Plasmons describe collective oscillations of electrons. They have a fundamental role in the dynamic responses of electron systems and form the basis of research into optical metamaterials. Plasmons of two-dimensional massless electrons, as present in graphene, show unusual behaviour that enables new tunable plasmonic metamaterials and, potentially, optoelectronic applications in the terahertz frequency range. Here we explore plasmon excitations in engineered graphene micro-ribbon arrays. We demonstrate that graphene plasmon resonances can be tuned over a broad terahertz frequency range by changing micro-ribbon width and in situ electrostatic doping. The ribbon width and carrier doping dependences of graphene plasmon frequency demonstrate power-law behaviour characteristic of two-dimensional massless Dirac electrons. The plasmon resonances have remarkably large oscillator strengths, resulting in prominent room-temperature optical absorption peaks. In comparison, plasmon absorption in a conventional two-dimensional electron gas was observed only at 4.2 K (refs 13, 14). The results represent a first look at light-plasmon coupling in graphene and point to potential graphene-based terahertz metamaterials.

Significance A new class of heterostructures consisting of layered transition metal dichalcogenide components can be designed and built by van der Waals (vdW) stacking of individual monolayers into functional multilayer structures. Nonetheless, the optoelectronic properties of this new type of vdW heterostructure are unknown. Here, we investigate artificial semiconductor heterostructures built from single-layer WSe 2 and MoS 2 . We observe spatially direct absorption but spatially indirect emission in this heterostructure, with strong interlayer coupling of charge carriers. The coupling at the hetero-interface can be readily tuned by inserting hexagonal BN dielectric layers into the vdW gap. The generic nature of this interlayer coupling is expected to yield a new family of semiconductor heterostructures having tunable optoelectronic properties through customized composite layers.

Electron valley, a degree of freedom that is analogous to spin, can lead to novel topological phases in bilayer graphene. A tunable bandgap can be induced in bilayer graphene by an external electric field, and such gapped bilayer graphene is predicted to be a topological insulating phase protected by no-valley mixing symmetry, featuring quantum valley Hall effects and chiral edge states. Observation of such chiral edge states, however, is challenging because inter-valley scattering is induced by atomic-scale defects at real bilayer graphene edges. Recent theoretical work has shown that domain walls between AB- and BA-stacked bilayer graphene can support protected chiral edge states of quantum valley Hall insulators. Here we report an experimental observation of ballistic (that is, with no scattering of electrons) conducting channels at bilayer graphene domain walls. We employ near-field infrared nanometre-scale microscopy (nanoscopy) to image in situ bilayer graphene layer-stacking domain walls on device substrates, and we fabricate dual-gated field effect transistors based on the domain walls. Unlike single-domain bilayer graphene, which shows gapped insulating behaviour under a vertical electrical field, bilayer graphene domain walls feature one-dimensional valley-polarized conducting channels with a ballistic length of about 400 nanometres at 4 kelvin. Such topologically protected one-dimensional chiral states at bilayer graphene domain walls open up opportunities for exploring unique topological phases and valley physics in graphene.

Electrons moving in graphene behave as massless Dirac fermions, and they exhibit fascinating low-frequency electrical transport phenomena. Their dynamic response, however, is little known at frequencies above one terahertz (THz). Such knowledge is important not only for a deeper understanding of the Dirac electron quantum transport, but also for graphene applications in ultrahigh speed THz electronics and IR optoelectronics. In this paper, we report the first measurement of high-frequency conductivity of graphene from THz to mid-IR at different carrier concentrations. The conductivity exhibits Drude-like frequency dependence and increases dramatically at THz frequencies, but its absolute strength is substantially lower than theoretical predictions. This anomalous reduction of free electron oscillator strength is corroborated by corresponding changes in graphene interband transitions, as required by the sum rule.Our surprising observation indicates that many-body effects and Dirac fermion-impurity interactions beyond current transport theories are important for Dirac fermion electrical response in graphene.

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Characterizing and ultimately controlling the heterogeneity underlying biomolecular functions, quantum behavior of complex matter, photonic materials, or catalysis requires large-scale spectroscopic imaging with simultaneous specificity to structure, phase, and chemical composition at nanometer spatial resolution. However, as with any ultrahigh spatial resolution microscopy technique, the associated demand for an increase in both spatial and spectral bandwidth often leads to a decrease in desired sensitivity. We overcome this limitation in infrared vibrational scattering-scanning probe near-field optical microscopy using synchrotron midinfrared radiation. Tip-enhanced localized light-matter interaction is induced by low-noise, broadband, and spatially coherent synchrotron light of high spectral irradiance, and the near-field signal is sensitively detected using heterodyne interferometric amplification. We achieve sub-40-nm spatially resolved, molecular, and phonon vibrational spectroscopic imaging, with rapid spectral acquisition, spanning the full midinfrared (700-5,000 cm) with few cm −1 spectral resolution. We demonstrate the performance of synchrotron infrared nanospectroscopy on semiconductor, biomineral, and protein nanostructures, providing vibrational chemical imaging with subzeptomole sensitivity.any properties and functions of natural or synthetic materials are defined by chemically or structurally distinct phases, domains, or interfaces on length scales of a few nanometers to micrometers. Characterizing these heterogeneities has long driven the development of advanced microscopy techniques, with notable advances in electron (1), photoemission (2), X-ray (3), and superresolution (4) microscopies. Although extremely effective, these techniques have strict sample requirements: either they operate in vacuum, are limited by electron or X-ray beam damage, or rely on labeling with exogenous fluorophores.In contrast, infrared (IR) vibrational spectroscopic imaging is minimally invasive, requires little sample preparation, is applicable in situ and under ambient conditions, and provides intrinsic chemical contrast and spectroscopic identification for a wide range of materials (5), including living cells (6) and tissues (7,8). The spatial resolution, however, is diffraction-limited to 2-10 μm, depending on wavelength. Moreover, high signal-to-noise spectra even at this low resolution are only possible with a source of high spectral irradiance (9). Subwavelength imaging has been achieved to some extent through point-spread function deconvolution (10, 11) and attenuated total reflection techniques (12). However, the micrometer-size wavelength of IR radiation, in general, has fundamentally limited its application for the characterization of essentially any mesoscopic, heterogeneous material where chemical information at the nanoscale is desired.Infrared scattering-scanning near-field microscopy (IR s-SNOM) overcomes the diffraction limit by scattering incident light with the typically metallic tip of an atomic for...

The critical role in surface reactions and heterogeneous catalysis of metal atoms with low coordination numbers, such as found at atomic steps and surface defects, is firmly established. But despite the growing availability of tools that enable detailed in situ characterization, so far it has not been possible to document this role directly. Surface properties can be mapped with high spatial resolution, and catalytic conversion can be tracked with a clear chemical signature; however, the combination of the two, which would enable high-spatial-resolution detection of reactions on catalytic surfaces, has rarely been achieved. Single-molecule fluorescence spectroscopy has been used to image and characterize single turnover sites at catalytic surfaces, but is restricted to reactions that generate highly fluorescing product molecules. Herein the chemical conversion of N-heterocyclic carbene molecules attached to catalytic particles is mapped using synchrotron-radiation-based infrared nanospectroscopy with a spatial resolution of 25 nanometres, which enabled particle regions that differ in reactivity to be distinguished. These observations demonstrate that, compared to the flat regions on top of the particles, the peripheries of the particles-which contain metal atoms with low coordination numbers-are more active in catalysing oxidation and reduction of chemically active groups in surface-anchored N-heterocyclic carbene molecules.

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