Temporal and spatial tracking of ultrafast light-induced strain and polarization modulation in a ferroelectric thin film.

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 BiFeO3 thin film by ultrashort light pulses. To map the light-induced deformation of the BiFeO3 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.

Vapor Phase Ammonia Curing to Improve the Mechanical Properties of Antireflection Optical Coatings Designed for Power Laser Optics.

Projects of inertial confinement fusion using lasers need numerous optical components whose coatings allow the increase in their transmission and their resistance to high laser fluence. A coating process based on the self-assembly of sol-gel silica nanoparticles and a post-treatment with ammonia vapor over the surfaces of the optical components ("ammonia curing process") was developed and successfully optimized for industrial production. Manufacturing such antireflective coatings has clear advantages: (i) it is much cheaper than conventional top-down processes; (ii) it is well adapted to large-sized optical components and large-scale production; and (iii) it gives low optical losses in transmission and high resistances to laser fluence. The post-treatment was achieved by a simple exposition of optical components to room-temperature ammonia vapors. The resulting curing process induced strong optical and mechanical changes at the interface and was revealed to be of paramount importance since it reinforced the adhesion and abrasion resistance of the components so that the optical components could be handled easily. Here, we discuss how such coatings were characterized and how the initial thin nanoparticle film was transformed from a brittle film to a resistant coating from the ammonia curing process.

Ultrafast tunable modulation of light polarization at terahertz frequencies.

Controlling light polarization is one of the most essential routines in modern optical technology. Since the demonstration of optical pulse shaping by spatial light modulators and its potential in controlling the quantum reaction pathways, it paved the way for many applications as a coherent control of the photoionization process or as polarization shaping of terahertz (THz) pulses. Here, we evidenced efficient nonresonant and noncollinear χ(2)-type light-matter interaction in femtosecond polarization-sensitive time-resolved optical measurements. Such nonlinear optical interaction of visible light and ultrashort THz pulses leads to THz modulation of visible light polarization in bulk LiNbO3 crystal. Theoretical simulations based on the wave propagation equation capture the physical processes underlying this nonlinear effect. Apart from the observed tunable polarization modulation of visible pulses at ultrahigh frequencies, this physical phenomenon can be envisaged in THz depth-profiling of materials.

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.

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.

Femtosecond imaging of nonlinear acoustics in gold.

We have developed a high-sensitivity, low-noise femtosecond imaging technique based on pump-probe time-resolved measurements with a standard CCD camera. The approach used in the experiment is based on lock-in acquisitions of images generated by a femtosecond laser probe synchronized to modulation of a femtosecond laser pump at the same rate. This technique allows time-resolved imaging of laser-excited phenomena with femtosecond time resolution. We illustrate the technique by time-resolved imaging of the nonlinear reshaping of a laser-excited picosecond acoustic pulse after propagation through a thin gold layer. Image analysis reveals the direct 2D visualization of the nonlinear acoustic propagation of the picosecond acoustic pulse. Many ultrafast pump-probe investigations can profit from this technique because of the wealth of information it provides over a typical single diode and lock-in amplifier setup, for example it can be used to image ultrasonic echoes in biological samples.

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.

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.

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.