Single up-conversion nanocrystal as a local temperature probe of electrically heated silver nanowire.

Luminescence thermometry is a powerful technique for monitoring temperature in a sensitive, remote (through light), and minimally invasive manner. Up to now, many macroscopic and microscopic luminescence temperature probes exploiting different temperature sensing schemes have been investigated, with the majority of the studies using aggregates of nanothermometers. This work presents isolated single up-converting NaYF4:Er3+/Yb3+ nanocrystals as functional temperature indicators operating in a standard confocal microscopy configuration. More specifically, the nanocrystals were used to monitor the temperature of a single silver nanowire, whose temperature was controlled electrically via the Joule process. We demonstrate that individual nanocrystals placed near the nanowire can precisely determine the temperature distribution in its surroundings. These results, which combine nanoscopic heat generation with temperature readout using isolated nanocrystals, represent an essential step for the application of isolated single nanoprobes for luminescence thermometry at the nanoscale.

Efficient optimization of SHG hotspot switching in plasmonic nanoantennas using phase-shaped laser pulses controlled by neural networks.

We present a novel procedure for manipulating the near-field of plasmonic nanoantennas using neural network-controlled laser pulse-shaping. For our model systems we numerically studied the spatial distribution of the second harmonic response of L-shaped nanoantennas illuminated by broadband laser pulses. We first show that a trained neural network can be used to predict the relative intensity of the second-harmonic hotspots of the nanoantenna for a given spectral phase and that it can be employed to deterministically switch individual hotspots on and off on sub-diffraction length scale by shaping the spectral phase of the laser pulse. We then demonstrate that a neural network trained on a 90 nm × 150 nm nano-L can, in addition, efficiently predict the hotspot intensities in an antenna with different aspect ratio, after minimal further training, for varying spectral phases. These results could lead to novel applications of machine-learning and optical control to nanoantennas and nanophotonics components.

Silver nanowires as receiving-radiating nanoantennas in plasmon-enhanced up-conversion processes.

We demonstrate efficient coupling between plasmons in a single silver nanowire and nanocrystals doped with rare earth ions, α-NaYF4:Er(3+)/Yb(3+). Plasmonic interaction results in a sevenfold increase of the up-converted emission of nanocrystals located in the vicinity of the nanowires as well as much faster luminescence decays. The enhancement of the emission can be precisely controlled by the polarization of the excitation laser and is significantly stronger for polarization parallel to the nanowire antennas. Imaging of angular-resolved emission patterns in the Fourier plane reveals plasmon-mediated luminescence, where the up-converted radiation is emitted via the nanowire antennas as leakage radiation.

Electrical excitation of surface plasmons by an individual carbon nanotube transistor.

We demonstrate here the realization of an integrated, electrically driven, source of surface plasmon polaritons. Light-emitting individual single-walled carbon nanotube field effect transistors were fabricated in a plasmonic-ready platform. The devices were operated at ambient conditions to act as an electroluminescence source localized near the contacting gold electrodes. We show that photon emission from the semiconducting channel can couple to propagating surface plasmons developing in the electrical terminals. Our results show that a common functional element can be operated for two different platforms emphasizing thus the high degree of compatibility between state-of-the-art nano-optoelectronics devices and a plasmonic architecture.

Influence of metallic and dielectric nanowire arrays on the photoluminescence properties of P3HT thin films.

The optical properties of organic semiconductor thin films deposited on nanostructured surfaces are investigated using time-resolved two-photon photoluminescence (PL) microscopy. The surfaces consist of parallel aligned metallic or dielectric nanowires forming well-defined arrays on glass substrates. Keeping the nanowire dimensions constant and varying only their spacing from 40 to 400 nm, we study the range of different types of nanowire-semiconductor interactions. For silver nanowires and spacings below 100 nm, the PL intensity and lifetime of P3HT and MDMO-PPV decrease rapidly due to the short-ranged metal-induced quenching that dominates the PL response with respect to a possible plasmonic enhancement of optical transition rates. In the case of P3HT however, we observe an additional longer-ranged reduction of non-radiative losses for both metallic and dielectric nanowires that is not observed for MDMO-PPV. Excitation polarization dependent measurements indicate that this reduction is due to self-assembly of the P3HT polymer chains along the nanowires. In conclusion, nanostructured surfaces, when fabricated across large areas, could be used to control film morphologies and to improve energy transport and collection efficiencies in P3HT-based solar cells.

Making graphene luminescent by oxygen plasma treatment.

We show that strong photoluminescence (PL) can be induced in single-layer graphene using an oxygen plasma treatment. The PL is spatially uniform across the flakes and connected to elastic scattering spectra distinctly different from those of gapless pristine graphene. Oxygen plasma can be used to selectively convert the topmost layer when multilayer samples are treated.

Mechanism of near-field Raman enhancement in one-dimensional systems.

We develop a theory of near-field Raman enhancement in one-dimensional systems, and report supporting experimental results for carbon nanotubes. The enhancement is established by a laser-irradiated nanoplasmonic structure acting as an optical antenna. The near-field Raman intensity is inversely proportional to the 10th power of the separation between the enhancing structure and the one-dimensional system. Experimental data obtained from single-wall carbon nanotubes indicate that the Raman enhancement process is not significantly influenced by the specific phonon eigenvector, and is mainly defined by the properties of the nanoplasmonic structure.

Tip-enhanced near-field optical microscopy of carbon nanotubes.

We review recent experimental studies on single-walled carbon nanotubes on substrates using tip-enhanced near-field optical microscopy (TENOM). High-resolution optical and topographic imaging with sub 15 nm spatial resolution is shown to provide novel insights into the spectroscopic properties of these nanoscale materials. In the case of semiconducting nanotubes, the simultaneous observation of Raman scattering and photoluminescence (PL) is possible, enabling a direct correlation between vibrational and electronic properties on the nanoscale. So far, applications of TENOM have focused on the spectroscopy of localized phonon modes, local band energy renormalizations induced by charge carrier doping, the environmental sensitivity of nanotube PL, and inter-nanotube energy transfer. At the end of this review we discuss the remaining limitations and challenges in this field.

Raman spectroscopy of graphene edges.

Graphene edges are of particular interest since their orientation determines the electronic properties. Here we present a detailed Raman investigation of graphene flakes with edges oriented at different crystallographic directions. We also develop a real space theory for Raman scattering to analyze the general case of disordered edges. The position, width, and intensity of G and D peaks are studied as a function of the incident light polarization. The D-band is strongest for polarization parallel to the edge and minimum for perpendicular. Raman mapping shows that the D peak is localized in proximity of the edge. For ideal edges, the D peak is zero for zigzag orientation and large for armchair, allowing in principle the use of Raman spectroscopy as a sensitive tool for edge orientation. However, for real samples, the D to G ratio does not always show a significant dependence on edge orientation. Thus, even though edges can appear macroscopically smooth and oriented at well-defined angles, they are not necessarily microscopically ordered.

A novel approach to detect and characterize the scattering patterns of single Au nanoparticles using confocal microscopy.

We demonstrate a novel optical method for characterizing single Au nanoparticles by acquiring their scattering patterns. This technique combines confocal microscopy and higher-order laser modes for detecting the light scattered by sub-wavelength-sized nanoobjects. The optical patterns are generated by the coherent superposition of the field scattered by individual metallic particles and the excitation field reflected at the cover slide-air interface and provide information about the particles' position, orientation, size and shape. Detectable changes in the full width at half maximum (FWHM) of the signal intensity permit to distinguish between 20- and 60-nm diameter Au spheres. The confocal images are also very sensitive to the particle's geometry and polarizability, that is, Au nanospheres, Au nanorods and triangular Au nanoplates give different characteristic patterns if the excitation wavelength is varied.

Rayleigh imaging of graphene and graphene layers.

We investigate graphene and graphene layers on different substrates by monochromatic and white-light confocal Rayleigh scattering microscopy. The image contrast depends sensitively on the dielectric properties of the sample as well as the substrate geometry and can be described quantitatively using the complex refractive index of bulk graphite. For a few layers (<6), the monochromatic contrast increases linearly with thickness. The data can be adequately understood by considering the samples behaving as a superposition of single sheets that act as independent two-dimensional electron gases. Thus, Rayleigh imaging is a general, simple, and quick tool to identify graphene layers, which is readily combined with Raman scattering, that provides structural identification.

Near-field Raman spectroscopy using a sharp metal tip.

Near-field Raman spectroscopy with a spatial resolution of 20 nm is demonstrated by raster scanning a sharp metal tip over the sample surface. The method is used to image vibrational modes of single-walled carbon nanotubes. By combining optical and topographical signals rendered by the single-walled carbon nanotubes, we can separate near-field and far-field contributions and quantify the observed Raman enhancement factors.

Near-field second-harmonic generation induced by local field enhancement.

The field near a sharp metal tip can be strongly enhanced if irradiated with an optical field polarized along the tip axis. We demonstrate that the enhanced field gives rise to local second-harmonic (SH) generation at the tip surface thereby creating a highly confined photon source. A theoretical model for the excitation and emission of SH radiation at the tip is developed and it is found that this source can be represented by a single on-axis oscillating dipole. The model is experimentally verified by imaging the spatial field distribution of strongly focused laser modes.