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Density Functional Theory (DFT) calculations not only allow to predict the vibrational and optical properties of solids but also to understand and disentangle the mechanisms playing a key role in the generation of coherent optical phonons. Recent experiments performed on a Bi$_2$Te$_3$ nanofilm have shown that a THz pulse launches at least a coherent $A_{1g}^1$ phonon as the transient transmittance measured using an isotropic detection scheme displays oscillations with a frequency matching the frequency of the $A_{1g}^1$ mode measured in Raman experiments. Such an observation can be explained by invoking either a sum frequency process or cubic/quartic phonon-phonon couplings as considered for Bi$_2$Se$_3$, a parent compound of Bi$_2$Te$_3$. By resorting to group theory and calculating energy surfaces from first-principles, the main phonon-phonon couplings can be identified. Furthermore, a minimal model can be built to compute the dynamics of the Raman active modes coupled to the infrared active mode driven by the experimental THz pulse. Our model firmly establishes that cubic phonon-phonon interactions are relevant as the agreement between the computed and experimental transmittance is noteworthy., Comment: 6 pages, 3 figures, submitted to Physical Review Letters

Superlattices are materials created by the alternating growth of two chemically different materials. The direct consequence of creating a superlattice is the folding of the Brillouin zone which gives rise to additional electronic bands and phonon modes. This has been successfully exploited to achieve new transport and optical properties in semiconductor superlattices, for example. Here, we show that multiferroic BiFeO$_3$/LaFeO$_3$ superlattices are more than just periodic chemical stacking. Using transmission electron microscopy, X-ray diffraction and first-principles calculations, we demonstrate the existence of a new order of FeO$_6$ octahedra, with a period along the growth direction about twice that of the chemical supercell, i.e. a superorder. The effect of this new structural order on the lattice dynamics is studied with ultrafast optical pump-probe experiments. While a mode at 1.2 THz is attributed solely to the chemical modulation of the superlattice, the existence of another 0.7 THz mode seems to be explained only by a double Brillouin zone folding in agreement with the structural description. Our work shows that multiferroic BiFeO$_3$/LaFeO$_3$ superlattices can be used to tune the spectrum of coherent THz phonons, and potentially that of magnons or electromagnons.

The dielectric properties of Bi$_2$Te$_3$, a layered compound crystallizing in a rhombohedral structure, are investigated by means of first-principles calculations at the random phase approximation level. A special attention is devoted to the anisotropy in the dielectric function and to the local field effects that strongly renormalize the optical properties in the UV-visible range when the electric field is polarized along the stacking axis. Furthermore, both the Born effective charges for each atom and the zone center phonon frequencies and eigenvectors needed to describe the dielectric response in the infrared range are computed. Our theoretical near-normal incidence reflectivity spectras in both the UV-visible and infrared range are in fairly good agreement with the experimental spectras, provided that the free carriers Drude contribution arising from defects is included in the infrared response. The anisotropic plasmon frequencies entering the Drude model are computed within the rigid band approximation, suggesting that a measurement of the reflectivity in the infrared range for both polarizations might allow to infer not only the type of doping but also the level of doping., Comment: 29 pages, 10 figures

As sadly known, forest fires are part of a set of natural disasters that have always affected regions of the world typically characterized by a tropical climate with long periods of drought. However, due to climate changes of the recent years, other regions of our planet that were not affected by this plague have also had to deal with this phenomenon. One of them is certainly the Italian peninsula, and especially the regions of southern Italy. For this reason, the scientific community, and in particular that one of the remote sensing, plays an important role in the development of reliable techniques to provide useful support to the competent authorities. Therefore, in this work, the capability of the Normalized Differential Water Index (NDWI), derived from spaceborne remote sensing (RS) data, is assessed to monitor the forest fires occurred on a specific study area during the summer of 2017: the volcano Vesuvius, near Naples (in Campania, Italy). In particular, the index is obtained from Sentinel-2 multispectral images of the European Space Agency (ESA), which are free of charge and open accessible. Moreover, the twin Sentinel-2 (S-2) sensors allows to overcome some restrictions on time delivery and high frequency observation. These requirements are goodly matched by other spaceborne sensors, such as MODIS and VIIRS satellites, but at the expense of a lower spatial resolution., Comment: 4 pages, 2 tables, 4 figures, IGARSS 2020

Disordered optical media are an emerging class of materials capable of strongly scattering light. Their study is relevant to investigate transport phenomena and for applications in imaging, sensing and energy storage. While such materials can be used to generate coherent light, their directional emission is typically hampered by their very multiple scattering nature. Here, we tune the out-of-plane directionality of coherent Raman light scattered by a fractal network of silicon nanowires. By visualizing Rayleigh scattering, photoluminescence and weakly localized Raman light from the random network of nanowires via real-space microscopy and Fourier imaging, we gain insight on the light transport mechanisms responsible for the material's inelastic coherent signal and for its directionality. The possibility of visualizing and manipulating directional coherent light in such networks of nanowires opens venues for fundamental studies of light propagation in disordered media as well as for the development of next generation optical devices based on disordered structures, inclusive of sensors, light sources and optical switches.

Phase change alloys have seen widespread use from rewritable optical discs to the present day interest in their use in emerging neuromorphic computing architectures. In spite of this enormous commercial interest, the physics of carriers in these materials is still not fully understood. Here, we describe the time and space dependence of the coupling between photoexcited carriers and the lattice in both the amorphous and crystalline states of one phase change material, GeTe. We study this using a time-resolved optical technique called picosecond acoustic method to investigate the \textit{in situ} thermally assisted amorphous to crystalline phase transformation in GeTe. Our work reveals a clear evolution of the electron-phonon coupling during the phase transformation as the spectra of photoexcited acoustic phonons in the amorphous ($a$-GeTe) and crystalline ($\alpha$-GeTe) phases are different. In particular and surprisingly, our analysis of the photoinduced acoustic pulse duration in crystalline GeTe suggests that a part of the energy deposited during the photoexcitation process takes place over a distance that clearly exceeds that defined by the pump light skin depth. In the opposite, the lattice photoexcitation process remains localized within that skin depth in the amorphous state. We then demonstrate that this is due to supersonic diffusion of photoexcited electron-hole plasma in the crystalline state. Consequently these findings prove the existence of a non-thermal transport of energy which is much faster than lattice heat diffusion.

Enabling the light-control of complex systems on ultra-short timescales gives rise to rich physics with promising applications. While crucial, the quantitative determination of both the longitudinal and shear photo-induced strains still remains challenging. Here, by scrutinizing asymmetric Bragg peaks pairs $(\pm h01)$ using picosecond time-resolved X-ray diffraction experiments in BiFeO$_3$, we simultaneously determine the longitudinal and shear strains. The relative amplitude of those strains can be explained only if both thermal and non-thermal processes contribute to the acoustic phonon photogeneration process. Importantly, we also reveal a difference of the dynamical response of the longitudinal strain with respect to the shear one due to an interplay of quasi-longitudinal and quasi-transverse acoustic modes, well reproduced by our model.

Remote Sensing applications can benefit from a relatively fine spatial resolution multispectral (MS) images and a high revisit frequency ensured by the twin satellites Sentinel-2. Unfortunately, only four out of thirteen bands are provided at the highest resolution of 10 meters, and the others at 20 or 60 meters. For instance the Short-Wave Infrared (SWIR) bands, provided at 20 meters, are very useful to detect active fires. Aiming to a more detailed Active Fire Detection (AFD) maps, we propose a super-resolution data fusion method based on Convolutional Neural Network (CNN) to move towards the 10-m spatial resolution the SWIR bands. The proposed CNN-based solution achieves better results than alternative methods in terms of some accuracy metrics. Moreover we test the super-resolved bands from an application point of view by monitoring active fire through classic indices. Advantages and limits of our proposed approach are validated on specific geographical area (the mount Vesuvius, close to Naples) that was damaged by widespread fires during the summer of 2017., Comment: 8 pages, 6 figures

Clear anomalies in the lattice thermal expansion (deviation from linear variation) and elastic properties (softening of the sound velocity) at the antiferromagnetic-to-paramagnetic transition are observed in the prototypical multiferroic BiFeO3 using a combination of picosecond acoustic pump-probe and high-temperature X-ray diffraction experiments. Similar anomalies are also evidenced using first-principles calculations supporting our experimental findings. Those calculations in addition to a simple Landau-like model we also developed allow to understand the elastic softening and lattice change at T_N as a result of magnetostriction combined with electrostrictive and magnetoelectric couplings which renormalize the elastic constants of the high-temperature reference phase when the critical T_N temperature is reached.

Time-domain Brillouin scattering is an all-optical experimental technique based on ultrafast lasers applied for generation and detection of coherent acoustic pulses on time durations of picoseconds and length scales of nanometers. In transparent materials scattering of the probe laser beam by the coherent phonons permits imaging of sample inhomogeneity. The transient optical reflectivity of the sample recorded by the probe beam as the acoustic nanopulse propagates in space contains information on the acoustical, optical, and acousto-optical parameters of the material under study. The experimental method is based on a heterodyning where weak light pulses scattered by the coherent acoustic phonons interfere at the photodetector with probe light pulses of significantly higher amplitude reflected from various interfaces of the sample. The time-domain Brillouin scattering imaging is based on Brillouin scattering and has the potential to provide all the information that researchers in material science, physics, chemistry, biology etc., get with classic frequency-domain Brillouin scattering of light. It can be viewed as a replacement for Brillouin scattering and Brillouin microscopy in all investigations where nanoscale spatial resolution is either required or advantageous. Here we review applications of time-domain Brillouin scattering for imaging of nanoporous films, ion-implanted semiconductors and dielectrics, texture in polycrystalline materials and inside vegetable and animal cells, and for monitoring the transformation of nanosound caused by nonlinearity and focusing. We also discuss the perspectives and the challenges for the future., Comment: This article has been accepted by Applied Physics Reviews. After it is published, it will be found at https://aip.scitation.org/journal/are. Copyright (2018) Vitalyi E. Gusev and Pascal Ruello. This article is distributed under a Creative Commons Attribution (CC BY) License

The way nuclear motion affects electronic responses has become a very hot topic in materials science. Coherent acoustic phonons can dynamically modify optical, magnetic and mechanical properties at ultrasonic frequencies, with promising applications as sensors and transducers. Here, by means of ultrafast broadband deep-ultraviolet spectroscopy, we demonstrate that coherent acoustic phonons confined in anatase TiO$_2$ nanoparticles can selectively modulate the oscillator strength of the two-dimensional bound excitons supported by the material. We use many-body perturbation-theory calculations to reveal that the deformation potential is the mechanism behind the generation of the observed coherent acoustic wavepackets. Our results offer a route to manipulate and dynamically tune the properties of excitons in the deep-ultraviolet at room temperature.

The coherent manipulation of excitons in bulk semiconductors via the lattice degrees of freedom is key to the development of acousto-optic and acousto-excitonic devices. Wide-bandgap transition metal oxides exhibit strongly bound excitons that are interesting for applications in the deep-ultraviolet, but their properties have remained elusive due to the lack of efficient generation and detection schemes in this spectral range. Here, we perform ultrafast broadband deep-ultraviolet spectroscopy on anatase TiO$_2$ single crystals at room temperature, and reveal a dramatic modulation of the exciton peak amplitude due to coherent acoustic phonons. This modulation is comparable to those of nanostructures where exciton-phonon coupling is enhanced by quantum confinement, and is accompanied by a giant exciton shift of 30-50 meV. We model these results by many-body perturbation theory and show that the deformation potential coupling within the nonlinear regime is the main mechanism for the generation and detection of the coherent acoustic phonons. Our findings pave the way to the design of exciton control schemes in the deep-ultraviolet with propagating strain pulses.

We report GHz longitudinal as well as shear acoustic phonons photoexcitation and photodetection using femtosecond laser pulses in a spin-crossover molecular crystal. From our experimental observation of time domain Brillouin scattering triggered by the photoexcitation of acoustic waves across the low-spin (LS) to high-spin (HS) thermal crossover, we reveal a link between molecular spin state and photoexcitation of coherent GHz acoustic phonons. In particular, we experimentally evidence an unconventional non-thermal pathway for the laser excitation of GHz phonons. We also provide experimental insight on the optical and mechanical parameters evolution across the LS/HS spin crossover temperature T$_{1/2}$.

We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonon generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon. These results demonstrate how it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures.

Ultrafast lattice dynamics of few quintuple layers of topological insulator (TI) Bi$_2$Te$_3$ is studied with time-resolved optical pump-probe spectroscopy. Both optical and acoustic phonons are photogenerated and detected. Here, in order to get new insights on the out-of-equilibrium electron-phonon coupling and phonons dynamics in confined TI, different nanostructures have been investigated (single or polycrystalline QLs assemblies and nano-crystallized islands). Contrary to previous literature claims, we show that even for nanostructures containing only 10 quintuple layers (QLs), the symmetric A1g(I) coherent optical phonon is efficiently photogenerated and no restriction due to the structural confinement appears. We also observe that whatever the arrangement of the nanostructures, the A1g(I) optical phonon features are similar (lifetime). We also report the observation of confined coherent acoustic phonons propagating from QLs to QLs whose spectrum is, this time, very sensitive to the atomic arrangement. In the case of the single crystalline ultrathin film, the time of flight analysis of these acoustic phonons provides direct estimate of the elastic properties of these nanostructures as well as some estimates of Van der Waals interactions between QLs.

Ultrafast laser excited hot electrons can transport energy supersonically far from the region where they are initially produced. We show that this ultrafast energy transport is responsible of the emission of coherent acoustic phonons deeply beneath the free surface of a copper metal sample. In particular we demonstrate that enough energy carried by these hot electrons over a distance as large as 220nm at room temperature in copper can be converted into coherent acoustic phonons. In order to demonstrate this effect, several configurations of time-resolved optical experiments of time of flight of coherent acoustic phonons and of hot electrons have been performed., Comment: 8 pages, 4 figures