Gwenaelle Vaudel

Giant ultrafast photo-induced shear strain in ferroelectric BiFeO3

Generation of strain using light is a key issue for future development of ultrasonic devices. Up to now, photo-induced GHz-THz acoustic phonons have been mainly explored in metals and semiconductors, and in artificial nanostructures to enhance their phononic emission. However, despite their inherent strong polarization (providing natural asymmetry) and superior piezoelectric properties, ferroelectric oxides have been only poorly regarded. Here, by using ultrafast optical pump-probe measurements, we show that photogeneration/photodetection of coherent phonons in BiFeO3 ferroelectric leads, at room temperature, to the largest intensity ratio ever reported of GHz transverse acoustic wave versus the longitudinal one. It is found that the major mechanism involved corresponds to screening of the internal electric fields by light-induced charges, which in turn induces stress by inverse piezoelectric effect. This giant opto-acoustic response opens new perspectives for the use of ferroelectric oxides in ultrahigh frequency acoustic devices and the development of new GHz-THz acoustic sources.

Nanoscale noncontact subsurface investigations of mechanical and optical properties of nanoporous low-k material thin film.

Revealing defects and inhomogeneities of physical and chemical properties beneath a surface or an interface with in-depth nanometric resolution plays a pivotal role for a high degree of reliability in nanomanufacturing processes and in materials science more generally. (1, 2) Nanoscale noncontact depth profiling of mechanical and optical properties of transparent sub-micrometric low-k material film exhibiting inhomogeneities is here achieved by picosecond acoustics interferometry. On the basis of the optical detection through the time-resolved Brillouin scattering of the propagation of a picosecond acoustic pulse, depth profiles of acoustical velocity and optical refractive index are measured simultaneously with spatial resolution of tens of nanometers. Furthermore, measuring the magnitude of this Brillouin signal provides an original method for depth profiling of photoelastic moduli. This development of a new opto-acoustical nanometrology paves the way for in-depth inspection and for subsurface nanoscale imaging of inorganic- and organic-based materials.

Elasticity of an Assembly of Disordered Nanoparticles Interacting via Either van der Waals-Bonded or Covalent-Bonded Coating Layers

Tailoring physical and chemical properties at the nanoscale by assembling nanoparticles currently paves the way for new functional materials. Obtaining the desired macroscopic properties is usually determined by a perfect control of the contact between nanoparticles. Therefore, the physics and chemistry of nanocontacts are one of the central issues for the design of the nanocomposites. Since the birth of atomic force microscopy, crucial advances have been achieved in the quantitative evaluation of van der Waals and Casimir forces in nanostructures and of adhesion between the nanoparticles. We present here an investigation, by a noncontact method, of the elasticity of an assembly of nanoparticles interacting via either van der Waals-bonded or covalent-bonded coating layers. We demonstrate indeed that the ultrafast opto-acoustic technique, based on the generation and detection of hypersound by femtosecond laser pulses, is very sensitive to probe the properties of the nanocontacts. In particular, we observe and evaluate how much the subnanometric molecules present at nanocontacts influence the coherent acoustic phonon propagation along the network of the interconnected silica nanoparticles. Finally, we show that this ultrafast opto-acoustic technique provides quantitative estimates of the rigidity/stiffness of the nanocontacts.

Photoexcitation of gigahertz longitudinal and shear acoustic waves in BiFeO3 multiferroic single crystal

Using femtosecond laser pulses, coherent GHz acoustic phonons are efficiently photogenerated and photodetected in BiFeO3 (BFO) multiferroic single crystal. Due to the crystal lattice symmetry, longitudinal as well as two transverse acoustic modes are generated and detected, and the corresponding sound velocities are determined. This provides the opportunity to experimentally evaluate the elastic coefficients of the multiferroic compound BiFeO3 that have been estimated so far only through ab initio calculations. The knowledge of the elastic properties of BFO is highly desired for BFO integration in nanoelectronic devices. Moreover, our findings highlight also that BFO may be a good candidate for light-controlled coherent acoustic phonons sources.

Picosecond acoustics in p-doped piezoelectric semiconductors

We demonstrate by experiment and theoretical analysis that the presence of built-in electric fields near the (111) and (1¯1¯1¯) surfaces of p-doped GaAs causes efficient generation of acoustic waves due to the laser-induced inverse piezoelectric effect. At the same time, the generation efficiency from the electron-hole-phonon deformation potential is shown to be reduced. The polarity of the acoustic pulse is inverted when changing the laser irradiated surface from (111) to (1¯1¯1¯). The results have ramifications for optically controlled piezoelectric ultrasound transducers.

Jones matrix formalism for the theory of picosecond shear acoustic pulse detection

A theoretical analysis of the transient optical reflectivity of a sample by a normalized Jones matrix is presented. The off-diagonal components of the normalized matrix are identified with the complex rotation of the polarization ellipse. Transient optical polarimetry is a relevant technique to detect shear acoustic strain pulses propagating normally to the surface of an optically isotropic sample. Moreover, polarimetry has a selective sensitivity to shear waves, as this technique cannot detect longitudinal waves that propagate normally to the sample surface.

Ultrafast acousto-plasmonics in gold nanoparticle superlattices

We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonon generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon. These results demonstrate how it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures.

Depth-profiling of elastic and optical inhomogeneities in transparent materials by picosecond ultrasonic interferometry: Theory

The theoretical backgrounds for the depth-profiling of the optically transparent materials by picosecond ultrasonic interferometry are developed. The mathematical description of the light reflection from inhomogeneous transparent films or coatings is proposed. The inhomogeneity can be caused both by the film synthesis (intrinsic stationary inhomogeneity) and by the short acoustic transients launched in the film (time-dependent inhomogeneity). The theory indicates that the measurements of the complex optical reflectivity time evolution, caused by acoustic strain pulse propagation in such films, offer various possibilities to extract the depth profiles of intrinsic inhomogeneous distributions of mechanical/acoustical, optical, and acousto-optical parameters of the films. In particular it is proposed how the measurements of the transient complex optical reflectivity by the femtosecond optical interferometers, operating with light of different polarizations and probing the tested samples at different angles o...

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

The ability to generate efficient giga–terahertz coherent acoustic phonons with femtosecond laser makes acousto-optics a promising candidate for ultrafast light processing, which faces electronic device limits intrinsic to complementary metal oxide semiconductor technology. Modern acousto-optic devices, including optical mode conversion process between ordinary and extraordinary light waves (and vice versa), remain limited to the megahertz range. Here, using coherent acoustic waves generated at tens of gigahertz frequency by a femtosecond laser pulse, we reveal the mode conversion process and show its efficiency in ferroelectric materials such as BiFeO3 and LiNbO3. Further to the experimental evidence, we provide a complete theoretical support to this all-optical ultrafast mechanism mediated by acousto-optic interaction. By allowing the manipulation of light polarization with gigahertz coherent acoustic phonons, our results provide a novel route for the development of next-generation photonic-based devices and highlight new capabilities in using ferroelectrics in modern photonics.

Transition from piezoelectric to deformation potential mechanism of hypersound photogeneration in n-doped GaAs semiconductors

Both experiments with deeply penetrating femtosecond laser pulses and theoretical analysis demonstrate that at low laser fluences on (111) and (1−1−1−) surfaces of n-doped GaAs semiconductors the hypersound generation mechanism is the inverse piezoelectric effect. The transient electric field causing the inverse piezoelectric effect is due to the spatial separation in the built-in near-surface electric field of the electrons and holes photoexcited directly in the depletion region and also of those photoexcited outside the depletion region and diffusing toward it. However, with increasing laser fluence the amplitude of the acoustic signal generated by laser-induced transient electric fields saturates and the hypersound generation through electron–hole–phonon deformation potential mechanism becomes predominant. The peculiar dependencies of the hypersound amplitude and phase on pump laser fluence reveal the transition between the two physical mechanisms of optoacoustic conversion. The phase of the acoustic s...