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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. [ABSTRACT FROM AUTHOR]

Spin/charge interconversion mechanisms provide an essential handle to generate and detect spin currents. Their applications at different timescales are critical in spintronics since they cover a technologically relevant broadband spectrum. While the inverse spin Hall effect is known to be robust from quasi-static to sub-picosecond timescales, the conversion efficiency evolution of the inverse Edelstein effect has not been addressed yet. In this work, we report that while the quasi-static response of the inverse Edelstein effect can be comparable to that of the most efficient inverse spin Hall systems, a drastic drop of efficiency is observed in the terahertz (THz) regime. This behavior at the sub-picosecond timescale is qualitatively understood from the dependence of the inverse Edelstein effect on the energy distribution of spin-carrier entities, which is different between thermalized carriers in the quasi-static regime and hot carriers generated by light pulses. This finding is supported by the pump-laser wavelength dependence in the THz regime for the inverse Edelstein effect, which offers a promising route for tunability of spintronic devices. [ABSTRACT FROM AUTHOR]

Bimetallic Au/Ag core–shell cuboid nanoparticles (NPs) exhibit a complex plasmonic response dominated by a dipolar longitudinal mode and higher-order transverse modes in the near-UV, which may be exploited for a range of applications. In this paper, we take advantage of the strong signature of these modes in the NP ultrafast transient optical response, measured by pump-probe transient absorption (TA) spectroscopy, to explore the NP vibrational landscape. The fast Fourier transform analysis of the TA dynamics reveals specific vibration modes in the frequency range 15–150 GHz, further studied by numerical simulations based on the finite element method. While bare Au nanorods exhibit extensional and breathing modes, the bimetallic NPs undergo more complex motions, involving the displacement of facets, edges and corners. The amplitude and frequency of these modes are shown to depend on the Ag shell thickness, as the silver load modifies the NP aspect ratio and mass. Moreover, the contributions of the vibrational modes to the experimental TA spectra are shown to vary with the probe laser wavelength at which the signal is monitored. Using the combined simulations of the NP elastic and optical properties, we elucidate this influence by analyzing the effect of the mechanisms involved in the acousto-plasmonic coupling. [ABSTRACT FROM AUTHOR]

The transient electronic and molecular structure arising from photoinduced charge transfer in transition metal complexes is studied by X-ray powder diffraction with a 100 fs temporal and atomic spatial resolution. Crystals containing a dense array of Fe(II)-tris(bipyridine) ([Fe(bpy)3]2 +) complexes and their PF6 - counterions display pronounced changes of electron density that occur within the first 100 fs after two-photon excitation of a small fraction of the [Fe(bpy)3]2 + complexes. Transient electron density maps derived from the diffraction data reveal a transfer of electronic charge from the Fe atoms and-so far unknown-from the PF6 - counterions to the bipyridine units. Such charge transfer (CT) is connected with changes of the inter-ionic and the Fe-bipyridine distances. An analysis of the electron density maps demonstrates the many-body character of charge transfer which affects approximately 30 complexes around a directly photoexcited one. The many-body behavior is governed by the long-range Coulomb forces in the ionic crystals and described by the concept of electronic polarons. [ABSTRACT FROM AUTHOR]

The interaction of intense femtosecond pulses with metals allows for generating ultrashort hard x-rays. In contrast to plasma theories, tunneling from the target into vacuum is introduced as electron generation step, followed by vacuum acceleration in the laser field and re-entrance into the target to generate characteristic x-rays and Bremsstrahlung. For negligible space charge in vacuum, the Kα flux is proportional to the incident intensity and the wavelength squared, suggesting a strong enhancement of the x-ray flux by mid-infrared driving pulses. This prediction is in quantitative agreement with experiments on femtosecond Cu Kα generation. [ABSTRACT FROM AUTHOR]

Ultrafast structural dynamics in the condensed phase represents a key topic of current physics, chemistry and materials science. Femtosecond hard X-ray pulses are important structure probes that have been applied in time-resolved X-ray absorption and diffraction. Optical pump/X-ray probe schemes with compact laser-driven table-top sources have allowed for tiny changes of diffracted intensity to be measured with X-ray photon statistics, which has set the ultimate sensitivity limit. To address the strong quest for a higher X-ray flux, here we present the first hard X-ray plasma source driven by intense mid-infrared sub-100-fs pulses at 3.9 μm. The comparably long optical period allows for accelerating electrons from the Cu target to very high kinetic energies and for generating a characteristic Kα flux of 109 photons per pulse, 25 times more than with our 800 nm driver. Theoretical simulations account for the experimental results in a wide range of driving fields and predict a further enhancement of X-ray flux. [ABSTRACT FROM AUTHOR]

X-Ray diffraction provides insight into the distribution of electronic charge in crystals. Equilibrium electron distributions have been determined with high spatial resolution by recording and analysing a large number of diffraction peaks under stationary conditions. In contrast, transient electron densities during and after structure-changing processes are mainly unknown. Recently, we have introduced femtosecond X-ray powder diffraction from polycrystalline samples to determine transient electron density maps with a spatial resolution of 0.03 nm and a temporal resolution of 100 fs. In a pump–probe approach with a laser-driven tabletop hard X-ray source, optically induced structure changes are resolved in time by diffracting the hard X-ray probe pulses at different time delays from the excited powder sample and recording up to several tens of reflections simultaneously. Time-dependent changes of the atomic arrangement in the crystal lattice as well as modified electron densities are derived from the diffraction data. As a prototypical field-driven process, we address here quasi-instantaneous changes of electron density in LiBH4, LiH and NaBH4 in response to a non-resonant strong optical field. The light-induced charge relocation in LiBH4 and NaBH4 exhibits an electron transfer from the anion (BHSTACKABOVE−/ABOVEBELOW4/BELOW/STACK) to the respective cation. The distorted geometry of the BH4 tetrahedron in LiBH4 leads to different contributions of the H atoms to electron transfer. LiH displays a charge transfer from Li to H, i.e., an increase of the ionicity of LiH in the presence of the strong electric field. This unexpected behavior originates from strong electron correlations in LiH as is evident from a comparison with quasi-particle bandstructures calculated within the Coulomb-hole-plus-screened-exchange (COHSEX) formalism. [ABSTRACT FROM AUTHOR]

We study the quasi-instantaneous change of electron density in the unit cells of LiH and NaBH4 in response to a nonresonant strong optical field. We determine for the first time the related transient electron density maps, applying femtosecond x-ray powder diffraction as a structure probe. The light-induced charge relocation in NaBH4 exhibits an electron transfer from the anion (BH-4) to the Na+ cation. In contrast, LiH displays the opposite behavior, i.e., an increase of the ionicity of LiH in the presence of the strong electric field. This behavior originates from strong electron correlations in LiH, as is evident from a comparison with quasiparticle band structures calculated within the Coulomb-hole-plus-screened-exchange formalism. [ABSTRACT FROM AUTHOR]

Thedependence of the spectral width of the longitudinal localizedsurface plasmon resonance (LSPR) of individual gold nanorods protectedby a silica shell is investigated as a function of their size. Experimentswere performed using the spatial modulation spectroscopy techniquethat permits determination of both the spectral characteristics ofthe LSPR of an individual nanoparticle and its morphology. The measuredLSPR is shown to broaden with reduction of both the nanorod lengthand its diameter, which is in contrast with the predictions of existingclassical and quantum theoretical models. This behavior can be reproducedassuming the LSPR width linearly depends on the inverse of an effectivelength proportional to the square root of the particle surface withthe same slope as that recently determined for silica-coated silvernanospheres. [ABSTRACT FROM AUTHOR]

The acoustic vibration modes of spherical composite nanoparticles formed by a core and an arbitrary number of shells are computed using a semianalytic approach based on elastic theory. The modes observed in time-resolved pump-probe experiments are identified in the case of metal-dielectric-based spherical composite nanoparticles, and results are illustrated in the case of Ag@SiO2 core-shell nanoparticles. The presence of a light dielectric shell is shown to only weakly shift the frequency of the dominant mode observed in time-resolved experiments. Moreover, a large impact of the mechanical contact between the different materials forming the particle on the vibrational mode frequency and damping is predicted, offering the possibility of experimentally addressing this parameter. [ABSTRACT FROM AUTHOR]

Abstract: Laser-induced breakdown spectroscopy (LIBS) has been applied to analyze trace elements contained in fresh vegetables. A quadrupled Nd:YAG laser is used in the experiments for ablation. Analyzed samples come from local markets and represent frequently consumed vegetables. For a typical root vegetable, such as potato, spectral analysis of the plasma emission reveals more than 400 lines emitted by 27 elements and 2 molecules, C2 and CN. Among these species, one can find trace as well as ultra-trace elements. A space-resolved analysis of several trace elements with strong emissions is then applied to typical root, stem and fruit vegetables. The results from this study demonstrate the potential of an interesting tool for botanical and agricultural studies as well for food quality/safety and environment pollution assessment and control. [Copyright &y& Elsevier]

The temperature dependence of the thermal boundary resistivity is investigated in glass-embedded Ag particles of radius 4.5 nm, in the temperature range from 300 to 70 K, using all-optical time-resolved nanocalorimetry. The present results provide a benchmark for theories aiming at explaining the thermal boundary resistivity at the interface between metal nanoparticles and their environment, a topic of great relevance when tailoring thermal energy delivery from nanoparticles as for applications in nanomedicine and thermal management at the nanoscale. [ABSTRACT FROM AUTHOR]

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.

The effects of the dielectric environment on the optical extinction spectra of gold nanorods were quantitatively studied using individual bare and silica-coated nanorods. The dispersion and amplitude of their extinction cross-section, dominated by absorption for the investigated sizes, were measured using spatial modulation spectroscopy (SMS). The experimental results were compared to calculations from a numerical model that included environmental features present in the measurements and the morphology and size of the corresponding nanorods measured by transmission electron microscopy. The combination of these experimental and theoretical tools permits a detailed interpretation of the optical properties of the individual nanorods. The measured optical extinction spectra and the extinction cross-section amplitudes were well reproduced by the numerical model for silica-coated gold nanorods, for which the silica shell provides a controlled environment. In contrast, additional environmental factors had to be assumed in the model for bare nanorods, stressing the importance of controlling and characterizing the experimental conditions when measuring the optical response of bare surface-deposited single metal nanoparticles.

The acoustic vibrations of metal nanoparticles encapsulated in a dielectric shell (Ag@SiO(2)) were investigated using a time-resolved femtosecond technique. The measured vibration periods significantly differ from those predicted for the bare metal cores and, depending on the relative core and shell sizes, were found to be either larger or smaller than them. These results show that the vibration of the whole core-shell particle is excited and detected. Moreover, vibrational periods are in excellent agreement with the predictions of a model based on continuum thermoelasticity. However, such agreement is obtained only if a good mechanical contact of the metal and dielectric parts of the core-shell particle is assumed, providing a unique way to probe this contact in multimaterial or hybrid nano-objects.

The acoustic response of surface-controlled metal (Pt) nanoparticles is investigated in the small size range, between 1.3 and 3 nm (i.e., 75-950 atoms), using time-resolved spectroscopy. Acoustic vibration of the nanoparticles is demonstrated, with frequencies ranging from 1.1 to 2.6 THz, opening the way to the development of THz acoustic resonators. The frequencies, measured with a noncontact optical method, are in excellent agreement with the prediction of a macroscopic approach based on the continuous elastic model, together with the bulk material elastic constants. This demonstrates the validity of this model at the nanoscale and the weak impact of size reduction on the elastic properties of a material, even for nanoparticles formed by less than 100 atoms.