The discovery of graphene has ignited intensive interest in two-dimensional layered materials (2DLMs). These 2DLMs represent a new class of nearly ideal 2D material systems for exploring fundamental chemistry and physics at the limit of single-atom thickness, and have the potential to open up totally new technological opportunities beyond the reach of existing materials. In general, there are a wide range of 2DLMs in which the atomic layers are weakly bonded together by van der Waals interactions and can be isolated into single or few-layer nanosheets. The van der Waals interactions between neighboring atomic layers could allow much more flexible integration of distinct materials to nearly arbitrarily combine and control different properties at the atomic scale. The transition metal dichalcogenides (TMDs) (e.g., MoS2, WSe2) represent a large family of layered materials, many of which exhibit tunable band gaps that can undergo a transition from an indirect band gap in bulk crystals to a direct band gap in monolayer nanosheets. These 2D-TMDs have thus emerged as an exciting class of atomically thin semiconductors for a new generation of electronic and optoelectronic devices. Recent studies have shown exciting potential of these atomically thin semiconductors, including the demonstration of atomically thin transistors, a new design of vertical transistors, as well as new types of optoelectronic devices such as tunable photovoltaic devices and light emitting devices. In parallel, there have also been considerable efforts in developing diverse synthetic approaches for the rational growth of various forms of 2D materials with precisely controlled chemical composition, physical dimension, and heterostructure interface. Here we review the recent efforts, progress, opportunities and challenges in exploring the layered TMDs as a new class of atomically thin semiconductors.

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have recently emerged as a new class of atomically thin semiconductors for diverse electronic, optoelectronic, and valleytronic applications. To explore the full potential of these 2D semiconductors requires a precise control of their band gap and electronic properties, which represents a significant challenge in 2D material systems. Here we demonstrate a systematic control of the electronic properties of 2D-TMDs by creating mixed alloys of the intrinsically p-type WSe2 and intrinsically n-type WS2 with variable alloy compositions. We show that a series of WS2xSe2-2x alloy nanosheets can be synthesized with fully tunable chemical compositions and optical properties. Electrical transport studies using back-gated field effect transistors demonstrate that charge carrier types and threshold voltages of the alloy nanosheet transistors can be systematically tuned by adjusting the alloy composition. A highly p-type behavior is observed in selenium-rich alloy, which gradually shifts to lightly p-type, and then switches to lightly n-type characteristics with the increasing sulfur atomic ratio, and eventually evolves into highly n-doped semiconductors in sulfur-rich alloys. The synthesis of WS2xSe2-2x nanosheets with tunable optical and electronic properties represents a critical step toward rational design of 2D electronics with tailored spectral responses and device characteristics.

All systems GO! An intracellular protease sensor is based on the covalent conjugate of graphene oxide and peptide substrates with fluorophore labels. The conjugate can be delivered into live cells and provides specific, high‐contrast imaging of caspase‐3 activation (see picture; orange=cell penetration peptide, blue/black=caspase‐3 peptide probe).

The design and synthesis of a novel rhodamine spirolactam derivative and its application in fluorescent detections of Cu(2+) in aqueous solution and living cells are reported. The signal change of the chemosensor is based on a specific metal ion induced reversible ring-opening mechanism of the rhodamine spirolactam. It exhibits a highly sensitive "turn-on" fluorescent response toward Cu(2+) in aqueous solution with an 80-fold fluorescence intensity enhancement under 10 equiv of Cu(2+) added. This indicates that the synthesized chemosensor effectively avoided the fluorescence quenching for the paramagnetic nature of Cu(2+) via its strong binding capability toward Cu(2+). With the experimental conditions optimized, the probe exhibits a dynamic response range for Cu(2+) from 8.0 x 10(-7) to 1.0 x 10(-5) M, with a detection limit of 3.0 x 10(-7) M. The response of the chemosensor for Cu(2+) is instantaneous and reversible. Most importantly, both the color and fluorescence changes of the chemosensor are remarkably specific for Cu(2+) in the presence of other heavy and transition metal ions (even those that exist in high concentration), which meet the selective requirements for biomedical and environmental monitoring application. The proposed chemosensor has been used for direct measurement of Cu(2+) content in river water samples and imaging of Cu(2+) in living cells with satisfying results, which further demonstrates its value of practical applications in environmental and biological systems.

On the basis of the remarkable difference in affinity of graphene (GO) with ssDNA containing a different number of bases in length, we for the first time report a GO-DNAzyme based biosensor for amplified fluorescence "turn-on" detection of Pb(2+). A FAM-labeled DNAzyme-substrate hybrid acted as both a molecular recognition module and signal reporter and GO as a superquencher. By taking advantage of the super fluorescence quenching efficiency of GO, our proposed biosensor exhibits a high sensitivity toward the target with a detection limit of 300 pM for Pb(2+), which is lower than previously reported for catalytic beacons. Moreover, with the choice of a classic Pb(2+)-dependent GR-5 DNAzyme instead of 8-17 DNAzyme as the catalytic unit, the newly designed sensing system also shows an obviously improved selectivity than previously reported methods. Moreover, the sensing system was used for the determination of Pb(2+) in river water samples with satisfying results.

Messenger RNA (mRNA) is, by its nature, transient, beginning with transcription and ending with degradation, but with a period of processing and transport in between. As such, the spatiotemporal dynamics of specific mRNA molecules are difficult to image and detect inside living cells, and this has been a significant challenge for the chemical and biomedical communities. To solve this problem, we have developed a targeted, self-delivered, and photocontrolled aptamer-based molecular beacon (MB) for intracellular mRNA analysis. An internalizing aptamer connected via a double-stranded DNA structure is used as a carrier probe (CP) for cell-specific delivery of the MB designed to signal target mRNA. A light activation strategy was employed by inserting two photolabile groups in the CP sequence, enabling control over the MB's intracellular function. After being guided to their target cells via specific binding of aptamer AS1411 to nucleolin on the cell membrane, light illumination releases the MB for mRNA monitoring. Consequently, the MB is able to perform live-cell mRNA imaging with precise spatiotemporal control, while the CP acts as both a tracer for intracellular distribution of the MB before photoinitiation, and an internal reference for mRNA ratiometric detection.

Blood glucose monitoring has attracted extensive attention because diabetes mellitus is a worldwide public health problem. Here, we reported an upconversion fluorescence detection method based on manganese dioxide (MnO2)-nanosheet-modified upconversion nanoparticles (UCNPs) for rapid, sensitive detection of glucose levels in human serum and whole blood. In this strategy, MnO2 nanosheets on the UCNP surface serve as a quencher. UCNP fluorescence can make a recovery by the addition of H2O2, which can reduce MnO2 to Mn(2+), and the glucose can thus be monitored based on the enzymatic conversion of glucose by glucose oxidase to generate H2O2. Because of the nonautofluorescent assays offered by UCNPs, the developed method has been applied to monitor glucose levels in human serum and whole blood samples with satisfactory results. The proposed approach holds great potential for diabetes mellitus research and clinical diagnosis. Meanwhile, this nanosystem is also generalizable and can be easily expanded to the detection of various H2O2-involved analytes.

Cell membrane-anchored biochemical sensors that allow real-time monitoring of the interactions of cells with their microenvironment would be powerful tools for studying the mechanisms underlying various biological processes, such as cell metabolism and signaling. Despite the significance of these techniques, unfortunately, their development has lagged far behind due to the lack of a desirable membrane engineering method. Here, we propose a simple, efficient, biocompatible, and universal strategy for one-step self-construction of cell-surface sensors using diacyllipid-DNA conjugates as the building and sensing elements. The sensors exploit the high membrane-insertion capacity of a diacyllipid tail and good sensing performance of the DNA probes. Based on this strategy, we have engineered specific DNAzymes on the cell membrane for metal ion assay in the extracellular microspace. The immobilized DNAzyme showed excellent performance for reporting and semiquantifying both exogenous and cell-extruded target metal ions in real time. This membrane-anchored sensor could also be used for multiple target detection by having different DNA probes inserted, providing potentially useful tools for versatile applications in cell biology, biomedical research, drug discovery, and tissue engineering.