Vincent Juvé

En passant de l’état massif à la nanoparticule les matériaux métalliques voient certaines de leurs caractéristiques modifiées de manière notable comme par exemple les propriétés optiques avec l’apparition d’une résonance dans le spectre optique, la Résonance Plasmon de Surface Localisée (RPSL) responsable du changement de couleur des nanoparticules métalliques. Les propriétés vibrationnelles et thermiques de nanoparticules métalliques ont été étudiées à l’aide d’une technique de Spectroscopie Femtoseconde. Nous avons montré qu’il était possible d’exciter et de détecter optiquement des fréquences de vibrations mécaniques dans le domaine térahertz pour des nanoparticules de platine composées de moins de cent atomes. D’autre part l’augmentation des effets dus aux interfaces a été mis en évidence sur les propriétés thermiques de nanoparticules d’or et d’argent. La résistance thermique à l’interface, résistance de Kapitza, voit son rôle augmenter lors du transfert thermique à l’échelle nanométrique. Une corrélation entre les valeurs mesurées et les impédances acoustiques des matériaux composants les interfaces a été mise en évidence. Nous avons aussi montré qu’elle augmente quand la température diminue de 300K à 70K. Les propriétés optiques de nanoparticules non sphériques ont été étudiées à l’aide de la Spectroscopie à Modulation Spatiale. Cette technique a permis de repérer puis de caractériser des nano-bâtonnets d’or individuels. Nous avons montré que la largeur spectrale de la RPSL est fortement dépendante de la géométrie des nanoparticules (diamètre et longueur). Cette double dépendance n’est pas prédite par les modèles classiques ou quantique existants

In this perspectives paper, we discuss the role of optical anisotropy in detecting coherent acoustic phonons in a time-domain Brillouin experiment. First, we present the general theoretical background to the optical detection of acoustic phonons in a uniaxial material. We then illustrate this theory experimentally by studying highly birefringent BiFeO3 material as a case study. We demonstrate how the amplitude of the time-domain Brillouin signal of both longitudinal and shear phonons can be controlled by selecting the polarization of the probe beam (ordinary or extraordinary). Using classical electrodynamics combined with first-principles calculation of photoelastic coefficients, we find a good qualitative agreement with experiments. Besides the general demonstration of the importance of optical anisotropy, we demonstrate that BiFeO3 exhibits comparable photoelastic coefficients to the technologically significant LiNbO3 and LiTaO3 materials. These findings could lead to the development of BiFeO3-based sub-THz acousto-optic devices. In addition to ferroelectrics, our comprehensive description of the coherent acoustic phonon detection process could, in the future, be extended to other birefringent functional oxides such as TiO2, ZnO, and distorted perovskite systems (ABO3), as well as polar semiconductors such as GaN and two-dimensional and van der Waals materials.

In this paper, we develop a method that combines optical birefringence properties and time-domain Brillouin scattering microscopy to determine in situ the optical axis orientation of each single micrometer size grain in a polycrystalline sample. We illustrate the method by investigating the room temperature multiferroic material BiFeO3 where the optical axis coincides with the ferroelectric polarization direction. We are able to find the grain orientation and also provide the sound velocity (longitudinal and transverse) since the method is based on the Brillouin scattering process. These advances open interesting perspectives for probing the anisotropy of a micrometer size grain with an extension to the evaluation of the ferroelastic domain orientation in a non-contact and non-destructive manner.

Superlattices are materials created by the alternating growth of two chemically different materials. The direct consequence of creating a superlattice is the folding of the Brillouin zone, which gives rise to additional electronic bands and phonon modes. This phenomenon has been successfully exploited to achieve new transport and optical properties in semiconductor superlattices. Here, we show that multiferroic BiFeO3/LaFeO3 superlattices exhibit several structural orders parallel and perpendicular to the growth direction, not existing in individual bulk materials. Using transmission electron microscopy, x-ray diffraction, and first-principles calculations, we reveal in particular a new long-range order of tilted FeO6 octahedra, with a period along the growth direction about twice that of the chemical supercell, i.e., a superorder. The effect of this new structural order on the phonon dynamics is studied with ultrafast optical pump-probe experiments. While a folded-mode at 1.2 THz is attributed solely to the chemical modulation of the superlattice, the existence of another 0.7 THz mode seems to be explained only by a double Brillouin zone folding in agreement with the structural out-of-plane superorder. Our work shows that multiferroic BiFeO3/LaFeO3 superlattices can be used to tune the spectrum of coherent THz phonons, and potentially that of magnons or electromagnons.

Ultrashort light pulses induce rapid deformations of crystalline lattices. In ferroelectrics, lattice deformations couple directly to the polarization, which opens the perspective to modulate the electric polarization on an ultrafast time scale. Here, we report on the temporal and spatial tracking of strain and polar modulation in a single-domain BiFeO ₃ thin film by ultrashort light pulses. To map the light-induced deformation of the BiFeO ₃ unit cell, we perform time-resolved optical reflectivity and time-resolved x-ray diffraction. We show that an optical femtosecond laser pulse generates not only longitudinal but also shear strains. The longitudinal strain peaks at a large amplitude of 0.6%. The access of both the longitudinal and shear strains enables to quantitatively reconstruct the ultrafast deformation of the unit cell and to infer the corresponding reorientation of the ferroelectric polarization direction in space and time. Our findings open new perspectives for ultrafast manipulation of strain-coupled ferroic orders.

Spin/charge interconversion mechanisms provide an essential handle to generate and detect spin currents. Their applications at different timescales are critical in spintronics since they cover a technologically relevant broadband spectrum. While the inverse spin Hall effect is known to be robust from quasi-static to sub-picosecond timescales, the conversion efficiency evolution of the inverse Edelstein effect has not been addressed yet. In this work, we report that while the quasi-static response of the inverse Edelstein effect can be comparable to that of the most efficient inverse spin Hall systems, a drastic drop of efficiency is observed in the terahertz (THz) regime. This behavior at the sub-picosecond timescale is qualitatively understood from the dependence of the inverse Edelstein effect on the energy distribution of spin-carrier entities, which is different between thermalized carriers in the quasi-static regime and hot carriers generated by light pulses. This finding is supported by the pump-laser wavelength dependence in the THz regime for the inverse Edelstein effect, which offers a promising route for tunability of spintronic devices.

Bimetallic Au/Ag core–shell cuboid nanoparticles (NPs) exhibit a complex plasmonic response dominated by a dipolar longitudinal mode and higher-order transverse modes in the near-UV, which may be exploited for a range of applications. In this paper, we take advantage of the strong signature of these modes in the NP ultrafast transient optical response, measured by pump-probe transient absorption (TA) spectroscopy, to explore the NP vibrational landscape. The fast Fourier transform analysis of the TA dynamics reveals specific vibration modes in the frequency range 15–150 GHz, further studied by numerical simulations based on the finite element method. While bare Au nanorods exhibit extensional and breathing modes, the bimetallic NPs undergo more complex motions, involving the displacement of facets, edges and corners. The amplitude and frequency of these modes are shown to depend on the Ag shell thickness, as the silver load modifies the NP aspect ratio and mass. Moreover, the contributions of the vibrational modes to the experimental TA spectra are shown to vary with the probe laser wavelength at which the signal is monitored. Using the combined simulations of the NP elastic and optical properties, we elucidate this influence by analyzing the effect of the mechanisms involved in the acousto-plasmonic coupling.

We report the generation of coherent acoustic phonons in materials with terahertz ultrashort pulses. This is demonstrated in metals and topological insulators by exciting an acoustic eigenmode in nanometric-sized thin films. The efficiency of the coupling is quadratic in the terahertz electric field strength within the range of investigation. Owing to a quantitative comparison between terahertz and near-infrared ultrashort pulse excitations, we show that the process of acoustic phonon generation by terahertz radiation is mainly driven by thermoelastic stress. While for the near-infrared light excitation the lattice temperature increase comes from a rapid energy transfer from the hot carriers to the phonon bath during carrier intraband relaxation, the thermoelastic stress induced by the terahertz electric field is linked to the scattering of the accelerated electrons leading to an ultrafast Joule effect.