Synthesis of Vacancy-Controlled Copper Iodide Semiconductor for High-Performance p-Type Thin-Film Transistors.

Copper iodide (CuI) has emerged as a promising p-type semiconductor material owing to its excellent carrier mobility, high transparency, and solution processability. Although CuI has potential for numerous applications, including perovskite solar cells, photovoltaic devices, and thin-film transistors (TFTs), the close relationship between the anion vacancy generation and the charge transport mechanism in CuI-based devices is underexplored. In this study, we propose solution-processed p-type CuI TFTs which were subject to the thermal annealing process in air and vacuum atmospheres at temperatures of 100, 200, and 300 °C. The chemical states and surface morphologies of the CuI thin films were systematically investigated, revealing the generation of iodine vacancy states and the reduction of carrier concentration, as well as increased film density and grain size according to the annealing condition. Further, the effective role of the Al2O3 passivation layer on the electrical characteristics of the solution-processed CuI TFTs is demonstrated for the first time, where the Al2O3 precursor greatly enhanced the electrical performance of the CuI TFTs, exhibiting a field-effect mobility of 4.02 cm2/V·s, a subthreshold swing of 0.61 V/decade, and an on/off current ratio of 1.12 × 104, which exceed the values of CuI TFTs reported so far. Based on the synergistic effects of the annealing process and the passivation layer that engineered the iodine vacancy state and morphology of CuI, the proposed CuI TFTs with the Al2O3 passivation layer showed excellent reliability under 100 times repeated operation and long-term stability over 216 h, where the transfer curves slightly shifted in the positive direction of 1.36 and 1.88 V measured at a current level of 10-6 A for the reliability and stability tests, respectively. Thus, this work opens a new window for solution-processed p-type CuI TFTs with excellent stability for developing next-generation complementary logic circuits.

Charge Transfer Dynamics of Doped Graphene Electrodes for Organic Light-Emitting Diodes.

Atomically thin graphene has attracted immense attention as a future transparent electrode for flat-panel displays owing to its excellent conductivity, optical transparency, and flexibility. In particular, a graphene doping process is essential for implementing graphene-based high-performance devices, and the development of a transparent cathode with a low work function is required to simplify the integration process of thin-film transistors and organic light-emitting diodes (OLEDs) into active matrix displays. In this study, a transparent n-doped graphene cathode is proposed for implementing inverted OLEDs through two types of cesium (Cs)-based doping techniques: a dipping method using wet chemicals and an evaporation method under a vacuum atmosphere. The changes in the chemical structures and work functions of the n-doped graphene electrodes, as well as their surface morphologies and transmittances, were systematically investigated. The n-type doping mechanism of graphene was investigated, and a close relationship between the electrical charge transfer characteristics of graphene transistors and the formation of C-O-Cs complexes was revealed. Finally, an effective Cs-doped graphene electrode was developed, exhibiting a dramatically decreased work function while maintaining high transmittance; therefore, the Cs-doped graphene cathode was successfully integrated with inverted OLEDs with a bottom-light emission structure that exhibited enhanced external quantum efficiency of graphene cathode-based OLEDs. Thus, our findings provide a better understanding of the doping strategies and potential of n-doped graphene as a transparent cathode for developing high-performance future displays.

Enhanced Triboelectric Nanogenerator Based on Tungsten Disulfide via Thiolated Ligand Conjugation.

Two-dimensional transition-metal dichalcogenides (TMDs) are of particular interest as a new active material for future triboelectric nanogenerators (TENGs) owing to their excellent electrical properties, optical transparency, flexibility, ultrathin thickness, and biocompatibility. Here, we propose a new approach to engineer the surface of TMDs via conjugation with thiolated ligands having different alkane chain lengths and to develop TMD-based TENG devices that exhibit enhanced output performance for the first time. The triboelectric charging behaviors of ligand-conjugated TMDs are successfully investigated, and the electrical output performance of TMD TENGs based on TMD-to-polymer device geometries with a vertical contact-separation mode is dramatically improved, exhibiting an output voltage of 12.2 V and a power density of 138 mW/m2. Furthermore, the ligand-conjugated TMD TENG device exhibits a highly stable operation under repeated contact and separation over 10 000 cycles, as well as high chemical stability, as a result of novel defect engineering via thiolated ligand conjugation. Detailed investigation reveals that the improved performance of the ligand-conjugated TMD TENG device originates from the synergistic effect of defect engineering and the p-type doping effect of TMDs, correlated with the increased electric potential difference between triboelectric layers. These findings provide a new potential of TMDs as a promising building block for the next-generation energy harvesting system.

Synthesis of Ultrathin Metal Nanowires with Chemically Exfoliated Tungsten Disulfide Nanosheets.

Transition metal dichalcogenides (TMDs) have attracted great interest owing to their fascinating properties with atomically thin nature. Although TMDs have been exploited for diverse applications, the effective role of TMDs in the synthesis of metal nanowires has not been explored. Here, we propose a new approach to synthesize ultrathin metal nanowires using TMDs for the first time. High-quality ultrathin nanowires with an average diameter of 11.3 nm are successfully synthesized for realizing high-performance transparent conductors that exhibit excellent conductivity and transparency with low haze. The growth mechanism is carefully investigated using high-resolution transmission electron microscopy, and growth of nanowires with tunable diameters is achieved by controlling the nanosheet dimension. Finally, we unravel the important role of TMDs acting as both reducing and nucleating agents. Therefore, our work provides a new strategy of the TMD as an innovative material for the growth of metal nanowires as a promising building block in next-generation optoelectronics.

Stretchable thin-film transistors with molybdenum disulfide channels and graphene electrodes.

Two-dimensional (2D) materials including graphene and transition metal dichalcogenides (TMDCs) have attracted great interest as new electronic materials, given their superior properties such as optical transparency, mechanical flexibility, and stretchability, especially for application in next-generation displays. In particular, the integration of graphene and TMDCs enables the implementation of 2D materials-based thin-film transistors (TFTs) in stretchable displays, given that TFTs are the fundamental element of various modern devices. In the present study, we demonstrate chemical-vapor-deposited molybdenum disulfide and graphene-based TFTs on a polymer substrate and investigate the electrical characteristics of TFTs under mechanical deformation to determine the stretchability of our devices. Furthermore, the mechanisms leading to TFT performance degradation are investigated, as they relate to the change in the contact resistance that is closely associated with the relative deformation of 2D materials under mechanical stress. Therefore, the synergetic integration of 2D materials with versatile electrical properties provides an important strategy for creating 2D materials-based stretchable TFTs, thus extending the excellent potential of 2D materials as innovative materials for stretchable active-matrix displays.

Antibacterial Activities of Graphene Oxide-Molybdenum Disulfide Nanocomposite Films.

Two-dimensional (2D) nanomaterials, such as graphene-based materials and transition metal dichalcogenide (TMD) nanosheets, are promising materials for biomedical applications owing to their remarkable cytocompatibility and physicochemical properties. On the basis of their potent antibacterial properties, 2D materials have potential as antibacterial films, wherein the 2D nanosheets are immobilized on the surface and the bacteria may contact with the basal planes of 2D nanosheets dominantly rather than contact with the sharp edges of nanosheets. To address these points, in this study, we prepared an effective antibacterial surface consisting of representative 2D materials, i.e., graphene oxide (GO) and molybdenum disulfide (MoS2), formed into nanosheets on a transparent substrate for real device applications. The antimicrobial properties of the GO-MoS2 nanocomposite surface toward the Gram-negative bacteria Escherichia coli were investigated, and the GO-MoS2 nanocomposite exhibited enhanced antimicrobial effects with increased glutathione oxidation capacity and partial conductivity. Furthermore, direct imaging of continuous morphological destruction in the individual bacterial cells having contacts with the GO-MoS2 nanocomposite surface was characterized by holotomographic (HT) microscopy, which could be used to detect the refractive index (RI) distribution of each voxel in bacterial cell and reconstruct the three-dimensional (3D) mapping images of bacteria. In this regard, the decreases in both the volume (67.2%) and the dry mass (78.8%) of bacterial cells that came in contact with the surface for 80 min were quantitatively measured, and releasing of intracellular components mediated by membrane and oxidative stress was observed. Our findings provided new insights into the antibacterial properties of 2D nanocomposite film with label-free tracing of bacterial cell which improve our understanding of antimicrobial activities and opened a window for the 2D nanocomposite as a practical antibacterial film in biomedical applications.

Healing Graphene Defects Using Selective Electrochemical Deposition: Toward Flexible and Stretchable Devices.

Graphene produced by chemical-vapor-deposition inevitably has defects such as grain boundaries, pinholes, wrinkles, and cracks, which are the most significant obstacles for the realization of superior properties of pristine graphene. Despite efforts to reduce these defects during synthesis, significant damages are further induced during integration and operation of flexible and stretchable applications. Therefore, defect healing is required in order to recover the ideal properties of graphene. Here, the electrical and mechanical properties of graphene are healed on the basis of selective electrochemical deposition on graphene defects. By exploiting the high current density on the defects during the electrodeposition, metal ions such as silver and gold can be selectively reduced. The process is universally applicable to conductive and insulating substrates because graphene can serve as a conducting channel of electrons. The physically filled metal on the defects improves the electrical conductivity and mechanical stretchability by means of reducing contact resistance and crack density. The healing of graphene defects is enabled by the solution-based room temperature electrodeposition process, which broadens the use of graphene as an engineering material.