The formation of a dense and uniform thin layer on the substrates is crucial for the fabrication of high-performance perovskite solar cells (PSCs) containing formamidinium with multiple cations and mixed halide anions. The concentration of defect states, which reduce a cell’s performance by decreasing the open-circuit voltage and short-circuit current density, needs to be as low as possible. We show that the introduction of additional iodide ions into the organic cation solution, which are used to form the perovskite layers through an intramolecular exchanging process, decreases the concentration of deep-level defects. The defect-engineered thin perovskite layers enable the fabrication of PSCs with a certified power conversion efficiency of 22.1% in small cells and 19.7% in 1-square-centimeter cells.

Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells

Transparent electronics is today one of the most advanced topics for a wide range of device applications. The key components are wide bandgap semiconductors, where oxides of different origins play an important role, not only as passive component but also as active component, similar to what is observed in conventional semiconductors like silicon. Transparent electronics has gained special attention during the last few years and is today established as one of the most promising technologies for leading the next generation of flat panel display due to its excellent electronic performance. In this paper the recent progress in n- and p-type oxide based thin-film transistors (TFT) is reviewed, with special emphasis on solution-processed and p-type, and the major milestones already achieved with this emerging and very promising technology are summarizeed. After a short introduction where the main advantages of these semiconductors are presented, as well as the industry expectations, the beautiful history of TFTs is revisited, including the main landmarks in the last 80 years, finishing by referring to some papers that have played an important role in shaping transparent electronics. Then, an overview is presented of state of the art n-type TFTs processed by physical vapour deposition methods, and finally one of the most exciting, promising, and low cost but powerful technologies is discussed: solution-processed oxide TFTs. Moreover, a more detailed focus analysis will be given concerning p-type oxide TFTs, mainly centred on two of the most promising semiconductor candidates: copper oxide and tin oxide. The most recent data related to the production of complementary metal oxide semiconductor (CMOS) devices based on n- and p-type oxide TFT is also be presented. The last topic of this review is devoted to some emerging applications, finalizing with the main conclusions. Related work that originated at CENIMAT|I3N during the last six years is included in more detail, which has led to the fabrication of high performance n- and p-type oxide transistors as well as the fabrication of CMOS devices with and on paper.

Oxide Semiconductor Thin‐Film Transistors: A Review of Recent Advances

Lead halide perovskite solar cells have recently attracted tremendous attention because of their excellent photovoltaic efficiencies. However, the poor stability of both the perovskite material and the charge transport layers has so far prevented the fabrication of devices that can withstand sustained operation under normal conditions. Here, we report a solution-processed lead halide perovskite solar cell that has p-type NiOx and n-type ZnO nanoparticles as hole and electron transport layers, respectively, and shows improved stability against water and oxygen degradation when compared with devices with organic charge transport layers. Our cells have a p–i–n structure (glass/indium tin oxide/NiOx/perovskite/ZnO/Al), in which the ZnO layer isolates the perovskite and Al layers, thus preventing degradation. After 60 days storage in air at room temperature, our all-metal-oxide devices retain about 90% of their original efficiency, unlike control devices made with organic transport layers, which undergo a complete degradation after just 5 days. The initial power conversion efficiency of our devices is 14.6 ± 1.5%, with an uncertified maximum value of 16.1%. Using metal oxides for both the hole- and electron-transport layers in perovskite solar cells significantly improves their stability compared with devices containing organic transport layers.

Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers

Optical transparency, tunable conducting properties and easy processability make metal oxides key materials for advanced optoelectronic devices. This Review discusses recent advances in the synthesis of these materials and their use in applications. Metal oxides (MOs) are the most abundant materials in the Earth's crust and are ingredients in traditional ceramics. MO semiconductors are strikingly different from conventional inorganic semiconductors such as silicon and III–V compounds with respect to materials design concepts, electronic structure, charge transport mechanisms, defect states, thin-film processing and optoelectronic properties, thereby enabling both conventional and completely new functions. Recently, remarkable advances in MO semiconductors for electronics have been achieved, including the discovery and characterization of new transparent conducting oxides, realization of p-type along with traditional n-type MO semiconductors for transistors, p–n junctions and complementary circuits, formulations for printing MO electronics and, most importantly, commercialization of amorphous oxide semiconductors for flat panel displays. This Review surveys the uniqueness and universality of MOs versus other unconventional electronic materials in terms of materials chemistry and physics, electronic characteristics, thin-film fabrication strategies and selected applications in thin-film transistors, solar cells, diodes and memories.

Metal oxides for optoelectronic applications

Methylammonium Chloride Induces Intermediate Phase Stabilization for Efficient Perovskite Solar Cells

Solution-processed silver nanowire networks are one of the promising candidates to replace a traditional indium tin oxide as next-generation transparent and flexible electrodes due to their ease of processing, moderate flexibility, high transparency, and low sheet resistance. To date, however, high stability of the nanowire networks remains a major challenge because the long-term usages of these electrodes are limited by their poor thermal and chemical stabilities. Existing methods for addressing this challenge mainly focus on protecting the nanowire network with additional layers that require vacuum processes, which can lead to an increment in manufacturing cost. Here, we report a straightforward strategy of a sol–gel processing as a fast and robust way to improve the stabilities of silver nanowires. Compared with reported nanoparticles embedded in nanowire networks, better thermal and chemical stabilities are achieved via sol–gel coating of TiO2 over the silver nanowire networks. The conformal surface c...

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Highly Robust Silver Nanowire Network for Transparent Electrode.

We investigated the formation of ultraviolet (UV)-assisted directly patternable solution-processed oxide semiconductor films and successfully fabricated thin-film transistors (TFTs) based on these films. An InGaZnO (IGZO) solution that was modified chemically with benzoylacetone (BzAc), whose chelate rings decomposed via a π–π* transition as result of UV irradiation, was used for the direct patterning. A TFT was fabricated using the directly patterned IGZO film, and it had better electrical characteristics than those of conventional photoresist (PR)-patterned TFTs. In addition, the nitric acid (HNO3) and acetylacetone (AcAc) modified In2O3 (NAc-In2O3) solution exhibited both strong UV absorption and high exothermic reaction. This method not only resulted in the formation of a low-energy path because of the combustion of the chemically modified metal-oxide solution but also allowed for photoreaction-induced direct patterning at low temperatures.

Low-temperature metal-oxide thin-film transistors formed by directly photopatternable and combustible solution synthesis.

We employ mixed self-assembled monolayers of carboranethiols to alter the work function of gold and silver systematically. We use isomers of symmetric carboranethiol cage molecules to vary molecular dipole moments and directions, which enable work function tunability over a wide range with minimal alterations in surface energy. Mixed monolayers of carboranethiol isomers provide an ideal platform for the study and fabrication of solution-processed organic field-effect transistors; improved device performance is demonstrated by interface engineering.

https://pubs.acs.org/doi/pdf/10.1021/nl501081q

Interface Control in Organic Electronics Using Mixed Monolayers of Carboranethiol Isomers

Ultrasensitive field-effect transistor-based biosensors using quasi-two-dimensional metal oxide semiconductors were demonstrated. Quasi-two-dimensional low-dimensional metal oxide semiconductors were highly sensitive to electrical perturbations at the semiconductor–bio interface and showed competitive sensitivity compared with other nanomaterial-based biosensors. Also, the solution process made our platform simple and highly reproducible, which was favorable compared with other nanobioelectronics. A quasi-two-dimensional In2O3-based pH sensor showed a small detection limit of 0.0005 pH and detected the glucose concentration at femtomolar levels. Detailed electrical characterization unveiled how the device’s parameters affect the biosensor sensitivity, and lowest detectable charge was extrapolated, which was consistent with the experimental data.

Quasi-Two-Dimensional Metal Oxide Semiconductors Based Ultrasensitive Potentiometric Biosensors.

We investigated aqueous metal complex-based oxide semiconductor films formed with various ligands, such as chloride, acetate, fluoride, and nitrate. Nitrate ligand-based indium(III) precursor was easily decomposed at low temperature due to the replacement of all nitrate ions with water during solvation to form the hexaaqua indium(III) cation ([In(H2O)6]3+). Hexaaqua indium(III) cation was a key complex to realize high-quality oxide films at low temperature. Additionally, Al2O3-based high-k dielectric was also employed by using a nitrate precursor, and the hexaaqua aluminum(III) cation ([Al(H2O)6]3+) was confirmed. This complex-based Al2O3 film showed high breakdown voltage and stable capacitance under high frequency operation compared to organic solvent-based Al2O3 films. We successfully demonstrated aqueous-based In2O3 TFTs with Al2O3 high-k gate dielectrics formed at 250 °C with a wide gate voltage operation and high saturation mobility and on/off ratio of 36.31 ± 2.29 cm2 V–1 s–1 and over 107, respecti...

You Seung Rim

Papers

Highly Robust Silver Nanowire Network for Transparent Electrode.

Low-temperature metal-oxide thin-film transistors formed by directly photopatternable and combustible solution synthesis.

Interface Control in Organic Electronics Using Mixed Monolayers of Carboranethiol Isomers

Quasi-Two-Dimensional Metal Oxide Semiconductors Based Ultrasensitive Potentiometric Biosensors.

Hexaaqua Metal Complexes for Low-Temperature Formation of Fully Metal Oxide Thin-Film Transistors