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Shock waves generated by laser pulses have been gaining attention for biological and medical applications in which shock-induced cell membrane deformation influences cell permeation. However, the mechanisms through which the deformation of cell membranes affects permeability remain mostly unknown because of the difficulty of observing in real time the transient and dynamic behaviors of the shock waves and the cells. Here we present an all-optical measurement method that can quantitatively capture the pressure distribution of the propagating shock wave and simultaneously monitor the dynamic behavior of cell membranes. Using this method, we find that the profile of the shock wave dictates the cell membrane permeation. The results suggest a possible mechanism of membrane permeation where sharp pressure gradients create pores on the membrane. Our measurement will foster further understanding of the interaction of shock waves with cells, while the proposed mechanism advances biological and medical applications of shock waves. While shock waves are widely used in clinical and biological research due to their ability to deform the cell’s membrane and its permeability, the mechanisms of such interaction are still unclear. Here, the authors propose a method that allows to monitor the dynamic deformation of a cell’s membrane in response to shock waves and its effect on permeability.

International audience; 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.

We use femtosecond extreme ultraviolet pulses derived from a free electron laser to excite and probe surface acoustic waves (SAWs) on the (001) surface of single crystal SrTiO3. SAWs are generated by a pair of 39.9 nm pulses crossed at the sample with the crossing angle defining the SAW wavelength at 84 nm. Detection of SAWs is performed via diffraction of a time-delayed 13.3 nm probe pulse by SAW-induced surface ripples. Despite the low reflectivity of the sample in the extreme ultraviolet range, the reflection mode detection is found to be efficient because of an increase in the diffraction efficiency for shorter wavelengths. We describe a methodology for extracting the SAW attenuation in the presence of a thermal grating, which is based on measuring the decay of oscillations at twice the SAW frequency. The proposed approach can be used to study ultrahigh frequency SAWs in a broad range of materials and will bridge the wave vector gap in surface phonon spectroscopy between Brillouin scattering and He atom scattering.

Chirality and chiral molecules are key elements in modern chemical and biochemical industries. Individual addressing, and the eventual separation of chiral enantiomers has been and still is an important elusive task in molecular physics and chemistry, and a variety of methods has been introduced over the years to achieve this goal. Here, we theoretically demonstrate that a pair of cross-polarized THz pulses interacting with chiral molecules through their permanent dipole moments induces an enantioselective orientation of these molecules. This orientation persists for a long time, exceeding the duration of the THz pulses by several orders of magnitude, and its dependency on temperature and pulses' parameters is investigated. The persistent orientation may enhance the deflection of the molecules in inhomogeneous electromagnetic fields, potentially leading to viable separation techniques., 9 pages, 5 figures

Ionic motion significantly contributes to conductivity in devices such as memory, switches, and rechargeable batteries. In our work, we experimentally demonstrate that intense terahertz electric-field transients can be used to manipulate ions in a superionic conductor, namely Na^{+} β-alumina. The cations trapped in the local potential minima are accelerated using single-cycle terahertz pulses, thereby inducing a macroscopic current flow on a subpicosecond timescale. Our results clearly show that single-cycle terahertz pulses can be used to significantly modulate the nature of superionic conductors and could possibly serve as a basic tool for application in future electronic devices.

Impact-induced erosion is the ablation of matter caused by being physically struck by another object. While this phenomenon is known, it is empirically challenging to study mechanistically because of the short timescales and small length scales involved. Here, we resolve supersonic impact erosion in situ with micrometer- and nanosecond-level spatiotemporal resolution. We show, in real time, how metallic microparticles (~10-μm) cross from the regimes of rebound and bonding to the more extreme regime that involves erosion. We find that erosion in normal impact of ductile metallic materials is melt-driven, and establish a mechanistic framework to predict the erosion velocity., Supersonic particle impacts can cause permanent damage to space vehicles and satellites, but how exactly remains unclear. Here, the authors visualise for the first time the high impact of single tin microparticles on a tin substrate and show erosion of ductile metallic materials is melt-driven.

International audience; We demonstrate that time-domain Brillouin scattering (TDBS), a technique based on an ultrafast pump-probe approach, is sensitive to phase transitions and apply it to the study of structural changes of 8CB liquid crystals at different temperatures across the isotropic, nematic, smectic and crystalline phases. We investigate the viscoelastic properties of 8CB squeezed in a narrow gap, from nanometer to submicrometer thickness range, and conclude on the long-range molecular structuring of the smectic phase. These TDBS results reveal that confinement effects favor structuring of the smectic phase into a crystalline-like phase that can be observed at extended distances far beyond the molecular dimensions.

We describe a high-speed single-shot multi-frame interferometric imaging technique enabling multiple interferometric images with femtosecond exposure time over a 50 ns event window to be recorded, following a single laser-induced excitation event. The stroboscopic illumination of a framing camera is made possible through the use of a doubling cavity that produces a femtosecond pulse train that is synchronized to the gated exposure windows of the individual frames of the camera. The imaging system utilizes a Michelson interferometer to extract phase and ultimately displacement information. We demonstrate the method by monitoring laser-induced deformation and the propagation of high-amplitude acoustic waves in a silicon nitride membrane. The method is applicable to a wide range of fast irreversible phenomena such as crack branching, shock-induced material damage, cavitation, and dielectric breakdown., U.S. Army Research Office (Contract W911NF-18-2-0048)

Transition metal oxides possess complex free energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained $\mathrm{La_{0.67}Ca_{0.33}MnO_3}$, optical excitation with a sub-100 fs pulse above $2\ \mathrm{mJ/cm^2}$ leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multi-step process. We conclude that the phase transition is driven by partial charge order melting, followed by growth of the persistent metallic phase on longer timescales. A time-dependent Ginzburg-Landau model can describe the fast dynamics of the reflectivity, followed by longer timescale in-growth of the metallic phase., 5 pages plus 7 pages supplement, 4 figures plus 2 figures supplement

Shock waves in condensed matter are of great importance for many areas of science and technology ranging from inertially confined fusion to planetary science and medicine. In laboratory studies of shock waves, there is a need in developing diagnostic techniques capable of measuring parameters of materials under shock with high spatial resolution. Here, time-resolved interferometric imaging is used to study laser-driven focusing shock waves in a thin liquid layer in an all-optical experiment. Shock waves are generated in a 10 µm-thick layer of water by focusing intense picosecond laser pulses into a ring of 95 µm radius. Using a Mach-Zehnder interferometer and time-delayed femtosecond laser pulses, we obtain a series of images tracing the shock wave as it converges at the center of the ring before reemerging as a diverging shock, resulting in the formation of a cavitation bubble. Through quantitative analysis of the interferograms, density profiles of shocked samples are extracted. The experimental geometry used in our study opens prospects for spatially resolved spectroscopic studies of materials under shock compression., Massachusetts Institute of Technology. Institute for Soldier Nanotechnologies (Contract W911NF-13-D-0001)

Spatially patterned extreme ultraviolet light pulses can be used for probing multiple dynamical processes at the nanoscale., Advances in developing ultrafast coherent sources operating at extreme ultraviolet (EUV) and x-ray wavelengths allow the extension of nonlinear optical techniques to shorter wavelengths. Here, we describe EUV transient grating spectroscopy, in which two crossed femtosecond EUV pulses produce spatially periodic nanoscale excitations in the sample and their dynamics is probed via diffraction of a third time-delayed EUV pulse. The use of radiation with wavelengths down to 13.3 nm allowed us to produce transient gratings with periods as short as 28 nm and observe thermal and coherent phonon dynamics in crystalline silicon and amorphous silicon nitride. This approach allows measurements of thermal transport on the ~10-nm scale, where the two samples show different heat transport regimes, and can be applied to study other phenomena showing nontrivial behaviors at the nanoscale, such as structural relaxations in complex liquids and ultrafast magnetic dynamics.

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We present results of time-domain Brillouin scattering (TDBS) to determine the local temperature of liquids. 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 are shown to demonstrate the usefulness of TDBS as a temperature probe. Keywords: acoustic; thermal conductivity; spectroscopy, United States. Department of Energy (Grant DE-FG02-00ER15087), National Science Foundation (U.S.) (Grant CHE-0616939), National Science Foundation (U.S.) (Grant DMR-0414895), France. Agence nationale de la recherche (Grant ANR-12-BS09-0031-0)

Optics express 27(19), 26547-26568 (2019)., A theory of terahertz generation using a superposition of beamlets is developed. It is shown how such an arrangement produces a distortion-free tilted pulse front. We analytically show how a superposition of beamlets produces terahertz radiation with greater efficiency and spatial homogeneity compared to tilted pulse fronts generated by diffraction gratings. The advantages are particularly notable for large pump bandwidths and beam sizes, suggesting better performance in the presence of cascading effects and for high energy pumping. Closed-form expressions for terahertz spectra and transients in three spatial dimensions are derived. Conditions for obtaining performance better than conventional tilted pulse fronts and bounds for optimal pump parameters are furnished., Published by Soc., Washington, DC

Time-resolved transient grating (TG) spectroscopy facilitates detailed studies of electron dynamics and transport phenomena by means of a periodic excitation of matter with coherent ultrashort light pulses. Several current and next generation free-electron laser (FEL) facilities provide fully coherent pulses with few femtosecond pulse durations and extreme ultraviolet (XUV) photon energies. Thus, they allow for transient grating experiments with periodicities as small as tens of nanometers and with element specific photon energies. Here, we demonstrate the element specificity of XUV TG (X-TG) experiments by tuning the photon energy across the Si L2,3-edge of Si3N4. We observe a shortening of the signal decay when increasing the XUV photon energy above the absorption edge. The analysis of the wavelength dependent signal shows that the faster decay is driven by the increase in the charge carrier density. From the decay constants the interband Auger coefficient at elevated temperatures and high electron densities has been determined.Time-resolved transient grating (TG) spectroscopy facilitates detailed studies of electron dynamics and transport phenomena by means of a periodic excitation of matter with coherent ultrashort light pulses. Several current and next generation free-electron laser (FEL) facilities provide fully coherent pulses with few femtosecond pulse durations and extreme ultraviolet (XUV) photon energies. Thus, they allow for transient grating experiments with periodicities as small as tens of nanometers and with element specific photon energies. Here, we demonstrate the element specificity of XUV TG (X-TG) experiments by tuning the photon energy across the Si L2,3-edge of Si3N4. We observe a shortening of the signal decay when increasing the XUV photon energy above the absorption edge. The analysis of the wavelength dependent signal shows that the faster decay is driven by the increase in the charge carrier density. From the decay constants the interband Auger coefficient at elevated temperatures and high electron dens...

"Hidden phases" are metastable collective states of matter that are typically not accessible on equilibrium phase diagrams. These phases can host exotic properties in otherwise conventional materials and hence may enable novel functionality and applications, but their discovery and access are still in early stages. Using intense terahertz electric field excitation, we show that an ultrafast phase transition into a hidden ferroelectric phase can be dynamically induced in the quantum paraelectric SrTiO$_3$. The induced lowering in crystal symmetry yields dramatic changes in the phonon excitation spectra. Our results demonstrate collective coherent control over material structure, in which a single-cycle field drives ions along the microscopic pathway leading directly to their locations in a new crystalline phase on an ultrafast timescale., 25 pages, 11 figures

As a type of fermions without counterpart in high energy physics, triply degenerate fermions show exotic physical properties, which are represented by triply degenerate nodal points in topological semimetals. Here, based on the space group theory analysis, we propose a practical guidance for seeking a topological semimetal with triply degenerate nodal points located at a symmetric axis, which is applicable to both symmorphic and nonsymmorphic crystals. By using this guidance in combination with the first-principles electronic structure calculations, we predict a class of triply degenerate topological semimetals $R{\mathrm{Rh}}_{6}{\mathrm{Ge}}_{4}\phantom{\rule{4pt}{0ex}}(R=\text{Y},\text{La},\text{Lu})$. In these compounds, the triply degenerate nodal points are located at the $\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}A$ axis and not far from the Fermi level. Especially, ${\mathrm{LaRh}}_{6}{\mathrm{Ge}}_{4}$ has a pair of triply degenerate nodal points located at just $\ensuremath{\sim}3$ meV below the Fermi level. Considering the fact that the single crystals of $R{\mathrm{Rh}}_{6}{\mathrm{Ge}}_{4}$ have been synthesized experimentally, the $R{\mathrm{Rh}}_{6}{\mathrm{Ge}}_{4}$ class of compounds will be an appropriate platform for studying exotic physical properties of triply degenerate topological semimetals.

Dynamic fracture of borosilicate glass through focusing of high-amplitude nanosecond surface acoustic waves (SAWs) at the micron scale is investigated in an all-optical experiment. SAWs are generated by a picosecond laser excitation pulse focused into a ring-shaped spot on the sample surface. Interferometric images capture the SAW as it converges towards the center, focuses, and subsequently diverges. Above a laser energy threshold, damage at the acoustic focal point is observed. Numerical calculations help us determine the time evolution of the stress distribution. We find that the glass withstands a local tensile stress of at least 6 GPa without fracture. Keyword: Dynamic fracture; Surface acoustic waves; Interferometry; Glass, United States. Army Research Office (Agreement W911NF-13-D-001 and W911NF-18-2-0048), United States. Office of Naval Research (Grant N000141512694), United States. Department of Energy (Award DE-SC0018091)

Multidimensional spectroscopy in the visible and infrared spectral ranges has become a powerful technique to retrieve dynamic correlations and couplings in wide-ranging systems by utilizing multiple correlated light-matter interactions. Its extension to the terahertz (THz) regime of the electromagnetic spectrum, where rich material degrees of freedom reside, however, has been progressing slowly. This chapter reviews some of the THz-frequency two-dimensional (2D) spectroscopy techniques and experimental results realized in recent years. Examples include gas molecule rotations, spin precessions in magnetic systems, and liquid molecular dynamics studied by 2D THz or hybrid 2D THz-Raman spectroscopy techniques. The methodology shows promising applications to different THz-frequency degrees of freedom in various chemical systems and processes.

We investigate the excitation of coherent acoustic and optical phonons by ultrashort extreme ultraviolet (EUV) pulses produced by a free electron laser. Two crossed femtosecond EUV (wavelength 12.7 nm) pulses are used to excite coherent phonons at a wavelength of 280 nm, which are detected via diffraction of an optical probe beam. Longitudinal and surface acoustic waves are measured in BK-7 glass, diamond, and Bi4Ge3O12; in the latter material, the excitation of a coherent optical phonon mode is also observed. We discuss probing different acoustic modes in reflection and transmission geometries and frequency mixing of surface and bulk acoustic waves in the signal. The use of extreme ultraviolet radiation will allow the creation of tunable GHz to THz acoustic sources in any material without the need to fabricate transducer structures. The contribution by the MIT group was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Award No. DE-FG02-00ER15087. The JILA group graciously acknowledges support from the Department of Energy BES Award No. DE-FG02-99ER14982 and the Gordon and Betty Moore Foundation's EPiQS Initiative through Grant No. GBMF: 4538, and J.K. acknowledges support from an SRC Fellowship. The Elettra group acknowledges the European Research Council Grant No. 202804-TIMER. A.C. and T.F. acknowledge the Swiss NSF through the NCCR-MUST.

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 large bubble clouds at the smallest laser excitation rings. Our technique of shock-driven bubble cavitation opens interesting perspectives for the investigation of shock-induced single-bubble or multibubble cavitation phenomena in thin liquids.

A supervised machine learning algorithm, called locally adaptive discriminant analysis (LADA), has been developed to locate boundaries between identifiable image features that have varying intensities. LADA is an adaptation of image segmentation, which includes techniques that find the positions of image features (classes) using statistical intensity distributions for each class in the image. In order to place a pixel in the proper class, LADA considers the intensity at that pixel and the distribution of intensities in local (nearby) pixels. This paper presents the use of LADA to provide, with statistical uncertainties, the positions and shapes of features within ultrafast images of shock waves. We demonstrate the ability to locate image features including crystals, density changes associated with shock waves, and material jetting caused by shock waves. This algorithm can analyze images that exhibit a wide range of physical phenomena because it does not rely on comparison to a model. LADA enables analysis of images from shock physics with statistical rigor independent of underlying models or simulations., United States. Office of Naval Research (Grant N00014-16-1-2090), United States. Office of Naval Research (Grant N00014-15-1-2694)

Focusing of high-amplitude surface acoustic waves leading to material damage is visualized in an all-optical experiment. The optical setup includes a lens and an axicon that focuses an intense picosecond excitation pulse into a ring-shaped pattern at the surface of a gold-coated glass substrate. Optical excitation induces a surface acoustic wave (SAW) that propagates in the plane of the sample and converges toward the center. The evolution of the SAW profile is monitored using interferometry with a femtosecond probe pulse at variable time delays. The quantitative analysis of the full-field images provides direct information about the surface displacement profiles, which are compared to calculations. The high stress at the focal point leads to the removal of the gold coating and, at higher excitation energies, to damage of the glass substrate. The results open the prospect for testing material strength on the microscale using laser-generated SAWs., United States. Army Research Office. Institute for Soldier Nanotechnologies (contract number W911NF-13-D-0001), Centre national de la recherche scientifique (France) (grant Projet International de Coopération Scientifique)

We demonstrate the agreement between first-principles calculations and experimental measurements of size effects in thermal transport in SiGe alloys without fitting parameters. Transient thermal grating (TTG) is used to measure the effect of the grating period on the temperature decay. The virtual crystal approximation under the density-functional-theory framework combined with impurity scattering is used to determine the phonon properties for the exact alloy composition of the measured samples. With these properties, classical size effects are calculated for the experimental geometry of reflection mode TTG using the recently developed variational solution to the phonon Boltzmann transport equation, which is verified against established Monte Carlo simulations. We find agreement between theoretical predictions and experimental measurements in the reduction of thermal conductivity (as much as fourfold of the bulk value) across grating periods spanning one order of magnitude. This paper provides a framework for the study of size effects in thermal transport in opaque materials.

Nature's highly efficient light-harvesting antennae, such as those found in green sulfur bacteria, consist of supramolecular building blocks that self-assemble into a hierarchy of close-packed structures. In an effort to mimic the fundamental processes that govern nature's efficient systems, it is important to elucidate the role of each level of hierarchy: from molecule, to supramolecular building block, to close-packed building blocks. Here, we study the impact of hierarchical structure. We present a model system that mirrors nature's complexity: cylinders self-assembled from cyanine-dye molecules. Our work reveals that even though close-packing may alter the cylinders' soft mesoscopic structure, robust delocalized excitons are retained: Internal order and strong excitation-transfer interactions-prerequisites for efficient energy transport-are both maintained. Our results suggest that the cylindrical geometry strongly favors robust excitons; it presents a rational design that is potentially key to nature's high efficiency, allowing construction of efficient light-harvesting devices even from soft, supramolecular materials.

Direct mesoscale measurements of radiation-induced changes in the mechanical properties of bulk materials remain difficult to perform. Most widely used characterization techniques are either macro- or microscale in nature, focusing on overall properties or overly small areas for analysis. Linking the atomic structure of irradiated materials directly with their radiation-affected properties remains one of the largest unmet challenges in radiation materials science. By measuring the change in surface acoustic wave speed as a function of relative orientation on metallic single crystals, we demonstrate that transient grating (TG) spectroscopy experiments have the sensitivity necessary to detect radiation-induced material property changes. We also show that classical molecular dynamics (MD) simulations can be used to accurately simulate orientation-based changes in surface acoustic wave speed in TG experiments, by comparing with experimental measurements and theoretical predictions. The agreement between theory, simulation, and experiment gives confidence in classical MD as a predictive tool to simulate defect-based changes in elastic properties, which cannot yet be fully treated by theory. This ability is of critical importance for the informed use of TG spectroscopy to measure material property changes induced by radiation damage, which may vary by amounts formerly too small for reliable in situ detection. Finally, our MD simulation framework is used to study the effect of an imposed vacancy population on the acoustic response of several materials. The results of these studies indicate that TG experiments are well suited to the ex situ and in situ study of radiation-induced material property changes., National Science Foundation (U.S.) (Grant 1122374), National Science Foundation (U.S.) (Grant CHE-1111557), Transatomic Power (Award 023875-001), U.S. Nuclear Regulatory Commission (MIT Nuclear Education Faculty Development Program. Grant NRC-HQ- 84-15-G-0045)

Ultrafast two-dimensional spectroscopy utilizes correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum. Its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. Here we report ultrafast two-dimensional terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by three terahertz field-dipole interactions. The nonlinear time-domain orientation signals are mapped into the frequency domain in two-dimensional rotational spectra which reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state., 31 pages, 14 figures

© 2016 American Physical Society. The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.