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Mott insulators are a class of strongly correlated materials with emergent properties important for modern electronics applications. The key property for application is the Electric Mott insulator to metal Transitions (EMT) whose proposed mechanism is related to the creation of hot electrons by electric field triggering an electronic avalanche after a time delay. This model suggests that the direct creation of hot carriers thanks to a laser pulse should drastically affect the EMT. We have tested this idea by performing pump-pump-probe experiments on single crystals of the Mott insulator GaTa4Se8, whereby electric and laser pulses simultaneously excite the crystal while electric probe monitors its conductivity. Our results show that the concomitant application of femtosecond laser pulse reduced the time delay of EMT by a factor up to. Measurements performed with different laser wavelengths and fluences support moreover that the EMT is driven by a hot carriers generation mechanism.

Der LIESST-Effekt (“light-induced excited spin state trapping”) in Eisen(II)-Spinubergangsverbindungen, das heist, die lichtinduzierte Population des High-spin-Zustands (S=2) unterhalb der thermischen Ubergangstemperatur, wurde vor 30 Jahren entdeckt. Fur die Einstrahlung in Metall-Ligand-Charge-Transfer(MLCT)-Banden der Low-spin-Spezies (S=0) geht die anerkannte Relaxationskaskade in etwa 150 fs vom ursprunglich angeregten 1MLCT-Zustand uber den 3MLCT-Zustand direkt in den High-spin-Zustand, wobei die tiefenergetischen Ligandenfeld(LF)-Zustande umgangen werden. Die Beobachtung von LIESST und reverse-LIESST mittels Einstrahlung direkt in die LF-Banden in Systemen mit nur hochenergetischen MLCT-Zustanden zeigt, dass diese dennoch eine Rolle spielen. Hier identifizieren wir den ersten angeregten S=1-LF-Zustand als Zwischenzustand mit einer Lebensdauer von 39 ps in der Kaskade von reverse-LIESST, die auf die Anregung in den spinerlaubten LF-Ubergang der high-spin Spezies im NIR folgt.

We used the newly developed low-$\alpha$mode of SOLEIL synchrotron to observe optically induced strain waves in 200nm bismuth thin-films.

We discuss the capacity of ultrafast broadband spectroscopy to become a test bed for investigating dynamics of metals driven far from equilibrium by a femtosecond laser pulse. A controversy in conventional description of the reflectivity of metals is looked upon by means of pump–probe white light set-up.

The family of materials (EDO-TTF)2XF6 represents quasi-one-dimensional ¼ filled systems exhibiting insulator-to-metal (I-M) phase transition at thermal equilibrium. (EDO-TTF)2PF6 is known to undergo a photoinduced I-M conversion with cooperative response to light excitation. Here we use femtosecond pump-probe experiments to study the photoresponse of (EDO-TTF)2SbF6 made of a larger counter-anion SbF6 compared to the well studied (EDO-TTF)2PF6. In the early stage of the photoinduced process, we reveal a multi-component coherent oscillating feature. The evolution of this feature with excitation density and temperature points to the local nature of the photoswitching in (EDO-TTF)2SbF6. At longer timescale, we did not detect the features associated with the transformation to the M phase, albeit observed in the PF 6 derivative. We propose a scenario whereby the bigger size of the counter-anion in (EDO-TTF)2SbF6 hinders the establishment of this transformation at macroscopic scale.

We report GHz longitudinal as well as shear acoustic phonon 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 the molecular spin state and photoexcitation of coherent GHz acoustic phonons. In particular, we experimentally evidence a non-thermal pathway for the laser excitation of GHz phonons. We also provide experimental insights into the optical and mechanical parameters evolving across the LS/HS spin crossover temperature range.

The optical control of materials and related physical properties (electronic state, magnetic, optical...) by laser irradiation has gained tremendous interest within the emerging field of photoinduced phase transitions. Light-induced changes of molecular systems involve subtle coupling between the electronic and structural degrees of freedom, which are essential to stabilize the photo-excited state, different in nature from the stable state. Therefore the new experimental field of photocrystallography plays a key role. Its outreach goes far beyond simple structural analysis under laser excitation. By playing on different physical parameters and developing the techniques and analysis, one can investigate new out of equilibrium physics through light-driven cooperative dynamics and transformations in materials, or follow a chemical reaction in real time [1]. The use of photo-crystallography allows to investigate the nature, the mechanisms and the dynamics of photoinduced phase transitions. Here we will present photocrystallography studies of the photo-switching process in spin-crossover materials. On the one hand, ultrafast diffraction allows to follow the structural dynamics [2] and to probe the different processes following femtosecond laser excitation. Recent studies performed on the LCLS X-FEL have shown that the structural molecular changes, with the characteristic Fe-N bond elongation, occur within 160 fs. On the other hand, we will present investigations on the effect of light excitation on spin-state concentration waves, which may be of aperiodic nature (Figure, [3]). Time-resolved x-ray diffraction studies reveal that the high symmetry phase is reached only after milliseconds.

International audience; Light-induced excited spin-state trapping (LIESST) in iron(II) spin-crossover compounds, that is, the light-induced population of the high-spin (S=2) state below the thermal transition temperature, was discovered thirty years ago. For irradiation into metal-ligand charge transfer (MLCT) bands of the low-spin (S=0) species the acknowledged sequence takes the system from the initially excited 1MLCT to the high-spin state via the 3MLCT state within ca. 150 fs, thereby bypassing low-lying ligand-field (LF) states. Nevertheless, these play a role, as borne out by the observation of LIESST and reverse-LIESST on irradiation directly into the LF bands for systems with only high-energy MLCT states. Herein we elucidate the ultrafast reverse-LIESST pathway by identifying the lowest energy S=1 LF state as an intermediate state with a lifetime of 39 ps for the light-induced high-spin to low-spin conversion on irradiation into the spin-allowed LF transition of the high-spin species in the NIR.

International audience; The emergence of the field of photo-induced transformation triggered by intense and ultra-short light pulse in a material has opened a new route to acting on matter. It combines many of today's issues such as far away from equilibrium phenomena, coherence and quantum control, complex correlations and non linear responsiveness, inter-conversion of energy and information. The advent of ultrafast structural dynamics motivated developing new tools to directly watch how matter works, by probing the time- and length-scales on which photo-induced processes take place. Different points will be briefly overviewed: (i) the development of laser pump and X-ray probe for watching ultrafast structural dynamics, (ii) the physical features resulting from this way of impacting materials by light, (iii) the presentation of some examples investigated by time-resolved X-ray diffraction and diffuse scattering experiments to illustrate the complex structural dynamics of a photo-induced transformation.

International audience; We report here on the ultrafast photo-switching dynamics of a Fe(II) molecular material [Fe(PM-AzA)2(NCS)2]. It undergoes a thermal spin-crossover which can be detected by magnetic measurements or by optical reflectivity. We use here femtosecond optical reflectivity to study the ultrafast photo-switching dynamics. Our results indicate that the HS state is reached from the LS state within less than 100 fs, through an intermediate MLCT state. This ultrafast relaxation from the electronic excited state towards the structurally relaxed HS state is followed by a vibrational cooling of the hot HS molecules within ≈1 ps timescale.

International audience; We report on the spin state photoswitching dynamics triggered by a femtosecond laser of [(TPA)FeIII(TCC)]+ cations in a new salt with SbF6- anions. Femtosecond optical pump-probe spectroscopy and picosecond X-ray diffraction techniques were combined to investigate the different steps of the out-of-equilibrium dynamics. The obtained results are very consistent with the ones previously reported for the PF6- salts. If the ultra-fast responses of the cations in both salts are similar, the spin conversion due to laser heating is slightly shifted to higher temperature in the SbF6- salt, as its thermal crossover occurs at higher temperature.

International audience

International audience; We report the spin state photo-switching dynamics in two polymorphs of a spin-crossover molecular complex triggered by a femtosecond laser flash, as determined by combining femtosecond optical pump-probe spectroscopy and picosecond X-ray diffraction techniques. The light-driven transformations in the two polymorphs are compared. Combining both techniques and tracking how the X-ray data correlate with optical signals allow understanding of how electronic and structural degrees of freedom couple and play their role when the switchable molecules interact in the active crystalline medium. The study sheds light on crossing the border between femtochemistry at the molecular scale and femtoswitching at the material scale.

International audience; We study by 100 picosecond X-ray diffraction the photo-switching dynamics of single crystal of the orthorhombic polymorph of the spin-crossover complex [(TPA)Fe(TCC)]PF(6), in which TPA = tris(2-pyridyl methyl)amine, TCC(2-) = 3,4,5,6-Cl(4)-Catecholate(2-). In the frame of the emerging field of dynamical structural science, this is made possible by using optical pump/X-ray probe techniques, which allow following in real time structural reorganization at intra- and intermolecular levels associated with the change of spin state in the crystal. We use here the time structure of the synchrotron radiation generating 100 picosecond X-ray pulses, coupled to 100 fs laser excitation. This study has revealed a rich variety of structural reorganizations, associated with the different steps of the dynamical process. Three consecutive regimes are evidenced in the time domain: 1) local molecular photo-switching with structural reorganization at constant volume, 2) volume relaxation with inhomogeneous distribution of local temperatures, 3) homogenization of the crystal in the transient state 100 µs after laser excitation. These findings are fundamentally different from those of conventional diffraction studies of long-lived photoinduced high spin states. The time-resolution used here with picosecond X-ray diffraction probes different physical quantities on their intrinsic time-scale, shedding new light on the successive processes driving macroscopic switching in a functionalized material. These results pave the way for structural studies away from equilibrium and represent a first step toward femtosecond crystallography.

International audience; In this paper we put on solid ground the optical time-resolved study of spin-state photoinduced switching in an Fe(III) compound whose structural dynamics have been recently unveiled. We provide the experimental evidence of complex dynamics, occurring in succession, and spanning ten decades in time. We show that in addition to the ultrafast photoinduced molecular switching occurring on the subpicosecond timescale, there exists two additional switching processes significantly affecting the fate of the macroscopic material: one driven by elastic interactions as volume expansion occurs on a tens of nanoseconds timescale, and another one associated with heat diffusion and thermal switching taking place on a tens of microseconds timescale.

International audience; The birth of the field of photoinduced phase transitions was strongly influenced by the conceptual viewpoint expressed by Professor Y. Toyozawa on the condensation of relaxed excitons. Since this first period, twenty years ago, this young field has been expanding rapidly along a diversity of directions. Nowadays, it goes hand in hand with the challenges of today's science: emergence, nonlinearity, coherence, far away from equilibrium, for example. The control of the functionality of a material via photoexcited states poses many new fundamental questions. Some of them will be overviewed: (i) the nature of the control parameters and the nature of the relevant collective variables, especially the order parameters, which characterize the evolution of the system, (ii) the difference between photoinduced transformations under continuous light irradiation and those resulting from an ultrashort laser pulse, (iii) the physical mechanisms of ultrafast photoinduced phase transitions from the formation and proliferation of phototransformed entities to the softening of a collective mode.

International audience; Fast and ultra-fast time-resolved diffraction is a fantastic tool for directly observing the structural dynamics of a material rearrangement during the transformation induced by an ultra-short laser pulse. The paper illustrates this ability using the dynamics of photoinduced molecular switching in the solid state probed by 100 ps X-ray diffraction. This structural information is crucial for establishing the physical foundations of how to direct macroscopic photoswitching in materials. A key feature is that dynamics follow a complex pathway from molecular to material scales through a sequence of processes. Not only is the pathway indirect, the nature of the dynamical processes along the pathway depends on the timescale. This dictates which types of degrees of freedom are involved in the subsequent dynamics or kinetics and which are frozen or statistically averaged. We present a recent investigation of the structural dynamics in multifunctional spin-crossover materials, which are prototypes of molecular bistability in the solid state. The time-resolved X-ray diffraction results show that the dynamics span from subpicosecond molecular photoswitching followed by volume expansion (on a nanosecond timescale) and additional thermoswitching (on a microsecond timescale).

We are developing and exploring the imaging performance of, an in vivo, in-line holography, x-ray phase-contrast, micro-CT system with an ultrafast laser-based x-ray (ULX) source. By testing and refining our system, and by performing computer simulations, we plan to improve system performance in terms of contrast resolution and multi-energy imaging to a level beyond what can be obtained using a conventional microfocal x-ray tube. Initial CT projection sets at single energy (Mo K(alpha) and K(beta) lines) were acquired in the Fresnel regime and reconstructed for phantoms and a euthanized mouse. We also performed computer simulations of phase-contrast micro-CT scans for low-contrast, soft-tissue, tumor imaging. We determined that, in order to perform a phase-contrast, complete micro-CT scan using ULX, the following conditions must be met: (i) the x-ray source needs to be stable during the scan; (ii) the laser focal spot size needs to be less than 10 mum for source-to-object distance greater than 30 cm; (iii) the laser light intensity on the target needs to be in the range of 5 x 10(17) to 5 x 10(19) W/cm(2); (iv) the ablation protection system needs to allow uninterrupted scans; (v) the laser light focusing on the target needs to remain accurate during the entire scan; (vi) a fresh surface of the target must be exposed to consecutive laser shots during the entire scan; (vii) the effective detector element size must be less than 12 mum. Based on the results obtained in this research project, we anticipate that the new 10 Hz, 200 TW laser with 50 W average power that is being commissioned at ALLS will allow us practical implementation of in vivo x-ray phase-contrast micro-CT.

We have identified two polymorphs of the molecular complex [(TPA)Fe(III)(TCC)]PF6 [TPA = tris(2-pyridylmethyl)amine and TCC = 3,4,5,6-tetrachlorocatecholate dianion]: one is monoclinic and the other is orthorhombic. By lowering the temperature both undergo a thermal spin-crossover between a high-spin (S = 5/2) and a low-spin (S = 1/2) state, which we detected by magnetic, optical and X-ray diffraction measurements. The thermal crossover is only slightly shifted between the polymorphs. Their crystalline structures consist of similar cation layers alternating with PF6 anion layers, packed differently in the two polymorphs. The magnetic and optical properties of the polymorphs are presented.

International audience; We investigate the out-of-equilibrium switching dynamics of a molecular Fe(III) spin-crossover solid triggered by a femtosecond laser flash. The time-resolved x-ray diffraction and optical results show that the dynamics span from subpicosecond local photoswitching followed by volume expansion (nanosecond) and thermal switching (microsecond). We present a physical picture of the consecutive steps in the photoswitching of molecular materials.

International audience; We report here the first observation of the photoinduced insulating-to-metal phase transition in the (EDO-TTF)2SbF6 salt, which occurs on the picosecond time-scale. The time-resolved optical experiments performed with 80 fs time-resolution demonstrate that the dynamical process involves several low-frequency phonons, as the crystalline structure is destabilized upon laser excitation.

This paper presents different aspects of x-ray diffraction techniques for material science: investigation of symmetry breaking, electron density analysis, diffuse scattering, aperiodic systems and time-resolved experiments.

International audience; We report here on the photo-switching dynamics of a Fe(III) molecular material undergoing a spin-crossover. The thermal spin conversion is observed by magnetic and spectroscopic measurements, as well as imaging. The photoinducedswitching dynamics between the low-spin and the high-spinstates is studied with a femtosecond optical pump-probe technique. The results demonstrate that the switching occurs within a time-scale shorter than one picosecond.

Nickel nanowires present >90% absorption in an effective skin-depth ~1 mum, making efficient X-ray converters. We present new theoretical and experimental results for intensities from small-signal up to very clean relativistic pulses.

Nickel nanowires present >90% absorption in an absorption depth ~1 µm, making efficient x-ray converters at high energy-densities. We present new theoretical and experimental results for intensities from small-signal up to relativistic ultrafast pulses.

We have investigated theoretically the mean absorbed dose to the mouse in our newly constructed, in-line holography, x-ray phase-contrast, in-vivo, micro-CT system with an ultrafast laser-based x-ray (ULX) source. We assumed that the effective mouse diameter was 30 mm and the x-ray detector required minimum 30 μGy per frame to produce high quality images. The following laser target-filter combinations were considered: Ag-Ag, Mo-Mo, Sn- Sn. In addition, we considered narrow-pass multilayer x-ray mirrors. The corresponding ULX spectra were obtained using a CZT solid-state spectrometer. The approach used for dose computation was similar to human dose estimation. The mouse was modeled as a tissue-equivalent cylinder located at the isocenter with diameter 30 mm and density 1g/cm3. A layer of dermis (skin and fur) with 1 mm thickness was also modeled. Imparted energy per volume was estimated for 1 keV wide x-ray energy intervals in the 6-100 keV range. Monte Carlo simulations were performed using the SIERRA code previously validated using 30 mm diameter PMMA phantom. The results obtained indicate that: a) the mean absorbed dose for ULX is less than or equal to that from a W-anode micro-CT tube operating at 30-40 kVp with 0.5 or 1.0 mm Al; b) for filter thickness above 100 μm, Sn-Sn results in the highest dose, followed by Ag-Ag and Mo-Mo; c) the multilayer x-ray mirror with FWHM ≤ 10 keV produces significantly lower dose than metallic foil filters. We conclude that ULX can provide better dose utilization than a microfocal x-ray tube for in vivo microtomography applications.

We have investigated experimentally and theoretically the imaging performance of our newly constructed in-line holography x-ray phase-contrast imaging system with an ultrafast laser-based x-ray source. Projection images of nylon fibers with diameters in the 10-330 μm range were obtained using an ultrafast (100 Hz, 28 fs, 40 mJ) laser-based x-ray source with Mo and Ta targets and Be filter, and Gaussian spatial-intensity distribution (FWHMS = 5 μm). A cooled CCD camera (24 μm pitch) with a Gd 2 OS 2 screen coupled via 1:1 optical taper was used (FWHMD = 50 μm). We have investigated nylon-fiber image quality vs. imaging setup geometry and x-ray spectra. The following parameters were evaluated: contrast, signal-to-noise ratio (SNR), resolution, and sampling. In addition, we performed theoretical simulation of image formation for the same objects but within a wide range of geometrical parameters. The rigorous wave-optical formalism was used for modeling of the free-space propagation of x-rays from the object plane to the detector, and the "projection approximation" was used. We found reasonable agreement between predictions of our analytical model and the experiments. We conclude that: a) Optimum magnification maximizing contrast and SNR is almost independent of the source-to-detector ( R ) distance and depends strongly on the diameter of the fiber. b) The corresponding maximum values of the contrast and SNR are almost linear with respect to R; the optimum magnification decreases with fiber diameter. c) The minimum diameter of fiber defines the minimum source-to-object distance R 1 if R is fixed and the object is moved.

Recent progress in high intensity ultrafast laser systems provides the opportunity to produce laser plasma x-ray sources exhibiting broad spectrum and high average x-ray flux that are well adapted to x-ray absorption measurements. In this paper, the development of a laser based x-ray absorption near edge structure (XANES) beamline exhibiting high repetition rate by using the Advanced Laser Light Source (ALLS) facility 100 Hz laser system (100 mJ, 35 fs at 800 nm) is presented. This system is based on a broadband tantalum solid target soft x-ray source and a grazing incidence grating spectrometer in the 1-5 nm wavelength range. To demonstrate the high potential of this laser based XANES technique in condensed matter physics, material science, or biology, measurements realized with several samples are presented: VO2 vanadium L edge, Si3N4 nitrogen K edge, and BPDA/PPD polyimide carbon K edge. The characteristics of this laser based beamline are discussed in terms of brightness, signal to noise ratio, and compared to conventional synchrotron broadband x-ray sources which allow achieving similar measurements. Apart from the very compact size and the relative low cost, the main advantages of such a laser based soft x-ray source are the picosecond pulse duration and the perfect synchronization between this x-ray probe and a laser pulse excitation which open the way to the realization of time resolved x-ray absorption measurements with picosecond range time resolution to study the dynamics of ultrafast processes and phase transition.

The 2D projection phase-contrast imaging performance of the ultrafast laser-based x-ray (ULX) source has been investigated. The potential of such a novel x-ray source has been assessed by imaging a reference object (Contrast Detail Evaluation phantom) in the in-line holography geometry and by applying a simple 1D numerical model to the data analysis. The results indicate that the ULX is a promising technique for 2D projection phase-contrast imaging and for implementation of phase-contrast micro-Computed Tomography (μ-CT). This is because by using high contrast laser pulse ULX simultaneously provides a very small x-ray source size along with a high average x-ray flux. In addition, due to the ultrashort x-ray burst duration, ULX might allow practical implementation of ultrafast phase-contrast stroboscopy and time-of-flight based electronic scatter rejection. This technique is also of interest for time resolved radiography to follow shock waves and radiative fronts propagating in an opaque matter.

International audience; The spin-crossover compound [(TPA)Fe(TCC)]PF6 was experimentally investigated using time-resolved optical pump and supercontinuum probe technique. Changes of VIS optical density at thermal equilibrium of a crystal with different high-spin/low-spin fractions are compared to changes recorded picoseconds after femtosecond laser excitation. A white light snapshot of the high-spin state at 180 K is extracted from time-resolved spectra. Our results indicate that the temperature of the electronic state affects the absorption spectra of high- and low-spin states.

The ability of certain materials to change its ground state due to laser excitation has arisen a lot of opportunities for light-control of material properties. The field of photo-induced phase transitions counts a rich variety of chemical and physical processes triggered by light-matter interactions involved during the phase transition process. Recently it was reported that elastically driven cooperativity leads to the amplification of spin state in molecular crystals and prolonged the lifetime of the transient state with an ultra-short laser pulse. The cooperative response appears during the propagation of non-linear coherent strain waves, in other words shock waves, coupled with the order parameter field. Shock waves can be seen as a new challenging pathway to achieve a permanently switched state with appropriate excitations.First, we introduce time-resolved single-shot imaging combined with the laser shock focusing technique that makes it possible to generate, acoustically focus, and directly visualize under a microscope shock waves propagating and focusing along the sample surface. The spatial separation of the laser-influenced and strain-influenced regions makes it possible to disentangle the material changes produced solely by the shock waves. Second, we present experimental results involving the shock-focusing technique to materials undergoing phase transitions linked with a macroscopic change of their volume (spin-crossover systems, Mott insulators). Post-mortem analyses of the samples confirm permanent phase transition under specific experimental conditions. These innovative results open doors for a generic elastically driven cooperativity.; La capacité de certains matériaux à changer d'état fondamental sous excitation laser a ouvert un champ de recherche autour de la manipulation de leurs propriétés par la lumière. Les processus chimiques et physiques mis alors en jeu sont riches et complexes. Dans ce contexte, le rôle prédominant de la coopérativité élastique pour l’amplification et la stabilisation de la transition a été mis en évidence récemment dans un matériau à transitions de spin irradié par laser. Ces observations font apparaître la perspective de commuter de façon permanente certaines propriétés des matériaux par des ultrasons non-linéaires, des ondes de choc excitées par laser.Dans un premier temps, nous introduisons le dispositif expérimental d’imagerie mono-coup résolu en temps, associée à la technique de focalisation des ondes de chocs excitées par laser au niveau de la surface de l’échantillon. La séparation spatiale des régions irradiées par le laser et influencées par les ondes de choc propagatives permet de discerner clairement les changements du matériaux induits uniquement par les ondes de choc. Dans un second temps, nous présentons nos résultats expérimentaux en lien avec cette technique innovante, aux matériaux dont les changements de phases impliquent un changement de volume macroscopique (systèmes spin-crossover, isolants de Mott). Des analyses post-mortem des échantillons ont permis de confirmer, dans certaines conditions expérimentales, une modification permanente de la phase du matériau par action de l'onde de choc. Ces résultats ouvrent des perspectives pour la généralisation à de nombreux matériaux du phénomène de coopérativité élastique donnant lieu à des transition permanent

The ability of certain materials to change its ground state due to laser excitation has arisen a lot of opportunities for light-control of material properties. The field of photo-induced phase transitions counts a rich variety of chemical and physical processes triggered by light-matter interactions involved during the phase transition process. Recently it was reported that elastically driven cooperativity leads to the amplification of spin state in molecular crystals and prolonged the lifetime of the transient state with an ultra-short laser pulse. The cooperative response appears during the propagation of non-linear coherent strain waves, in other words shock waves, coupled with the order parameter field. Shock waves can be seen as a new challenging pathway to achieve a permanently switched state with appropriate excitations.First, we introduce time-resolved single-shot imaging combined with the laser shock focusing technique that makes it possible to generate, acoustically focus, and directly visualize under a microscope shock waves propagating and focusing along the sample surface. The spatial separation of the laser-influenced and strain-influenced regions makes it possible to disentangle the material changes produced solely by the shock waves. Second, we present experimental results involving the shock-focusing technique to materials undergoing phase transitions linked with a macroscopic change of their volume (spin-crossover systems, Mott insulators). Post-mortem analyses of the samples confirm permanent phase transition under specific experimental conditions. These innovative results open doors for a generic elastically driven cooperativity., La capacité de certains matériaux à changer d'état fondamental sous excitation laser a ouvert un champ de recherche autour de la manipulation de leurs propriétés par la lumière. Les processus chimiques et physiques mis alors en jeu sont riches et complexes. Dans ce contexte, le rôle prédominant de la coopérativité élastique pour l’amplification et la stabilisation de la transition a été mis en évidence récemment dans un matériau à transitions de spin irradié par laser. Ces observations font apparaître la perspective de commuter de façon permanente certaines propriétés des matériaux par des ultrasons non-linéaires, des ondes de choc excitées par laser.Dans un premier temps, nous introduisons le dispositif expérimental d’imagerie mono-coup résolu en temps, associée à la technique de focalisation des ondes de chocs excitées par laser au niveau de la surface de l’échantillon. La séparation spatiale des régions irradiées par le laser et influencées par les ondes de choc propagatives permet de discerner clairement les changements du matériaux induits uniquement par les ondes de choc. Dans un second temps, nous présentons nos résultats expérimentaux en lien avec cette technique innovante, aux matériaux dont les changements de phases impliquent un changement de volume macroscopique (systèmes spin-crossover, isolants de Mott). Des analyses post-mortem des échantillons ont permis de confirmer, dans certaines conditions expérimentales, une modification permanente de la phase du matériau par action de l'onde de choc. Ces résultats ouvrent des perspectives pour la généralisation à de nombreux matériaux du phénomène de coopérativité élastique donnant lieu à des transition permanent