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Register a new userExtraordinary nonlinear plasmonics in graphene nanoislands
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Added by
F. Javier Garcia de Abajo
Publication date
2014
fields
Physics
and research's language is
English
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Nonlinear optical processes rely on the intrinsically weak interactions between photons enabled by their coupling with matter. Unfortunately, many applications in nonlinear optics are severely hindered by the small response of conventional materials. Metallic nanostructures partially alleviate this situation, as the large light enhancement associated with their localized plasmons amplifies their nonlinear response to record high levels. Graphene hosts long-lived, electrically tunable plasmons that also interact strongly with light. Here we show that the nonlinear polarizabilities of graphene nanoislands can be electrically tuned to surpass by several orders of magnitude those of metal nanoparticles of similar size. This extraordinary behavior extends over the visible and near-infrared for islands consisting of hundreds of carbon atoms doped with moderate carrier densities. Our quantum-mechanical simulations of the plasmon-enhanced optical response of nanographene reveal this material as an ideal platform for the development of electrically tunable nonlinear optical nanodevices.
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In recent years, we have seen a rapid progress in the field of graphene plasmonics, motivated by graphenes unique electrical and optical properties, tunabilty, long-lived collective excitation and their extreme light confinement. Here, we review the basic properties of graphene plasmons; their energy dispersion, localization and propagation, plasmon-phonon hybridization, lifetimes and damping pathways. The application space of graphene plasmonics lies in the technologically significant, but relatively unexploited terahertz to mid-infrared regime. We discuss emerging and potential applications, such as modulators, notch filters, polarizers, mid-infrared photodetectors, mid-infrared vibrational spectroscopy, among many others.
We demonstrate the controlled preparation of heteroepitaxial diamond nano- and microstructures on silicon wafer based iridium films as hosts for single color centers. Our approach uses electron beam lithography followed by reactive ion etching to pattern the carbon layer formed by bias enhanced nucleation on the iridium surface. In the subsequent chemical vapor deposition process, the patterned areas evolve into regular arrays of (001) oriented diamond nano-islands with diameters of <500nm and a height of approx. 60 nm. In the islands, we identify single SiV color centers with narrow zero phonon lines down to 1 nm at room temperature.
We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonon generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon. These results demonstrate how it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures.
We determined the lattice dynamics of metastable, surface-stabilized $alpha$-phase FeSi$_2$ nanoislands epitaxially grown on the Si(111) surface with average heights and widths ranging from 1.5 to 20 nm and 18 to 72 nm, respectively. The crystallographic orientation, surface morphology and local crystal structure of the nanoislands were investigated by reflection high-energy electron diffraction, atomic force microscopy and X-ray absorption spectroscopy. The Fe-partial phonon density of states (PDOS), obtained by nuclear inelastic scattering, exhibits a pronounced damping and broadening of the spectral features with decreasing average island height. First-principles calculations of the polarization-projected Si- and Fe-partial phonon dispersions and PDOS enable the disentanglement of the contribution of the $xy$- and $z$-polarized phonons to the experimental PDOS. Modeling of the experimental data with the theoretical results unveils an enhanced damping of the $z$-polarized phonons for islands with average sizes below 10 nm. This phenomenon is attributed to the fact that the low-energy $z$-polarized phonons couple to the low-energy surface/interface vibrational modes. The thermodynamic and elastic properties obtained from the experimental data show a pronounced size-dependent behavior.
To understand the band bending caused by metal contacts, we study the potential and charge density induced in graphene in response to contact with a metal strip. We find that the screening is weak by comparison with a normal metal as a consequence of the ultra-relativistic nature of the electron spectrum near the Fermi energy. The induced potential decays with the distance from the metal contact as x^{-1/2} and x^{-1} for undoped and doped graphene, respectively, breaking its spatial homogeneity. In the contact region the metal contact can give rise to the formation of a p-p, n-n, p-n junction (or with additional gating or impurity doping, even a p-n-p junction) that contributes to the overall resistance of the graphene sample, destroying its electron-hole symmetry. Using the work functions of metal-covered graphene recently calculated by Khomyakov et al. [Phys. Rev. B 79, 195425 (2009)] we predict the boundary potential and junction type for different metal contacts.
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