Strong plasmon reflection at nanometer-size gaps in monolayer graphene on SiC.

We employ tip-enhanced infrared near-field microscopy to study the plasmonic properties of epitaxial quasi-free-standing monolayer graphene on silicon carbide. The near-field images reveal propagating graphene plasmons, as well as a strong plasmon reflection at gaps in the graphene layer, which appear at the steps between the SiC terraces. When the step height is around 1.5 nm, which is two orders of magnitude smaller than the plasmon wavelength, the reflection signal reaches 20% of its value at graphene edges, and it approaches 50% for step heights as small as 5 nm. This intriguing observation is corroborated by numerical simulations and explained by the accumulation of a line charge at the graphene termination. The associated electromagnetic fields at the graphene termination decay within a few nanometers, thus preventing efficient plasmon transmission across nanoscale gaps. Our work suggests that plasmon propagation in graphene-based circuits can be tailored using extremely compact nanostructures, such as ultranarrow gaps. It also demonstrates that tip-enhanced near-field microscopy is a powerful contactless tool to examine nanoscale defects in graphene.

Optical field enhancement by strong plasmon interaction in graphene nanostructures.

The ability of plasmons to enhance the electromagnetic field intensity in the gap between metallic nanoparticles derives from their strong optical confinement relative to the light wavelength. The spatial extension of plasmons in doped graphene has recently been shown to be boldly reduced with respect to conventional plasmonic metals. Here, we show that graphene nanostructures are capable of capitalizing such strong confinement to yield unprecedented levels of field enhancement, well beyond what is found in noble metals of similar dimensions (~ tens of nanometers). We perform realistic, quantum-mechanical calculations of the optical response of graphene dimers formed by nanodisks and nanotriangles, showing a strong sensitivity of the level of enhancement to the type of carbon edges near the gap region, with armchair edges favoring stronger interactions than zigzag edges. Our quantum-mechanical description automatically incorporates nonlocal effects that are absent in classical electromagnetic theory, leading to over an order of magnitude higher enhancement in armchair structures. The classical limit is recovered for large structures. We predict giant levels of light concentration for dimers ~200 nm, leading to infrared-absorption enhancement factors ~10(8). This extreme light enhancement and confinement in nanostructured graphene has great potential for optical sensing and nonlinear devices.

Tunable molecular plasmons in polycyclic aromatic hydrocarbons.

We show that chemically synthesized polycyclic aromatic hydrocarbons (PAHs) exhibit molecular plasmon resonances that are remarkably sensitive to the net charge state of the molecule and the atomic structure of the edges. These molecules can be regarded as nanometer-sized forms of graphene, from which they inherit their high electrical tunability. Specifically, the addition or removal of a single electron switches on/off these molecular plasmons. Our first-principles time-dependent density-functional theory (TDDFT) calculations are in good agreement with a simpler tight-binding approach that can be easily extended to much larger systems. These fundamental insights enable the development of novel plasmonic devices based upon chemically available molecules, which, unlike colloidal or lithographic nanostructures, are free from structural imperfections. We further show a strong interaction between plasmons in neighboring molecules, quantified in significant energy shifts and field enhancement, and enabling molecular-based plasmonic designs. Our findings suggest new paradigms for electro-optical modulation and switching, single-electron detection, and sensing using individual molecules.

Gated tunability and hybridization of localized plasmons in nanostructured graphene.

Graphene has emerged as an outstanding material for optoelectronic applications due to its high electronic mobility and unique doping capabilities. Here we demonstrate electrical tunability and hybridization of plasmons in graphene nanodisks and nanorings down to 3.7 µm light wavelength. By electrically doping patterned graphene arrays with an applied gate voltage, we observe radical changes in the plasmon energy and strength, in excellent quantitative agreement with rigorous analytical theory. We further show evidence of an unexpected increase in plasmon lifetime with growing energy. Plasmon hybridization and electrical doping in nanorings of suitably chosen nanoscale dimensions are key elements for bringing the optical response of graphene closer to the near-infrared, where it can provide a robust, integrable platform for light modulation, switching, and sensing.

Optical nano-imaging of gate-tunable graphene plasmons.

The ability to manipulate optical fields and the energy flow of light is central to modern information and communication technologies, as well as quantum information processing schemes. However, because photons do not possess charge, a way of controlling them efficiently by electrical means has so far proved elusive. A promising way to achieve electric control of light could be through plasmon polaritons­coupled excitations of photons and charge carriers­in graphene. In this two-dimensional sheet of carbon atoms, it is expected that plasmon polaritons and their associated optical fields can readily be tuned electrically by varying the graphene carrier density. Although evidence of optical graphene plasmon resonances has recently been obtained spectroscopically, no experiments so far have directly resolved propagating plasmons in real space. Here we launch and detect propagating optical plasmons in tapered graphene nanostructures using near-field scattering microscopy with infrared excitation light. We provide real-space images of plasmon fields, and find that the extracted plasmon wavelength is very short­more than 40 times smaller than the wavelength of illumination. We exploit this strong optical field confinement to turn a graphene nanostructure into a tunable resonant plasmonic cavity with extremely small mode volume. The cavity resonance is controlled in situ by gating the graphene, and in particular, complete switching on and off of the plasmon modes is demonstrated, thus paving the way towards graphene-based optical transistors. This successful alliance between nanoelectronics and nano-optics enables the development of active subwavelength-scale optics and a plethora of nano-optoelectronic devices and functionalities, such as tunable metamaterials, nanoscale optical processing, and strongly enhanced light­matter interactions for quantum devices and biosensing applications.

Complete optical absorption in periodically patterned graphene.

We demonstrate that 100% light absorption can take place in a single patterned sheet of doped graphene. General analysis shows that a planar array of small particles with losses exhibits full absorption under critical-coupling conditions provided the cross section of each individual particle is comparable to the area of the lattice unit cell. Specifically, arrays of doped graphene nanodisks display full absorption when supported on a substrate under total internal reflection and also when lying on a dielectric layer coating a metal. Our results are relevant for infrared light detectors and sources, which can be made tunable via electrostatic doping of graphene.

Quantum finite-size effects in graphene plasmons.

Graphene plasmons are emerging as an alternative solution to noble metal plasmons, adding the advantages of tunability via electrostatic doping and long lifetimes. These excitations have been so far described using classical electrodynamics, with the carbon layer represented by a local conductivity. However, the question remains, how accurately is such a classical description representing graphene? What is the minimum size for which nonlocal and quantum finite-size effects can be ignored in the plasmons of small graphene structures? Here, we provide a clear answer to these questions by performing first-principles calculations of the optical response of doped nanostructured graphene obtained from a tight-binding model for the electronic structure and the random-phase approximation for the dielectric response. The resulting plasmon energies are in good agreement with classical local electromagnetic theory down to ∼10 nm sizes, below which plasmons split into several resonances that emphasize the molecular character of the carbon structures and the quantum nature of their optical excitations. Additionally, finite-size effects produce substantial plasmon broadening compared to homogeneous graphene up to sizes well above 20 nm in nanodisks and 10 nm in nanoribbons. The atomic structure of edge terminations is shown to be critical, with zigzag edges contributing to plasmon broadening significantly more than armchair edges. This study demonstrates the ability of graphene nanostructures to host well-defined plasmons down to sizes below 10 nm, and it delineates a roadmap for understanding their main characteristics, including the role of finite size and nonlocality, thus providing a solid background for the emerging field of graphene nanoplasmonics.

Graphene plasmon waveguiding and hybridization in individual and paired nanoribbons.

Plasmons in doped graphene exhibit relatively large confinement and long lifetime compared to noble-metal plasmons. Here, we study the propagation properties of plasmons guided along individual and interacting graphene nanoribbons. Besides their tunability via electrostatic gating, an additional handle to control these excitations is provided by the dielectric environment and the relative arrangement of the interacting waveguides. Plasmon interaction and hybridization in pairs of neighboring aligned ribbons are shown to be strong enough to produce dramatic modifications in the plasmon field profiles. We introduce a universal scaling law that considerably simplifies the analysis an understanding of these plasmons. Our work provides the building blocks to construct graphene plasmon circuits for future compact plasmon devices with potential application to optical signal processing, infrared sensing, and quantum information technology.

Enhanced bandwidth and reduced dispersion through stacking multiple optical metamaterials.

All-semiconductor, highly anisotropic metamaterials provide a straightforward path to negative refraction in the mid-infrared. However, their usefulness in applications is restricted by strong frequency dispersion and limited spectral bandwidth. In this work, we show that by stacking multiple metamaterials of varying thickness and doping into one compound metamaterial, bandwidth is increased by 27% over a single-stack metamaterial, and dispersion is reduced.

Hypergratings: nanophotonics in planar anisotropic metamaterials.

We present a technique capable of producing subwavelength focal spots in planar nonresonant structures not limited to the near-field of the source. The approach combines the diffraction gratings that generate the high-wave-vector-number modes and planar slabs of homogeneous anisotropic metamaterials that propagate these waves and combine them at the subwavelength focal spots. In a sense, the technique combines the benefits of Fresnel lens, near-field zone plates, hyperlens, and superlens and at the same time resolves their fundamental limitations. Several realizations of the proposed technique for visible, near-IR, and mid-IR frequencies are proposed, and their performance is analyzed theoretically and numerically. Generalizations of the developed approach for subdiffractional imaging and on-chip photonics are suggested.