Flexible and Transparent Thin-Film Transistors Based on Two-Dimensional Materials for Active-Matrix Display.

Two-dimensional (2D) materials have attracted significant attention because of their outstanding electrical, mechanical, and optical characteristics. Because all of the conducting (graphene), semiconducting (molybdenum disulfide, MoS2), and insulating (hexagonal boron nitride, h-BN) components can be constructed from 2D materials, thin-film transistors based on 2D materials (2D TFTs) have been developed. However, scaling-up is necessary for these technologies to go beyond their initial implementation using the mechanical exfoliation method. Furthermore, it would be beneficial to find a method to realize high flexibility and/or transparency to their full potential. In this study, large-scale, flexible, and transparent 2D TFTs are developed and demonstrated as a backplane in active-matrix organic light-emitting diodes (AMOLEDs). With the optical chemical vapor deposition of the 2D materials, flexible (bending radius < 1 mm) and transparent (transmittance > 70%) TFTs with high electrical performances (mobility ≈ 10 cm2 V-1 s-1, on/off current ratio > 106) can be achieved. Furthermore, 2D TFTs are integrated into OLEDs by connecting the source electrode of the TFT to the anode of the OLED via a single graphene film, thus demonstrating pixel-by-pixel driving through a 2D TFT array in an active-matrix configuration.

Pyridinic-N-Doped Graphene Paper from Perforated Graphene Oxide for Efficient Oxygen Reduction.

We report a simple approach to fabricate a pyridinic-N-doped graphene film (N-pGF) without high-temperature heat treatment from perforated graphene oxide (pGO). pGO is produced by a short etching treatment with hydrogen peroxide. GO perforation predominated in a short etching time (∼1 h), inducing larger holes and defects compared to pristine GO. The pGO is advantageous to the formation of a pyridinic N-doped graphene because of strong NH3 adsorption on vacancies with oxygen functional groups during the nitrogen-doping process, and the pyridinic-N-doped graphene exhibits good electrocatalytic activity for oxygen reduction reaction (ORR). Using rotating-disk electrode measurements, we confirm that N-pGF undergoes a four-electron-transfer process during the ORR in alkaline and acidic media by possessing sufficient diffusion pathways and readily available ORR active sites for efficient mass transport. A comparison between Pt/N-pGF and commercial Pt/C shows that Pt/N-pGF has superior performance, based on its more positive onset potential and higher limiting diffusion current at -0.5 V.

Synergetic electrode architecture for efficient graphene-based flexible organic light-emitting diodes.

Graphene-based organic light-emitting diodes (OLEDs) have recently emerged as a key element essential in next-generation displays and lighting, mainly due to their promise for highly flexible light sources. However, their efficiency has been, at best, similar to that of conventional, indium tin oxide-based counterparts. We here propose an ideal electrode structure based on a synergetic interplay of high-index TiO2 layers and low-index hole-injection layers sandwiching graphene electrodes, which results in an ideal situation where enhancement by cavity resonance is maximized yet loss to surface plasmon polariton is mitigated. The proposed approach leads to OLEDs exhibiting ultrahigh external quantum efficiency of 40.8 and 62.1% (64.7 and 103% with a half-ball lens) for single- and multi-junction devices, respectively. The OLEDs made on plastics with those electrodes are repeatedly bendable at a radius of 2.3 mm, partly due to the TiO2 layers withstanding flexural strain up to 4% via crack-deflection toughening.

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.

Metal-etching-free direct delamination and transfer of single-layer graphene with a high degree of freedom.

A method of graphene transfer without metal etching is developed to minimize the contamination of graphene in the transfer process and to endow the transfer process with a greater degree of freedom. The method involves direct delamination of single-layer graphene from a growth substrate, resulting in transferred graphene with nearly zero Dirac voltage due to the absence of residues that would originate from metal etching. Several demonstrations are also presented to show the high degree of freedom and the resulting versatility of this transfer method.

Large-area single-layer MoSe2 and its van der Waals heterostructures.

Layered structures of transition metal dichalcogenides stacked by van der Waals interactions are now attracting the attention of many researchers because they have fascinating electronic, optical, thermoelectric, and catalytic properties emerging at the monolayer limit. However, the commonly used methods for preparing monolayers have limitations of low yield and poor extendibility into large-area applications. Herein, we demonstrate the synthesis of large-area MoSe2 with high quality and uniformity by selenization of MoO3 via chemical vapor deposition on arbitrary substrates such as SiO2 and sapphire. The resultant monolayer was intrinsically doped, as evidenced by the formation of charged excitons under low-temperature photoluminescence analysis. A van der Waals heterostructure of MoSe2 on graphene was also demonstrated. Interestingly, the MoSe2/graphene heterostructures show strong quenching of the characteristic photoluminescence from MoSe2, indicating the rapid transfer of photogenerated charge carriers between MoSe2 and graphene. The development of highly controlled heterostructures of two-dimensional materials will further promote advances in the physics and chemistry of reduced dimensional systems and will provide novel applications in electronics and optoelectronics.

Laser-induced solid-phase doped graphene.

There have been numerous efforts to improve the performance of graphene-based electronic devices by chemical doping. Most studies have focused on gas-phase doping with chemical vapor deposition. However, that requires a complicated transfer process that causes undesired doping and defects by residual polymers. Here, we report a solid-phase synthesis of doped graphene by means of silicon carbide (SiC) substrate including a dopant source driven by pulsed laser irradiation. This method provides in situ direct growth of doped graphene on an insulating SiC substrate without a transfer step. A numerical simulation on the temperature history of the SiC surface during laser irradiation reveals that the surface temperature of SiC can be accurately controlled to grow nitrogen-doped graphene from the thermal decomposition of nitrogen-doped SiC. Laser-induced solid-phase doped graphene is highly promising for the realization of graphene-based nanoelectronics with desired functionalities.