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H. Cailleau

Publications and source records attributed to H. Cailleau.

3 recordsLinked to original sources

Strain Wave Pathway to Semiconductor-to-Metal Transition revealed by time resolved X-ray powder diffraction

Thanks to the remarkable developments of ultrafast science, one of today's challenges is to modify material state by controlling with a light pulse the coherent motions that connect two different phases. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a macroscopic transformation pathway for the semiconducting-to-metal transition with large volume change in bistable Ti$_3$O$_5$ nanocrystals. Femtosecond powder X-ray diffraction allowed us to quantify the structural deformations associated with the photoinduced phase transition on relevant time scales. We monitored the early intra-cell distortions around absorbing metal dimers, but also long range crystalline deformations dynamically governed by acoustic waves launched at the laser-exposed Ti$_3$O$_5$ surface. We rationalize these observations with a simplified elastic model, demonstrating that a macroscopic transformation occurs concomitantly with the propagating acoustic wavefront on the picosecond timescale, several decades earlier than the subsequent thermal processes governed by heat diffusion.

cond-mat.mtrl-sci

Ultrafast non-thermal laser excitation of gigahertz longitudinal and shear acoustic waves in spin-crossover molecular crystals [$Fe(PM-AzA)_{2}$$(NCS)_{2}$]

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$_{1/2}$.

cond-mat.mtrl-sci

Ultrafast Spectral Weight Transfer in RBaCo2O6-delta (R=Sm, Gd, and Tb): A Role of Electronic Correlation in Photoinduced Phase Transition

We performed femtosecond reflection spectroscopy on a series of perovskite-type cobalt oxide $R$BaCo$_2$O$_{6-δ}$ ($R$=Sm, Gd, and Tb) crystals, in which the electronic transfer was controlled by $R$. The transient reflectivity and the optical conductivity ($σ^{\rm PI}(ω)$) obtained by Kramers-Kronig analysis showed an ultrafast change within a time resolution ($\approx 150$ fs) at room temperature and the appearance of signals of a hidden state different from the high temperature metallic state. The transferred spectral weight in $σ^{\rm PI}(ω)$ upon photoexcitation sensitively depended on the $R$-species, indicating an important role of electronic correlation in the photoexcited state.

cond-mat.str-el