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.
The ability to modulate light at high speeds is of paramount importance for telecommunications, information processing, and medical imaging technologies. This has stimulated intense efforts to master optoelectronic switching at visible and near-infra
red frequencies, although coping with current computer speeds in integrated architectures still remains a major challenge. As a partial success, midinfrared light modulation has been recently achieved through gating patterned graphene. Here we show that atomically thin noble metal nanoislands can extend optical modulation to the visible and near-infrared spectral range. We find plasmons in thin metal nanodisks to produce similar absorption cross-sections as spherical particles of the same diameter. Using realistic levels of electrical doping, plasmons are shifted by about half their width, thus leading to a factor-of-two change in light absorption. These results, which we substantiate on microscopic quantum theory of the optical response, hold great potential for the development of electrical visible and near-infrared light modulation in integrable, nanoscale devices.
Electron energy-loss spectroscopy (EELS) performed in transmission electron microscopes is shown to directly render the photonic local density of states (LDOS) with unprecedented spatial resolution, currently below the nanometer. Two special cases ar
e discussed in detail: (i) 2D photonic structures with the electrons moving along the translational axis of symmetry and (ii) quasi-planar plasmonic structures under normal incidence. Nanophotonics in general and plasmonics in particular should benefit from these results connecting the unmatched spatial resolution of EELS with its ability to probe basic optical properties like the photonic LDOS.
Light transmission through 2D subwavelength hole arrays in perfect-conductor films is shown to be complete (100%) at some resonant wavelengths even for arbitrarily narrow holes. Conversely, the reflection on a 2D planar array of non-absorbing scatter
ers is shown to be complete at some wavelengths regardless how weak the scatterers are. These results are proven analytically and corroborated by rigorous numerical solution of Maxwells equations. This work supports the central role played by dynamical diffraction during light transmission through subwavelength hole arrays and it provides a systematics to analyze more complex geometries and many of the features observed in connection with transmission through hole arrays.
