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Equilibrium gigahertz acoustics reveals long-range confinement in liquids
Authors:
Ievgeniia Chaban,
Thomas Pezeril
Abstract:
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 fl…
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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.
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Submitted 3 August, 2026;
originally announced August 2026.
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High-power laser beam shaping using a metasurface for shock excitation and focusing at the microscale
Authors:
Yun Kai,
Jet Lem,
Marcus Ossiander,
Maryna L. Meretska,
Vyacheslav Sokurenko,
Steven E. Kooi,
Federico Capasso,
Keith A. Nelson,
Thomas Pezeril
Abstract:
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 lever…
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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.
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Submitted 17 July, 2023; v1 submitted 11 October, 2022;
originally announced October 2022.
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Additive Laser Excitation of Giant Nonlinear Surface Acoustic Wave Pulses
Authors:
Jude Deschamps,
Yun Kai,
Jet Lem,
Ievgeniia Chaban,
Alexey Lomonosov,
Abdelmadjid Anane,
Steven E. Kooi,
Keith A. Nelson,
Thomas Pezeril
Abstract:
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 a…
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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.
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Submitted 11 July, 2023; v1 submitted 28 September, 2022;
originally announced September 2022.
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Direct Observation of Coherent Longitudinal and Shear Acoustic Phonons in TaAs Using Ultrafast X-ray Diffraction
Authors:
Min-Cheol Lee,
N. Sirica,
S. W. Teitelbaum,
A. Maznev,
T. Pezeril,
R. Tutchton,
V. Krapivin,
G. A. de la Pena,
Y. Huang,
L. X. Zhao,
G. F. Chen,
B. Xu,
R. Yang,
J. Shi,
J. Zhu,
D. A. Yarotski,
X. G. Qiu,
K. A. Nelson,
M. Trigo,
D. A. Reis,
R. P. Prasankumar
Abstract:
Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal…
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Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures.
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Submitted 28 February, 2022; v1 submitted 13 November, 2020;
originally announced November 2020.
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Time-domain Brillouin Scattering as a Local Temperature Probe in Liquids
Authors:
I. Chaban,
H. D. Shin,
C. Klieber,
R. Busselez,
V. Gusev,
Keith A. Nelson,
T. Pezeril
Abstract:
We present results of time-domain Brillouin scattering (TDBS) to determine the local temperature of liquids in contact to an optical transducer. TDBS is based on an ultrafast pump-probe technique to determine the light scattering frequency shift caused by the propagation of coherent acoustic waves in a sample. Since the temperature influences the Brillouin scattering frequency shift, the TDBS sign…
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We present results of time-domain Brillouin scattering (TDBS) to determine the local temperature of liquids in contact to an optical transducer. TDBS is based on an ultrafast pump-probe technique to determine the light scattering frequency shift caused by the propagation of coherent acoustic waves in a sample. Since the temperature influences the Brillouin scattering frequency shift, the TDBS signal probes the local temperature of the liquid. Results for the extracted Brillouin scattering frequencies recorded at different liquid temperatures and at different laser powers - i.e. different steady state background temperatures- are shown to demonstrate the usefulness of TDBS as a temperature probe. This TDBS experimental scheme is a first step towards the investigation of ultrathin liquids measured by GHz ultrasonic probing.
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Submitted 15 September, 2018;
originally announced September 2018.
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Single-bubble and multi-bubble cavitation in water triggered by laser-driven focusing shock waves
Authors:
D. Veysset,
U. Gutiérrez-Hernández,
L. Dresselhaus-Cooper,
F. De Colle,
S. Kooi,
K. A. Nelson,
P. A. Quinto-Su,
T. Pezeril
Abstract:
In this study a single laser pulse spatially shaped into a ring is focused into a thin water layer, creating an annular cavitation bubble and cylindrical shock waves: an outer shock that diverges away from the excitation laser ring and an inner shock that focuses towards the center. A few nanoseconds after the converging shock reaches the focus and diverges away from the center, a single bubble nu…
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In this study a single laser pulse spatially shaped into a ring is focused into a thin water layer, creating an annular cavitation bubble and cylindrical shock waves: an outer shock that diverges away from the excitation laser ring and an inner shock that focuses towards the center. A few nanoseconds after the converging shock reaches the focus and diverges away from the center, a single bubble nucleates at the center. The inner diverging shock then reaches the surface of the annular laser-induced bubble and reflects at the boundary, initiating nucleation of a tertiary bubble cloud. In the present experiments, we have performed time-resolved imaging of shock propagation and bubble wall motion. Our experimental observations of single-bubble cavitation and collapse and appearance of ring-shaped bubble clouds are consistent with our numerical simulations that solve a one dimensional Euler equation in cylindrical coordinates. The numerical results agree qualitatively with the experimental observations of the appearance and growth of bubble clouds at the smallest laser excitation rings. Our technique of shock-driven bubble cavitation opens novel perspectives for the investigation of shock-induced single-bubble or multi-bubble cavitation phenomena in thin liquids.
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Submitted 29 March, 2018; v1 submitted 20 September, 2017;
originally announced September 2017.
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Time-domain Brillouin scattering assisted by diffraction gratings
Authors:
Osamu Matsuda,
Thomas Pezeril,
Ievgeniia Chaban,
Kentaro Fujita,
Vitalyi Gusev
Abstract:
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 dif…
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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.
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Submitted 26 April, 2017;
originally announced April 2017.
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Time-domain Brillouin scattering for the determination of laser-induced temperature gradients in liquids
Authors:
I. Chaban,
D. Shin,
C. Klieber,
R. Busselez,
V. Gusev,
Keith A. Nelson,
T. Pezeril
Abstract:
We present an optical technique based on ultrafast photoacoustics to precisely determine the local temperature distribution profile in liquid samples in contact with a laser heated optical transducer. This ultrafast pump-probe experiment uses time-domain Brillouin scattering (TDBS) to locally determine the light scattering frequency shift. As the temperature influences the Brillouin scattering fre…
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We present an optical technique based on ultrafast photoacoustics to precisely determine the local temperature distribution profile in liquid samples in contact with a laser heated optical transducer. This ultrafast pump-probe experiment uses time-domain Brillouin scattering (TDBS) to locally determine the light scattering frequency shift. As the temperature influences the Brillouin scattering frequency, the TDBS signal probes the local laser-induced temperature distribution in the liquid. We demonstrate the relevance and the sensitivity of this technique for the measurement of the absolute laser-induced temperature gradient of a glass forming liquid prototype, glycerol, at different laser pump powers - i.e. different steady state background temperatures. Complementarily, our experiments illustrate how this TDBS technique can be applied to measure thermal diffusion in complex multilayer systems in contact to a surrounding liquid.
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Submitted 17 October, 2017; v1 submitted 3 February, 2017;
originally announced February 2017.
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Ultrafast non-thermal laser excitation of gigahertz longitudinal and shear acoustic waves in spin-crossover molecular crystals [$Fe(PM-AzA)_{2}$$(NCS)_{2}$]
Authors:
T. Parpiiev,
M. Servol,
M. Lorenc,
I. Chaban,
E. Collet,
H. Cailleau,
P. Ruello,
G. Chastanet,
T. Pezeril
Abstract:
We report GHz longitudinal as well as shear acoustic phonons photoexcitation and photodetection using femtosecond laser pulses in a spin-crossover molecular crystal. From our experimental observation of time domain Brillouin scattering triggered by the photoexcitation of acoustic waves across the low-spin (LS) to high-spin (HS) thermal crossover, we reveal a link between molecular spin state and p…
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We report GHz longitudinal as well as shear acoustic phonons photoexcitation and photodetection using femtosecond laser pulses in a spin-crossover molecular crystal. From our experimental observation of time domain Brillouin scattering triggered by the photoexcitation of acoustic waves across the low-spin (LS) to high-spin (HS) thermal crossover, we reveal a link between molecular spin state and photoexcitation of coherent GHz acoustic phonons. In particular, we experimentally evidence an unconventional non-thermal pathway for the laser excitation of GHz phonons. We also provide experimental insight on the optical and mechanical parameters evolution across the LS/HS spin crossover temperature T$_{1/2}$.
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Submitted 17 October, 2017; v1 submitted 12 April, 2016;
originally announced April 2016.
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Nonlinear acousto-magneto-plasmonics
Authors:
Vasily V. Temnov,
Ilya Razdolski,
Thomas Pezeril,
Denys Makarov,
Denis Seletskiy,
Alexey Melnikov,
Keith A. Nelson
Abstract:
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 re…
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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.
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Submitted 21 February, 2016;
originally announced February 2016.
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Ultrafast electron-phonon-magnon interactions at noble metal-ferromagnet interfaces
Authors:
V. Shalagatskyi,
O. Kovalenko,
V. Shumylo,
A. Alekhin,
G. Vaudel,
T. Pezeril,
V. S. Vlasov,
A. M. Lomonosov,
V. E. Gusev,
D. Makarov,
V. V. Temnov
Abstract:
Ultrafast optical excitation of gold-cobalt bilayers triggers the nontrivial interplay between the electronic, acoustic, and magnetic degrees of freedom. Laser-heated electrons generated at the gold-air interface diffuse through the layer of gold and strongly overheat the lattice in cobalt resulting in the emission of ultrashort acoustic pulses and generation of exchange-coupled magnons. Time-reso…
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Ultrafast optical excitation of gold-cobalt bilayers triggers the nontrivial interplay between the electronic, acoustic, and magnetic degrees of freedom. Laser-heated electrons generated at the gold-air interface diffuse through the layer of gold and strongly overheat the lattice in cobalt resulting in the emission of ultrashort acoustic pulses and generation of exchange-coupled magnons. Time-resolved optical measurements allow for extracting the thermal boundary (Kapitza) resistances at metal/metal interfaces and the hot electron diffusion length in ferromagnetic materials. Both the experimental data and the analytical treatment of the two-temperature model reveal the role of the Kapitza resistance in transient lattice overheating.
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Submitted 27 July, 2017; v1 submitted 29 November, 2015;
originally announced November 2015.
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Ultrafast Acousto-Plasmonics in Gold Nanoparticles Superlattice
Authors:
P. Ruello,
A. Ayouch,
G. Vaudel,
T. Pezeril,
N. Delorme,
S. Sato,
K. Kimura,
V. Gusev
Abstract:
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 estima…
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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.
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Submitted 8 July, 2015;
originally announced July 2015.
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Nonlinear Acoustics at GHz Frequencies in a Viscoelastic Fragile Glass Former
Authors:
Christoph Klieber,
Vitalyi E. Gusev,
Thomas Pezeril,
Keith A. Nelson
Abstract:
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 pr…
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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.
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Submitted 13 March, 2014;
originally announced March 2014.
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Coherent acoustic phonons emission in copper driven by super-diffusive hot electrons
Authors:
M. Lejman,
V. Shalagatsky,
A. Kovalenko,
T. Pezeril,
V. V. Temnov,
P. Ruello
Abstract:
Ultrafast laser excited hot electrons can transport energy supersonically far from the region where they are initially produced. We show that this ultrafast energy transport is responsible of the emission of coherent acoustic phonons deeply beneath the free surface of a copper metal sample. In particular we demonstrate that enough energy carried by these hot electrons over a distance as large as 2…
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Ultrafast laser excited hot electrons can transport energy supersonically far from the region where they are initially produced. We show that this ultrafast energy transport is responsible of the emission of coherent acoustic phonons deeply beneath the free surface of a copper metal sample. In particular we demonstrate that enough energy carried by these hot electrons over a distance as large as 220nm at room temperature in copper can be converted into coherent acoustic phonons. In order to demonstrate this effect, several configurations of time-resolved optical experiments of time of flight of coherent acoustic phonons and of hot electrons have been performed.
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Submitted 19 April, 2013;
originally announced April 2013.
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Magnetization switching by ultrashort acoustic pulses
Authors:
O. Kovalenko,
T. Pezeril,
V. V. Temnov
Abstract:
It is shown theoretically that a single a few picoseconds long acoustic pulse can reverse magnetization in a magneto-strictive material Terfenol-D. Following giant magneto-elastic changes of free energy density the magnetization vector is kicked out of a local in-plane energy mininum and decays into another minimum. For acoustic pulse duration significantly shorter than magnetization precession pe…
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It is shown theoretically that a single a few picoseconds long acoustic pulse can reverse magnetization in a magneto-strictive material Terfenol-D. Following giant magneto-elastic changes of free energy density the magnetization vector is kicked out of a local in-plane energy mininum and decays into another minimum. For acoustic pulse duration significantly shorter than magnetization precession period $τ_{ac}$<<$T_{prec}$, the switching threshold is determined by the {\it acoustic pulse area}, i.e. pulse integral in time domain, similar to coherent phenomena in optics. Simulation results are summarized in a magneto-acoustic switching diagram and discussed in the context of all-optical magnetization switching by circularly polarized light pulses.
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Submitted 4 December, 2012;
originally announced December 2012.
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Direct Visualization of Laser-Driven Focusing Shock Waves
Authors:
Thomas Pezeril,
Gagan Saini,
David Veysset,
Steve Kooi,
Piotr Fidkowski,
Raul Radovitzky,
Keith A. Nelson
Abstract:
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…
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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.
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Submitted 6 April, 2011;
originally announced April 2011.