Heykel Aouani

Bright Unidirectional Fluorescence Emission of Molecules in a Nanoaperture with Plasmonic Corrugations

Controlling the fluorescence emission from nanoscale quantum emitters is a key element for a wide range of applications, from efficient analytical sensing to quantum information processing. Enhancing the fluorescence intensity and narrowing the emission directivity are both essential features to achieve a full control of fluorescence, yet this is rarely obtained simultaneously with optical nanoantennas. Here we report that gold nanoapertures surrounded by periodic corrugations transform standard fluorescent molecules into bright unidirectional sources. We obtain enhancement factors of the fluorescence count rate per molecule up to 120 fold simultaneously with a directional emission of the fluorescence into a narrow angular cone in the direction normal to the sample plane. The bright emission and narrow directionality enable the detection of single molecules with a low numerical aperture objective, and improve the effectiveness of fluorescence-based applications. We thoroughly quantify the increased light-matter coupling as well as the radiation pattern intensity. These results are highly relevant for the development of single molecule sensing, single-photon sources, and light emitting devices.

Third-harmonic-upconversion enhancement from a single semiconductor nanoparticle coupled to a plasmonic antenna.

The ability to convert low-energy quanta into a quantum of higher energy is of great interest for a variety of applications, including bioimaging, drug delivery and photovoltaics. Although high conversion efficiencies can be achieved using macroscopic nonlinear crystals, upconverting light at the nanometre scale remains challenging because the subwavelength scale of materials prevents the exploitation of phase-matching processes. Light-plasmon interactions that occur in nanostructured noble metals have offered alternative opportunities for nonlinear upconversion of infrared light, but conversion efficiency rates remain extremely low due to the weak penetration of the exciting fields into the metal. Here, we show that third-harmonic generation from an individual semiconductor indium tin oxide nanoparticle is significantly enhanced when coupled within a plasmonic gold dimer. The plasmonic dimer acts as a receiving optical antenna, confining the incident far-field radiation into a near field localized at its gap; the indium tin oxide nanoparticle located at the plasmonic dimer gap acts as a localized nonlinear transmitter upconverting three incident photons at frequency ω into a photon at frequency 3ω. This hybrid nanodevice provides third-harmonic-generation enhancements of up to 10(6)-fold compared with an isolated indium tin oxide nanoparticle, with an effective third-order susceptibility up to 3.5 × 10(3) nm V(-2) and conversion efficiency of 0.0007%. We also show that the upconverted third-harmonic emission can be exploited to probe the near-field intensity at the plasmonic dimer gap.

Multiresonant Broadband Optical Antennas As Efficient Tunable Nanosources of Second Harmonic Light

We report the experimental realization of efficient tunable nanosources of second harmonic light with individual multiresonant log-periodic optical antennas. By designing the nanoantenna with a bandwidth of several octaves, simultaneous enhancement of fundamental and harmonic fields is observed over a broad range of frequencies, leading to a high second harmonic conversion efficiency, together with an effective second order susceptibility within the range of values provided by widespread inorganic crystals. Moreover, the geometrical configuration of the nanoantenna makes the generated second harmonic signal independent from the polarization of the fundamental excitation. These results open new possibilities for the development of efficient integrated nonlinear nanodevices with high frequency tunability.

Plasmonic Antennas for Directional Sorting of Fluorescence Emission

Spontaneous emission of fluorescent molecules or quantum dots is radiated along all directions when emitters are diluted in a liquid solution, which severely limits the amount of collected light. Besides, the emission direction does not carry any useful information and cannot be used to sort different molecules. To go beyond these limits, optical antennas have been recently introduced as conceptual tools to control the radiation properties for nanoemitters fixed on a substrate. Despite intense recent research, controlling the luminescence directivity remains a challenge for emitters with random positions and orientations, which is a key for several biomolecular screening applications. Here, we present full directional control of the fluorescence emission from molecules in water solution by an optical antenna made of a nanoaperture surrounded by a periodic set of shallow grooves in a gold film. For each emission wavelength, the fluorescence beam can be directed along a specific direction with a given angular width, hereby realizing a micrometer-size dispersive antenna. We demonstrate the fluorescence beaming results from an interference phenomenon and provide physical optics guidelines to control the fluorescence directivity by tuning the groove-nanoaperture distance. This photon-sorting capability provides a new approach for high-sensitivity screening of molecular species in solution.

Ultrasensitive broadband probing of molecular vibrational modes with multifrequency optical antennas.

Optical antennas represent an enabling technology for enhancing the detection of molecular vibrational signatures at low concentrations and probing the chemical composition of a sample in order to identify target molecules. However, efficiently detecting different vibrational modes to determine the presence (or the absence) of a molecular species requires a multispectral interrogation in a window of several micrometers, as many molecules present informative fingerprint spectra in the mid-infrared between 2.5 and 10 μm. As most nanoantennas exhibit a narrow-band response because of their dipolar nature, they are not suitable for such applications. Here, we propose the use of multifrequency optical antennas designed for operating with a bandwidth of several octaves. We demonstrate that surface-enhanced infrared absorption gains in the order of 10(5) can be easily obtained in a spectral window of 3 μm with attomolar concentrations of molecules, providing new opportunities for ultrasensitive broadband detection of molecular species via vibrational spectroscopy techniques.

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

Optical-fiber-microsphere for remote fluorescence correlation spectroscopy

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

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

Fluorescence correlation spectroscopy (FCS) is a versatile method that would greatly benefit to remote optical-fiber fluorescence sensors. However, the current state-of-the-art struggles with high background and low detection sensitivities that prevent the extension of fiber-based FCS down to the single-molecule level. Here we report the use of an optical fiber combined with a latex microsphere to perform FCS analysis. The sensitivity of the technique is demonstrated at the single molecule level thanks to a photonic nanojet effect. This offers new opportunities for reducing the bulky microscope setup and extending FCS to remote or in vivo applications.

Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations

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.

Colloidal quantum dots as probes of excitation field enhancement in photonic antennas.

We investigate the influence of circular corrugations surrounding a central nanoaperture to further enhance the fluorescence count rate per emitter and control its emission directionality. Adding a single corrugation already allows to significantly increase the fluorescence signal as compared to a bare nanoaperture. A complete fluorescence characterization quantifies the excitation and emission gains contributing to the fluorescence enhancement process as the number of corrugations is increased.