Olivier Demichel

Delocalization of Nonlinear Optical Responses in Plasmonic Nanoantennas.

Remote excitation and emission of two-photon luminescence and second-harmonic generation are observed in micrometer long gold rod optical antennas upon local illumination with a tightly focused near-infrared femtosecond laser beam. We show that these nonlinear radiations are emitted from the entire antenna and the measured far-field angular patterns bear the information regarding the nature and origins of the respective nonlinear processes. We demonstrate that the nonlinear responses are locally induced by a propagating surface plasmon at the excitation frequency, enabling thereby a polariton-mediated spatial tailoring and design of coherent and incoherent nonlinear responses.

Near-Field Properties of Plasmonic Nanostructures with High Aspect Ratio

Using the Greens dyad technique based on cuboidal meshing, we compute the electromagnetic field scattered by metal nanorods with high aspect ratio. We investigate the effect of the meshing shape on the numerical simulations. We observe that discretizing the object with cells with aspect ratios similar to the objects aspect ratio improves the computations, without degrading the convergency. We also compare our numerical simulations to finite element method and discuss further possible improvements.

High-order modes in cavity-resonator-integrated guided-mode resonance filters (CRIGFs).

Cavity-resonator-integrated guided-mode resonance filters (CRIGFs) are optical filters based on weak coupling by a grating between a free-space propagating optical mode and a guided mode, like guided-mode resonance filters (GMRFs). As compared to GMRFs they offer narrowband reflection with small aperture and high angular acceptance. We report experimental characterization and theoretical modeling of unexpected high-order reflected modes in such devices. Using coupled-mode modeling and moiré analysis we provide physical insight on key mechanisms ruling CRIGF properties. This model could serve as a simple and efficient framework to design new reflectors with tailored spatial and spectral modal reflectivities.

Selective excitation of bright and dark plasmonic resonances of single gold nanorods.

Plasmonic dark modes are pure near-field resonances since their dipole moments are vanishing in far field. These modes are particularly interesting to enhance nonlinear light-matter interaction at the nanometer scale because radiative losses are mitigated therefore increasing the intrinsic lifetime of the resonances. However, the excitation of dark modes by standard far field approaches is generally inefficient because the symmetry of the electromagnetic near-field distribution has a poor overlap with the excitation field. Here, we demonstrate the selective optical excitation of bright and dark plasmonic modes of single gold nanorods by spatial phase-shaping the excitation beam. Using two-photon luminescence measurements, we unambiguously identify the symmetry and the order of the emitting modes and analyze their angular distribution by Fourier-space imaging.

Improving the transmittance of an epsilon-near-zero-based wavefront shaper

Although epsilon-near-zero (ENZ) metamaterials offer many unconventional ways to play with light, the optical impedance mismatch with surroundings can limit the efficiency of future devices. We report here on the improvement of the transmittance of an ENZ wavefront shaper. In this Letter, we first address the way to enhance the transmittance of a plane wave through a layer of ENZ material, thanks to a numerical optimization approach based on the transfer matrix method. We then transpose the one-dimensional approach to a two-dimensional case where the emission of a dipole is shaped into a plane wave by an ENZ device with a design that optimizes the transmittance. As a result, we demonstrate a transmittance efficiency of 15% that is four orders of magnitude higher than previous devices proposed in the literature for wavefront shaping applications. This Letter aims to pave the way for future efficient ENZ devices by offering new strategies to optimize the transmittance through ENZ materials.

Hot electron generation and dynamics within plasmonic nano-antenna (Conference Presentation)

Hot carriers are energetic photoexcited carriers driving a large range of chemicophysical mechanisms. At the nanoscale, an efficient generation of these carriers is facilitated by illuminating plasmonic antennas. However, the ultrafast relaxation rate severally impedes their deployment in future hot-carrier based devices. In this paper, we report on the picosecond relaxation dynamics of hot carriers in plasmonic monocrystalline gold nanoantennas. The ultrafast dynamics of the hot carriers is experimentally investigated by interrogating the nonlinear photoluminescence response of the antenna [1]. From this investigation, we reveal some leverages to control the dynamics of such hot carriers within nano antenna. In particular, an increase by a factor up to five of this dynamics (from 0.5 ps to 2.5 ps) is observed for resonant nanoantenna compared to off-resonance antenna and when excitation power increases. By a two temperature model we model quantitatively the dynamics of hot carriers and we demonstrate the nonlinear generation of these carriers. The control over the carrier dynamics should allow to employ their energy more effieciently within physico-chemical processes. In a second part, we investigate the hot carrier dynamics with a spectrally resolved two-pulse correlation configuration, and demonstrate that the relaxation of the photoexcited carriers depends of their energies relative to the Fermi level. We find a 60% variation in the relaxation rate for electron−hole pair energies ranging from ca. 0.2 to 1.8 eV. The quantitative relationship between hot-carrier energy and relaxation dynamics is an important finding for optimizing hot-carrier-assisted processes and shed new light on the intricacy of nonlinear photoluminescence in plasmonic [2]. [1] O. Demichel et al, ACS Photonics 3, 791 (2016) [2] R. Mejard et al, ACS Photonics 3, 1482 (2016)

Hot electrons and nonlinear optical nanoantennas

The large field enhancement generated at the surface of a resonant plasmonic nanoparticle, or optical antennas, is the key mechanism that eventually led to the development of nonlinear plasmonics [1-2]. While the resonance may boost the nonlinear yield of an adjacent structure or surrounding medium, it was soon realized that optical antennas possess nonlinear coefficients comparable or exceeding those of standard nonlinear optical materials [3]. We discuss here two nonlinear optical processes — incoherent multi-photon luminescence (MPL) and coherent second-harmonic generation (SHG) — emitted from gold rod optical antennas upon local illumination with a tightly focused femtosecond near-infrared laser beam.

Silicon-microring into a fiber laser cavity for high-repetition-rate pulse train generation

In 1997, Yoshida et al. inserted a Fabry-Perot filter in a modulation instability fiber laser cavity [1], the free spectral range (FSR) of the Fabry-Perot fixed the RF to 115 GHz; however the pulsed laser was poorly stable. Since then, lasers of increasing performance have been demonstrated using variants of this method. In 2012, Peccianti et al. demonstrated the first fiber laser harmonically mode-locked by integrated high-finesse microresonator [2]. The doped silica, on-chip microresonator provided both high spectral selectivity and nonlinearity, thus promoting the dynamics pulsed at 200 GHz. By using a silicon microring resonator (SMRR), this approach lead to the recent realization of 110 GHz-RF mode-locked fiber laser [3]. Working with silicon takes advantage of the huge investment and experience from the microelectronics industry, and contributes to the development of a monolithic platform for optoelectronics [4]. The high Kerr nonlinearity of silicon is instrumental to induce mode locking with low pumping threshold. However, at the main telecom wavelength (1.55 μm), two photo absorption, free-carriers dispersion and their thermalization have to be considered [5], and can be detrimental to formation of the ultrafast dynamics.

Towards an efficient epsilon near-zero-based wavefront shaper

Although epsilon-near-zero (ENZ) metamaterials offer many unconventional ways to play with light, the optical impedance mismatch with surroundings can limit the efficiency of future devices. An original example of ENZ-based applications is the wavefront shaping, but up to now devices have transmission efficiency as low as 10-5 [1]. Here, we report strategies to enhance the transmittance through ENZ layer and we demonstrate an enhancement by four orders of magnitude of the transmittance, which reaches up to 15% in the context of ENZ-based wavefront shaping [2].

Single-Crystal vs Polycrystalline Gold: A Non-linear-Optics Analysis

Standard gold in the field of plasmonics is obtained by evaporation or sputtering and therefore is polycrystalline. Yet, this gold presents numbers of drawbacks such as roughness, grains and ill-defined electronic band diagrams in addition to the lack of reproducibility from one instrument to another. It is, thus, beneficial to turn to a metal production that can enable well-defined and controlled gold parameters. To that end, we have explored the wet synthesis of gold nanoplates which represents a simple and robust means of obtaining single-crystal gold (Guo Z, Zhang Y, DuanMu Y, Xu L, Xie S, Gu N, Colloids Surf A 278:33–38, 2006). The synthesized nanoplates are from 50 to less than 100 nm in thickness and can span over micrometers in lateral dimensions corresponding to areas of several hundreds of μm2. They can thus be considered as thin film material perfectly suitable for plasmonic applications.