arXiv subjects

Thomas Pezeril

Publications and source records attributed to Thomas Pezeril.

11 recordsLinked to original sources

arXiv2026

Equilibrium gigahertz acoustics reveals long-range confinement in liquids

Understanding how the mechanical properties of liquids confined within nanometer-scale gaps differ from bulk behavior is central to biophysics, lubrication, catalysis, electrochemistry, and surface science. Yet the characterization of ultrathin confined liquids remains challenging, as many existing approaches rely on destructive or intrusive contact-based techniques, mostly measuring the liquid flow in the low frequency regime. Here, we present a non-invasive, all-optical technique based on ultrafast laser ultrasonics that probes confined liquids at equilibrium in the gigahertz frequency range. The method measures the phase and amplitude of time-domain Brillouin scattering signals transmitted through liquid layers whose thickness is varied step by step with subnanometer effective sampling. Supported by numerical modeling of acoustic propagation and optical detection, these signals allow us to extract the thickness-dependent acoustic velocity and attenuation of confined liquids. We show that nanometric confinement modifies the GHz acoustic response of glycerol, the liquid crystal 8CB, and a butyl-based ionic liquid over unexpectedly long spatial scales. These effects extend from a few nanometers to several tens of nanometers and reveal bound interfacial layers, acoustic stiffening, and enhanced solid-like behavior under confinement. Our results open a route to probing liquid confinement in a scarcely explored regime: dynamically measured at gigahertz frequencies, yet sufficiently weakly perturbative to preserve the equilibrium confined state.

cond-mat.soft↗

arXiv2025

Shocking a Shock Wave for Nonlinear Summation of GPa Pressures

Exploring shock-shock interactions has been limited by experimental constraints, particularly in laser-induced shock experiments due to specialized equipment requirements. Herein, we introduce a tabletop approach to systematically investigate the excitation and superposition of dual laser-induced shock waves in water. Utilizing two laser pulses, spatio-temporally separated and focused into a confined water layer, we identify the optimal superposition leading to the highest combined shock pressure. Our results demonstrate that combining two shock waves each of $\sim$0.6~GPa pressure yields an overall shock pressure of $\sim$3~GPa. Our findings, suggesting an inherent nonlinear summation from the laser excitation process itself and highlights a new pathway for energy-efficient laser shock wave excitation.

physics.app-ph↗

arXiv2025

Quantification of Ultrafast Nonlinear Photothermal and Photoacoustic Effects in Molecular Thin Films via Time-Domain Brillouin Scattering

Improving the efficiency of photothermal (PT) therapies and photoacoustic (PA) imaging at the microscopic scale hinges on developing multiphoton-absorbing photothermal molecules or contrast agents that operate in the near-infrared (NIR) range. These advanced agents or molecules will enable excitation with NIR lasers, in an improved transparency range for biological tissues, while enabling minute, highly localized spatial control of the excitation area. However, progress in this field requires innovative experimental techniques to characterize photothermal and photoacoustic effects under multiphoton excitation. In this article, we showcase a study of a model organometallic molecular compound excited via two-photon absorption (2PA) using femtosecond laser pulses. Based on a time-domain Brillouin scattering technique, well adapted for investigating ultrafast nonlinear optical absorption processes in ultrathin films on substrates, we determine the effective nonlinear absorption coefficients of the compound directly linked to PT/PA. Our findings provide a practical approach for exploring and optimizing nonlinear PT/PA absorbers and contrast agents.

physics.optics↗

arXiv2022

High-power laser beam shaping using a metasurface for shock excitation and focusing at the microscale

Achieving high repeatability and efficiency in laser-induced strong shock wave excitation remains a significant technical challenge, as evidenced by the extensive efforts undertaken at large-scale national laboratories to optimize the compression of light element pellets. In this study, we propose and model a novel optical design for generating strong shocks at a tabletop scale. Our approach leverages the spatial and temporal shaping of multiple laser pulses to form concentric laser rings on condensed matter samples. Each laser ring initiates a two-dimensional focusing shock wave that overlaps and converges with preceding shock waves at a central point within the ring. We present preliminary experimental results for a single ring configuration. To enable high-power laser focusing at the micron scale, we demonstrate experimentally the feasibility of employing dielectric metasurfaces with exceptional damage threshold, experimentally determined to be 1.1 J/cm2, as replacements for conventional optics. These metasurfaces enable the creation of pristine, high-fluence laser rings essential for launching stable shock waves in materials. Herein, we showcase results obtained using a water sample, achieving shock pressures in the gigapascal (GPa) range. Our findings provide a promising pathway towards the application of laser-induced strong shock compression in condensed matter at the microscale.

physics.optics↗

arXiv2022

Additive Laser Excitation of Giant Nonlinear Surface Acoustic Wave Pulses

The laser ultrasonics technique perfectly fits the needs for non-contact, non-invasive, non-destructive mechanical probing of samples of mm to nm sizes. This technique is however limited to the excitation of low-amplitude strains, below the threshold for optical damage of the sample. In the context of strain engineering of materials, alternative optical techniques enabling the excitation of high amplitude strains in a non-destructive optical regime are seeking. We introduce here a non-destructive method for laser-shock wave generation based on additive superposition of multiple laser-excited strain waves. This technique enables strain generation up to mechanical failure of a sample at pump laser fluences below optical ablation or melting thresholds. We demonstrate the ability to generate nonlinear surface acoustic waves (SAWs) in Nb:SrTiO$_3$ substrates, at typically 1 kHz repetition rate, with associated strains in the percent range and pressures close to 100 kbars. This study paves the way for the investigation of a host of high-strength SAW-induced phenomena, including phase transitions in conventional and quantum materials, plasticity and a myriad of material failure modes, chemistry and other effects in bulk samples, thin layers, or two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2022

Nonlinear optical absorption in nanoscale films revealed through ultrafast acoustics

Herein we describe a novel spinning pump-probe photoacoustic technique developed to study nonlinear absorption in thin films. As a test case, an organic polycrystalline thin film of quinacridone, a well-known pigment, with a thickness in the tens of nanometers range, is excited by a femtosecond laser pulse which generates a time-domain Brillouin scattering signal. This signal is directly related to the strain wave launched from the film into the substrate and can be used to quantitatively extract the nonlinear optical absorption properties of the film itself. Quinacridone exhibits both quadratic and cubic laser fluence dependence regimes which we show to correspond to two- and three-photon absorption processes. This technique can be broadly applied to materials that are difficult or impossible to characterize with conventional transmittance-based measurements including materials at the nanoscale, prone to laser damage, with very weak nonlinear properties, opaque or highly scattering.

physics.optics↗

arXiv2018

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 LiNbO$_3$ 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.

physics.app-ph↗

arXiv2017

Time-domain Brillouin scattering assisted by diffraction gratings

Absorption of ultrashort laser pulses in a metallic grating deposited on a transparent sample launches coherent compression/dilatation acoustic pulses in directions of different orders of acoustic diffraction. Their propagation is detected by the delayed laser pulses, which are also diffracted by the metallic grating, through the measurement of the transient intensity change of the first order diffracted light. The obtained data contain multiple frequency components which are interpreted by considering all possible angles for the Brillouin scattering of light achieved through the multiplexing of the propagation directions of light and coherent sound by the metallic grating. The emitted acoustic field can be equivalently presented as a superposition of the plane inhomogeneous acoustic waves, which constitute an acoustic diffraction grating for the probe light. Thus, the obtained results can also be interpreted as a consequence of probe light diffraction by both metallic and acoustic gratings. The realized scheme of time-domain Brillouin scattering with metallic grating operating in reflection mode provides access to acoustic frequencies from the minimal to the maximal possible in a single experimental configuration for the directions of probe light incidence and scattered light detection. This is achieved by monitoring of the backward and forward Brillouin scattering processes in parallel. Applications include measurements of the acoustic dispersion, simultaneous determination of sound velocity and optical refractive index, and evaluation of the samples with a single direction of possible optical access.

physics.app-ph↗

arXiv2016

Nonlinear acousto-magneto-plasmonics

We review the recent progress in experimental and theoretical research of interactions between the acoustic, magnetic and plasmonic transients in hybrid metal-ferromagnet multilayer structures excited by ultrashort laser pulses. The main focus is on understanding the nonlinear aspects of the acoustic dynamics in materials as well as the peculiarities in the nonlinear optical and magneto-optical response. For example, the nonlinear optical detection is illustrated in details by probing the static magneto-optical second harmonic generation in gold-cobalt-silver trilayer structures in Kretschmann geometry. Furthermore, we show experimentally how the nonlinear reshaping of giant ultrashort acoustic pulses propagating in gold can be quantified by time-resolved plasmonic interferometry and how these ultrashort optical pulses dynamically modulate the optical nonlinearities. The effective medium approximation for the optical properties of hybrid multilayers facilitates the understanding of novel optical detection techniques. In the discussion we highlight recent works on the nonlinear magneto-elastic interactions, and strain-induced effects in semiconductor quantum dots.

cond-mat.mes-hall↗

arXiv2014

Nonlinear Acoustics at GHz Frequencies in a Viscoelastic Fragile Glass Former

Using a picosecond pump-probe ultrasonic technique, we study the propagation of high-amplitude, laser-generated longitudinal coherent acoustic pulses in the viscoelastic fragile glass former DC704. We observe an increase of almost ten percent in acoustic pulse propagation speed of its leading shock front at the highest optical pump fluence which is a result of the supersonic nature of nonlinear propagation in the viscous medium. From our measurement we deduce the nonlinear acoustic parameter of the glass former in the GHz frequency range across the glass transition temperature.

cond-mat.mtrl-sci↗

arXiv2011

Direct Visualization of Laser-Driven Focusing Shock Waves

Cylindrically or spherically focusing shock waves have been of keen interest for the past several decades. In addition to fundamental study of materials under extreme conditions, cavitation, and sonoluminescence, focusing shock waves enable myriad applications including hypervelocity launchers, synthesis of new materials, production of high-temperature and high-density plasma fields, and a variety of medical therapies. Applications in controlled thermonuclear fusion and in the study of the conditions reached in laser fusion are also of current interest. Here we report on a method for direct real-time visualization and measurement of laser-driven shock generation, propagation, and 2D focusing in a sample. The 2D focusing of the shock front is the consequence of spatial shaping of the laser shock generation pulse into a ring pattern. A substantial increase of the pressure at the convergence of the acoustic shock front is observed experimentally and simulated numerically. Single-shot acquisitions using a streak camera reveal that at the convergence of the shock wave in liquid water the supersonic speed reaches Mach 6, corresponding to the multiple gigapascal pressure range 30 GPa.

cond-mat.mtrl-sci↗