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

The effects of high-pressure annealing were investigated using amorphous InGaZnO (a-IGZO) thin-film transistors (TFTs). The fabricated device annealed at 5 atm in H2O ambient showed the best electrical characteristics and stability under positive bias temperature stress (PBTS). This was attributed to mainly a reduction in the band bending at the overlap between the source–drain (S/D) electrodes and the etch stop layer (ESL). This is originated from the recovery of charge-trapping sites at in- and bottom-ESLs due to defect passivation with the aid of high-pressure thermal annealing at 5 atm in H2O ambient.

Effects of high-pressure H2O-annealing on amorphous IGZO thin-film transistors

Investigation of solution-processed amorphous SrInZnO thin film transistors

β-Ga2O3 Schottky barrier diodes (SBDs) were demonstrated with Ni Schottky contact deposited by the confined magnetic field-based sputtering (CMFS) method. A shallow interfacial layer was formed by the diffusion of Ni into β-Ga2O3 after post-annealing treatment, which significantly influenced the electrical performance of the CMFS-Ni/β-Ga2O3 SBDs. The CMFS method was used to vary the Schottky barrier height and the ideality factor from 0.84 to 1.33 eV and 1.20 to 1.04, respectively. The leakage current of the CMFS-SBDs was only 10% of the leakage current using E-beam Ni-based SBDs, and the thermal stability of the CMFS-SBDs also was much higher than that of the E-beam Ni SBDs. We confirmed that the effective diffusion of Ni atoms could substitute for Ga through the activation of the β-Ga2O3 with CMFS.

Effective surface diffusion of nickel on single crystal β-Ga2O3 for Schottky barrier modulation and high thermal stability

Nanoribbon- and nanowire-based field-effect transistors (FETs) have attracted significant attention due to their high surface-to-volume ratios, which make them effective as chemical and biological sensors. However, the conventional nanofabrication of these devices is challenging and costly, posing a major barrier to widespread use. We report a high-throughput approach for producing arrays of ultrathin (∼3 nm) In2O3 nanoribbon FETs at the wafer scale. Uniform films of semiconducting In2O3 were prepared on Si/SiO2 surfaces via a sol-gel process prior to depositing Au/Ti metal layers. Commercially available high-definition digital versatile discs were employed as low-cost, large-area templates to prepare polymeric stamps for chemical lift-off lithography, which selectively removed molecules from self-assembled monolayers functionalizing the outermost Au surfaces. Nanoscale chemical patterns, consisting of one-dimensional lines (200 nm wide and 400 nm pitch) extending over centimeter length scales, were etched into the metal layers using the remaining monolayer regions as resists. Subsequent etch processes transferred the patterns into the underlying In2O3 films before the removal of the protective organic and metal coatings, revealing large-area nanoribbon arrays. We employed nanoribbons in semiconducting FET channels, achieving current on-to-off ratios over 107 and carrier mobilities up to 13.7 cm2 V-1 s-1. Nanofabricated structures, such as In2O3 nanoribbons and others, will be useful in nanoelectronics and biosensors. The technique demonstrated here will enable these applications and expand low-cost, large-area patterning strategies to enable a variety of materials and design geometries in nanoelectronics.

You Seung Rim

Papers

Effects of high-pressure H2O-annealing on amorphous IGZO thin-film transistors

Investigation of solution-processed amorphous SrInZnO thin film transistors

Effective surface diffusion of nickel on single crystal β-Ga2O3 for Schottky barrier modulation and high thermal stability

Large-Area, Ultrathin Metal-Oxide Semiconductor Nanoribbon Arrays Fabricated by Chemical Lift-Off Lithography

Preparation of Al-doped ZnO thin film deposited at room temperature