Pablo Albella

All-optical control of a single plasmonic nanoantenna–ITO hybrid

We demonstrate experimentally picosecond all-optical control of a single plasmonic nanoantenna embedded in indium tin oxide (ITO). We identify a picosecond response of the antenna-ITO hybrid system, which is distinctly different from transient bleaching observed for gold antennas on a nonconducting SiO(2) substrate. Our experimental results can be explained by the large free-carrier nonlinearity of ITO, which is enhanced by plasmon-induced hot-electron injection from the gold nanoantenna into the conductive oxide. The combination of tunable antenna-ITO hybrids with nanoscale plasmonic energy transfer mechanisms, as demonstrated here, opens a path for new ultrafast devices to produce nanoplasmonic switching and control.

Real-space mapping of Fano interference in plasmonic metamolecules

An unprecedented control of the spectral response of plasmonic nanoantennas has recently been achieved by designing structures that exhibit Fano resonances. This new insight is paving the way for a variety of applications, such as biochemical sensing and surface-enhanced Raman spectroscopy. Here we use scattering-type near-field optical microscopy to map the spatial field distribution of Fano modes in infrared plasmonic systems. We observe in real space the interference of narrow (dark) and broad (bright) plasmonic resonances, yielding intensity and phase toggling between different portions of the plasmonic metamolecules when either their geometric sizes or the illumination wavelength is varied.

Experimental verification of the spectral shift between near- and far-field peak intensities of plasmonic infrared nanoantennas.

Theory predicts a distinct spectral shift between the near- and far-field optical response of plasmonic antennas. Here we combine near-field optical microscopy and far-field spectroscopy of individual infrared-resonant nanoantennas to verify experimentally this spectral shift. Numerical calculations corroborate our experimental results. We furthermore discuss the implications of this effect in surface-enhanced infrared spectroscopy.

Plasmonic nickel nanoantennas.

The fundamental optical properties of pure nickel nanostructures are studied by far-field extinction spectroscopy and optical near-field microscopy, providing direct experimental evidence of the existence of particle plasmon resonances predicted by theory. Experimental and calculated near-field maps allow for unambiguous identification of dipolar plasmon modes. By comparing calculated near-field and far-field spectra, dramatic shifts are found between the near-field and far-field plasmon resonances, which are much stronger than in gold nanoantennas. Based on a simple damped harmonic oscillator model to describe plasmonic resonances, it is possible to explain these shifts as due to plasmon damping.

Longitudinal and transverse coupling in infrared gold nanoantenna arrays: long range versus short range interaction regimes

Interaction between micrometer-long nanoantennas within an array considerably modifies the plasmonic resonant behaviour; for fundamental resonances in the infrared already at micrometer distances. In order to get systematic knowledge on the relationship between infrared plasmonic resonances and separation distances dx and dy in longitudinal and transverse direction, respectively, we experimentally studied the optical extinction spectra for rectangularly ordered lithographic gold nanorod arrays on silicon wafers. For small dy, strong broadening of resonances and strongly decreased values of far-field extinction are detected which come along with a decreased near-field intensity, as indicated by near-field amplitude maps of the interacting nanoantennas. In contrast, near-field interaction over small dx does only marginally broaden the resonance. Our findings set a path for optimum design of rectangular nanorod lattices for surface enhanced infrared spectroscopy.

Shape matters: plasmonic nanoparticle shape enhances interaction with dielectric substrate.

Numerical analyses of the ultraviolet and visible plasmonic spectra measured from hemispherical gallium nanostructures on dielectric substrates reveal that resonance frequencies are quite sensitive to illumination angle and polarization in a way that depends on nanostructure size, shape, and substrate. Large, polarization-dependent splittings arise from the broken symmetry of hemispherical gallium nanoparticles on sapphire substrates, inducing strong interactions with the substrate that depend sensitively on the angle of illumination and the nanoparticle diameter.

Analysis of the Spectral Behavior of Localized Plasmon Resonances in the Near- and Far-Field Regimes

The angular spectrum representation of electromagnetic fields scattered by metallic particles much smaller than the incident wavelength is used to interpret and analyze the spectral response of localized surface plasmon resonances (LSPs) both in the near-field and far-zone regimes. The previously observed spectral redshift and broadening of the LSP peak, as one moves from the far-zone to the near-field region of the scatterer, is analyzed on studying the role and contribution of the evanescent and propagating plane wave components of the emitted field. For such dipolar particles, it is found that the evanescent waves are responsible for those broadenings and shifts. Further, we prove that the shift is a universal phenomenon, and hence, it constitutes a general law, its value increasing as the imaginary part of the nanostructure permittivity grows. Our results should be of use for the prediction and interpretation of the spectral behavior in applications where the excitation of LSPs yield field enhancements like those assisting surface-enhanced Raman spectroscopy or equivalent processes.

Switchable directional scattering of electromagnetic radiation with subwavelength asymmetric silicon dimers.

High refractive index dielectric nanoparticles show high promise as a complementary nanophotonics platform due to compared with plasmonic nanostructures low absorption losses and the co-existence of magnetic and electric resonances. Here we explore their use as resonantly enhanced directional scatterers. We theoretically demonstrate that an asymmetric dimer of silicon nanoparticles shows tuneable directional scattering depending on the frequency of excitation. This is due to the interference between electric and magnetic dipoles excited in each nanoparticle, enabling directional control of the scattered light. Interestingly, this control can be achieved regardless of the polarization direction with respect to the dimer axis; however, difference in the polarization can shift the wavelengths at which the directional scattering is achieved. We also explore the application of such an asymmetric nanoantenna as a tuneable routing element in a nanometer scale, suggesting applications in optical nanocircuitry.

Detection of deep-subwavelength dielectric layers at terahertz frequencies using semiconductor plasmonic resonators

Plasmonic bowtie antennas made of doped silicon can operate as plasmonic resonators at terahertz (THz) frequencies and provide large field enhancement close to their gap. We demonstrate both experimentally and theoretically that the field confinement close to the surface of the antenna enables the detection of ultrathin (100 nm) inorganic films, about 3750 times thinner than the free space wavelength. Based on model calculations, we conclude that the detection sensitivity and its variation with the thickness of the deposited layer are related to both the decay of the local THz field profile around the antenna and the local field enhancement in the gap of the bowtie antenna. This large field enhancement has the potential to improve the detection limits of plasmon-based biological and chemical sensors.

Interference, coupling, and nonlinear control of high-order modes in single asymmetric nanoantennas

We investigate theoretically and experimentally the structure of plasmonic modes in individual asymmetric dimer antennas. Plasmonic near-field coupling of high-order modes results in hybridization of bright and dark modes of the individual nanorods, leading to an anticrossing of the coupled resonances. For two bright modes, hybridization results in a capacitive red shift and super-radiant broadening. We show that the properties of asymmetric dimers can be used for nonlinear control of spectral modes and demonstrate such a nonlinear effect by measuring the modulation of a hybrid asymmetric dimer--ITO antenna. With use of full electrodynamical calculations, we find that the properties of the near-field nonlinear responses are distinctly different from the far-field, which opens up new routes for nonlinear control of plasmonic nanosystems.