Mathieu Kociak

Zeptomol Detection Through Controlled Ultrasensitive Surface-Enhanced Raman Scattering

SERS permits identifying the nature of molecules in extremely low concentrations, but it is hindered by poor enhancement or low reproducibility. We demonstrate controllable approximately 10(10) signal amplification reaching the zeptomol detection limit for a nonresonant molecule by sandwiching the analyte between the tips of star-shaped gold nanoparticles and a planar gold surface using a simple synthetic procedure. This unprecedented control over light-intensity amplification opens a new avenue toward high-yield, fully reproducible, SERS-based, zeptomol detection and holds promise for nonlinear optics applications at the single-particle level.

Superconductivity in Ropes of Single-Walled Carbon Nanotubes

We report measurements on ropes of single-walled carbon nanotubes (SWNT) in low-resistance contact to nonsuperconducting (normal) metallic pads, at low voltage and at temperatures down to 70 mK. In one sample, we find a 2 orders of magnitude resistance drop below 0.55 K, which is destroyed by a magnetic field of the order of 1 T, or by a dc current greater than 2.5 microA. These features strongly suggest the existence of superconductivity in ropes of SWNT.

Probing the photonic local density of states with electron energy loss spectroscopy

Electron energy loss spectroscopy performed in transmission electron microscopes is shown to directly render the photonic local density of states with unprecedented spatial resolution, currently below the nanometer. Two special cases are discussed in detail: (i) 2D photonic structures with the electrons moving along the translational axis of symmetry and (ii) quasiplanar plasmonic structures under normal incidence. Nanophotonics in general and plasmonics, in particular, should benefit from these results connecting the unmatched spatial resolution of electron energy loss spectroscopy with its ability to probe basic optical properties such as the photonic local density of states.

Nanometer Scale Spectral Imaging of Quantum Emitters in Nanowires and Its Correlation to Their Atomically Resolved Structure

We report the spectral imaging in the UV to visible range with nanometer scale resolution of closely packed GaN/AlN quantum disks in individual nanowires using an improved custom-made cathodoluminescence system. We demonstrate the possibility to measure full spectral features of individual quantum emitters as small as 1 nm and separated from each other by only a few nanometers and the ability to correlate their optical properties to their size, measured with atomic resolution. The direct correlation between the quantum disk size and emission wavelength provides evidence of the quantum confined Stark effect leading to an emission below the bulk GaN band gap for disks thicker than 2.6 nm. With the help of simulations, we show that the internal electric field in the studied quantum disks is smaller than what is expected in the quantum well case. We show evidence of a clear dispersion of the emission wavelengths of different quantum disks of identical size but different positions along the wire. This dispersion is systematically correlated to a change of the diameter of the AlN shell coating the wire and is thus attributed to the related strain variations along the wire. The present work opens the way both to fundamental studies of quantum confinement in closely packed quantum emitters and to characterizations of optoelectronic devices presenting carrier localization on the nanometer scale.

Ultraviolet Photodetector Based on GaN/AlN Quantum Disks in a Single Nanowire

We report the demonstration of single-nanowire photodetectors relying on carrier generation in GaN/AlN QDiscs. Two nanowire samples containing QDiscs of different thicknesses are analyzed and compared to a reference binary n-i-n GaN nanowire sample. The responsivity of a single wire QDisc detector is as high as 2 x 10(3) A/W at lambda = 300 nm at room temperature. We show that the insertion of an axial heterostructure drastically reduces the dark current with respect to the binary nanowires and enhances the photosensitivity factor (i.e., the ratio between the photocurrent and the dark current) up to 5 x 10(2) for an incoming light intensity of 5 mW/cm(2). Photocurrent spectroscopy allows identification of the spectral contribution related to carriers generated within large QDiscs, which lies below the GaN band gap due to the quantum confined Stark effect.

Plasmon Spectroscopy and Imaging of Individual Gold Nanodecahedra: A Combined Optical Microscopy, Cathodoluminescence, and Electron Energy-Loss Spectroscopy Study

Imaging localized plasmon modes in noble-metal nanoparticles is of fundamental importance for applications such as ultrasensitive molecular detection. Here, we demonstrate the combined use of optical dark-field microscopy (DFM), cathodoluminescence (CL), and electron energy-loss spectroscopy (EELS) to study localized surface plasmons on individual gold nanodecahedra. By exciting surface plasmons with either external light or an electron beam, we experimentally resolve a prominent dipole-active plasmon band in the far-field radiation acquired via DFM and CL, whereas EELS reveals an additional plasmon mode associated with a weak dipole moment. We present measured spectra and intensity maps of plasmon modes in individual nanodecahedra in excellent agreement with boundary-element method simulations, including the effect of the substrate. A simple tight-binding model is formulated to successfully explain the rich plasmon structure in these particles encompasing bright and dark modes, which we predict to be fully observable in less lossy silver decahedra. Our work provides useful insight into the complex nature of plasmon resonances in nanoparticles with pentagonal symmetry.

Two-Dimensional Quasistatic Stationary Short Range Surface Plasmons in Flat Nanoprisms

We report on the nanometer scale spectral imaging of surface plasmons within individual silver triangular nanoprisms by electron energy loss spectroscopy and on related discrete dipole approximation simulations. A dependence of the energy and intensity of the three detected modes as function of the edge length is clearly identified both experimentally and with simulations. We show that for experimentally available prisms (edge lengths ca. 70 to 300 nm) the energies and intensities of the different modes show a monotonic dependence as function of the aspect ratio of the prisms. For shorter or longer prisms, deviations to this behavior are identified thanks to simulations. These modes have symmetric charge distribution and result from the strong coupling of the upper and lower triangular surfaces. They also form a standing wave in the in-plane direction and are identified as quasistatic short range surface plasmons of different orders as emphasized within a continuum dielectric model. This model explains in simple terms the measured and simulated energy and intensity changes as function of geometric parameters. By providing a unified vision of surface plasmons in platelets, such a model should be useful for engineering of the optical properties of metallic nanoplatelets.

Ultralocal Modification of Surface Plasmons Properties in Silver Nanocubes

The plasmonic properties of individual subwavelength-sized silver nanocubes are mapped with nanometric spatial resolution by means of electron energy-loss spectroscopy in a scanning transmission electron microscope. Three main features with different energies and spatial behavior (two peaked at the corners, one on the edges) are identified and related to previous measurements on ensemble or individual nanoparticles. The highly subwavelength mapping of the energy position and intensity of the excitations shows that the surface plasmon modes, localized at specific areas of the particles, for example, the corners or the edges, are modified by their size, the presence of a substrate, and the very local environment. Helped by discrete dipole approximation numerical simulations, we discuss how local modifications of the environment affect the global modes of the particles. In particular, we show both experimentally and theoretically that absorption resonances at different corners of the same nanocube are largely independent of each other in energy and intensity. Our findings provide a better understanding of the spatial coherence of the surface plasmons in nanoparticles but also give useful insights about their roles in the nanoparticle sensing properties.

Electron energy-gain spectroscopy

We introduce electron energy-gain spectroscopy as a tool to yield information on local optical excitations of nanostructured systems using transmission electron microscopes equipped with external optical illumination. The new spectroscopy combines the superb spatial resolution of electron microscopes with unprecedented energy resolution below the milli-electron-volt level, only limited by the bandwidth of the external light. The analysis of energy gain events should reveal hyperfine details in the optical response of individual nanostructures (e.g. plasmons in nanoparticles). Our conclusions rely on a general formalism capable of describing light absorption by fast electrons moving in vacuum near an illuminated nanostructure, thus paving the way towards new light-assisted electron- and ion-acceleration schemes. Energy gain probabilities are shown to be comparable to those observed in energy loss experiments for reasonable illumination intensity.

Acoustoelectric Effects in Carbon Nanotubes

We show that it is possible to detect mechanical bending modes on 1µm long ropes of single walled-carbon nanotubes suspended between 2 metallic contacts. This is done by measuring either their dc resistance in a region of strong temperature dependence (in the vicinity of superconducting or metal-insulator transition), or their critical current. The vibrations are excited by a radio-frequency electric field produced by an antenna located in the vicinity of the sample. We analyze the mechanism of detection of the mechanical resonances in terms of heating and phase breaking effects.