We present the science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems, targeting an evolution in technology, that might lead to impacts and benefits reaching into most areas of society. This roadmap was developed within the framework of the European Graphene Flagship and outlines the main targets and research areas as best understood at the start of this ambitious project. We provide an overview of the key aspects of graphene and related materials (GRMs), ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries. We also define an extensive list of acronyms in an effort to standardize the nomenclature in this emerging field.

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Science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems

Two rich and vibrant fields of investigation, graphene physics and plasmonics, strongly overlap Not only does graphene possess intrinsic plasmons that are tunable and adjustable, but a combination of graphene with noble-metal nanostructures promises a variety of exciting applications for conventional plasmonics The versatility of graphene means that graphene-based plasmonics may enable the manufacture of novel optical devices working in different frequency ranges, from terahertz to the visible, with extremely high speed, low driving voltage, low power consumption and compact sizes Here we review the field emerging at the intersection of graphene physics and plasmonics

Graphene plasmonics

The stability of two-dimensional (2D) layers and membranes is subject of a long standing theoretical debate. According to the so called Mermin-Wagner theorem, long wavelength fluctuations destroy the long-range order for 2D crystals. Similarly, 2D membranes embedded in a 3D space have a tendency to be crumpled. These dangerous fluctuations can, however, be suppressed by anharmonic coupling between bending and stretching modes making that a two-dimensional membrane can exist but should present strong height fluctuations. The discovery of graphene, the first truly 2D crystal and the recent experimental observation of ripples in freely hanging graphene makes these issues especially important. Beside the academic interest, understanding the mechanisms of stability of graphene is crucial for understanding electronic transport in this material that is attracting so much interest for its unusual Dirac spectrum and electronic properties. Here we address the nature of these height fluctuations by means of straightforward atomistic Monte Carlo simulations based on a very accurate many-body interatomic potential for carbon. We find that ripples spontaneously appear due to thermal fluctuations with a size distribution peaked around 70 \AA which is compatible with experimental findings (50-100 \AA) but not with the current understanding of stability of flexible membranes. This unexpected result seems to be due to the multiplicity of chemical bonding in carbon.

Intrinsic ripples in graphene

Controlling the bandstructure through local-strain engineering is an exciting avenue for tailoring optoelectronic properties of materials at the nanoscale. Atomically thin materials are particularly well-suited for this purpose because they can withstand extreme nonhomogeneous deformations before rupture. Here, we study the effect of large localized strain in the electronic bandstructure of atomically thin MoS2. Using photoluminescence imaging, we observe a strain-induced reduction of the direct bandgap and funneling of photogenerated excitons toward regions of higher strain. To understand these results, we develop a nonuniform tight-binding model to calculate the electronic properties of MoS2 nanolayers with complex and realistic local strain geometries, finding good agreement with our experimental results.

https://digital.csic.es/bitstream/10261/94671/1/Local%20strain.pdf

Local strain engineering in atomically thin MoS2.

We review the problem of electron-electron interactions in graphene. Starting from the screening of long range interactions in these systems, we discuss the existence of an emerging Dirac liquid of Lorentz invariant quasi-particles in the weak coupling regime, and strongly correlated electronic states in the strong coupling regime. We also analyze the analogy and connections between the many-body problem and the Coulomb impurity problem. The problem of the magnetic instability and Kondo effect of impurities and/or adatoms in graphene is also discussed in analogy with classical models of many-body effects in ordinary metals. We show that Lorentz invariance plays a fundamental role and leads to effects that span the whole spectrum, from the ultraviolet to the infrared. The effect of an emerging Lorentz invariance is also discussed in the context of finite size and edge effects as well as mesoscopic physics. We also briefly discuss the effects of strong magnetic fields in single layers and review some of the main aspects of the many-body problem in graphene bilayers. In addition to reviewing the fully understood aspects of the many-body problem in graphene, we show that a plethora of interesting issues remain open, both theoretically and experimentally, and that the field of graphene research is still exciting and vibrant.

Electron-Electron Interactions in Graphene: Current Status and Perspectives

Recent theoretical proposals suggest that strain can be used to engineer graphene electronic states through the creation of a pseudo-magnetic field. This effect is unique to graphene because of its massless Dirac fermion-like band structure and particular lattice symmetry (C3v). Here, we present experimental spectroscopic measurements by scanning tunneling microscopy of highly strained nanobubbles that form when graphene is grown on a platinum (111) surface. The nanobubbles exhibit Landau levels that form in the presence of strain-induced pseudo-magnetic fields greater than 300 tesla. This demonstration of enormous pseudo-magnetic fields opens the door to both the study of charge carriers in previously inaccessible high magnetic field regimes and deliberate mechanical control over electronic structure in graphene or so-called "strain engineering."

https://science.sciencemag.org/content/sci/329/5991/544.full.pdf

Strain-Induced Pseudo–Magnetic Fields Greater Than 300 Tesla in Graphene Nanobubbles

Gate-controlled tuning of the charge carrier density in graphene devices provides new opportunities to control the behavior of molecular adsorbates. We have used scanning tunneling microscopy (STM) and spectroscopy (STS) to show how the vibronic electronic levels of 1,3,5-tris(2,2-dicyanovinyl)benzene molecules adsorbed onto a graphene/BN/SiO2 device can be tuned via application of a backgate voltage. The molecules are observed to electronically decouple from the graphene layer, giving rise to well-resolved vibronic states in dI/dV spectroscopy at the single-molecule level. Density functional theory (DFT) and many-body spectral function calculations show that these states arise from molecular orbitals coupled strongly to carbon–hydrogen rocking modes. Application of a back-gate voltage allows switching between different electronic states of the molecules for fixed sample bias.

/pdf/imaging-and-tuning-molecular-levels-at-the-surface-of-a-251irndnfn.pdf

Imaging and tuning molecular levels at the surface of a gated graphene device.

A monolayer 2D capping layer with high Young's modulus is shown to be able to effectively suppress the dewetting of underlying thin films of small organic semiconductor molecule, polymer, and polycrystalline metal, respectively. To verify the universality of this capping layer approach, the dewetting experiments are performed for single-layer graphene transferred onto polystyrene (PS), semiconducting thienoazacoronene (EH-TAC), gold, and also MoS2 on PS. Thermodynamic modeling indicates that the exceptionally high Young's modulus and surface conformity of 2D capping layers such as graphene and MoS2 substantially suppress surface fluctuations and thus dewetting. As long as the uncovered area is smaller than the fluctuation wavelength of the thin film in a dewetting process via spinodal decomposition, the dewetting should be suppressed. The 2D monolayer-capping approach opens up exciting new possibilities to enhance the thermal stability and expands the processing parameters for thin film materials without significantly altering their physical properties.

Preventing Thin Film Dewetting via Graphene Capping.

http://absimage.aps.org/image/MAR14/MWS_MAR14-2013-004691.pdf

Kacey Meaker

Papers

Strain-Induced Pseudo–Magnetic Fields Greater Than 300 Tesla in Graphene Nanobubbles

Imaging and tuning molecular levels at the surface of a gated graphene device.

Preventing Thin Film Dewetting via Graphene Capping.

Graphene Calisthenics: Straintronics of Graphene with Light-Reactive Azobenzene Polymer