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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., Comment: 30 pages (including supplementary text), 5 main figures, 9 supplementary figures; corrected author list

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 performed femtosecond reflection spectroscopy on a series of perovskite-type cobalt oxide $R$BaCo$_2$O$_{6-\delta}$ ($R$=Sm, Gd, and Tb) crystals, in which the electronic transfer was controlled by $R$. The transient reflectivity and the optical conductivity ($\sigma^{\rm PI}(\omega)$) 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 $\sigma^{\rm PI}(\omega)$ upon photoexcitation sensitively depended on the $R$-species, indicating an important role of electronic correlation in the photoexcited state.

Using inelastic neutron scattering, x-ray, neutron diffraction, and the first-principle calculation techniques, we show that the crystal structure of the two-dimensional quantum spin system (CuCl)LaNb$_2$O$_7$ is orthorhombic with $Pbam$ symmetry in which CuCl$_4$O$_2$ octahedra are tilted from their high symmetry positions and the Cu$^{2+} (s = 1/2)$ ions form a distorted square lattice. The dominant magnetic interactions are the fourth nearest neighbor antiferromagnetic interactions with a Cu-Cl--Cl-Cu exchange path, which lead to the formation of spin singlets. The two strongest interactions between the singlets are ferromagnetic, which makes (CuCl)LaNb$_2$O$_7$ the first system of ferromagnetically coupled Shastry-Sutherland quantum spin singlets.