal evaporation can deposit NiO x to give a better performance as a HTL with higher reproducibility than spin-coating.

ZnO:Ga-graded ITO electrodes to control interface between PCBM and ITO in planar perovskite solar cells.

Ga-doped ZnO (GZO)-graded layer, facilitating electron extraction from electron transport layer, was integrated on the surface of transparent indium tin oxide (ITO) cathode by using graded sputtering technique to improve the performance of planar n-i-p perovskite solar cells (PSCs). The thickness of graded GZO layer was controlled to optimize GZO-indium tin oxide (ITO) combined electrode for planar n-i-p PSCs. At optimized graded thickness of 15 nm, the GZO-ITO combined electrode showed an optical transmittance of 95%, a resistivity of 2.3 × 10-4 Ohm cm, a sheet resistance of 15.6 Ohm/square, and work function of 4.23 eV, which is well matched with the 4.0-eV lowest unoccupied molecular orbital of [6,6]-phenyl-C61-butyric acid methyl ester. Owing to enhanced extraction of electron by the graded GZO, the n-i-p PSC with GZO-ITO combined electrode showed higher power conversion efficiency (PCE) of 9.67% than the PCE (5.25%) of PSC with only ITO electrode without GZO-graded layer. In addition, the GZO integrated-ITO electrode acts as transparent electrode and electron extraction layer simultaneously due to graded mixing of the GZO at the surface region of ITO electrode.

Tetrahedral amorphous carbon prepared filter cathodic vacuum arc for hole transport layers in perovskite solar cells and quantum dots LEDs.

(ta-C) films coated through the filtered cathodic vacuum arc (FCVA) process as a hole transport layer (HTL) for perovskite solar cells (PSCs) and quantum dot light-emitting diodes (QDLEDs). The p-type ta-C film has several remarkable features, including ease of fabrication without the need for thermal annealing, reasonable electrical conductivity, optical transmittance, and a high work function. X-ray photoelectron spectroscopy and ultraviolet photoelectron spectroscopy examinations show that the electrical properties (sp3/sp2 hybridized bond) and work function of the ta-C HTL are appropriate for PSCs and QDLEDs. In addition, in order to correlate the performance of the devices, the optical, surface morphological, and structural properties of the FCVA-grown ta-C films with different thicknesses (5 ~ 20 nm) deposited on the ITO anode are investigated in detail. The optimized ta-C film with a thickness of 5 nm deposited on the ITO anode had a sheet resistance of 10.33 Ω-2, a resistivity of 1.34 × 10-4 Ω cm, and an optical transmittance of 88.97%. Compared to the reference PSC with p-NiO HTL, the PSC with 5 nm thick ta-C HTL yielded a higher power conversion efficiency (PCE, 10.53%) due to its improved fill factor. Further, the performance of QDLEDs with 5 nm thick ta-C hole injection layers (HIL) showed better than the performance of QDLEDs with different ta-C thicknesses. It is concluded that ta-C films have the potential to serve as HTL and HIL in next-generation PSCs and QDLEDs.

Flexible ITO films with atomically flat surfaces for high performance flexible perovskite solar cells.

We report high performance flexible Sn-doped In2O3 (ITO) films prepared by in-line type vertical plasma arc ion plating for high performance flexible perovskite solar cells. Even at room temperature deposition, the ion-plated ITO film showed a low sheet resistance of 15.75 Ohm per square, a high average optical transmittance of 85.88% and a small outer bending radius of 5 mm because energetic ITO ions accelerated to the substrate led to better crystallinity and adhesion than sputtered ITO films. In addition, the ion-plated ITO films showed atomically flat and smooth surfaces due to different growth mechanisms and the absence of resputtering effects during the ion plating process. Flexible perovskite solar cells fabricated on the ion-plated ITO electrodes showed a higher power conversion efficiency of 16.8% than the sputtered ITO-based perovskite solar cell, indicating the potential of ion plated ITO films as promising flexible and transparent electrodes for perovskite solar cells.

Effective passivation of Ag nanowire network by transparent tetrahedral amorphous carbon film for flexible and transparent thin film heaters.

We developed effective passivation method of flexible Ag nanowire (NW) network electrodes using transparent tetrahedral amorphous carbon (ta-C) film prepared by filtered cathode vacuum arc (FCVA) coating. Even at room temperature process of FCVA, the ta-C passivation layer effectively protect Ag NW network electrode and improved the ambient stability of Ag NW network without change of sheet resistance of Ag NW network. In addition, ta-C coated Ag NW electrode showed identical critical inner and outer bending radius to bare Ag NW due to the thin thickness of ta-C passivation layer. The time-temperature profiles demonstrate that the performance of the transparent and flexible thin film heater (TFH) with the ta-C/Ag NW network is better than that of a TFH with Ag NW electrodes due to thermal stability of FCVA grown ta-C layer. In addition, the transparent and flexible TFHs with ta-C/Ag NW showed robustness against external force due to its high hardness and wear resistance. This indicates that the FCVA coated ta-C is promising passivation and protective layer for chemically weak Ag NW network electrodes against sulfur in ambient.