Graphene’s success has shown that it is possible to create stable, single and few-atom-thick layers of van der Waals materials, and also that these materials can exhibit fascinating and technologically useful properties. Here we review the state-of-the-art of 2D materials beyond graphene. Initially, we will outline the different chemical classes of 2D materials and discuss the various strategies to prepare single-layer, few-layer, and multilayer assembly materials in solution, on substrates, and on the wafer scale. Additionally, we present an experimental guide for identifying and characterizing single-layer-thick materials, as well as outlining emerging techniques that yield both local and global information. We describe the differences that occur in the electronic structure between the bulk and the single layer and discuss various methods of tuning their electronic properties by manipulating the surface. Finally, we highlight the properties and advantages of single-, few-, and many-layer 2D materials in...

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Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene

Graphene-Like Two-Dimensional Materials

Circularly polarized light has been used to confine charge carriers in single-layer molybdenum disulphide entirely to a single energy-band valley, representing full valley polarization.

Control of valley polarization in monolayer MoS2 by optical helicity

A two-dimensional crystal of molybdenum disulfide (MoS2) monolayer is a photoluminescent direct gap semiconductor in striking contrast to its bulk counterpart. Exfoliation of bulk MoS2 via Li intercalation is an attractive route to large-scale synthesis of monolayer crystals. However, this method results in loss of pristine semiconducting properties of MoS2 due to structural changes that occur during Li intercalation. Here, we report structural and electronic properties of chemically exfoliated MoS2. The metastable metallic phase that emerges from Li intercalation was found to dominate the properties of as-exfoliated material, but mild annealing leads to gradual restoration of the semiconducting phase. Above an annealing temperature of 300 °C, chemically exfoliated MoS2 exhibit prominent band gap photoluminescence, similar to mechanically exfoliated monolayers, indicating that their semiconducting properties are largely restored.

Photoluminescence from Chemically Exfoliated MoS2

Most electronic devices exploit the electric charge of electrons, but it is also possible to build devices that rely on other properties of electrons. Spintronic devices, for example, make use of the spin of electrons. Valleytronics is a more recent development that relies on the fact that the conduction bands of some materials have two or more minima at equal energies but at different positions in momentum space. To make a valleytronic device it is necessary to control the number of electrons in these valleys, thereby producing a valley polarization. Single-layer MoS(2) is a promising material for valleytronics because both the conduction and valence band edges have two energy-degenerate valleys at the corners of the first Brillouin zone. Here, we demonstrate that optical pumping with circularly polarized light can achieve a valley polarization of 30% in pristine monolayer MoS(2). Our results, and similar results by Mak et al., demonstrate the viability of optical valley control and valley-based electronic and optoelectronic applications in MoS(2) monolayers.

Valley polarization in MoS2 monolayers by optical pumping

The band structure of MoS2 strongly depends on the number of layers, and a transition from indirect to direct-gap semiconductor has been observed recently for a single layer of MoS2. Single-layer MoS2 therefore becomes an efficient emitter of photoluminescence even at room temperature. Here, we report on scanning Raman and on temperature-dependent, as well as time-resolved photoluminescence measurements on single-layer MoS2 flakes prepared by exfoliation. We observe the emergence of two distinct photoluminescence peaks at low temperatures. The photocarrier recombination at low temperatures occurs on the few-picosecond timescale, but with increasing temperatures, a biexponential photoluminescence decay with a longer-lived component is observed.

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Low-temperature photocarrier dynamics in monolayer MoS2

Single- and few-layer MoS2 has recently gained attention as an interesting new material system for opto-electronics. Here, we report on scanning Raman measurements on few-layer MoS2 flakes prepared by exfoliation. We observe a Raman mode corresponding to a rigid shearing oscillation of adjacent layers. This mode appears at very low Raman shifts between 20 and 30 relative wavenumbers. Its position strongly depends on the number of layers, which we independently determine using AFM measurements and investigation of the other characteristic Raman modes. Raman spectroscopy of the shear mode therefore is a useful tool to determine the number of layers for few-layer MoS2 flakes.

Raman spectroscopy of the interlayer shear mode in few-layer MoS2 flakes

Single- and few-layer MoS2 has recently gained attention as an interesting material system for opto-electronics. Here, we report on scanning Raman measurements on few-layer MoS2 flakes prepared by exfoliation. We observe a Raman mode corresponding to a rigid shearing oscillation of adjacent layers. This mode appears at very low Raman shifts between 20 and 30 cm−1. Its position strongly depends on the number of layers, which we independently determine using atomic force microscopy and investigation of the other characteristic Raman modes. Raman spectroscopy of the shear mode, therefore, is a useful tool to determine the number of layers for few-layer MoS2 flakes.

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We have investigated antidot lattices, which were prepared on exfoliated graphene single layers via electron-beam lithography and ion etching, by means of scanning Raman spectroscopy. The peak positions, peak widths and intensities of the characteristic phonon modes of the carbon lattice have been studied systematically in a series of samples. In the patterned samples, we found a systematic stiffening of the G band mode, accompanied by a line narrowing, while the 2D mode energies are found to be linearly correlated with the G mode energies. We interpret this as evidence for p-type doping of the nanostructured graphene.

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Scanning Raman spectroscopy of graphene antidot lattices: Evidence for systematic p-type doping

We have investigated antidot lattices, which were prepared on exfoliated graphene single layers via electron-beam lithography and ion etching, by means of scanning Raman spectroscopy. The peak positions, peak widths, and intensities of the characteristic phonon modes of the carbon lattice have been studied systematically in a series of samples. In the patterned samples, we found a systematic stiffening of the G band phonon mode, accompanied by a line narrowing, while the 2D two-phonon mode energies are found to be linearly correlated with the G mode energies. We interpret this as evidence for p-type doping of the nanostructured graphene.

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Stefanie Heydrich

Papers

Low-temperature photocarrier dynamics in monolayer MoS2

Raman spectroscopy of the interlayer shear mode in few-layer MoS2 flakes

Raman spectroscopy of the interlayer shear mode in few-layer MoS2 flakes

Scanning Raman spectroscopy of graphene antidot lattices: Evidence for systematic p-type doping

Scanning Raman spectroscopy of graphene antidot lattices: Evidence for systematic p-type doping