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.

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.

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)'.

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.

High-Frequency Elastic Coupling at the Interface of van der Waals Nanolayers Imaged by Picosecond Ultrasonics.

Although the topography of van de Waals (vdW) layers and heterostructures can be imaged by scanning probe microscopy, high-frequency interface elastic properties are more difficult to assess. These can influence the stability, reliability, and performance of electronic devices that require uniform layers and interfaces. Here, we use picosecond ultrasonics to image these properties in vdW layers and heterostructures based on well-known exfoliable materials, i.e., InSe, hBN, and graphene. We reveal a strong, uniform elastic coupling between vdW layers over a wide range of frequencies of up to tens of gigahertz (GHz) and in-plane areas of 100 µm2. In contrast, the vdW layers can be weakly coupled to their supporting substrate, behaving effectively as free-standing membranes. Our data and analysis demonstrate that picosecond ultrasonics offers opportunities to probe the high-frequency elastic coupling of vdW nanolayers and image both "perfect" and "broken" interfaces between different materials over a wide frequency range, as required for future scientific and technological developments.

Evaluation of crack parameters by a nonlinear frequency-mixing laser ultrasonics method.

The local evaluation of several parameters of a crack is realized with a nonlinear laser ultrasonic method. The method is based on the sample excitation by two laser beams, independently intensity modulated at two cyclic frequencies ωH and ωL (ωH≫ωL) and on the detection of nonlinear frequency-mixing ultrasonic components at frequencies ωH±nωL (n an integer). Frequency-mixing is a nonlinear process originating from the modulation of the crack state at low frequency ωL by laser-induced thermo-elastic stresses, which causes in turn the modulation of the acoustic waves at frequency ωH reflected/transmitted by the crack. We carry experiments with increasing laser power and observe a non-monotonous variation in the amplitude of up to 6 nonlinear sidelobes. We also improve a previously introduced theoretical model which leads to interpreting the experimental observations by the combined action on the crack of the thermo-elastic waves at low frequency ωL and of the stationary thermo-elastic stresses at ω=0. The latter are induced by the average laser power absorbed by the sample. While thermo-elastic wave can periodically modulate the parameters of the crack up to its periodic opening/closing, the stationary heating could cause complete local closure of the crack. By fitting the experimental amplitude evolutions for all monitored sidelobes with the theoretically predicted ones, various local parameters of the crack are extracted, including its local width and effective rigidity.

Picosecond laser ultrasonics for imaging of transparent polycrystalline materials compressed to megabar pressures.

Picosecond laser ultrasonics is an all-optical experimental technique based on ultrafast high repetition rate lasers applied for the generation and detection of nanometric in length coherent acoustic pulses. In optically transparent materials these pulses can be detected not only on their arrival at the sample surfaces but also all along their propagation path inside the sample providing opportunity for imaging of the sample material spatial inhomogeneities traversed by the acoustic pulse. Application of this imaging technique to polycrystalline elastically anisotropic transparent materials subject to high pressures in a diamond anvil cell reveals their significant texturing/structuring at the spatial scales exceeding dimensions of the individual crystallites.

Combined laser ultrasonics, laser heating, and Raman scattering in diamond anvil cell system.

We developed a multi-functional in situ measurement system under high pressure equipped with a laser ultrasonics (LU) system, Raman device, and laser heating system (LU-LH) in a diamond anvil cell (DAC). The system consists of four components: (1) a LU-DAC system (probe and pump lasers, photodetector, and oscilloscope) and DAC; (2) a fiber laser, which is designed to allow precise control of the total power in the range from 2 to 100 W by changing the diode current, for heating samples; (3) a spectrometer for measuring the temperature of the sample (using black body radiation), fluorescence spectrum (spectrum of the ruby for pressure measurement), and Raman scattering measurements inside a DAC under high pressure and high temperature (HPHT) conditions; and (4) an optical system to focus laser beams on the sample and image it in the DAC. The system is unique and allows us to do the following: (a) measure the shear and longitudinal velocities of non-transparent materials under HPHT; (b) measure temperature in a DAC under HPHT conditions using Planck's law; (c) measure pressure in a DAC using a Raman signal; and (d) measure acoustical properties of small flat specimens removed from the DAC after HPHT treatment. In this report, we demonstrate that the LU-LH-DAC system allows measurements of velocities of the skimming waves in iron at 2580 K and 22 GPa.

Revealing sub-µm and µm-scale textures in H2O ice at megabar pressures by time-domain Brillouin scattering.

The time-domain Brillouin scattering technique, also known as picosecond ultrasonic interferometry, allows monitoring of the propagation of coherent acoustic pulses, having lengths ranging from nanometres to fractions of a micrometre, in samples with dimension of less than a micrometre to tens of micrometres. In this study, we applied this technique to depth-profiling of a polycrystalline aggregate of ice compressed in a diamond anvil cell to megabar pressures. The method allowed examination of the characteristic dimensions of ice texturing in the direction normal to the diamond anvil surfaces with sub-micrometre spatial resolution via time-resolved measurements of the propagation velocity of the acoustic pulses travelling in the compressed sample. The achieved imaging of ice in depth and in one of the lateral directions indicates the feasibility of three-dimensional imaging and quantitative characterisation of the acoustical, optical and acousto-optical properties of transparent polycrystalline aggregates in a diamond anvil cell with tens of nanometres in-depth resolution and a lateral spatial resolution controlled by pump laser pulses focusing, which could approach hundreds of nanometres.

Probing single-cell mechanics with picosecond ultrasonics.

The mechanical properties of cells play a key role in several fundamental biological processes, such as migration, proliferation, differentiation and tissue morphogenesis. The complexity of the inner cell composition and the intricate meshwork formed by transmembrane cell-substrate interactions demands a non-invasive technique to probe cell mechanics and cell adhesion at a subcell scale. In this paper we review the use of laser-generated GHz acoustic waves--a technique called picosecond ultrasonics (PU)--to probe the mechanical properties of single cells. We first describe applications to vegetal cells and biomimetic systems. We show how these systems can be used as simple models to understand more complex animal cells. We then present an opto-acoustic bio-transducer designed for in vivo measurements in physiological conditions. We illustrate the use of this transducer through the simultaneous probing of the density and compressibility of Allium cepa cells. Finally, we demonstrate that this technique can quantify animal-cell adhesion on metallic surfaces by analyzing the acoustic pulses reflected off the cell-metal interface. This innovative approach allows investigating quantitatively cell mechanics without fluorescent labels or mechanical contact to the cell.

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.

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.