Low-Cost, Scalable Fabrication of Multi-Dimensional Perovskite Solar Cells and Modules Assisted by Mechanical Scribing.

The performance and scalability of perovskite solar cells (PSCs) based on 3D formamidinium lead triiodide (FAPbI3) absorber are often hindered by defects at the surface and grain boundaries of the perovskite. To address this, the study demonstrates the use of pyrrolidinium iodide for the in situ formation of an energetically aligned 1D pyrrolidinium lead triiodide (PyPbI3) capping layer over the 3D FAbI3 perovskite. The thermodynamically stable PyPbI3 perovskitoids, formed through cation exchange reactions, effectively reduce surface and grain boundary defects in the FAPbI3 perovskite. In addition to improved phase stability, the resulting 1D/3D perovskite film forms a cascade energy band alignment with the other functional layers in PSCs, enabling a barrier-free interfacial charge transport. With a maximum power conversion efficiency (PCE) of ≈23.1% and ≈20.7% at active areas of 0.09 and 1.05 cm2, respectively, the 1D/3D PSCs demonstrate excellent performance and scalability. Leveraging this improved scalability, the study has successfully developed a mechanically-scribed 1D/3D perovskite mini-module with an unprecedentedly high PCE of ≈20.6% and a total power output of ≈270 mW at an active area of ≈13.0 cm2. The 1D/3D multi-dimensional perovskite film developed herein holds great promise for producing low-cost, high-performance perovskite photovoltaics at both the cell and module levels.

Efficient deep-blue electroluminescence from Ce-based metal halide.

Rare earth ions with d-f transitions (Ce3+, Eu2+) have emerged as promising candidates for electroluminescence applications due to their abundant emission spectra, high light conversion efficiency, and excellent stability. However, directly injecting charge into 4f orbitals remains a significant challenge, resulting in unsatisfied external quantum efficiency and high operating voltage in rare earth light-emitting diodes. Herein, we propose a scheme to solve the difficulty by utilizing the energy transfer process. X-ray photoelectron spectroscopy and transient absorption spectra suggest that the Cs3CeI6 luminescence process is primarily driven by the energy transfer from the I2-based self-trapped exciton to the Ce-based Frenkel exciton. Furthermore, energy transfer efficiency is largely improved by enhancing the spectra overlap between the self-trapped exciton emission and the Ce-based Frenkel exciton excitation. When implemented as an active layer in light-emitting diodes, they show the maximum brightness and external quantum efficiency of 1073 cd m-2 and 7.9%, respectively.

Development of High Efficiency, Spray-Coated Perovskite Solar Cells and Modules Using Additive-Engineered Porous PbI2 Films.

The development of anti-solvent free, scalable, and printable perovskite film is crucial to realizing the low-cost roll-to-roll development of perovskite solar cells (PSCs). Herein, large-area perovskite film fabrication is explored using a spray-assisted sequential deposition technique. How propylene carbonate (PC) solvent additive affects the transformation of lead halide (PbI2 ) into perovskite at room temperature is investigated. The result shows that PC-modified perovskite films exhibit a uniform, pinhole-free morphology with oriented grains compared with pristine perovskite films. The PC-modified perovskite film also has a prolonged fluorescence lifetime that indicates lower carrier recombination. The champion PSC devices based on PC-modified perovskite film realize a power conversion efficiency (PCE) of 20.5% and 19.3% at an active area (A) of 0.09 cm2 and 1 cm2 , respectively. The fabricated PSCs are stable and demonstrate ≥85% PCE retention following 60 days of exposure to ambient conditions. Furthermore, perovskite solar modules (A ≈ 13 cm2 ) that yield a PCE of 15.8% are fabricated. These results are among the best reported for the state-of-art spray-coated PSCs. Spray deposition coupled with a PC additive is highly promising for economical and high-output preparation of PSCs.

Room-Temperature Spray Deposition of Large-Area SnO2 Electron Transport Layer for High Performance, Stable FAPbI3 -Based Perovskite Solar Cells.

The performance and scalability of perovskite solar cells (PSCs) is highly dependent on the morphology and charge selectivity of the electron transport layer (ETL). This work demonstrates a high-speed (1800 mm min-1 ), room-temperature (25 °C-30 °C) deposition of large-area (62.5 cm2 ) tin oxide films using a multi-pass spray deposition technique. The spray-deposited SnO2 (spray-SnO2 ) films exhibit a controllable thickness, a unique granulate morphology and high transmittance (≈85% at 550 nm). The performance of the PSC based on spray-SnO2 ETL and formamidinium lead iodide (FAPbI3 )-based perovskite is highly consistent and reproducible, achieving a maximum efficiency of ≈20.1% at an active area (A) of 0.096 cm2 . Characterization results reveal that the efficiency improvement originates from the granular morphology of spray-SnO2 and high conversion rate of PbI2 in the perovskite. More importantly, spray-SnO2 films are highly scalable and able to reduce the efficiency roll-off that comes with the increase in contact-area between SnO2 and perovskite film. Based on the spray-SnO2 ETL, large-area PSC (A = 1.0 cm2 ) achieves an efficiency of ≈18.9%. Furthermore, spray-SnO2 ETL based PSCs also exhibit higher storage stability compared to the spin-SnO2 based PSCs.

An active carbon-nanotube polarizer-embedded electrode and liquid-crystal alignment.

We report a method for constructing an active optical polarizer using an aligned carbon nanotube (CNT) sheet that is flexible, bendable, transparent, conductive, and also serves to anchor liquid-crystal (LC) molecules. A horizontally aligned CNT sheet was obtained by mechanical stretching from a vertically grown CNT forest, which was then transferred onto a substrate. A liquid polymer was infiltrated into the CNT sheet followed by UV curing, while a part of the CNT sheet was still exposed on the film surface without polymer coating. The polymer-embedded CNT sheet (P-ECS) film with 10 layers of CNT sheets exhibited a good polarization efficiency of 87%, a sheet resistance of 340 Ω□-1, and excellent ability to align LC molecules. The high stability of the P-ECS film was confirmed from the very low variation of sheet resistance (2%) and transmittance (10%) observed during a bending test of 1000 cycles. In addition, a twisted nematic LC device constructed using the P-ECS films shows a good bright-dark switching performance. The P-ECS film functions simultaneously as a transparent electrode, a film-type polarizer, and a LC alignment layer, demonstrating the multi-functionality of the active CNT film. This study thus highlights a wide range of possible applications for active polarizers and flexible displays.

Enhancement of Photoluminescence Quantum Yield and Stability in CsPbBr3 Perovskite Quantum Dots by Trivalent Doping.

We determine the influence of substitutional defects on perovskite quantum dots through experimental and theoretical investigations. Substitutional defects were introduced by trivalent dopants (In, Sb, and Bi) in CsPbBr3 by ligand-assisted reprecipitation. We show that the photoluminescence (PL) emission peak shifts toward shorter wavelengths when doping concentrations are increased. Trivalent metal-doped CsPbBr3 enhanced the PL quantum yield (~10%) and air stability (over 10 days). Our findings provide new insights into the influence of substitutional defects on substituted CsPbBr3 that underpin their physical properties.

Dual Light Trapping and Water-Repellent Effects of a Flexible-Based Inverse Micro-Cone Array for Organic and Perovskite Solar Cells.

A simple and cost-effective fabrication process of a flexible-based inverse micro-cone array (i-MCA) structure textured on flexible transparent conductive electrodes (TCEs) was successfully demonstrated via a micro-imprinting process. The flexible i-MCA films exhibited an extremely high total transmittance of ∼93% and a haze of ∼95% with reduced reflectance while simultaneously demonstrating water-repellent properties. Introducing i-MCA on the illuminating side of organic solar cells (OSCs)- and perovskite solar cells-rigid glass substrate showed improved power conversion efficiencies (PCEs) due to the light trapping effect by multiple light bounces between cone array structures (forward scattering). This results in an increase of the optical path length in the photoactive layer. Similarly, flexible TCEs embedded with textured i-MCA increased the PCE by 14% for flexible OSCs. More importantly, i-MCA-TCE-based OSCs were highly flexible with 98% retention from the initial PCE at both 0° and at 60° even after 2000 bending cycles at a radius of 2 mm. This finding demonstrates that textured i-MCA is promising for improving: (a) the light harvesting efficiency of solar cells when installed in low-/high-latitude locations and (b) the wearable technology where a flexible device attached on curved objects could retain the PCE, even at an oblique angle, with respect to the normal incidence angle.

High-performance, color-tunable fiber shaped organic light-emitting diodes.

In recent years, extensive research has been undertaken to develop fiber-shaped optoelectronic devices, because they are aesthetically pleasing, light in weight, and exhibit superior light emitting properties when compared with conventional planar analogues. In this work, we have successfully developed hollow-fiber shaped organic light emitting diodes (HF-OLED) with an exceptionally high luminance and facile color tunability. The HF-OLED device was fabricated by hierarchically depositing amorphous indium-doped tin oxide electrode on a hollow-fiber, followed by the sequential deposition of light-emitting organic layers and Al cathode. The external quantum efficiency of the HF-OLED is more than ∼2.0 times higher than that of a planar-OLED. The experimental results are in good agreement with the output of optical simulations, revealing that the use of a hollow-fiber has contributed to a ∼2.3 times improvement in light extraction efficiency. Furthermore, the color emission of a single HF-OLED device could be easily tuned from a green to yellowish-green wavelength after the injection of a super-yellow solution. The novel color tunable nature of the HF-OLED further broadens its application in the field of modern lighting and display technology.

Vertically stacked nanocellulose tactile sensor.

Paper-based electronic devices are attracting considerable attention, because the paper platform has unique attributes such as flexibility and eco-friendliness. Here we report on what is claimed to be the firstly fully integrated vertically-stacked nanocellulose-based tactile sensor, which is capable of simultaneously sensing temperature and pressure. The pressure and temperature sensors are operated using different principles and are stacked vertically, thereby minimizing the interference effect. For the pressure sensor, which utilizes the piezoresistance principle under pressure, the conducting electrode was inkjet printed on the TEMPO-oxidized-nanocellulose patterned with micro-sized pyramids, and the counter electrode was placed on the nanocellulose film. The pressure sensor has a high sensitivity over a wide range (500 Pa-3 kPa) and a high durability of 104 loading/unloading cycles. The temperature sensor combines various materials such as poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS), silver nanoparticles (AgNPs) and carbon nanotubes (CNTs) to form a thermocouple on the upper nanocellulose layer. The thermoelectric-based temperature sensors generate a thermoelectric voltage output of 1.7 mV for a temperature difference of 125 K. Our 5 × 5 tactile sensor arrays show a fast response, negligible interference, and durable sensing performance.

Plasmonic Effect of Gold Nanostars in Highly Efficient Organic and Perovskite Solar Cells.

Herein, a novel strategy is presented for enhancing light absorption by incorporating gold nanostars (Au NSs) into both the active layer of organic solar cells (OSCs) and the rear-contact hole transport layer of perovskite solar cells (PSCs). We demonstrate that the power conversion efficiencies of OSCs and PSCs with embedded Au NSs are improved by 6 and 14%, respectively. We find that pegylated Au NSs are greatly dispersable in a chlorobenzene solvent, which enabled complete blending of Au NSs with the active layer. The plasmonic contributions and accelerated charge transfer are believed to improve the short-circuit current density and the fill factor. This study demonstrates the roles of plasmonic nanoparticles in the improved optical absorption, where the improvement in OSCs was attributed to surface plasmon resonance (SPR) and in PSCs was attributed to both SPR and the backscattering effect. Additionally, devices including Au NSs exhibited a better charge separation/transfer, reduced charge recombination rate, and efficient charge transport. This work provides a comprehensive understanding of the roles of plasmonic Au NS particles in OSCs and PSCs, including an insightful approach for the further development of high-performance optoelectronic devices.

Self-organized semiconductor nano-network on graphene.

A network structure consisting of nanomaterials with a stable structural support and charge path on a large area is desirable for various electronic and optoelectronic devices. Generally, network structures have been fabricated via two main strategies: (1) assembly of pre-grown nanostructures onto a desired substrate and (2) direct growth of nanomaterials onto a desired substrate. In this study, we utilized the surface defects of graphene to form a nano-network of ZnO via atomic layer deposition (ALD). The surface of pure and structurally perfect graphene is chemically inert. However, various types of point and line defects, including vacancies/adatoms, grain boundaries, and ripples in graphene are generated by growth, chemical or physical treatments. The defective sites enhance the chemical reactivity with foreign atoms. ZnO nanoparticles formed by ALD were predominantly deposited at the line defects and agglomerated with increasing ALD cycles. Due to the formation of the ZnO nano-network, the photocurrent between two electrodes was clearly changed under UV irradiation as a result of the charge transport between ZnO and graphene. The line patterned ZnO/graphene (ZnO/G) nano-network devices exhibit sensitivities greater than ten times those of non-patterned structures. We also confirmed the superior operation of a fabricated flexible photodetector based on the line patterned ZnO/G nano-network.

Ultra-Smooth, Fully Solution-Processed Large-Area Transparent Conducting Electrodes for Organic Devices.

A novel approach for the fabrication of ultra-smooth and highly bendable substrates consisting of metal grid-conducting polymers that are fully embedded into transparent substrates (ME-TCEs) was successfully demonstrated. The fully printed ME-TCEs exhibited ultra-smooth surfaces (surface roughness ~1.0 nm), were highly transparent (~90% transmittance at a wavelength of 550 nm), highly conductive (sheet resistance ~4 Ω â—»-1), and relatively stable under ambient air (retaining ~96% initial resistance up to 30 days). The ME-TCE substrates were used to fabricate flexible organic solar cells and organic light-emitting diodes exhibiting devices efficiencies comparable to devices fabricated on ITO/glass substrates. Additionally, the flexibility of the organic devices did not degrade their performance even after being bent to a bending radius of ~1 mm. Our findings suggest that ME-TCEs are a promising alternative to indium tin oxide and show potential for application toward large-area optoelectronic devices via fully printing processes.

Silver Nanowire Transparent Conductive Electrodes for High-Efficiency III-Nitride Light-Emitting Diodes.

Silver nanowires (AgNWs) have been successfully demonstrated to function as next-generation transparent conductive electrodes (TCEs) in organic semiconductor devices owing to their figures of merit, including high optical transmittance, low sheet resistance, flexibility, and low-cost processing. In this article, high-quality, solution-processed AgNWs with an excellent optical transmittance of 96.5% at 450 nm and a low sheet resistance of 11.7 Ω/sq were demonstrated as TCEs in inorganic III-nitride LEDs. The transmission line model applied to the AgNW contact to p-GaN showed that near ohmic contact with a specific contact resistance of ~10(-3) Ωcm(2) was obtained. The contact resistance had a strong bias-voltage (or current-density) dependence: namely, field-enhanced ohmic contact. LEDs fabricated with AgNW electrodes exhibited a 56% reduction in series resistance, 56.5% brighter output power, a 67.5% reduction in efficiency droop, and a approximately 30% longer current spreading length compared to LEDs fabricated with reference TCEs. In addition to the cost reduction, the observed improvements in device performance suggest that the AgNWs are promising for application as next-generation TCEs, to realise brighter, larger-area, cost-competitive inorganic III-nitride light emitters.

Ultrasmooth, extremely deformable and shape recoverable Ag nanowire embedded transparent electrode.

Transparent electrodes have been widely used in electronic devices such as solar cells, displays, and touch screens. Highly flexible transparent electrodes are especially desired for the development of next generation flexible electronic devices. Although indium tin oxide (ITO) is the most commonly used material for the fabrication of transparent electrodes, its brittleness and growing cost limit its utility for flexible electronic devices. Therefore, the need for new transparent conductive materials with superior mechanical properties is clear and urgent. Ag nanowire (AgNW) has been attracting increasing attention because of its effective combination of electrical and optical properties. However, it still suffers from several drawbacks, including large surface roughness, instability against oxidation and moisture, and poor adhesion to substrates. These issues need to be addressed before wide spread use of metallic NW as transparent electrodes can be realized. In this study, we demonstrated the fabrication of a flexible transparent electrode with superior mechanical, electrical and optical properties by embedding a AgNW film into a transparent polymer matrix. This technique can produce electrodes with an ultrasmooth and extremely deformable transparent electrode that have sheet resistance and transmittance comparable to those of an ITO electrode.

Designed synthesis and stacking architecture of solid and mesoporous TiO(2) nanoparticles for enhancing the light-harvesting efficiency of dye-sensitized solar cells.

We fabricated solid and mesoporous TiO2 nanoparticles (NPs) with relatively large primary sizes of approximately 200 nm via inorganic templates for aero-sol-gel and subsequent aqueous-washing processes. The amount of dye molecules adsorbed by the internal pores in the mesoporous TiO2 NPs was increased by creating the nanopores within the solid TiO2 NPs. Simultaneously, the light-scattering effect of the mesoporous TiO2 NPs fabricated by this approach was secured by maintaining their spherical shape and relatively large average size. By precisely accumulating the fabricated solid or mesoporous 200 nm diameter TiO2 NPs on top of a conventional 25 nm diameter TiO2 NP-based underlayer, we could systematically examine the effect of the solid and mesoporous TiO2 NPs on the photovoltaic performance of dye-sensitized solar cells (DSSCs). Consequently, the stacking architecture of the mesoporous TiO2 NP-based overlayer, which functioned as both a light-scattering and dye-supporting medium, on top of a conventional solid TiO2 NP-based underlayer in a DSSC photoelectrode (i.e., double-layer structures) was found to be very promising for significantly improving the photovoltaic properties of conventional solid TiO2 NP single-layer-based DSSCs.

Preparation of flexible organic solar cells with highly conductive and transparent metal-oxide multilayer electrodes based on silver oxide.

We report that significantly more transparent yet comparably conductive AgOx films, when compared to Ag films, are synthesized by the inclusion of a remarkably small amount of oxygen (i.e., 2 or 3 atom %) in thin Ag films. An 8 nm thick AgOx (O/Ag=2.4 atom %) film embedded between 30 nm thick ITO films (ITO/AgOx/ITO) achieves a transmittance improvement of 30% when compared to a conventional ITO/Ag/ITO electrode with the same configuration by retaining the sheet resistance in the range of 10-20 Ω sq(-1). The high transmittance provides an excellent opportunity to improve the power-conversion efficiency of organic solar cells (OSCs) by successfully matching the transmittance spectral range of the electrode to the optimal absorption region of low band gap photoactive polymers, which is highly limited in OSCs utilizing conventional ITO/Ag/ITO electrodes. An improvement of the power-conversion efficiency from 4.72 to 5.88% is achieved from highly flexible organic solar cells (OSCs) fabricated on poly(ethylene terephthalate) polymer substrates by replacing the conventional ITO/Ag/ITO electrode with the ITO/AgOx/ITO electrode. This novel transparent electrode can facilitate a cost-effective, high-throughput, room-temperature fabrication solution for producing large-area flexible OSCs on heat-sensitive polymer substrates with excellent power-conversion efficiencies.

Highly efficient hybrid thin-film solar cells using a solution-processed hole-blocking layer.

We report the origin of the improvement of the power conversion efficiency (PCE) of hybrid thin-film solar cells when a soluble C(60) derivative, [6,6]-phenyl-C(61)-butyric acid methyl ester (PCBM), is introduced as a hole-blocking layer. The PCBM layer could establish better interfacial contact by decreasing the reverse dark-saturation current density, resulting in a decrease in the probability of carrier recombination. The PCE of this optimized device reached a maximum value of 8.34% and is the highest yet reported for hybrid thin-film solar cells.

High efficiency inorganic/organic hybrid tandem solar cells.

Hybrid tandem solar cells comprising an inorganic bottom cell and an organic top cell have been designed and fabricated. The interlayer combination and thickness matching were optimized in order to increase the overall photovoltaic conversion efficiency. A maximum power conversion efficiency of 5.72% was achieved along with a V(oc) of 1.42 V, reaching as high as 92% of the sum of the subcell V(oc) values.

ZnO nanosheets decorated with CdSe and TiO2 for the architecture of dye-sensitized solar cells.

Pure and TiO2- and CdSe-deposited ZnO nanosheets aligned vertically to the surface of ITO (Indium tin oxide) are prepared using electrodeposition, which is used for building blocks of dye sensitized solar cell. A significant improvement in the photovoltaic efficiency can be obtained by depositing TiO2 or CdSe on ZnO. Photoluminescence spectra show that the TiO2 and CdSe nanostructures suppress the recombination of the electron-hole pair of ZnO. We suggest that the interface charge transfer at TiO2-ZnO and CdSe-ZnO should be responsible for the suppression of the electron-hole pair recombination and enhanced solar cell efficiency by TiO2 and CdSe nanostructures.