Carbon nanowall-based gas sensors for carbon dioxide gas detection.

Carbon nanowalls (CNWs) have attracted significant attention for gas sensing applications due to their exceptional material properties such as large specific surface area, electric conductivity, nano- and/or micro-porous structure, and high charge carrier mobility. In this work, CNW films were synthesized and used to fabricate gas sensors for carbon dioxide (CO2) gas sensing. The CNW films were synthesized using an inductively-coupled plasma (ICP) plasma-enhanced chemical vapor deposition (PECVD) method and their structural and morphological properties were characterized using Raman spectroscopy and electron microscopy. The obtained CNW films were used to fabricate gas sensors employing interdigitated gold (Au) microelectrodes. The gas sensors were fabricated using both direct synthesis of CNW films on interdigitated Au microelectrodes on quartz and also transferring presynthesized CNW films onto interdigitated Au microelectrodes on glass. The CO2gas-sensing properties of fabricated devices were investigated for different concentrations of CO2gas and temperature-ranges. The sensitivities of fabricated devices were found to have a linear dependence on the concentration of CO2gas and increase with temperature. It was revealed that devices, in which CNW films have a maze-like structure, perform better compared to the ones that have a petal-like structure. A sensitivity value of 1.18% was obtained at 500 ppm CO2concentration and 100 °C device temperature. The CNW-based gas sensors have the potential for the development of easy-to-manufacture and efficient gas sensors for toxic gas monitoring.

Stepping toward Portable Optoelectronics with SnO2 Quantum Dot-Based Electron Transport Layers.

With a power conversion efficiency (PCE) of more than 25%, perovskite solar cells (PSCs) have shown an immense potential application for solar energy conversion. Owing to lower manufacturing costs and facile processibility via printing techniques, PSCs can easily be scaled up to an industrial scale. The device performance of printed PSCs has been improving steadily with the development and optimization of the printing process for the device functional layers. Various kinds of SnO2 nanoparticle (NP) dispersion solutions including commercial ones are used to print the electron transport layer (ETL) of printed PSCs, and high processing temperatures are often required to obtain ETLs with optimum quality. This, however, limits the application of SnO2 ETLs in printed and flexible PSCs. In this work, the use of an alternative SnO2 dispersion solution based on SnO2 quantum dots (QDs) to fabricate ETLs of printed PSCs on flexible substrates is reported. A comparative analysis of the performance and properties of the obtained devices with the devices fabricated employing ETLs made with a commercial SnO2 NP dispersion solution is carried out. The ETLs made with SnO2 QDs are shown to improve the performance of devices by ∼11% on average compared to the ETLs made with SnO2 NPs. It is found that employing SnO2 QDs can reduce trap states in the perovskite layer and improve charge extraction in devices.

Solution-Processed SnO2 Quantum Dots for the Electron Transport Layer of Flexible and Printed Perovskite Solar Cells.

Flexible and printed perovskite solar cells (PSCs) fabricated on lightweight plastic substrates have many excellent potential applications in emerging new technologies including wearable and portable electronics, the internet of things, smart buildings, etc. To fabricate flexible and printed PSCs, all of the functional layers of devices should be processed at low temperatures. Tin oxide is one of the best metal oxide materials to employ as the electron transport layer (ETL) in PSCs. Herein, the synthesis and application of SnO2 quantum dots (QDs) to prepare the ETL of flexible and printed PSCs are demonstrated. SnO2 QDs are synthesized via a solvothermal method and processed to obtain aqueous and printable ETL ink solutions with different QD concentrations. PSCs are fabricated using a slot-die coating method on flexible plastic substrates. The solar cell performance and spectral response of the obtained devices are characterized using a solar simulator and an external quantum efficiency measurement system. The ETLs prepared using 2 wt% SnO2 QD inks are found to produce devices with a high average power conversion efficiency (PCE) along with a 10% PCE for a champion device. The results obtained in this work provide the research community with a method to prepare fully solution-processed SnO2 QD-based inks that are suitable for the deposition of SnO2 ETLs for flexible and printed PSCs.

A Morphological Study of Solvothermally Grown SnO2 Nanostructures for Application in Perovskite Solar Cells.

Tin(IV) oxide (SnO2) nanostructures, which possess larger surface areas for transporting electron carriers, have been used as an electron transport layer (ETL) in perovskite solar cells (PSCs). However, the reported power conversion efficiencies (PCEs) of this type of PSCs show a large variation. One of the possible reasons for this phenomenon is the low reproducibility of SnO2 nanostructures if they are prepared by different research groups using various growth methods. This work focuses on the morphological study of SnO2 nanostructures grown by a solvothermal method. The growth parameters including growth pressure, substrate orientation, DI water-to-ethanol ratios, types of seed layer, amount of acetic acid, and growth time have been systematically varied. The SnO2 nanomorphology exhibits a different degree of sensitivity and trends towards each growth factor. A surface treatment is also required for solvothermally grown SnO2 nanomaterials for improving photovoltaic performance of PSCs. The obtained results in this work provide the research community with an insight into the general trend of morphological changes in SnO2 nanostructures influenced by different solvothermal growth parameters. This information can guide the researchers to prepare more reproducible solvothermally grown SnO2 nanomaterials for future application in devices.

Self-Powered Organometal Halide Perovskite Photodetector with Embedded Silver Nanowires.

Metal-semiconductor-metal (MSM) configuration of perovskite photodetectors (PPDs) suggests easy and low-cost manufacturing. However, the basic structures of MSM PPDs include vertical and lateral configurations, which require the use of expensive materials such as transparent conductive oxides or/and sophisticated fabrication techniques such as lithography. Integrating metallic nanowire-based electrodes into the perovskite photo-absorber layer to form one-half of the MSM PPD structure could potentially resolve the key issues of both configurations. Here, a manufacturing of solution-processed and self-powered MSM PPDs with embedded silver nanowire electrodes is demonstrated. The embedding of silver nanowire electrode into the perovskite layer is achieved by treating the silver nanowire/perovskite double layer with a methylamine gas vapor. The evaporated gold layer is used as the second electrode to form MSM PPDs. The prepared MSM PPDs show a photoresponsivity of 4 × 10-5 AW-1 in the UV region and 2 × 10-5 AW-1 in the visible region. On average, the devices exhibit a photocurrent of 1.1 × 10-6 A under white light (75 mW cm-2) illumination with an ON/OFF ratio of 83.4. The results presented in this work open up a new method for development and fabrication of simple, solution-processable MSM self-powered PPDs.

Effect of Electron and Proton Irradiation on Structural and Electronic Properties of Carbon Nanowalls.

In this work, a complex experimental study of the effect of electron and proton ionizing radiation on the properties of carbon nanowalls (CNWs) is carried out using various state-of-the-art materials characterization techniques. CNW layers on quartz substrates were exposed to 5 MeV electron and 1.8 MeV proton irradiation with accumulated fluences of 7 × 1013 e/cm2 and 1012 p/cm2, respectively. It is found that depending on the type of irradiation (electron or proton), the morphology and structural properties of CNWs change; in particular, the wall density decreases, and the sp2 hybridization component increases. The morphological and structural changes in turn lead to changes in the electronic, optical, and electrical characteristics of the material, in particular, change in the work function, improvement in optical transmission, an increase in the surface resistance, and a decrease in the specific conductivity of the CNW films. Lastly, this study highlights the potential of CNWs as nanostructured functional materials for novel high-performance radiation-resistant electronic and optoelectronic devices.

Physical properties of carbon nanowalls synthesized by the ICP-PECVD method vs. the growth time.

Investigation of the physical properties of carbon nanowall (CNW) films is carried out in correlation with the growth time. The structural, electronic, optical and electrical properties of CNW films are investigated using electron microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, UV-Vis spectroscopy, Hall Effect measurement system, Four Point Probing system, and thermoelectric measurements. Shorter growth time results in thinner CNW films with a densely spaced labyrinth structure, while a longer growth time results in thicker CNW films with a petal structure. These changes in morphology further lead to changes in the structural, optical, and electrical properties of the CNW.

Solution-processed antireflective coating for back-contact perovskite solar cells.

Back-contact architectures for perovskite solar cells eliminate parasitic-absorption losses caused by the electrode and charge collection layers but increase surface reflection due to the high refractive index mismatch at the air/perovskite interface. To mitigate this, a ∼85 nm thick layer of poly(methyl methacrylate) (PMMA), with a refractive index between those of air and perovskite, has been applied as an antireflective coating. Transfer matrix modelling is used to determine the ideal PMMA layer thickness, with UV-Vis spectroscopy measurements used to confirm the increase in absorption that arises through the application of the antireflective coating. The deposition of a thin film of PMMA via spin coating onto a solar cell results in a 20-30% relative increase in short circuit current density and stable power output density.

PMMA Thin Film with Embedded Carbon Quantum Dots for Post-Fabrication Improvement of Light Harvesting in Perovskite Solar Cells.

Perovskite solar cells (PSCs) with a standard sandwich structure suffer from optical transmission losses due to the substrate and its active layers. Developing strategies for compensating for the losses in light harvesting is of significant importance to achieving a further enhancement in device efficiencies. In this work, the down-conversion effect of carbon quantum dots (CQDs) was employed to convert the UV fraction of the incident light into visible light. For this, thin films of poly(methyl methacrylate) with embedded carbon quantum dots (CQD@PMMA) were deposited on the illumination side of PSCs. Analysis of the device performances before and after application of CQD@PMMA photoactive functional film on PSCs revealed that the devices with the coating showed an improved photocurrent and fill factor, resulting in higher device efficiency.

Cellulose Nanocrystal-Templated Tin Dioxide Thin Films for Gas Sensing.

Porous tin dioxide is an important low-cost semiconductor applied in electronics, gas sensors, and biosensors. Here, we present a versatile template-assisted synthesis of nanostructured tin dioxide thin films using cellulose nanocrystals (CNCs). We demonstrate that the structural features of CNC-templated tin dioxide films strongly depend on the precursor composition. The precursor properties were studied by using low-temperature nuclear magnetic resonance spectroscopy of tin tetrachloride in solution. We demonstrate that it is possible to optimize the precursor conditions to obtain homogeneous precursor mixtures and therefore highly porous thin films with pore dimensions in the range of 10-20 nm (ABET = 46-64 m2 g-1, measured on powder). Finally, by exploiting the high surface area of the material, we developed a resistive gas sensor based on CNC-templated tin dioxide. The sensor shows high sensitivity to carbon monoxide (CO) in ppm concentrations and low cross-sensitivity to humidity. Most importantly, the sensing kinetics are remarkably fast; both the response to the analyte gas and the signal decay after gas exposure occur within a few seconds, faster than in standard SnO2-based CO sensors. This is attributed to the high gas accessibility of the very thin porous film.

Dipole-field-assisted charge extraction in metal-perovskite-metal back-contact solar cells.

Hybrid organic-inorganic halide perovskites are low-cost solution-processable solar cell materials with photovoltaic properties that rival those of crystalline silicon. The perovskite films are typically sandwiched between thin layers of hole and electron transport materials, which efficiently extract photogenerated charges. This affords high-energy conversion efficiencies but results in significant performance and fabrication challenges. Herein we present a simple charge transport layer-free perovskite solar cell, comprising only a perovskite layer with two interdigitated gold back-contacts. Charge extraction is achieved via self-assembled monolayers and their associated dipole fields at the metal-perovskite interface. Photovoltages of ~600 mV generated by self-assembled molecular monolayer modified perovskite solar cells are equivalent to the built-in potential generated by individual dipole layers. Efficient charge extraction results in photocurrents of up to 12.1 mA cm-2 under simulated sunlight, despite a large electrode spacing.Simplified device concepts may become important for the development of low cost photovoltaics. Lin et al. report solar cells based on interdigitated gold back-contacts and metal halide perovskites where charge extraction is assisted via a dipole field generated by self-assembled molecular monolayers.

Directional Charge-Carrier Transport in Oriented Benzodithiophene Covalent Organic Framework Thin Films.

Charge-carrier transport in oriented COF thin films is an important factor for realizing COF-based optoelectronic devices. We describe how highly oriented electron-donating benzodithiophene BDT-COF thin films serve as a model system for a directed charge-transport study. Oriented BDT-COF films were deposited on different electrodes with excellent control over film roughness and topology, allowing for high-quality electrode-COF interfaces suitable for device fabrication. Hole-only devices were constructed to study the columnar hole mobility of the BDT-COF films. The transport measurements reveal a clear dependency of the measured hole mobilities on the BDT-COF film thickness, where thinner films showed about two orders of magnitude higher mobilities than thicker ones. Transport measurements under illumination yielded an order of magnitude higher mobility than in the dark. In-plane electrical conductivity values of up to 5 × 10-7 S cm-1 were obtained for the oriented films. Impedance measurements of the hole-only devices provided further electrical description of the oriented BDT-COF films in terms of capacitance, recombination resistance, and dielectric constant. An exceptionally low dielectric constant value of approximately 1.7 was estimated for the BDT-COF films, a further indication of their highly porous nature. DFT and molecular-dynamics simulations were carried out to gain further insights into the relationships between the COF layer interactions, electronic structure, and the potential device performance.

Passivation of PbS Quantum Dot Surface with l-Glutathione in Solid-State Quantum-Dot-Sensitized Solar Cells.

Surface oxidation of quantum dots (QDs) is one of the biggest challenges in quantum dot-sensitized solar cells (QDSCs), because it introduces surface states that enhance electron-hole recombination and degrade device performance. Protection of QDs from surface oxidation by passivating the surface with organic or inorganic layers can be one way to overcome this issue. In this study, solid-state QDSCs with a PbS QD absorber layer were prepared from thin mesoporous TiO2 layers by the successive ionic layer adsorption/reaction (SILAR) method. Spiro-OMeTAD was used as the organic p-type hole transporting material (HTM). The effects on the solar cell performance of passivating the surface of the PbS QDs with the tripeptide l-glutathione (GSH) were investigated. Current-voltage characteristics and external quantum efficiency measurements of the solar cell devices showed that GSH-treatment of the QD-sensitized TiO2 electrodes more than doubled the short circuit current and conversion efficiency. Impedance spectroscopy, intensity-modulated photovoltage and photocurrent spectroscopy analysis of the devices revealed that the enhancement in solar cell performance of the GSH-treated cells originates from improved charge injection from PbS QDs into the conduction band of TiO2. Time-resolved photoluminescence decay measurements show that passivation of the surface of QDs with GSH ligands increases the exciton lifetime in the QDs.