Coherent Phonons in van der Waals MoSe2/WSe2 Heterobilayers.

The increasing role of two-dimensional (2D) devices requires the development of new techniques for ultrafast control of physical properties in 2D van der Waals (vdW) nanolayers. A special feature of heterobilayers assembled from vdW monolayers is femtosecond separation of photoexcited electrons and holes between the neighboring layers, resulting in the formation of Coulomb force. Using laser pulses, we generate a 0.8 THz coherent breathing mode in MoSe2/WSe2 heterobilayers, which modulates the thickness of the heterobilayer and should modulate the photogenerated electric field in the vdW gap. While the phonon frequency and decay time are independent of the stacking angle between the MoSe2 and WSe2 monolayers, the amplitude decreases at intermediate angles, which is explained by a decrease in the photogenerated electric field between the layers. The modulation of the vdW gap by coherent phonons enables a new technology for the generation of THz radiation in 2D nanodevices with vdW heterobilayers.

Elastic moduli and refractive index of γ-Ge3N4.

Germanium nitride, having cubic spinel structure, γ-Ge3N4, is a wide band-gap semiconductor with a large exciton binding energy that exhibits high hardness, elastic moduli and elevated thermal stability up to approximately 700°C. Experimental data on its bulk and shear moduli (B0 and G0, respectively) are strongly limited, inconsistent and, thus, require verification. Moreover, earlier first-principles density functional calculations provided significantly scattering B0 values but consistently predicted G0 much higher than the so far available experimental value. Here, we examined the elasticity of polycrystalline γ-Ge3N4, densified applying high pressures and temperatures, using the techniques of laser ultrasonics (LU) and Brillouin light scattering (BLS) and compared with our extended first-principles calculations. From the LU measurements, we obtained its longitudinal- and Rayleigh wave sound velocities and, taking into account the sample porosity, derived B0 = 322(44) GPa and G0 = 188(7) GPa for the dense polycrystalline γ-Ge3N4. While our calculations underestimated B0 by approximately 17%, most of the predicted G0 matched well with our experimental value. Combining the LU- and BLS data and taking into account the elastic anisotropy, we determined the refractive index of γ-Ge3N4 in the visible range of light to be n = 2.4, similarly high as that of diamond or GaN, and matching our calculated value. This article is part of the theme issue 'Exploring the length scales, timescales and chemistry of challenging materials (Part 1)'.

Coherent Phononics of van der Waals Layers on Nanogratings.

Strain engineering can be used to control the physical properties of two-dimensional van der Waals (2D-vdW) crystals. Coherent phonons, which carry dynamical strain, could push strain engineering to control classical and quantum phenomena in the unexplored picosecond temporal and nanometer spatial regimes. This intriguing approach requires the use of coherent GHz and sub-THz 2D phonons. Here, we report on nanostructures that combine nanometer thick vdW layers and nanogratings. Using an ultrafast pump-probe technique, we generate and detect in-plane coherent phonons with frequency up to 40 GHz and hybrid flexural phonons with frequency up to 10 GHz. The latter arises from the periodic modulation of the elastic coupling of the vdW layer at the grooves and ridges of the nanograting. This creates a new type of a tailorable 2D periodic phononic nanoobject, a flexural phononic crystal, offering exciting prospects for the ultrafast manipulation of states in 2D materials in emerging quantum technologies.

Giant Photoelasticity of Polaritons for Detection of Coherent Phonons in a Superlattice with Quantum Sensitivity.

The functionality of phonon-based quantum devices largely depends on the efficiency of the interaction of phonons with other excitations. For phonon frequencies above 20 GHz, generation and detection of the phonon quanta can be monitored through photons. The photon-phonon interaction can be enormously strengthened by involving an intermediate resonant quasiparticle, e.g., an exciton, with which a photon forms a polariton. In this work, we discover a giant photoelasticity of exciton-polaritons in a short-period superlattice and exploit it to detect propagating acoustic phonons. We demonstrate that 42 GHz coherent phonons can be detected with extremely high sensitivity in the time domain Brillouin oscillations by probing with photons in the spectral vicinity of the polariton resonance.

Gigahertz Optomechanical Photon-Phonon Transduction between Nanostructure Lines.

High-frequency surface phonons have a myriad of applications in telecommunications and sensing, but their generation and detection have often been limited to transducers occupying micron-scale regions because of the use of two-dimensional transducer arrays. Here, by means of transient reflection spectroscopy we experimentally demonstrate optically coupled nanolocalized gigahertz surface phonon transduction based on a gold nanowire emitter arranged parallel to linear gold nanorod receiver arrays, that is, quasi-one-dimensional emitter-receivers. We investigate the response up to 10 GHz of these individual optoacoustic and acousto-optic transducers, respectively, by exploiting plasmon-polariton longitudinal resonances of the nanorods. We also demonstrate how the surface phonon detection efficiency is highly dependent on the nanorod orientation with respect to the phonon wave vector, which constrains the symmetry of the detectable modes, and on the nanorod acoustic resonance spectrum. Applications include nanosensing.

Ultra-short photoacoustic pulse generation through hot electron pressure in two-dimensional electron gas.

Launching ultrashort femtosecond photoacoustic pulses with multi-terahertz bandwidth will find broad applications from fundamental acoustics in 2D materials and THz-acoustic and phonon spectroscopy to nondestructive detection in opaque materials with a sub-nanometer resolution. Here we report the generation of ultra-short 344 fs photoacoustic pulses with a 2.1 THz bandwidth from interfacial two-dimensional electron gas using optical femtosecond excitation. A comparison with simulation supports the dominant contribution of hot electron pressure and the ultrafast electron relaxation to produce pulsewidth shorter than the acoustic transit time across the electron wavefunction. Our simulation further indicates the possibility to generate <200 fs photoacoustic pulse.

Ultrafast tunable modulation of light polarization at terahertz frequencies.

Controlling light polarization is one of the most essential routines in modern optical technology. Since the demonstration of optical pulse shaping by spatial light modulators and its potential in controlling the quantum reaction pathways, it paved the way for many applications as a coherent control of the photoionization process or as polarization shaping of terahertz (THz) pulses. Here, we evidenced efficient nonresonant and noncollinear χ(2)-type light-matter interaction in femtosecond polarization-sensitive time-resolved optical measurements. Such nonlinear optical interaction of visible light and ultrashort THz pulses leads to THz modulation of visible light polarization in bulk LiNbO3 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.

Nonlinear acoustics at GHz frequencies in a viscoelastic fragile glass former.

Using a picosecond pump-probe ultrasonic technique, we study the propagation of high-amplitude, laser-generated longitudinal coherent acoustic pulses in the viscoelastic fragile glass former DC704. We observe an increase of almost 10% in acoustic pulse propagation speed 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 gigahertz frequency range across the glass transition temperature.

Graphene-to-substrate energy transfer through out-of-plane longitudinal acoustic phonons.

Practically, graphene is often deposited on substrates. Given the major substrate-induced modification of properties and considerable energy transfer at the interface, the graphene-substrate interaction has been widely discussed. However, the proposed mechanisms were restricted to the two-dimensional (2D) plane and interface, while the energy conduction in the third dimension is hardly considered. Herein, we disclose the transfer of energy perpendicular to the interface of the combined system of the 2D graphene and the 3D base. More precisely, our observation of the energy dissipation of optically excited graphene via emitting out-of-plane longitudinal acoustic phonon into the substrate is presented. By applying nanoultrasonic spectroscopy with a piezoelectric nanolayer embedded in the substrate, we found that under photoexcitation by a femtosecond laser pulse graphene can emit longitudinal coherent acoustic phonons (CAPs) with frequencies over 1 THz into the substrate. In addition, the waveform of the CAP pulse infers that the photocarriers and sudden lattice heating in graphene caused modification of graphene-substrate bond and consequently generated longitudinal acoustic phonons in the substrate. The direct observation of this unexplored graphene-to-substrate vertical energy transfer channel can bring new insights into the understanding of the energy dissipation and limited transport properties of supported graphene.

Structural heterogeneities at the origin of acoustic and transport anomalies in glycerol glass-former.

By means of large scale molecular dynamics simulations, we explore mesoscopic properties of prototypical glycerol glass-former above and below the glass transition. The model used, in excellent agreement with various experimental techniques, permits to carefully study the structure and the vibrational dynamics. We find that a medium range order is present in glycerol glass-former and arises from hydrogen bond network extension. The characteristic size of the structural heterogeneities is related to the anomalous properties of acoustic vibrations (Rayleigh scattering, "mode softening," and Boson Peak) in the glassy state. Finally the characteristic size of these heterogeneities, nearly constant in temperature, is also connected to the cross-over between structural relaxation and diffusion in liquid glycerol.

Optically Controlled Nano-Transducers Based on Cleaved Superlattices for Monitoring Gigahertz Surface Acoustic Vibrations.

Surface acoustic waves (SAWs) convey energy at subwavelength depths along surfaces. Using interdigital transducers (IDTs) and opto-acousto-optic transducers (OAOTs), researchers have harnessed coherent SAWs with nanosecond periods and micrometer localization depth for various applications. These applications include the sensing of small amount of materials deposited on surfaces, assessing surface roughness and defects, signal processing, light manipulation, charge carrier and exciton transportation, and the study of fundamental interactions with thermal phonons, photons, magnons, and more. However, the utilization of cutting-edge OAOTs produced through surface nanopatterning techniques has set the upper limit for coherent SAW frequencies below 100 GHz, constrained by factors such as the quality and pitch of the surface nanopattern, not to mention the electronic bandwidth limitations of the IDTs. In this context, unconventional optically controlled nanotransducers based on cleaved superlattices (SLs) are here presented as an alternative solution. To demonstrate their viability, we conducted proof-of-concept experiments using ultrafast lasers in a pump-probe configuration on SLs made of alternating AlxGa1-xAs and AlyGa1-yAs layers with approximately 70 nm periodicity and cleaved along their growth direction to produce a periodic nanostructured surface. The acoustic vibrations, generated and detected by laser beams incident on the cleaved surface, span a range from 40 to 70 GHz, corresponding to the generalized surface Rayleigh mode and bulk modes within the dispersion relation. This exploration shows that, in addition to SAWs, cleaved SLs offer the potential to observe surface-skimming longitudinal and transverse acoustic waves at GHz frequencies. This proof-of-concept demonstration below 100 GHz in nanoacoustics using such an unconventional platform might be useful for realizing sub-THz to THz coherent surface acoustic vibrations in the future, as SLs can be epitaxially grown with atomic-scale layer width and quality.

Sound velocity mapping from GHz Brillouin oscillations in transparent materials by optical incidence from the side of the sample.

Time-domain Brillouin scattering (TDBS) is an all-optical experimental technique for investigating transparent materials based on laser picosecond ultrasonics. Its application ranges from imaging thin-films, polycrystalline materials and biological cells to physical properties such as residual stress, temperature gradients and nonlinear coherent nano-acoustic pulses. When the sample refractive index is spatially uniform and known in TDBS, analysis by windowed Fourier transforms allows one to depth-profile the sound velocity. Here, we present a new method in TDBS for extracting sound velocity without a knowledge of the refractive index, by use of probe light obliquely incident on a side face-as opposed to the usual top face-of the sample. We demonstrate this method using a fused silica sample with a titanium transducer film and map the sound velocity in the depth direction. In future, it should be possible to map the sound velocity distribution in three dimensions in inhomogeneous samples, with applications to the imaging of biological cells.

Time-domain Brillouin scattering theory for probe light and acoustic beams propagating at an angle and acousto-optic interaction at material interfaces.

A theory has been developed to interpret time-domain Brillouin scattering (TDBS) experiments involving coherent acoustic pulse (CAP) and light pulse beams propagating at an angle to each other. It predicts the influence of the directivity pattern of their acousto-optic interaction on TDBS signals when heterodyne detection of acoustically scattered light is in backward direction to incident light. The theory reveals relationships between the carrier frequency, amplitude and duration of acoustically induced "wave packets" in light transient reflectivity signals, and factors such as CAP duration, widths of light and sound beams, and their interaction angle. It describes the transient dynamics of these wave packets when the light and CAP encounter material interfaces, and how the light scattering by the incident CAP transforms into scattering by the reflected and transmitted CAPs. The theory suggests that single-point TDBS experiments can determine not only depth positions of buried interfaces but also their local inclinations/orientations.

Time-domain Brillouin scattering for evaluation of materials interface inclination: Application to photoacoustic imaging of crystal destruction upon non-hydrostatic compression.

Time-domain Brillouin scattering (TDBS) is a developing technique for imaging/evaluation of materials, currently used in material science and biology. Three-dimensional imaging and characterization of polycrystalline materials has been recently reported, demonstrating evaluation of inclined material boundaries. Here, the TDBS technique is applied to monitor the destruction of a lithium niobate single crystal upon non-hydrostatic compression in a diamond anvil cell. The 3D TDBS experiments reveal, among others, modifications of the single crystal plate with initially plane-parallel surfaces, caused by non-hydrostatic compression, the laterally inhomogeneous variations of the plate thickness and relative inclination of opposite surfaces. Our experimental observations, supported by theoretical interpretation, indicate that TDBS enables the evaluation of materials interface orientation/inclination locally, from single point measurements, avoiding interface profilometry. A variety of observations reported in this paper paves the way to further expansion of the TDBS imaging use to analyze fascinating processes/phenomena occurring when materials are subjected to destruction.

Probing of laser-induced crack modulation by laser-monitored surface waves and surface skimming bulk waves.

All-optical monitoring of the nonlinear motion of a surface-breaking crack is reported. Crack closing is induced by quasi-continuous laser heating, while Rayleigh surface acoustic pulses and bulk longitudinal surface skimming acoustic pulses are also generated and detected by lasers. By exploiting the strong dependence of the acoustic pulses reflection and transmission efficiency on the state-open or closed-of the contacts between the crack faces, the parametric modulation of ultrasonic pulses is achieved. It is observed that bulk acoustic waves skimming along the surface can be more sensitive to crack motion than Rayleigh surface waves.

Ballistic dynamics of flexural thermal movements in a nanomembrane revealed with subatomic resolution.

Flexural oscillations of freestanding films, nanomembranes, and nanowires are attracting growing attention for their importance to the fundamental physical and optical properties and device applications of two-dimensional and nanostructured (meta)materials. Here, we report on the observation of short-time scale ballistic motion in the flexural mode of a nanomembrane cantilever, driven by thermal fluctuation of flexural phonons, including measurements of ballistic velocities and displacements performed with subatomic resolution, using a free electron edge-scattering technique. Within intervals <10 µs, the membrane moves ballistically at a constant velocity, typically ~300 µm/s, while Brownian-like dynamics emerge for longer observation periods. Access to the ballistic regime provides verification of the equipartition theorem and Maxwell-Boltzmann statistics for flexural modes and can be used in fast thermometry and mass sensing during atomic absorption/desorption processes on the membrane.

In-Situ Imaging of a Light-Induced Modification Process in Organo-Silica Films via Time-Domain Brillouin Scattering.

We applied time-domain Brillouin scattering (TDBS) for the characterization of porogen-based organosilicate glass (OGS) films deposited by spin-on-glass technology and cured under different conditions. Although the chemical composition and porosity measured by Fourier-transform infrared (FTIR) spectroscopy and ellipsometric porosimetry (EP) did not show significant differences between the films, remarkable differences between them were revealed by the temporal evolution of the Brillouin frequency (BF) shift of the probe light in the TDBS. The observed modification of the BF was a signature of the light-induced modification of the films in the process of the TDBS experiments. It correlated to the different amount of carbon residue in the samples, the use of ultraviolet (UV) femtosecond probe laser pulses in our optical setup, and their intensity. In fact, probe radiation with an optical wavelength of 356 nm appeared to be effective in removing carbon residue through single-photon absorption processes, while its two-photon absorption might have led to the breaking of Si-CH3 bonds in the OSG matrix. The quantum chemical calculations confirmed the latter possibility. This discovery demonstrates the possibility of local modifications of OSG films with a nanometric resolution via nonlinear optical processes, which could be important, among other applications, for the creation of active surface sites in the area-selective deposition of atomic layers.

All-optical probing of the nonlinear acoustics of a crack.

Experiments with an all-optical method for the study of the nonlinear acoustics of cracks in solids are reported. Nonlinear acoustic waves are initiated by the absorption of radiation from a pair of laser beams intensity modulated at two different frequencies. The detection of acoustic waves at mixed frequencies, absent in the frequency spectrum of the heating lasers, by optical interferometry or deflectometry provides unambiguous evidence of the elastic nonlinearity of the crack. The high contrast in crack imaging achieved by remote optical monitoring of the nonlinear acoustic processes is due to the strong dependence of the efficiency of optoacoustic conversion on the state of the crack. The highest acoustic nonlinearity is observed in the transitional state of the crack, which is intermediate between the open and the closed ones.

Evaluation of Optical and Acoustical Properties of Ba1-xSrxTiO3 Thin Film Material Library via Conjugation of Picosecond Laser Ultrasonics with X-ray Diffraction, Energy Dispersive Spectroscopy, Electron Probe Micro Analysis, Scanning Electron and Atomic Force Microscopies.

Wide-range continuous spatial variation of the film composition in lateral compositionally graded epitaxial films requires the development of high throughput measurement techniques for their local and non-destructive characterization with the highest possible spatial resolution. Here we report on the first application of the picosecond laser ultrasonics (PLU) technique for the evaluation of acoustical and optical parameters of lateral compositionally graded film, the Ba1-xSrxTiO3 (0 ≤ x ≤ 1) material library. The film was not dedicatedly prepared for its opto-acousto-optic evaluation by PLU, exhibiting significant lateral variations in thickness and surface roughness. Therefore, the achieved measurements of the sound velocity and of the optical refractive index, and characterization of the surface roughness confirm the robustness of the PLU technique for thin film evaluation. We hope that the first measurements of the acoustical and optical properties of epitaxial grown Ba1-xSrxTiO3 (0 ≤ x ≤ 1) by PLU technique accomplished here provide the parameters required for more extended predictive design of the phononic, photonic and phoxonic mirrors and cavities with superior properties/functionalities for novel multifunctional nanodevices.

Photoacoustic 3-D imaging of polycrystalline microstructure improved with transverse acoustic waves.

Non-invasive fast imaging of grain microstructure of polycrystalline ceria with sub-micrometric spatial resolution is performed via time-domain Brillouin scattering. The propagation of a nanoacoustic pulse is monitored down to 8 µm deep in a 30 × 30 µm2 area. Grains boundaries are reconstructed in three-dimensions via a two-step processing method, relying on the wavelet synchro-squeezed transform and the alphashape algorithm. Imaging contrast is improved by taking advantage of stronger sensitivity to anisotropy of transverse acoustic waves, compared with longitudinal waves. Utilization of transverse waves in the image processing reveals additional boundaries, confirmed by an electron backscattering diffraction pattern but not discerned using longitudinal waves. A buried inclined interface between differently oriented grains is identified by monitoring changes in amplitude (phase) of the portion of the signal associated with transverse (longitudinal) waves. Estimates of the inclination angle of this interface prove the sensitivity of our laser ultrasonic method to image inclined boundaries.