Pascal Ruello

Physical mechanisms of coherent acoustic phonons generation by ultrafast laser action

In this review we address the microscopic mechanisms that are involved in the photogeneration processes of GHz-THz coherent acoustic phonons (CAP) induced by an ultrafast laser pulse. Understanding and describing the underlying physics is necessary indeed for improving the future sources of coherent acoustic phonons useful for the non-destructive testing optoacoustic techniques. Getting more physical insights on these processes also opens new perspectives for the emerging field of the opto-mechanics where lattice motions (surface and/or interfaces ultrafast displacements, nanostructures resonances) are controlled by light. We will then remind the basics of electron-phonon and photon-phonon couplings by discussing the deformation potential mechanism, the thermoelasticity, the inverse piezoelectric effect and the electrostriction in condensed matter. Metals, semiconductors and oxide materials will be discussed. The contribution of all these mechanisms in the photogeneration process of sound will be illustrated over several examples coming from the rich literature.

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.

Depth-profiling of elastic inhomogeneities in transparent nanoporous low-k materials by picosecond ultrasonic interferometry

We achieve depth-profiling of the elasticity of a thin transparent film of a nanoporous low-k material using picosecond acoustic interferometry. The variation in the material properties with depth is extracted from time-resolved femtosecond optical reflectivity measurements. More than 40% of the variation in the longitudinal elastic modulus between the front and the back surfaces of an 800 nm thick nanoporous layer is mapped with a 40 nm spatial resolution. We attribute this variation to the spatially inhomogeneous UV curing of the film during fabrication.

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.

Electron doped (Sm1−x,Cax)MnO3 perovskite manganite as potential infrared thermochromic switch

We have synthesized (Sm1−x,Cax)MnO3 and related compositions to show their potential use as thermochromic switch in the infrared range. Depending on temperature or composition, the single phase is stabilized using the polyacrilamide gel process. Infrared transmittance was measured on selected samples in the 1,42–25μm range. Relative contrast up to 0.773 is measured in the 8–14μm range. Full opacity in the 8–14μm range occurs at temperatures between 273 and 300K, depending on the composition. The potential application of perovskites manganites as thermochromic infrared switch or coating is discussed.

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.