Supercapacitors with porous carbon structures have high energy storage capacity. However, the porous nature of the carbon electrode, composed mainly of carbon nanotubes (CNTs) and graphene oxide (GO) derivatives, negatively impacts the volumetric electrochemical characteristics of the supercapacitors because of poor packing density (<0.5 g cm(-3)). Herein, we report a simple method to fabricate highly dense and vertically aligned reduced graphene oxide (VArGO) electrodes involving simple hand-rolling and cutting processes. Because of their vertically aligned and opened-edge graphene structure, VArGO electrodes displayed high packing density and highly efficient volumetric and areal electrochemical characteristics, very fast electrolyte ion diffusion with rectangular CV curves even at a high scan rate (20 V/s), and the highest volumetric capacitance among known rGO electrodes. Surprisingly, even when the film thickness of the VArGO electrode was increased, its volumetric and areal capacitances were maintained.

We report on the interlayer screening effect of graphene using Kelvin probe force microscopy (KPFM). By using a gate device configuration that enables the supply of electronic carriers in graphene sheets, the vertical screening properties were studied from measuring the surface potential gradient. The results show layer-dependence of graphene sheets, as the number of graphene layers increases, the surface potential decreases exponentially. In addition, we calculate the work function-related information of the graphene layers using KPFM.

Nonvolatile memory devices using gold nanoparticles (AuNPs) and reduced graphene oxide (rGO) sheets were fabricated in both horizontal and vertical structures. The horizontal memory device, in which a singly and doubly overlayered semiconducting rGO channel was formed by simply using a spin-casting technique to connect two gold electrodes, was designed for understanding the origin of charging effects. AuNPs were chemically bound to the rGO channel through a π-conjugated molecular linker. The π-conjugated bifunctional molecular linker, 4-mercapto-benzenediazonium tetrafluoroborate (MBDT) salt, was newly synthesized and used as a molecular bridge to connect the AuNPs and rGOs. By using a self-assembly technique, the diazonium functional group of the MBDT molecular linker was spontaneously immobilized on the rGOs. Then, the monolayered AuNPs working as capacitors were covalently connected to the thiol groups of the MBDT molecules, which were attached to rGOs (AuNP-frGO). These covalent bonds were confirmed by XPS analyses. The current-voltage characteristics of both the horizontal and vertical AuNP-frGO memory devices showed noticeable nonlinear hysteresis, stable write-multiple read-erase-multiple read cycles over 1000 s, and a long retention time over 700 s. In addition, the vertical AuNP-frGO memory device showed a large current ON/OFF ratio and high stability.

A strong electrostatic MV(2+) -GQD nanocomposite provides an electrolyte-free flexible electrochromic device wih high durability. The positively charged MV(2+) and negatively charged GQD are strongly stabilized by non-covalent intermolecular forces (e.g., electrostatic interactions, π-π stacking interactions, and cation-π electron interactions), eliminating the need for an electrolyte. An electrolyte-free flexible electrochromic device fabricated from the GQD-supported MV(2+) exhibits stable performance under mechanical and thermal stresses.

A molecular ultra-thin film (for example, a molecular monolayer) with graphene electrodes would allow for the realization of superior stable, transparent and flexible electronics. A realistic prospect regarding the use of graphene in two-terminal molecular electronic devices is to fabricate a chemically stable, optically transparent, mechanically flexible and molecularly compatible junction. Here we report on a novel photo-switchable molecular monolayer, one side chemically and the other side physically anchored between the two graphene electrodes. The photo-switchable organic molecules specified with an electrophilic group are chemically self-assembled into a monolayer on the graphene bottom electrode, while the other end is physically contacted to the graphene top electrode; this arrangement provides excellent stability for a highly transparent and flexible molecular monolayer device with a high device yield due to soft contacts at the top electrode interface. Thus, the transparent graphene electrodes allow stable molecular photo-switching due to photoinduced changes in the molecular conformational length.

Reduction to the essential: A highly conductive and soft carbon interlayer of reduced graphene oxide (rGO) prevents the formation of a filamentary current path, achieving both high yield and true molecular effects in monolayer‐based molecular devices. Junctions of the rGO interlayer contacts with molecular monolayers elucidate the molecularly resolved electronic properties of molecular resistors and nonvolatile memories.

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A simple chemical method to obtain bulk quantities of N-doped, reduced graphene oxide (rGO) sheets (see figure) as an n-type semiconductor through the treatment of as-prepared GO sheets with the commonly used reducing reagent hydrazine, followed by rapid thermal annealing (RTA) is described.