Davy Gérard

Three-dimensional subwavelength confinement of light with dielectric microspheres

Dielectric microspheres are shown to be capable of confining light in a three-dimensional region of subwavelength dimensions when they are illuminated by tightly focused Gaussian beams. We show that a simple configuration, not involving resonances, permits one to reach an effective volume as small as 0.6 (lambda/n)(3). It is shown that this three-dimensional confinement arises from interferences between the field scattered by the sphere and the incident Gaussian beam containing high angular components.

Emission and excitation contributions to enhanced single molecule fluorescence by gold nanometric apertures

We detail the role of single nanometric apertures milled in a gold film to enhance the fluorescence emission of Alexa Fluor 647 molecules. Combining fluorescence correlation spectroscopy and lifetime measurements, we determine the respective contributions of excitation and emission in the observed enhanced fluorescence. We characterize a broad range of nanoaperture diameters from 80 to 310 nm, and highlight the link between the fluorescence enhancement and the local photonic density of states. These results are of great interest to increase the effectiveness of fluorescence-based single molecule detection and to understand the interaction between a quantum emitter and a nanometric metal structure.

Strong electromagnetic confinement near dielectric microspheres to enhance single-molecule fluorescence

Latex microspheres are used as a simple and low-cost means to achieve three axis electromagnetic confinement below the standard diffraction limit. We demonstrate their use to enhance the fluorescence fluctuation detection of single molecules. Compared to confocal microscopy with high numerical aperture, we monitor a detection volume reduction of one order of magnitude below the diffraction limit together with a 5-fold gain in the fluorescence rate per molecule. This offers new opportunities for a broad range of applications in biophotonics, plasmonics, optical data storage and ultramicroscopy.

Localized surface plasmon resonances in the ultraviolet from large scale nanostructured aluminum films

We report on a straightforward preparation method to obtain a dense layer of quasi-spherical aluminum nanoparticles over a large area. The method is based on rapid thermal annealing of a thin aluminum film deposited on a super-repellent substrate. Diameters ranging from 2 to 15 nm are obtained by varying the film thickness. Aluminum nanoparticles exhibit well-defined localized surface plasmon resonances in the ultraviolet range as revealed by extinction measurements and confirmed by Mie theory.

High-resolution imaging and spectroscopy of multipolar plasmonic resonances in aluminum nanoantennas.

We report on the high resolution imaging of multipolar plasmonic resonances in aluminum nanoantennas using electron energy loss spectroscopy (EELS). Plasmonic resonances ranging from near-infrared to ultraviolet (UV) are measured. The spatial distributions of the multipolar resonant modes are mapped and their energy dispersion is retrieved. The losses in the aluminum antennas are studied through the full width at half-maximum of the resonances, unveiling the weight of both interband and radiative damping mechanisms of the different multipolar resonances. In the blue-UV spectral range, high order resonant modes present a quality factor up to 8, two times higher than low order resonant modes at the same energy. This study demonstrates that near-infrared to ultraviolet tunable multipolar plasmonic resonances in aluminum nanoantennas with relatively high quality factors can be engineered. Aluminum nanoantennas are thus an appealing alternative to gold or silver ones in the visible and can be efficiently used for UV plasmonics.

Efficient excitation and collection of single- molecule fluorescence close to a dielectric microsphere

Dielectric microspheres illuminated by a tightly focused Gaussian beam can focus light on a tiny spot with subwavelength dimensions along the three directions of space. We report here a detailed experimental and theoretical study of the interaction between a single fluorescent molecule and this peculiar electromagnetic distribution. The microsphere increases the excitation intensity sensed by the molecule up to a factor of 2.2, while at the same time it allows for a collection efficiency of up to 60% by redirecting the light emitted at large incidences toward the optical axis. By combining these two effects, the number of collected fluorescence photons can be increased up to a factor of 5. We quantify the evolution of the excitation and collection contributions with the microsphere dimensions and compare our experimental findings with numerical simulations.

An angle-independent Frequency Selective Surface in the optical range

We suggest and numerically demonstrate a design for Frequency Selective Surfaces (FSS) operating in the optical (visible and near-infrared) range. The position and width of the FSS bandpass do not depend on the angle of incidence and polarization state of the incoming light, allowing high transmission at any angle. The FSS is formed by annular apertures perforated in a metal film and arranged in a square array. Angle- and polarization-independent transmission properties are demonstrated for silver. These results can be extended to other metals as well as to other frequency domains.

Disposable Microscope Objective Lenses for Fluorescence Correlation Spectroscopy Using Latex Microspheres

We explore the combination of a latex microsphere with a low NA lens to form a high performance optical system, and enable the detection of single molecules by fluorescence correlation spectroscopy (FCS). Viable FCS experiments at concentrations 1-1000 nM with different objectives costing less than

Nanoaperture-Enhanced Signal-to-Noise Ratio in Fluorescence Correlation Spectroscopy

40 are demonstrated. This offers a simple and low-cost alternative to the conventional complex microscope objectives.

Near-field probing of active photonic-crystal structures

The fluorescence enhancement found in gold nanoapertures is demonstrated to increase the signal-to-noise ratio (SNR) in fluorescence correlation spectroscopy (FCS). Starting from a general discussion on noise in FCS experiments, we show that fluorescence enhancement leads to a dramatic increase in the SNR. This prediction is confirmed by experiments where we report an experimental gain in SNR of about 1 order of magnitude, corresponding to a 100-fold reduction of the experiment duration. This technique is then applied to monitor the kinetics of a fast enzymatic cleavage reaction. This set of experiments evidence the feasibility of FCS analysis with fast integration times of about 1 s, opening the way to the monitoring of a variety of biochemical reactions at reduced time scales.