High-Mobility and High-Optical Quality Atomically Thin WS 2.

The rise of atomically thin materials has the potential to enable a paradigm shift in modern technologies by introducing multi-functional materials in the semiconductor industry. To date the growth of high quality atomically thin semiconductors (e.g. WS2) is one of the most pressing challenges to unleash the potential of these materials and the growth of mono- or bi-layers with high crystal quality is yet to see its full realization. Here, we show that the novel use of molecular precursors in the controlled synthesis of mono- and bi-layer WS2 leads to superior material quality compared to the widely used direct sulfidization of WO3-based precursors. Record high room temperature charge carrier mobility up to 52 cm2/Vs and ultra-sharp photoluminescence linewidth of just 36 meV over submillimeter areas demonstrate that the quality of this material supersedes also that of naturally occurring materials. By exploiting surface diffusion kinetics of W and S species adsorbed onto a substrate, a deterministic layer thickness control has also been achieved promoting the design of scalable synthesis routes.

Highly Efficient Rubrene-Graphene Charge-Transfer Interfaces as Phototransistors in the Visible Regime.

Atomically thin materials such as graphene are uniquely responsive to charge transfer from adjacent materials, making them ideal charge-transport layers in phototransistor devices. Effective implementation of organic semiconductors as a photoactive layer would open up a multitude of applications in biomimetic circuitry and ultra-broadband imaging but polycrystalline and amorphous thin films have shown inferior performance compared to inorganic semiconductors. Here, the long-range order in rubrene single crystals is utilized to engineer organic-semiconductor-graphene phototransistors surpassing previously reported photogating efficiencies by one order of magnitude. Phototransistors based upon these interfaces are spectrally selective to visible wavelengths and, through photoconductive gain mechanisms, achieve responsivity as large as 107 A W-1 and a detectivity of 9 × 1011 Jones at room temperature. These findings point toward implementing low-cost, flexible materials for amplified imaging at ultralow light levels.

Extraordinary linear dynamic range in laser-defined functionalized graphene photodetectors.

Graphene-based photodetectors have demonstrated mechanical flexibility, large operating bandwidth, and broadband spectral response. However, their linear dynamic range (LDR) is limited by graphene's intrinsic hot-carrier dynamics, which causes deviation from a linear photoresponse at low incident powers. At the same time, multiplication of hot carriers causes the photoactive region to be smeared over distances of a few micrometers, limiting the use of graphene in high-resolution applications. We present a novel method for engineering photoactive junctions in FeCl3-intercalated graphene using laser irradiation. Photocurrent measured at these planar junctions shows an extraordinary linear response with an LDR value at least 4500 times larger than that of other graphene devices (44 dB) while maintaining high stability against environmental contamination without the need for encapsulation. The observed photoresponse is purely photovoltaic, demonstrating complete quenching of hot-carrier effects. These results pave the way toward the design of ultrathin photodetectors with unprecedented LDR for high-definition imaging and sensing.

An integrated and multi-purpose microscope for the characterization of atomically thin optoelectronic devices.

Optoelectronic devices based on graphene and other two-dimensional (2D) materials, such as transition metal dichalcogenides (TMDs), are the focus of wide research interest. They can be the key to improving bandwidths in telecommunications, capacity in data storage, and new features in consumer electronics, safety devices, and medical equipment. The characterization of these emerging atomically thin materials and devices strongly relies on a set of measurements involving both optical and electronic instrumentation ranging from scanning photocurrent mapping to Raman and photoluminescence (PL) spectroscopy. Furthermore, proof-of-concept devices are usually fabricated from micro-meter size flakes, requiring microscopy techniques to characterize them. Current state-of-the-art commercial instruments offer the ability to characterize individual properties of these materials with no option for the in situ characterization of a wide enough range of complementary optical and electrical properties. Presently, the requirement to switch atomically thin materials from one system to another often radically affects the properties of these uniquely sensitive materials through atmospheric contamination. Here, we present an integrated, multi-purpose instrument dedicated to the optical and electrical characterization of devices based on 2D materials which is able to perform low frequency electrical measurements, scanning photocurrent mapping, and Raman, absorption, and PL spectroscopy in one single setup with full control over the polarization and wavelength of light. We characterize this apparatus by performing multiple measurements on graphene, transition metal dichalcogenides (TMDs), and Si. The performance and resolution of each individual measurement technique is found to be equivalent to that of commercially available instruments. Contrary to nowadays' commercial systems, a significant advantage of the developed instrument is that for the first time the integration of a wide range of complementary optoelectronic and spectroscopy characterization techniques is demonstrated in a single compact unit. Our design offers a versatile solution to face the challenges imposed by the advent of atomically thin materials in optoelectronic devices.

Fast and Highly Sensitive Ionic-Polymer-Gated WS2 -Graphene Photodetectors.

The combination of graphene with semiconductor materials in heterostructure photodetectors enables amplified detection of femtowatt light signals using micrometer-scale electronic devices. Presently, long-lived charge traps limit the speed of such detectors, and impractical strategies, e.g., the use of large gate-voltage pulses, have been employed to achieve bandwidths suitable for applications such as video-frame-rate imaging. Here, atomically thin graphene-WS2 heterostructure photodetectors encapsulated in an ionic polymer are reported, which are uniquely able to operate at bandwidths up to 1.5 kHz whilst maintaining internal gain as large as 106 . Highly mobile ions and the nanometer-scale Debye length of the ionic polymer are used to screen charge traps and tune the Fermi level of the graphene over an unprecedented range at the interface with WS2 . Responsivity R = 106 A W-1 and detectivity D* = 3.8 × 1011 Jones are observed, approaching that of single-photon counters. The combination of both high responsivity and fast response times makes these photodetectors suitable for video-frame-rate imaging applications.

Homogeneously Bright, Flexible, and Foldable Lighting Devices with Functionalized Graphene Electrodes.

Alternating current electroluminescent technology allows the fabrication of large area, flat and flexible lights. Presently the maximum size of a continuous panel is limited by the high resistivity of available transparent electrode materials causing a visible gradient of brightness. Here, we demonstrate that the use of the best known transparent conductor FeCl3-intercalated few-layer graphene boosts the brightness of electroluminescent devices by 49% compared to pristine graphene. Intensity gradients observed for high aspect ratio devices are undetectable when using these highly conductive electrodes. Flat lights on polymer substrates are found to be resilient to repeated and flexural strains.

Correction: Functional modulation and directed assembly of an enzyme through designed non-natural post-translation modification.

[This corrects the article DOI: 10.1039/C4SC03900A.].

Large-area functionalized CVD graphene for work function matched transparent electrodes.

The efficiency of flexible photovoltaic and organic light emitting devices is heavily dependent on the availability of flexible and transparent conductors with at least a similar workfunction to that of Indium Tin Oxide. Here we present the first study of the work function of large area (up to 9 cm(2)) FeCl3 intercalated graphene grown by chemical vapour deposition on Nickel, and demonstrate values as large as 5.1 eV. Upon intercalation, a charge density per graphene layer of 5 ⋅ 10(13) ± 5 ⋅ 10(12) cm(-2) is attained, making this material an attractive platform for the study of plasmonic excitations in the infrared wavelength spectrum of interest to the telecommunication industry. Finally, we demonstrate the potential of this material for flexible electronics in a transparent circuit on a polyethylene naphthalate substrate.

Functional modulation and directed assembly of an enzyme through designed non-natural post-translation modification.

Post-translational modification (PTM) modulates and supplements protein functionality. In nature this high precision event requires specific motifs and/or associated modification machinery. To overcome the inherent complexity that hinders PTM's wider use, we have utilized a non-native biocompatible Click chemistry approach to site-specifically modify TEM ß-lactamase that adds new functionality. In silico modelling was used to design TEM ß-lactamase variants with the non-natural amino acid p-azido-l-phenylalanine (azF) placed at functionally strategic positions permitting residue-specific modification with alkyne adducts by exploiting strain-promoted azide-alkyne cycloaddition. Three designs were implemented so that the modification would: (i) inhibit TEM activity (Y105azF); (ii) restore activity compromised by the initial mutation (P174azF); (iii) facilitate assembly on pristine graphene (W165azF). A dibenzylcyclooctyne (DBCO) with amine functionality was enough to modulate enzymatic activity. Modification of TEMW165azF with a DBCO-pyrene adduct had little effect on activity despite the modification site being close to a key catalytic residue but allowed directed assembly of the enzyme on graphene, potentially facilitating the construction of protein-gated carbon transistor systems.