Ultrafast Suppression of the Ferroelectric Instability in KTaO_{3}.

We use an x-ray free-electron laser to study the lattice dynamics following photoexcitation with ultrafast near-UV light (wavelength 266 nm, 50 fs pulse duration) of the incipient ferroelectric potassium tantalate, KTaO_{3}. By probing the lattice dynamics corresponding to multiple Brillouin zones through the x-ray diffuse scattering with pulses from the Linac Coherent Light Source (LCLS) (wavelength 1.3 Å and <10 fs pulse duration), we observe changes in the diffuse intensity associated with a hardening of the transverse acoustic phonon branches along Γ to X and Γ to M. Using force constants from density functional theory, we fit the quasiequilibrium intensity and obtain the instantaneous lattice temperature and density of photoexcited charge carriers. The density functional theory calculations demonstrate that photoexcitation transfers charge from oxygen 2p derived π-bonding orbitals to Ta 5d derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

Complex Contact-Based Dynamics of Microsphere Monolayers Revealed by Resonant Attenuation of Surface Acoustic Waves.

Contact-based vibrations play an essential role in the dynamics of granular materials. Significant insights into vibrational granular dynamics have previously been obtained with reduced-dimensional systems containing macroscale particles. We study contact-based vibrations of a two-dimensional monolayer of micron-sized spheres on a solid substrate that forms a microscale granular crystal. Measurements of the resonant attenuation of laser-generated surface acoustic waves reveal three collective vibrational modes that involve displacements and rotations of the microspheres, as well as interparticle and particle-substrate interactions. To identify the modes, we tune the interparticle stiffness, which shifts the frequency of the horizontal-rotational resonances while leaving the vertical resonance unaffected. From the measured contact resonance frequencies we determine both particle-substrate and interparticle contact stiffnesses and find that the former is an order of magnitude larger than the latter. This study paves the way for investigating complex contact-based dynamics of microscale granular crystals and yields a new approach to studying micro- to nanoscale contact mechanics in multiparticle networks.

Four-wave-mixing experiments with seeded free electron lasers.

The development of free electron laser (FEL) sources has provided an unprecedented bridge between the scientific communities working with ultrafast lasers and extreme ultraviolet (XUV) and X-ray radiation. Indeed, in recent years an increasing number of FEL-based applications have exploited methods and concepts typical of advanced optical approaches. In this context, we recently used a seeded FEL to demonstrate a four-wave-mixing (FWM) process stimulated by coherent XUV radiation, namely the XUV transient grating (X-TG). We hereby report on X-TG measurements carried out on a sample of silicon nitride (Si3N4). The recorded data bears evidence for two distinct signal decay mechanisms: one occurring on a sub-ps timescale and one following slower dynamics extending throughout and beyond the probed timescale range (100 ps). The latter is compatible with a slower relaxation (time decay > ns), that may be interpreted as the signature of thermal diffusion modes. From the peak intensity of the X-TG signal we could estimate a value of the effective third-order susceptibility which is substantially larger than that found in SiO2, so far the only sample with available X-TG data. Furthermore, the intensity of the time-coincidence peak shows a linear dependence on the intensity of the three input beams, indicating that the measurements were performed in the weak field regime. However, the timescale of the ultrafast relaxation exhibits a dependence on the intensity of the XUV radiation. We interpreted the observed behaviour as the generation of a population grating of free-electrons and holes that, on the sub-ps timescale, relaxes to generate lattice excitations. The background free detection inherent to the X-TG approach allowed the determination of FEL-induced electron dynamics with a sensitivity largely exceeding that of transient reflectivity and transmissivity measurements, usually employed for this purpose.

Dirac cone dispersion of acoustic waves in plates without phononic crystals (L).

Lamb waves in elastic plates exhibit Dirac-like cone dispersion at zero wavevector at the points of accidental degeneracy between longitudinal and transverse thickness resonances. The Lamb mode dispersion can be fine-tuned to yield a conical point by coating a plate with a layer of a different material and varying the thickness of the latter. Similarities and differences with respect to Dirac-like cone dispersion in phononic crystals and possible observable effects are discussed.

Anisotropy of the thermal conductivity in GaAs/AlAs superlattices.

We combine the transient thermal grating and time-domain thermoreflectance techniques to characterize the anisotropic thermal conductivities of GaAs/AlAs superlattices from the same wafer. The transient grating technique is sensitive only to the in-plane thermal conductivity, while time-domain thermoreflectance is sensitive to the thermal conductivity in the cross-plane direction, making them a powerful combination to address the challenges associated with characterizing anisotropic heat conduction in thin films. We compare the experimental results from the GaAs/AlAs superlattices with first-principles calculations and previous measurements of Si/Ge SLs. The measured anisotropy is smaller than that of Si/Ge SLs, consistent with both the mass-mismatch picture of interface scattering and with the results of calculations from density-functional perturbation theory with interface mixing included.

Interaction of a contact resonance of microspheres with surface acoustic waves.

We study the interaction of surface acoustic waves (SAWs) with a contact-based vibrational resonance of 1 µm silica microspheres forming a two-dimensional granular crystal adhered to a substrate. The laser-induced transient grating technique is used to excite SAWs and measure their dispersion. The measured dispersion curves exhibit "avoided crossing" behavior due to the hybridization of the SAWs with the microsphere resonance. We compare the measured dispersion curves with those predicted by our analytical model and find excellent agreement. The approach presented can be used to study the contact mechanics and adhesion of micro- and nanoparticles as well as the dynamics of microscale granular crystals.

Direct measurement of room-temperature nondiffusive thermal transport over micron distances in a silicon membrane.

The "textbook" phonon mean free path of heat carrying phonons in silicon at room temperature is ∼40 nm. However, a large contribution to the thermal conductivity comes from low-frequency phonons with much longer mean free paths. We present a simple experiment demonstrating that room-temperature thermal transport in Si significantly deviates from the diffusion model already at micron distances. Absorption of crossed laser pulses in a freestanding silicon membrane sets up a sinusoidal temperature profile that is monitored via diffraction of a probe laser beam. By changing the period of the thermal grating we vary the heat transport distance within the range ∼1-10 µm. At small distances, we observe a reduction in the effective thermal conductivity indicating a transition from the diffusive to the ballistic transport regime for the low-frequency part of the phonon spectrum.

Imaging phonon eigenstates and elucidating the energy storage characteristics of a honeycomb-lattice phononic crystal cavity.

We extend gigahertz time-domain imaging to a wideband investigation of the eigenstates of a phononic crystal cavity. Using omnidirectionally excited phonon wave vectors, we implement an ultrafast technique to experimentally probe the two-dimensional acoustic field inside and outside a hexagonal cavity in a honeycomb-lattice phononic crystal formed in a microscopic crystalline silicon slab, thereby revealing the confinement and mode volumes of phonon eigenstates-some of which are clearly hexapole in character-lying both inside and outside the phononic-crystal band gap. This allows us to obtain a quantitative measure of the spatial acoustic energy storage characteristics of a phononic crystal cavity. We also introduce a numerical approach involving toneburst excitation and the monitoring of the acoustic energy decay together with the integral of the Poynting vector to calculate the Q factor of the principal in-gap eigenmode, showing it to be limited by ultrasonic attenuation rather than by phonon leakage to the surrounding region.

Extreme ultraviolet transient gratings: A tool for nanoscale photoacoustics.

Collective lattice dynamics determine essential aspects of condensed matter, such as elastic and thermal properties. These exhibit strong dependence on the length-scale, reflecting the marked wavevector dependence of lattice excitations. The extreme ultraviolet transient grating (EUV TG) approach has demonstrated the potential of accessing a wavevector range corresponding to the 10s of nm length-scale, representing a spatial scale of the highest relevance for fundamental physics and forefront technology, previously inaccessible by optical TG and other inelastic scattering methods. In this manuscript we report on the capabilities of this technique in the context of probing thermoelastic properties of matter, both in the bulk and at the surface, as well as discussing future developments and practical considerations.

Dispersion of an acoustic pulse passing through a large-grained polycrystalline film.

Propagation of a short acoustic pulse through a polycrystalline film comprised of large randomly oriented elastically anisotropic grains is analyzed theoretically. For average grain size much larger than the film thickness, a short acoustic pulse launched normally into the film will traverse each grain in a time determined by the acoustic slowness in the direction normal to the film, which will depend on the local grain orientation. A typical measurement averages over a large number of grains resulting in the broadening of the composite output pulse. The resulting pulse shape is characterized by distinct features related to stationary values of the directionally dependent acoustic slowness of the crystalline material. Maxima and minima in the slowness yield discontinuities in the pulse shape, while saddle points yield logarithmic singularities. For cubic and hexagonal crystals, power law singularities result from cones of directions in which the slowness is a maximum or minimum. Numerical results, taking into account Gaussian broadening of the input pulse, are presented for thin film materials commonly encountered in picosecond ultrasonic experiments, such as copper, gold, and aluminum.

Coherent Brillouin spectroscopy in a strongly scattering liquid by picosecond ultrasonics.

In a modification of a picosecond ultrasonic technique, a short acoustic pulse is launched into a liquid sample by a laser pulse absorbed in a semitransparent transducer film and is detected via coherent Brillouin scattering of a time-delayed probe pulse. With both excitation and probing performed from the transducer side, the arrangement is suitable for in vivo study of biological tissues. The signal is collected from a micrometer-thick layer next to the transducer and is not affected by the diffuse scattering of probe light deeper in the sample. The setup, utilizing a 33 nm thick single crystal SrRuO(3) transducer film, is tested on a full fat milk sample, with 11 GHz acoustic frequency recorded.

Ray splitting in the reflection and refraction of surface acoustic waves in anisotropic solids.

This paper examines the conditions for, and provides examples of, ray splitting in the reflection and refraction of surface acoustic waves (SAW) in elastically anisotropic solids at straight obstacles such as edges, surface breaking cracks, and interfaces between different solids. The concern here is not with the partial scattering of an incident SAW's energy into bulk waves, but with the occurrence of more than one SAW ray in the reflected and/or transmitted wave fields, by analogy with birefringence in optics and mode conversion of bulk elastic waves at interfaces. SAW ray splitting is dependent on the SAW slowness curve possessing concave regions, which within the constraint of wave vector conservation parallel to the obstacle allows multiple outgoing SAW modes for certain directions of incidence and orientation of obstacle. The existence of pseudo-SAW for a given surface provides a further channel for ray splitting. This paper discusses some typical material configurations for which SAW ray splitting occurs. An example is provided of mode conversion entailing backward reflection or negative refraction. Experimental demonstration of ray splitting in the reflection of a laser generated SAW in GaAs(111) is provided. The calculation of SAW mode conversion amplitudes lies outside the scope of this paper.

Multi-frame interferometric imaging with a femtosecond stroboscopic pulse train for observing irreversible phenomena.

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.

Observation of second sound in graphite at temperatures above 100 K.

Wavelike thermal transport in solids, referred to as second sound, is an exotic phenomenon previously limited to a handful of materials at low temperatures. The rare occurrence of this effect restricted its scientific and practical importance. We directly observed second sound in graphite at temperatures above 100 kelvins by using time-resolved optical measurements of thermal transport on the micrometer-length scale. Our experimental results are in qualitative agreement with ab initio calculations that predict wavelike phonon hydrodynamics. We believe that these results potentially indicate an important role of second sound in microscale transient heat transport in two-dimensional and layered materials in a wide temperature range.

Nanoscale transient gratings excited and probed by extreme ultraviolet femtosecond pulses.

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.

Layer specific observation of slow thermal equilibration in ultrathin metallic nanostructures by femtosecond X-ray diffraction.

Ultrafast heat transport in nanoscale metal multilayers is of great interest in the context of optically induced demagnetization, remagnetization and switching. If the penetration depth of light exceeds the bilayer thickness, layer-specific information is unavailable from optical probes. Femtosecond diffraction experiments provide unique experimental access to heat transport over single digit nanometer distances. Here, we investigate the structural response and the energy flow in the ultrathin double-layer system: gold on ferromagnetic nickel. Even though the excitation pulse is incident from the Au side, we observe a very rapid heating of the Ni lattice, whereas the Au lattice initially remains cold. The subsequent heat transfer from Ni to the Au lattice is found to be two orders of magnitude slower than predicted by the conventional heat equation and much slower than electron-phonon coupling times in Au. We present a simplified model calculation highlighting the relevant thermophysical quantities.

Photo-excited charge carriers suppress sub-terahertz phonon mode in silicon at room temperature.

There is a growing interest in the mode-by-mode understanding of electron and phonon transport for improving energy conversion technologies, such as thermoelectrics and photovoltaics. Whereas remarkable progress has been made in probing phonon-phonon interactions, it has been a challenge to directly measure electron-phonon interactions at the single-mode level, especially their effect on phonon transport above cryogenic temperatures. Here we use three-pulse photoacoustic spectroscopy to investigate the damping of a single sub-terahertz coherent phonon mode by free charge carriers in silicon at room temperature. Building on conventional pump-probe photoacoustic spectroscopy, we introduce an additional laser pulse to optically generate charge carriers, and carefully design temporal sequence of the three pulses to unambiguously quantify the scattering rate of a single-phonon mode due to the electron-phonon interaction. Our results confirm predictions from first-principles simulations and indicate the importance of the often-neglected effect of electron-phonon interaction on phonon transport in doped semiconductors.

Lifetime of high-order thickness resonances of thin silicon membranes.

Femtosecond laser pulses are used to excite and probe high-order longitudinal thickness resonances at a frequency of ∼270 GHz in suspended Si membranes with thickness ranging from 0.4 to 15 µm. The measured acoustic lifetime scales linearly with the membrane thickness and is shown to be controlled by the surface specularity which correlates with roughness characterized by atomic force microscopy. Observed Q-factor values up to 2400 at room temperature result from the existence of a local maximum of the material Q in the sub-THz range. However, surface specularity would need to be improved over measured values of ∼0.5 in order to achieve high Q values in nanoscale devices. The results support the validity of the diffuse boundary scattering model in analyzing thermal transport in thin Si membranes.

Laser-induced transient grating setup with continuously tunable period.

We present a modification of the laser-induced transient grating setup enabling continuous tuning of the transient grating period. The fine control of the period is accomplished by varying the angle of the diffraction grating used to split excitation and probe beams. The setup has been tested by measuring dispersion of bulk and surface acoustic waves in both transmission and reflection geometries. The presented modification is fully compatible with optical heterodyne detection and can be easily implemented in any transient grating setup.