An Aqueous Process for Preparing Flexible Transparent Electrodes Using Non-Oxidized Graphene/Single-Walled Carbon Nanotube Hybrid Solution.

In this study, we prepared flexible and transparent hybrid electrodes based on an aqueous solution of non-oxidized graphene and single-walled carbon nanotubes. We used a simple halogen intercalation method to obtain high-quality graphene flakes without a redox process and prepared hybrid films using aqueous solutions of graphene, single-walled carbon nanotubes, and sodium dodecyl sulfate surfactant. The hybrid films showed excellent electrode properties, such as an optical transmittance of ≥90%, a sheet resistance of ~3.5 kΩ/sq., a flexibility of up to ε = 3.6% ((R) = 1.4 mm), and a high mechanical stability, even after 103 bending cycles at ε = 2.0% ((R) = 2.5 mm). Using the hybrid electrodes, thin-film transistors (TFTs) were fabricated, which exhibited an electron mobility of ~6.7 cm2 V-1 s-1, a current on-off ratio of ~1.04 × 107, and a subthreshold voltage of ~0.122 V/decade. These electrical properties are comparable with those of TFTs fabricated using Al electrodes. This suggests the possibility of customizing flexible transparent electrodes within a carbon nanomaterial system.

Fabrication of Large-Area Molybdenum Disulfide Device Arrays Using Graphene/Ti Contacts.

Two-dimensional (2D) molybdenum disulfide (MoS2) is the most mature material in 2D material fields owing to its relatively high mobility and scalability. Such noticeable properties enable it to realize practical electronic and optoelectronic applications. However, contact engineering for large-area MoS2 films has not yet been established, although contact property is directly associated to the device performance. Herein, we introduce graphene-interlayered Ti contacts (graphene/Ti) into large-area MoS2 device arrays using a wet-transfer method. We achieve MoS2 devices with superior electrical and photoelectrical properties using graphene/Ti contacts, with a field-effect mobility of 18.3 cm2/V∙s, on/off current ratio of 3 × 107, responsivity of 850 A/W, and detectivity of 2 × 1012 Jones. This outstanding performance is attributable to a reduction in the Schottky barrier height of the resultant devices, which arises from the decreased work function of graphene induced by the charge transfer from Ti. Our research offers a direction toward large-scale electronic and optoelectronic applications based on 2D materials.

Low-Power Complementary Logic Circuit Using Polymer-Electrolyte-Gated Graphene Switching Devices.

The modulation of the electrical properties of graphene and its device configurations for low-power consumption are important in developing graphene-based logic electronics. Here, we demonstrate the change in the charge transport in graphene from ambipolar to unipolar using surface charge transfer doping of the polymer electrolyte. Unipolar graphene field-effect transistors (GFETs) were obtained by the surface treatment of poly(acrylic acid) (PAA) for p-type and poly(ethyleneimine) (PEI) for n-type as polymer-electrolyte gates. In addition, lithium perchlorate (LiClO4) in a polymer matrix can be used for the low-gate voltage operation of GFETs (less than ±3 V) because of its high gating efficiency. Using polymer-electrolyte-gated GFETs, complementary graphene inverters were fabricated with a voltage swing of 57% and maximum voltage gain (Vgain) of 1.1 at a low supply voltage (VDD = 1 V). This is expected to facilitate the development of graphene-based logic devices with low-cost, low-power, and flexible electronics.

Effect of ribbon width on electrical transport properties of graphene nanoribbons.

There has been growing interest in developing nanoelectronic devices based on graphene because of its superior electrical properties. In particular, patterning graphene into a nanoribbon can open a bandgap that can be tuned by changing the ribbon width, imparting semiconducting properties. In this study, we report the effect of ribbon width on electrical transport properties of graphene nanoribbons (GNRs). Monolayer graphene sheets and Si nanowires (NWs) were prepared by chemical vapor deposition and a combination of nanosphere lithography and metal-assisted electroless etching from a Si wafer, respectively. Back-gated GNR field-effect transistors were fabricated on a heavily p-doped Si substrate coated with a 300 nm-thick SiO2 layer, by O2 reactive ion etching of graphene sheets using etch masks based on Si NWs aligned on the graphene between the two electrodes by a dielectrophoresis method. This resulted in GNRs with various widths in a highly controllable manner, where the on/off current ratio was inversely proportional to ribbon width. The field-effect mobility decreased with decreasing GNR widths due to carrier scattering at the GNR edges. These results demonstrate the formation of a bandgap in GNRs due to enhanced carrier confinement in the transverse direction and edge effects when the GNR width is reduced.

Control over Electron-Phonon Interaction by Dirac Plasmon Engineering in the Bi2Se3 Topological Insulator.

Understanding the mutual interaction between electronic excitations and lattice vibrations is key for understanding electronic transport and optoelectronic phenomena. Dynamic manipulation of such interaction is elusive because it requires varying the material composition on the atomic level. In turn, recent studies on topological insulators (TIs) have revealed the coexistence of a strong phonon resonance and topologically protected Dirac plasmon, both in the terahertz (THz) frequency range. Here, using these intrinsic characteristics of TIs, we demonstrate a new methodology for controlling electron-phonon interaction by lithographically engineered Dirac surface plasmons in the Bi2Se3 TI. Through a series of time-domain and time-resolved ultrafast THz measurements, we show that, when the Dirac plasmon energy is less than the TI phonon energy, the electron-phonon coupling is trivial, exhibiting phonon broadening associated with Landau damping. In contrast, when the Dirac plasmon energy exceeds that of the phonon resonance, we observe suppressed electron-phonon interaction leading to unexpected phonon stiffening. Time-dependent analysis of the Dirac plasmon behavior, phonon broadening, and phonon stiffening reveals a transition between the distinct dynamics corresponding to the two regimes as the Dirac plasmon resonance moves across the TI phonon resonance, which demonstrates the capability of Dirac plasmon control. Our results suggest that the engineering of Dirac plasmons provides a new alternative for controlling the dynamic interaction between Dirac carriers and phonons.

Sulfur vacancy-induced reversible doping of transition metal disulfides via hydrazine treatment.

Chemical doping of transition metal dichalcogenides (TMDCs) has drawn significant interest because of its applicability to the modification of electrical and optical properties of TMDCs. This is of fundamental and technological importance for high-efficiency electronic and optoelectronic devices. Here, we present a simple and facile route to reversible and controllable modulation of the electrical and optical properties of WS2 and MoS2via hydrazine doping and sulfur annealing. Hydrazine treatment of WS2 improves the field-effect mobilities, on/off current ratios, and photoresponsivities of the devices. This is due to the surface charge transfer doping of WS2 and the sulfur vacancies formed by its reduction, which result in an n-type doping effect. The changes in the electrical and optical properties are fully recovered when the WS2 is annealed in an atmosphere of sulfur. This method for reversible modulation can be applied to other transition metal disulfides including MoS2, which may enable the fabrication of two-dimensional electronic and optoelectronic devices with tunable properties and improved performance.

Chemically Functionalized, Well-Dispersed Carbon Nanotubes in Lithium-Doped Zinc Oxide for Low-Cost, High-Performance Thin-Film Transistors.

Surface-functionalized carbon nanotubes (CNTs) are introduced into lithium-doped ZnO thin-film transistors (TFTs) as an alternative to the conventional incorporation of an expensive element, indium. The crucial role of surface functionalization of CNTs is clarified with the demonstration of indium-free ZnO-based TFTs with a field-effect mobility of 28.6 cm(2) V(-1) s(-1) and an on/off current ratio of 9 × 10(6) for low-cost, high-performance electronics.

Low-temperature-grown continuous graphene films from benzene by chemical vapor deposition at ambient pressure.

There is significant interest in synthesizing large-area graphene films at low temperatures by chemical vapor deposition (CVD) for nanoelectronic and flexible device applications. However, to date, low-temperature CVD methods have suffered from lower surface coverage because micro-sized graphene flakes are produced. Here, we demonstrate a modified CVD technique for the production of large-area, continuous monolayer graphene films from benzene on Cu at 100-300 °C at ambient pressure. In this method, we extended the graphene growth step in the absence of residual oxidizing species by introducing pumping and purging cycles prior to growth. This led to continuous monolayer graphene films with full surface coverage and excellent quality, which were comparable to those achieved with high-temperature CVD; for example, the surface coverage, transmittance, and carrier mobilities of the graphene grown at 300 °C were 100%, 97.6%, and 1,900-2,500 cm(2) V(-1) s(-1), respectively. In addition, the growth temperature was substantially reduced to as low as 100 °C, which is the lowest temperature reported to date for pristine graphene produced by CVD. Our modified CVD method is expected to allow the direct growth of graphene in device manufacturing processes for practical applications while keeping underlying devices intact.

Isoindigo-Based Donor-Acceptor Conjugated Polymers for Air-Stable Nonvolatile Memory Devices.

Nonvolatile resistive memory devices based on a new low bandgap donor-acceptor (D-A) conjugated polymer, poly((E)-6,6'-bis(2,3-dihydrothieno[3,4-b][1,4]dioxine-5-yl)-1,1'-bis(2-octyldodecyl)-[3,3'-biindolinyi-dene]-2,2'-dione) (PIDED), which are fabricated and operated in ambient air, are reported. The D-A conjugated polymer is synthesized from 2,3-dihydrothieno[3,4-b][1,4]dioxine and isoindigo as an electron donor and an electron acceptor, respectively, using CH-arylation polymerization. The devices show nonvolatile, unipolar resistive switching behaviors with a high on/off current ratio (∼104), excellent endurance cycles (>200 cycles), and a long retention time (>104 s) in ambient air. These properties remain stable in ambient air over one year, demonstrating that the device performance is significantly unaffected by exposure to air as the isoindigo has strong electron-withdrawing character and the PIDED exhibits a high degree of crystallinity. This study may pave the way for use of practical nonvolatile organic memory devices operating in ambient air.

Graphene interlayer for current spreading enhancement by engineering of barrier height in GaN-based light-emitting diodes.

Pristine graphene and a graphene interlayer inserted between indium tin oxide (ITO) and p-GaN have been analyzed and compared with ITO, which is a typical current spreading layer in lateral GaN LEDs. Beyond a certain current injection, the pristine graphene current spreading layer (CSL) malfunctioned due to Joule heat that originated from the high sheet resistance and low work function of the CSL. However, by combining the graphene and the ITO to improve the sheet resistance, it was found to be possible to solve the malfunctioning phenomenon. Moreover, the light output power of an LED with a graphene interlayer was stronger than that of an LED using ITO or graphene CSL. We were able to identify that the improvement originated from the enhanced current spreading by inspecting the contact and conducting the simulation.

Sub-10 nm Graphene Nanoribbon Array field-effect transistors fabricated by block copolymer lithography.

Sub-10 nm Graphene Nanoribbon Arrays are fabricated over large areas by etching CVD-grown graphene. A mask is used made by the directed self-assembly of a cylindrical PS-b-PDMS block copolymer under solvent annealing guided by a removable template. The optimized solvent annealing process, surface-modified removable polymeric templates, and high Flory-Huggins interaction parameters of the block copolymer enable a highly aligned array of nanoribbons with low line edge roughness to be formed. This leads to a higher on/off ratio and stronger temperature dependence of the current for nanoribbon FETs, and a photocurrent which is 30 times larger compared to unpatterned graphene.

Diode-less bilayer oxide (WO(x)-NbO(x)) device for cross-point resistive memory applications.

The combination of a threshold switching device and a resistive switching (RS) device was proposed to suppress the undesired sneak current for the integration of bipolar RS cells in a cross-point array type memory. A simulation for this hybrid-type device shows that the matching of key parameters between switch element and memory element is an important issue. Based on the threshold switching oxides, a conceptual structure with a simple metal-oxide 1-oxide 2-metal stack was provided to accommodate the evolution trend. We show that electroformed W-NbO(x)-Pt devices can simultaneously exhibit both threshold switching and memory switching. A qualitative model was suggested to elucidate the unique properties in a W-NbO(x)-Pt stack, where threshold switching is associated with a localized metal-insulator transition in the NbO(x) bulk, and the bipolar RS derives from a redox at the tip of the localized filament at the WO(x)-NbO(x) interface. Such a simple metal-oxide-metal structure, with functionally separated bulk and interface effects, provides a fabrication advantage for future high-density cross-point memory devices.