arXiv subjects

G. Vaudel

Publications and source records attributed to G. Vaudel.

6 recordsLinked to original sources

arXiv2025

Nonlinear phononics in Bi$_2$Te$_3$ nanoscale thin films: A theoretical approach

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.

cond-mat.mtrl-sci↗

arXiv2024

Superorders and acoustic modes folding in BiFeO$_3$/LaFeO$_3$ superlattices

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.

cond-mat.mtrl-sci↗

arXiv2020

Non-thermal transport of energy driven by photoexcited carriers in switchable solid states of GeTe

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 ($α$-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.

cond-mat.mtrl-sci↗

arXiv2020

Ultrafast light-induced shear strain probed by time-resolved X-ray diffraction: the model multiferroic BiFeO$_3$ as a case study

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.

cond-mat.mtrl-sci↗

arXiv2017

Ultrafast electron-phonon-magnon interactions at noble metal-ferromagnet interfaces

Ultrafast optical excitation of gold-cobalt bilayers triggers the nontrivial interplay between the electronic, acoustic, and magnetic degrees of freedom. Laser-heated electrons generated at the gold-air interface diffuse through the layer of gold and strongly overheat the lattice in cobalt resulting in the emission of ultrashort acoustic pulses and generation of exchange-coupled magnons. Time-resolved optical measurements allow for extracting the thermal boundary (Kapitza) resistances at metal/metal interfaces and the hot electron diffusion length in ferromagnetic materials. Both the experimental data and the analytical treatment of the two-temperature model reveal the role of the Kapitza resistance in transient lattice overheating.

cond-mat.mtrl-sci↗

arXiv2015

Ultrafast Acousto-Plasmonics in Gold Nanoparticles Superlattice

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.

cond-mat.mtrl-sci↗