Julien Burgin

Damping of acoustic vibrations in gold nanoparticles

Studies of acoustic vibrations in nanometre-scale particles can provide fundamental insights into the mechanical properties of materials because it is possible to precisely characterize and control the crystallinity and geometry of such nanostructures. Metal nanoparticles are of particular interest because they allow the use of ultrafast laser pulses to generate and probe high-frequency acoustic vibrations, which have the potential to be used in a variety of sensing applications. So far, the decay of these vibrations has been dominated by dephasing due to variations in nanoparticle size. Such inhomogeneities can be eliminated by performing measurements on single nanoparticles deposited on a substrate, but unknown interactions between the nanoparticles and the substrate make it difficult to interpret the results of such experiments. Here, we show that the effects of inhomogeneous damping can be reduced by using bipyramidal gold nanoparticles with highly uniform sizes. The inferred homogeneous damping is due to the combination of damping intrinsic to the nanoparticles and the surrounding solvent; the latter is quantitatively described by a parameter-free model.

Surface Plasmon Resonance Properties of Single Elongated Nano-objects: Gold Nanobipyramids and Nanorods

The spectral characteristics (wavelength and line width) and the optical extinction cross-section of the longitudinal localized surface plasmon resonance (LSPR) of individual gold nanobipyramids have been quantitatively measured using the spatial modulation spectroscopy technique. The morphology of the same individual nanoparticles has been determined by transmission electron microscopy (TEM). The experimental results are thus interpreted with a numerical model using the TEM measured sizes of the particles as an input, and either including the substrate or assuming a mean homogeneous environment. Results are compared to those obtained for individual nanorods and also show the importance of the local environment of the particle on the detailed description of its spectral position and extinction amplitude.

Optical properties and relaxation processes at femtosecond scale of bimetallic clusters

The optical properties of Au-Ag and Ni-Ag clusters are measured by linear optical absorption spectroscopy and the time-resolved pump-probe femtosecond technique allowing a study of the influence of alloy or core-shell structure.

3D morphology of Au and Au@Ag nanobipyramids

The morphologies of Au and Au@Ag nanobipyramids were investigated using electron tomography. The 3D reconstruction reveals that the Au bipyramids have an irregular six-fold twinning structure with highly stepped dominant {151} facets. These short steps/edges stabilized via surface adsorbed CTAB favor the growth of silver on the lateral facets leading to strong blue shifts in longitudinal plasmon surface resonance.

Acoustic vibrations of Au nano-bipyramids and their modification under Ag deposition: a perspective for the development of nanobalances.

We investigated the acoustic vibrations of gold nanobipyramids and bimetallic gold-silver core-shell bipyramids, synthesized by wet chemistry techniques, using a high-sensitivity pump-probe femtosecond setup. Three modes were observed and characterized in the gold core particles for lengths varying from 49 to 170 nm and diameters varying from 20 to 40 nm. The two strongest modes have been associated with the fundamental extensional and its first harmonic, and a weak mode has been associated with the fundamental radial mode, in very good agreement with numerical simulations. We then derived linear laws linking the periods to the dimensions both experimentally and numerically. To go further, we investigated the evolution of these modes under silver deposition on gold core bipyramids. We studied the evolution of the periods of the extensional modes, which were found to be in good qualitative agreement with numerical simulations. Moreover, we observed a strong enhancement of the radial mode amplitude when silver is deposited: we are typically sensitive to the deposition of 40 attograms of silver per gold core particle. This opens up possible applications in the field of mass sensing, where metallic nanobalances have an important role to play, taking advantage of their robustness and versatility.

Femtosecond investigation of the non-instantaneous third-order nonlinear suceptibility in liquids and glasses

The symmetry of the noninstantaneous Kerr susceptibility is investigated in different liquids and glasses using a time-resolved two-beam energy transfer technique with pulses in the 100–15 fs range. The pulse duration dependence of the ratio of the isotropic χxxxx(3) to anisotropic χxyyx(3) tensor elements is demonstrated in liquid CS2 and in silica, showing that the elementary mechanisms mediating the observed optical beam energy transfers are modified for short pulses. This effect is ascribed to alteration of the nuclear contribution and increasing influence of the electronic one.

Femtosecond spectroscopy of defect modes in silica glasses

The D1 and D2 defect modes are investigated in the time domain in normal and densified silica using a high sensitivity femtosecond pump-probe technique with 15fs pulses. Their frequency and width are precisely determined even when they are partly masked by a broad background in spontaneous Raman spectroscopy. These results open up many possibility for investigation of local structures in glasses.

Femtosecond time-resolved investigation of the vibrational modes of vitreous GeO2

The vibrational response of vitreous GeO2 is investigated using an impulsive stimulated Raman scattering technique in the femtosecond regime. The results yield evidence for a weak vibrational mode ascribed to oxygen motion in three-membered planar ring structures. Its frequency and damping are determined and compared to theoretical predictions.