Two-Dimensional Disposable Graphene Sensor to Detect Na+ Ions.

The monitoring of Na+ ions distributed in the body has been indirectly calculated by the detection of Na+ ions in urine. We fabricated a two-dimensional (2D) Na+ ion sensor using a graphene ion-sensitive field-effect transistor (G-ISFET) and used fluorinated graphene as a reference electrode (FG-RE). We integrated G-ISFET and FG on a printed circuit board (PCB) designed in the form of a secure digital (SD) card to fabricate a disposable Na+ ion sensor. The sensitivity of the PCB tip to Na+ ions was determined to be -55.4 mV/dec. The sensor exhibited good linearity despite the presence of interfering ions in the buffer solution. We expanded the evaluation of the PCB tip to real human patient urine samples. The PCB tip exhibited a sensitivity of -0.36 mV/mM and linearly detected Na+ ions in human patient urine without any dilution process. We expect that G-ISFET with FG-RE can be used to realize a disposable Na+ ion sensor by serving as an alternative to Ag/AgCl reference electrodes.

Mechanistic Understanding of Improved Performance of Graphene Cathode Inverted Organic Light-Emitting Diodes by Photoemission and Impedance Spectroscopy.

Modification of multilayer graphene films was investigated for a cathode of organic light-emitting diodes (OLEDs). By doping the graphene/electron transport layer (ETL) interface with Li, the driving voltage of the OLED was reduced dramatically from 24.5 to 3.2 V at a luminance of 1000 cd/m2. The external quantum efficiency was also enhanced from 3.4 to 12.9%. Surface analyses showed that the Li doping significantly lowers the lowest unoccupied molecular orbital level of the ETL, thereby reducing the electron injection barrier and facilitating electron injection from the cathode. Impedance spectroscopy analyses performed on electron-only devices (EODs) revealed the existence of distributed trap states with a well-defined activation energy, which is successfully described by the Havriliak-Negami capacitance functions and the temperature-independent frequency dispersion parameters. In particular, the graphene EOD showed a unique high-frequency feature as compared to the indium tin oxide one, which could be explained by an additional parallel capacitance element.

Graphene Electrode Enabling Electrochromic Approaches for Daylight-Dimming Applications.

For environmental reason, buildings increasingly install smart windows, which can dim incoming daylight based on active electrochromic devices (ECDs). In this work, multi-layered graphene (MLG) was investigated as an ECD window electrode, to minimize carbon dioxide (CO2) emissions by decreasing the electricity consumption for building space cooling and heating and as an alternative to the transparent conductor tin-doped indium oxide (ITO) in order to decrease dependence on it. Various MLG electrodes with different numbers of graphene layers were prepared with environmentally friendly poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) to produce ECD cells. Tests demonstrated the reproducibility and uniformity in optical performance, as well as the flexibility of the ECD fabrication. With the optimized MLG electrode, the ECD cells exhibited a very fast switching response for optical changes from transparent to dark states of a few hundred msec.

Overcoming the efficiency limit of organic light-emitting diodes using ultra-thin and transparent graphene electrodes.

We propose an effective way to enhance the out-coupling efficiencies of organic light-emitting diodes (OLEDs) using graphene as a transparent electrode. In this study, we investigated the detrimental adsorption and internal optics occurring in OLEDs with graphene anodes. The optical out-coupling efficiencies of previous OLEDs with transparent graphene electrodes barely exceeded those of OLEDs with conventional transparent electrodes because of the weak microcavity effect. To overcome this issue, we introduced an internal random scattering layer for light extraction and reduced the optical absorption of the graphene by reducing the number of layers in the multilayered graphene film. The efficiencies of the graphene-OLEDs increased significantly with decreasing the number of graphene layers, strongly indicating absorption reduction. The maximum light extraction efficiency was obtained by using a single-layer graphene electrode together with a scattering layer. As a result, a widened angular luminance distribution with a remarkable external quantum efficiency and a luminous efficacy enhancement of 52.8% and 48.5%, respectively, was achieved. Our approach provides a demonstration of graphene-OLED having a performance comparable to that of conventional OLEDs.

Flexible Indium-Tin Oxide Crystal on Plastic Substrates Supported by Graphene Monolayer.

Flexible and crystallized indium-tin oxide (ITO) thin films were successfully obtained on plastic polyethylene terephthalate (PET) films with monolayered graphene as a platform. The highly crystalline ITO (c-ITO) was first fabricated on a rigid substrate of graphene on copper foil and it was subsequently transferred onto a PET substrate by a well-established technique. Despite the plasma damage during ITO deposition, the graphene layer effectively acted as a Cu-diffusion barrier. The c-ITO/graphene/PET electrode with the 60-nm-thick ITO exhibited a reasonable sheet resistance of ~45 Ω sq-1 and a transmittance of ~92% at a wavelength of 550 nm. The c-ITO on the monolayered graphene support showed significant enhancement in flexibility compared with the ITO/PET film without graphene because the atomically controlled monolayered graphene acted as a mechanically robust support. The prepared flexible transparent c-ITO/graphene/PET electrode was applied as the anode in a bulk heterojunction polymer solar cell (PSC) to evaluate its performance, which was comparable with that of the commonly used c-ITO/glass electrode. These results represent important progress in the fabrication of flexible transparent electrodes for future optoelectronics applications.

Stable angular emission spectra in white organic light-emitting diodes using graphene/PEDOT:PSS composite electrode.

In this work, we suggest a graphene/ poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) composite as a transparent electrode for stabilizing white emission of organic light-emitting diodes (OLEDs). Graphene/PEDOT:PSS composite electrodes have increased reflectance when compared to graphene itself, but their reflectance is still lower than that of ITO itself. Changes in the reflectance of the composite electrode have the advantage of suppressing the angular spectral distortion of white emission OLEDs and achieving an efficiency of 16.6% for white OLEDs, comparable to that achieved by graphene-only electrodes. By controlling the OLED structure to compensate for the two-beam interference effect, the CIE color coordinate change (Δxy) of OLEDs based on graphene/PEDOT:PSS composite electrodes is 0.018, less than that based on graphene-only electrode, i.e.,0.027.

A reliable and controllable graphene doping method compatible with current CMOS technology and the demonstration of its device applications.

The modulation of charge carrier concentration allows us to tune the Fermi level (E F) of graphene thanks to the low electronic density of states near the E F. The introduced metal oxide thin films as well as the modified transfer process can elaborately maneuver the amounts of charge carrier concentration in graphene. The self-encapsulation provides a solution to overcome the stability issues of metal oxide hole dopants. We have manipulated systematic graphene p-n junction structures for electronic or photonic application-compatible doping methods with current semiconducting process technology. We have demonstrated the anticipated transport properties on the designed heterojunction devices with non-destructive doping methods. This mitigates the device architecture limitation imposed in previously known doping methods. Furthermore, we employed E F-modulated graphene source/drain (S/D) electrodes in a low dimensional transition metal dichalcogenide field effect transistor (TMDFET). We have succeeded in fulfilling n-type, ambipolar, or p-type field effect transistors (FETs) by moving around only the graphene work function. Besides, the graphene/transition metal dichalcogenide (TMD) junction in either both p- and n-type transistor reveals linear voltage dependence with the enhanced contact resistance. We accomplished the complete conversion of p-/n-channel transistors with S/D tunable electrodes. The E F modulation using metal oxide facilitates graphene to access state-of-the-art complimentary-metal-oxide-semiconductor (CMOS) technology.

Graphene-coated meshes for electroactive flow control devices utilizing two antagonistic functions of repellency and permeability.

The wettability of graphene on various substrates has been intensively investigated for practical applications including surgical and medical tools, textiles, water harvesting, self-cleaning, oil spill removal and microfluidic devices. However, most previous studies have been limited to investigating the intrinsic and passive wettability of graphene and graphene hybrid composites. Here, we report the electrowetting of graphene-coated metal meshes for use as electroactive flow control devices, utilizing two antagonistic functions, hydrophobic repellency versus liquid permeability. Graphene coating was able to prevent the thermal oxidation and corrosion problems that plague unprotected metal meshes, while also maintaining its hydrophobicity. The shapes of liquid droplets and the degree of water penetration through the graphene-coated meshes were controlled by electrical stimuli based on the functional control of hydrophobic repellency and liquid permeability. Furthermore, using the graphene-coated metal meshes, we developed two active flow devices demonstrating the dynamic locomotion of water droplets and electroactive flow switching.

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.

Graphene-induced unusual microstructural evolution in Ag plated Cu foils.

Graphene-induced abnormal grain growth of Cu with a grain size of more than 1 mm(2) was observed on Cu-Ag alloy foil, and this phenomenon occurred only with graphene synthesis and only on the Cu-Ag alloy among various types of Cu foils.

Wetting-transparent graphene films for hydrophobic water-harvesting surfaces.

Wetting-transparent graphene films grown in situ by chemical vapor deposition on hydrophobic (roughened) copper surfaces offer excellent resistance to copper corrosion while maintaining the intrinsic hydrophobicity of the surface, enabling superior performance for water-harvesting applications.

Synthesis of CVD-graphene on rapidly heated copper foils.

Most chemical vapor deposition (CVD) systems used for graphene growth mainly employ convection and radiation heat transfer between the heating source and the metal catalyst in order to reach the activation temperature of the reaction, which in general leads to a long synthesis time and poor energy efficiency. Here, we report a highly time- and energy-efficient CVD setup, in which the metal catalyst (Cu) is designed to be physically contacted with a heating source to give quick heat transfer by conduction. The induced conduction heating enabled the usual effects of the pretreatment and annealing of Cu (i.e., annihilation of surface defects, impurities and contaminants) to be achieved in a significantly shorter time compared to conventional CVD. Notably, the rapid heating was observed to lead to larger grains of Cu with high uniformity as compared to the Cu annealed by conventional CVD, which are believed to be beneficial for the growth of high quality graphene. Through this CVD setup, bundles of high quality (∼252 Ω per square) and large area (over 16 inch) graphenes were able to be readily synthesized in 40 min in a significantly efficient way. When considering ease of scalability, high energy effectiveness and considerable productivity, our method is expected to be welcomed by industrialists.

Highly uniform growth of monolayer graphene by chemical vapor deposition on Cu-Ag alloy catalysts.

One of the major challenges for the practical application of graphene is the large scale synthesis of uniform films with high quality at lower temperature. Here, we demonstrate the use of Ag-plated Cu substrates in the synthesis of high-quality graphene films via chemical vapor deposition (CVD) of methane gas at temperatures as low as 900 °C. Various experimental analyses show that the plated Ag diffuses into Cu to form a uniform Cu-Ag alloy that suppresses the formation of multilayer nucleation and decreases the activation energy of precursor formation, leading to a lower synthesis temperature with enhanced monolayer coverage. In addition, we also observed an unusual Ag-assisted abnormal grain growth of Cu into the cube texture with larger grain sizes and reduced grain boundaries, which is believed to provide the homogeneous environment needed for uniform graphene growth.

Fast synthesis of high-performance graphene films by hydrogen-free rapid thermal chemical vapor deposition.

The practical use of graphene in consumer electronics has not been demonstrated since the size, uniformity, and reliability problems are yet to be solved to satisfy industrial standards. Here we report mass-produced graphene films synthesized by hydrogen-free rapid thermal chemical vapor deposition (RT-CVD), roll-to-roll etching, and transfer methods, which enabled faster and larger production of homogeneous graphene films over 400 × 300 mm(2) area with a sheet resistance of 249 ± 17 Ω/sq without additional doping. The properties of RT-CVD graphene have been carefully characterized by high-resolution transmission electron microscopy, Raman spectroscopy, chemical grain boundary analysis, and various electrical device measurements, showing excellent uniformity and stability. In particular, we found no significant correlation between graphene domain sizes and electrical conductivity, unlike previous theoretical expectations for nanoscale graphene domains. Finally, the actual application of the RT-CVD films to capacitive multitouch devices installed in the most sophisticated mobile phone was demonstrated.