Arnaud Arbouet

Plasmonic Pumping of Excitonic Photoluminescence in Hybrid MoS2–Au Nanostructures

We report on the fabrication of monolayer MoS2-coated gold nanoantennas combining chemical vapor deposition, e-beam lithography surface patterning, and a soft lift-off/transfer technique. The optical properties of these hybrid plasmonic-excitonic nanostructures are investigated using spatially resolved photoluminescence spectroscopy. Off- and in-resonance plasmonic pumping of the MoS2 excitonic luminescence showed distinct behaviors. For plasmonically mediated pumping, we found a significant enhancement (∼65%) of the photoluminescence intensity, clear evidence that the optical properties of the MoS2 monolayer are strongly influenced by the nanoantenna surface plasmons. In addition, a systematic photoluminescence broadening and red-shift in nanoantenna locations is observed which is interpreted in terms of plasmonic enhanced optical absorption and subsequent heating of the MoS2 monolayers. Using a temperature calibration procedure based on photoluminescence spectral characteristics, we were able to estimate the local temperature changes. We found that the plasmonically induced MoS2 temperature increase is nearly four times larger than in the MoS2 reference temperatures. This study shines light on the plasmonic-excitonic interaction in these hybrid metal/semiconductor nanostructures and provides a unique approach for the engineering of optoelectronic devices based on the light-to-current conversion.

Surface Plasmon Damping Quantified with an Electron Nanoprobe

Fabrication and synthesis of plasmonic structures is rapidly moving towards sub-nanometer accuracy in control over shape and inter-particle distance. This holds the promise for developing device components based on novel, non-classical electro-optical effects. Monochromated electron energy-loss spectroscopy (EELS) has in recent years demonstrated its value as a qualitative experimental technique in nano-optics and plasmonic due to its unprecedented spatial resolution. Here, we demonstrate that EELS can also be used quantitatively, to probe surface plasmon kinetics and damping in single nanostructures. Using this approach, we present from a large (>50) series of individual gold nanoparticles the plasmon Quality factors and the plasmon Dephasing times, as a function of energy/frequency. It is shown that the measured general trend applies to regular particle shapes (rods, spheres) as well as irregular shapes (dendritic, branched morphologies). The combination of direct sub-nanometer imaging with EELS-based plasmon damping analysis launches quantitative nanoplasmonics research into the sub-nanometer realm.

Plasmonic Nanoparticle Networks for Light and Heat Concentration

Self-assembled plasmonic nanoparticle networks (PNN) composed of chains of 12 nm diameter crystalline gold nanoparticles exhibit a longitudinally coupled plasmon mode centered at 700 nm. We have exploited this longitudinal absorption band to efficiently confine light fields and concentrate heat sources in the close vicinity of these plasmonic chain networks. The mapping of the two phenomena on the same superstructures was performed by combining two-photon luminescence and fluorescence polarization anisotropy imaging techniques. Besides the light and heat concentration, we show experimentally that the planar spatial distribution of optical field intensity can be simply modulated by controlling the linear polarization of the incident optical excitation. On the contrary, the heat production, which is obtained here by exciting the structures within the optically transparent window of biological tissues, is evenly spread over the entire PNN. This contrasts with the usual case of localized heating in continuous nanowires, thus opening opportunities for these networks in light-induced hyperthermia applications. Furthermore, we propose a unified theoretical framework to account for both the nonlinear optical and thermal near-fields around PNN. The associated numerical simulations, based on a Greens function formalism, are in excellent agreement with the experimental images. This formalism therefore provides a versatile tool for the accurate engineering of optical and thermodynamical properties of complex plasmonic colloidal architectures.

Optimal polarization conversion in coupled dimer plasmonic nanoantennas for metasurfaces

We demonstrate that polarization conversion in coupled dimer antennas, used in phase discontinuity metasurfaces, can be tuned by careful design. By controlling the gap width, a strong variation of the coupling strength and polarization conversion is found between capacitively and conductively coupled antennas. A theoretical two-oscillator model is proposed, which shows a universal scaling of the degree of polarization conversion with the energy splitting of the symmetric and antisymmetric modes supported by the antennas. Using single antenna spectroscopy, we find good agreement for the scaling of mode splitting and polarization conversion with gap width over the range from capacitive to conductive coupling. Next to linear polarization conversion, we demonstrate single-antenna linear to circular polarization conversion. Our results provide strategies for phase-discontinuity metasurfaces and ultracompact polarization optics.

Damping of the acoustic vibrations of individual gold nanoparticles.

In this letter, the ultrafast vibrational dynamics of individual gold nanorings has been investigated by femtosecond transient absorption spectroscopy. Two acoustic vibration modes have been detected and identified. The influence of the mechanical coupling at the nanoparticle/substrate interface on the acoustic vibrations of the nano-objects is discussed. Moreover, by changing the environment of the nanoring, we provide a clear evidence of the impact of the surrounding medium on the damping of the acoustic vibrations. Such results are reported here for the first time on individual nanoparticles. This work points out a new sensing method based on the sensitivity of the acoustic vibration damping to the surrounding medium.

Evaluation of infrared femtosecond laser ablation for the analysis of geomaterials by ICP-MS

The capabilities of an infrared (IR) Ti:sapphire femtosecond laser (≈800 nm) to ablate and analyze geomaterials such as monazite, zircon and synthetic glass reference materials is evaluated, with emphasis on U/Pb ratio determinations useful for dating accessory minerals in rocks. We particularly discuss the influence of pulse duration (respectively 60, 200, 350, 500, 670, 830, 2000 and 3000 fs) on the internal precision (2 min ablation), reproducibility over two weeks and accuracy of quadrupole ICP-MS measurements. The best results for all these criteria are obtained when using the shortest pulse duration (60 fs). It was found that internal precision and reproducibility were improved by a factor of 3 and 4, respectively, from picosecond to 60 fs pulsewidths. Reproducibility at this pulse duration for U/Pb ratio determinations is of 2% RSD or better, depending on the material analyzed, and this ratio is accurate within this uncertainty. Lead isotopic ratios also benefit from the shortest pulsewidth. They are measured at 60 fs with a precision (<0.5% RSD) approaching the limitations of quadrupole ICP-MS. Preliminary data were also obtained using the 3rd harmonic (≈266 nm) of the Ti:sapphire fundamental wavelength and they are compared with the infrared mode. There seems to be no obvious analytical benefit to switch from IR to UV in the femtosecond laser ablation regime. Analyses of zircon 91500 with IR pulses led to better repeatability, around 0.9% (10 values, 1σ), compared to 3% for the UV pulses. The accuracy appears to be comparable for the two wavelengths.

Acousto-plasmonic and surface-enhanced Raman scattering properties of coupled gold nanospheres/nanodisk trimers.

This work is devoted to the fundamental understanding of the interaction between acoustic vibrations and surface plasmons in metallic nano-objects. The acoustoplasmonic properties of coupled spherical gold nanoparticles and nanodisk trimers are investigated experimentally by optical transmission measurements and resonant Raman scattering experiments. For excitation close to resonance with the localized surface plasmons of the nanodisk trimers, we are able to detect several intense Raman bands generated by the spherical gold nanoparticles. On the basis of both vibrational dynamics calculations and Raman selection rules, the measured Raman bands are assigned to fundamental and overtones of the quadrupolar and breathing vibration modes of the spherical gold nanoparticles. Simulations of the electric near-field intensity maps performed at the Raman probe wavelengths showed strong localization of the optical energy in the vicinity of the nanodisk trimers, thus corroborating the role of the interaction between the acoustic vibrations of the spherical nanoparticles and the surface plasmons of the nanodisk trimers. Acoustic phonons surface enhanced Raman scattering is here demonstrated for the first time for such coupled plasmonic systems. This work paves the way to surface plasmon engineering for sensing the vibrational properties of nanoparticles.

Charge distribution induced inside complex plasmonic nanoparticles

We developed a versatile numerical technique to compute the three-dimensional charge distribution inside plasmonic nanoparticles. This method can be easily applied to investigate the charge distribution inside arbitrarily complex plasmonic nanostructures and to identify the nature of the multipolar plasmon modes involved at plasmonic resonances. Its ability to unravel the physical origin of plasmonic spectral features is demonstrated in the case of a single gold nanotriangle and of a gold nano-antenna. Finally, we show how the volume charge distribution can be used to define and compute the first terms of the multipolar expansion.

Gold nanoring trimers: a versatile structure for infrared sensing

In this work we report on the observation of surface plasmon properties of periodic arrays of gold nanoring trimers fabricated by electron beam lithography. It is shown that the localized surface plasmon resonances of such gold ring trimers occur in the infrared spectral region and are strongly influenced by the nanoring geometry and their relative positions. Based on numerical simulations of the optical extinction spectra and of the electric near-field intensity maps, the resonances are assigned to surface plasmon states arising from the strong intra-trimer electromagnetic interaction. We show that the nanoring trimer configuration allows for generating infrared surface plasmon resonances associated with strongly localized electromagnetic energy, thus providing plasmonic nanoresonators well-suited for sensing and surface enhanced near-infrared Raman spectroscopy.

AOPDF-shaped optical parametric amplifier output in the visible

Time shaping of ultra-short visible pulses has been performed using a specially designed acousto-optic programmable dispersive filter of 50% efficiency at the output of a two-stage non-collinear optical parametric amplifier. The set-up is compact and reliable. It provides a tunable shaped source in the visible with unique features: a 4-ps shaping window with preserved tunability over 500–650 nm, and pulses as short as 30 fs. Several-μJ output energy is easily obtained.