Martina Abb

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.

Photoconductively loaded plasmonic nanoantenna as building block for ultracompact optical switches

We propose and explore theoretically a new concept of ultrafast optical switches based on nonlinear plasmonic nanoantennas. The antenna nanoswitch operates on the transition from the capacitive to conductive coupling regimes between two closely spaced metal nanorods. By filling the antenna gap with amorphous silicon, progressive antenna-gap loading is achieved due to variations in the free-carrier density in the semiconductor. Strong modification of the antenna response is observed both in the far-field response and in the local near-field intensity. The large modulation depth, low switching threshold, and potentially ultrafast time response of antenna switches holds promise for applications ranging from integrated nanophotonic circuits to quantum information devices.

Surface-Enhanced Infrared Spectroscopy Using Metal Oxide Plasmonic Antenna Arrays

We successfully demonstrate surface-enhanced infrared spectroscopy using arrays of indium tin oxide (ITO) plasmonic nanoantennas. The ITO antennas show a strongly reduced plasmon wavelength, which holds promise for ultracompact antenna arrays and extremely subwavelength metamaterials. The strong plasmon confinement and reduced antenna cross section allows ITO antennas to be integrated at extremely high densities with no loss in performance due to long-range transverse interactions. By further reducing the spacing of antennas in the arrays, we access the regime of plasmonic near field coupling where the response is enhanced for both Au and ITO devices. Ultracompact ITO antennas with high spatial and spectral selectivity in spectroscopic applications offer a viable new platform for infrared plasmonics, which may be combined with other functionalities of these versatile materials in devices.

Ultrafast nonlinear control of progressively loaded, single plasmonic nanoantennas fabricated using helium ion milling

We demonstrate milling of partial antenna gaps and narrow conducting bridges with nanometer precision using a helium ion beam microscope. Single particle spectroscopy shows large shifts in the plasmonic mode spectrum of the milled antennas, associated with the transition from capacitive to conductive gap loading. A conducting bridge of nanometer height is found sufficient to shift the antenna from the capacitive to the conductive coupling regime, in agreement with circuit theory. Picosecond pump-probe spectroscopy reveals an enhanced nonlinear response for partially milled antennas, reaching an optimum value for an intermediate bridge height. Our results show that manipulation of the antenna load can be used to increase the nonlinear response of plasmonic antennas.

Ultrafast plasmonics using transparent conductive oxide hybrids in the epsilon-near-zero regime

The dielectric response of transparent conductive oxides near the bulk plasmon frequency is characterized by a refractive index less than vacuum. In analogy with x-ray optics, it is shown that this regime results in total external reflection and air-guiding of light. In addition, the strong reduction of the wavevector in the indium-tin oxide below that of free space enables a new surface plasmon polariton mode which can be excited without requiring a prism or grating coupler. Ultrafast control of the surface plasmon polariton mode is achieved with a modulation amplitude reaching 20%.

Hotspot-mediated ultrafast nonlinear control of multifrequency plasmonic nanoantennas

Plasmonic devices have a unique ability to concentrate and convert optical energy into a small volume. There is a tremendous interest in achieving active control of plasmon resonances, which would enable switchable hotspots for applications such as surface-enhanced spectroscopy and single molecule emission. The small footprint and strong-field confinement of plasmonic nanoantennas also holds great potential for achieving transistor-type devices for nanoscale-integrated circuits. To achieve such a functionality, new methods for nonlinear modulation are required, which are able to precisely tune the nonlinear interactions between resonant antenna elements. Here we demonstrate that resonant pumping of a nonlinear medium in a plasmonic hotspot produces an efficient transfer of optical Kerr nonlinearity between different elements of a multifrequency antenna. By spatially and spectrally separating excitation and readout, isolation of the hotspot-mediated ultrafast Kerr nonlinearity from slower, thermal effects is achieved.

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.

Transparent conducting oxides for active hybrid metamaterial devices

We present here a study of the combined nonlinear response of plasmonic antenna—transparent conducting oxide hybrids for activation of metamaterial devices. Nanoantenna layers consisting of randomly positioned gold nanodisk dimers are fabricated using hole-mask lithography. The nanoantenna layers are covered with a 20 nm thin layer of transparent conducting oxide (TCO). We investigate the response of atomic layer deposited aluminum-doped zinc oxide (AZO) next to indium–tin oxide (ITO) produced using sputter coating. We show that our results are in agreement with the hypothesis of fast electron-mediated cooling, facilitated by the Ohmic interface between the gold nanodisks and the TCO substrate, which appears a universal mechanism for providing a new hybrid functionality to active metamaterial devices.

Formation and Plasmonic Response of Self-Assembled Layers of Colloidal Gold Nanorods and Branched Gold Nanoparticles

The plasmonic properties of self-assembled layers of rod- and branched-shaped gold nanoparticles were investigated using optical techniques. Nanoparticles were synthesized by a surfactant-guided, seed-mediated growth method. The layers were obtained by gradual assembly of nanoparticles at the interface between a polar and a nonpolar solvent and were transferred to a glass slide. Polarization and angle-dependent extinction measurements showed that the layers made of gold nanorods were governed by an effective medium response. The response of the layers made by branched gold particles was characterized by random light scattering. Microscopic mapping of the spatial mode structure demonstrates a uniform optical response of the nanoparticle layers down to a submicrometer length scale.

Ultrafast dephasing of light in strongly scattering GaP nanowires

We demonstrate ultrafast dephasing in the random transport of light through a layer consisting of strongly scattering GaP nanowires. Dephasing results in a nonlinear intensity modulation of individual pseudomodes which is 100 times larger than that of bulk GaP. Different contributions to the nonlinear response are separated by using total transmission, white-light frequency correlation, and statistical pseudomode analysis. A dephasing time of 1.2±0.2  ps is found. Quantitative agreement is obtained with numerical model calculations which include photoinduced absorption and deformation of individual scatterers. Nonlinear dephasing of photonic eigenmodes opens up avenues for ultrafast control of random lasers, nanophotonic switches, and photon localization.