Synthesis and properties of free-standing monolayer amorphous carbon.

Bulk amorphous materials have been studied extensively and are widely used, yet their atomic arrangement remains an open issue. Although they are generally believed to be Zachariasen continuous random networks1, recent experimental evidence favours the competing crystallite model in the case of amorphous silicon2-4. In two-dimensional materials, however,  the corresponding questions remain unanswered. Here we report the synthesis, by laser-assisted chemical vapour deposition5, of centimetre-scale, free-standing, continuous and stable monolayer amorphous carbon, topologically distinct from disordered graphene. Unlike in bulk materials, the structure of monolayer amorphous carbon can be determined by atomic-resolution imaging. Extensive characterization by Raman and X-ray spectroscopy and transmission electron microscopy reveals the complete absence of long-range periodicity and a threefold-coordinated structure with a wide distribution of bond lengths, bond angles, and five-, six-, seven- and eight-member rings. The ring distribution is not a Zachariasen continuous random network, but resembles the competing (nano)crystallite model6. We construct a corresponding model that enables density-functional-theory calculations of the properties of monolayer amorphous carbon, in accordance with observations. Direct measurements confirm that it is insulating, with resistivity values similar to those of boron nitride grown by chemical vapour deposition. Free-standing monolayer amorphous carbon is surprisingly stable and deforms to a high breaking strength, without crack propagation from the point of fracture. The excellent physical properties of this stable, free-standing monolayer amorphous carbon could prove useful for permeation and diffusion barriers in applications such as magnetic recording devices and flexible electronics.

Nanometer thick elastic graphene engine.

Significant progress has been made in the construction and theoretical understanding of molecular motors because of their potential use. Here, we have demonstrated fabrication of a simple but powerful 1 nm thick graphene engine. The engine comprises a high elastic membrane-piston made of graphene and weakly chemisorbed ClF3 molecules as the high power volume changeable actuator, while a 532 nm LASER acts as the ignition plug. Rapid volume expansion of the ClF3 molecules leads to graphene blisters. The size of the blister is controllable by changing the ignition parameters. The estimated internal pressure per expansion cycle of the engine is about ∼10(6) Pa. The graphene engine presented here shows exceptional reliability, showing no degradation after 10,000 cycles.

Flexible graphene-PZT ferroelectric nonvolatile memory.

We report the fabrication of a flexible graphene-based nonvolatile memory device using Pb(Zr0.35,Ti0.65)O3 (PZT) as the ferroelectric material. The graphene and PZT ferroelectric layers were deposited using chemical vapor deposition and sol­gel methods, respectively. Such PZT films show a high remnant polarization (Pr) of 30 µC cm−2 and a coercive voltage (Vc) of 3.5 V under a voltage loop over ±11 V. The graphene­PZT ferroelectric nonvolatile memory on a plastic substrate displayed an on/off current ratio of 6.7, a memory window of 6 V and reliable operation. In addition, the device showed one order of magnitude lower operation voltage range than organic-based ferroelectric nonvolatile memory after removing the anti-ferroelectric behavior incorporating an electrolyte solution. The devices showed robust operation in bent states of bending radii up to 9 mm and in cycling tests of 200 times. The devices exhibited remarkable mechanical properties and were readily integrated with plastic substrates for the production of flexible circuits.

Graphene field-effect transistors with ferroelectric gating.

Recent experiments on ferroelectric gating have introduced a novel functionality, i.e., nonvolatility, in graphene field-effect transistors. A comprehensive understanding in the nonlinear, hysteretic ferroelectric gating and an effective way to control it are still absent. In this Letter, we quantitatively characterize the hysteretic ferroelectric gating using the reference of an independent background doping (n(BG)) provided by normal dielectric gating. More importantly, we prove that n(BG) can be used to control the ferroelectric gating by unidirectionally shifting the hysteretic ferroelectric doping in graphene. Utilizing this electrostatic effect, we demonstrate symmetrical bit writing in graphene-ferroelectric field-effect transistors with resistance change over 500% and reproducible no-volatile switching over 105 cycles.

Colossal Ultraviolet Photoresponsivity of Few-Layer Black Phosphorus.

Black phosphorus has an orthorhombic layered structure with a layer-dependent direct band gap from monolayer to bulk, making this material an emerging material for photodetection. Inspired by this and the recent excitement over this material, we studied the optoelectronics characteristics of high-quality, few-layer black phosphorus-based photodetectors over a wide spectrum ranging from near-ultraviolet (UV) to near-infrared (NIR). It is demonstrated for the first time that black phosphorus can be configured as an excellent UV photodetector with a specific detectivity ∼3 × 10(13) Jones. More critically, we found that the UV photoresponsivity can be significantly enhanced to ∼9 × 10(4) A W(-1) by applying a source-drain bias (VSD) of 3 V, which is the highest ever measured in any 2D material and 10(7) times higher than the previously reported value for black phosphorus. We attribute such a colossal UV photoresponsivity to the resonant-interband transition between two specially nested valence and conduction bands. These nested bands provide an unusually high density of states for highly efficient UV absorption due to the singularity of their nature.

Ultrathin organic solar cells with graphene doped by ferroelectric polarization.

Graphene has been employed as transparent electrodes in organic solar cells (OSCs) because of its good physical and optical properties. However, the electrical conductivity of graphene films synthesized by chemical vapor deposition (CVD) is still inferior to that of conventional indium tin oxide (ITO) electrodes of comparable transparency, resulting in a lower performance of OSCs. Here, we report an effective method to improve the performance and long-term stability of graphene-based OSCs using electrostatically doped graphene films via a ferroelectric polymer. The sheet resistance of electrostatically doped few layer graphene films was reduced to ∼70 Ω/sq at 87% optical transmittance. Such graphene-based OSCs exhibit an efficiency of 2.07% with a superior stability when compared to chemically doped graphene-based OSCs. Furthermore, OSCs constructed on ultrathin ferroelectric film as a substrate of only a few micrometers show extremely good mechanical flexibility and durability and can be rolled up into a cylinder with 7 mm diameter.

Tuning optical conductivity of large-scale CVD graphene by strain engineering.

A controllable optical anisotropy in CVD graphene is shown. The transparency in the visible range of pre-strained CVD graphene exhibits a periodic modulation as a function of polarization direction. The strain sensitivity of the optical response of graphene demonstrated here can be effectively utilized towards novel ultra-thin optical devices and strain sensing applications.

Unconventional transport through graphene on SrTiO3: a plausible effect of SrTiO3 phase-transitions.

High-k dielectric oxides are supposedly ideal gate-materials for ultra-high doping in graphene and other 2D-crystals. Here, we report a temperature-dependent electronic transport study on chemical vapor deposited-graphene gated with SrTiO3 (STO) thin film substrate. At carrier densities away from charge neutrality point the temperature-dependent resistivity of our graphene samples on both STO and SiO2/Si substrates show metallic behavior with contributions from Coulomb scattering and flexural phonons attributable to the presence of characteristic quasi-periodic nano-ripple arrays. Significantly, for graphene samples on STO substrates we observe an anomalous 'slope-break' in the temperature-dependent resistivity for T = 50 to 100 K accompanied by a decrease in mobility above 30 K. Furthermore, we observe an unusual decrease in the gate-induced doping-rate at low temperatures, despite an increase in dielectric constant of the substrate. We believe that a complex mechanism is at play as a consequence of the structural phase transition of the underlying substrate showing an anomalous transport behavior in graphene on STO. The anomalies are discussed in the context of Coulomb as well as phonon scattering.

Controlled hydrogenation of graphene sheets and nanoribbons.

The electronic properties of graphene sheets and nanoribbons with different degrees of hydrogenation have been investigated using a combination of charge transport and Raman spectroscopy experiments. The field-effect transistor mobility of graphene is shown to be highly sensitive to the treatment time during atomic hydrogen dose and follows an exponential decrease with time. Raman spectroscopy demonstrates linearly increasing defect-band intensity, and when considered together with transport data, the relationship between graphene mobility and the crystalline size of intact sp(2) carbon regions can be derived. Further, the increase in width of the voltage plateau for monolayer and bilayer graphene points to the formation of midgap states. For partially hydrogenated graphene, the temperature-dependent transport in these states shows a weak insulating behavior. A comparison of Raman spectrum and conductivity data of partially hydrogenated monolayer and bilayer graphene suggests that the latter is also quite susceptible to adsorption of hydrogen atoms, despite a stiffer lattice structure.