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S. Ravy

Publications and source records attributed to S. Ravy.

At least 19 recordsLinked to original sources

Vibrational and mechanical properties of the highly mismatched (Cd,Be)Te semiconductor alloy : Experiment and ab initio calculations

The (Cd, Be)Te semiconductor alloy that exhibits a dramatic mismatch in bond covalency and stiffness clarifying its vibrational and mechanical properties is used as a benchmark to test the limits of the percolation model (PM) worked out to explain the complex Raman spectra of the related but less contrasted (Zn, Be) chalcogenides. The test is done by way of experiment (x smaller than 0.11) combining Raman scattering with X ray diffraction at high pressure and ab initio calculations (x around 0, 0.5 and 1). The (macroscopic) bulk modulus B drops below the CdTe value on minor Be incorporation, at variance with a linear B versus x increase predicted ab initio, thus hinting at large anharmonic effects in the real crystal. Yet, no anomaly occurs at the microscopic (bond) scale as the regular bimodal PM Raman signal predicted ab initio for the BeTe bond in minority (x around 0 and 0.5) is (barely) detected experimentally. Although at large Be content (x around 1) the same bimodal signal relaxes down to inversion, an unprecedented case, specific pressure dependencies of the regular (x around 0 and 0.5) and inverted (x around 1) BeTe Raman doublets are in line with PM predictions. Hence, the PM applies as such to (Cd, Be)Te albeit in a relaxed form, without further refinement. This enhances the scheme validity as a generic descriptor of phonons in alloys.

cond-mat.mtrl-sci

Domain size effects on the dynamics of a charge density wave in 1T-TaS2

Recent experiments have shown that the high temperature incommensurate (I) charge density wave (CDW) phase of 1T-TaS2 can be photoinduced from the lower temperature, nearly commensurate (NC) CDW state. Here we report a time-resolved x-ray diffraction study of the growth process of the photoinduced I-CDW domains. The layered nature of the material results in a marked anisotropy in the size of the photoinduced domains of the I-phase. These are found to grow self-similarly, their shape remaining unchanged throughout the growth process. The photoinduced dynamics of the newly formed I-CDW phase was probed at various stages of the growth process using a double pump scheme, where a first pump creates I-CDW domains and a second pump excites the newly formed I-CDW state. We observe larger magnitudes of the coherently excited I-CDW amplitude mode in smaller domains, which suggests that the incommensurate lattice distortion is less stable for smaller domain sizes.

cond-mat.str-el

Watching the birth of a charge density wave order: diffraction study on nanometer-and picosecond-scales

Femtosecond time-resolved X-ray diffraction is used to study a photo-induced phase transition between two charge density wave (CDW) states in 1T-TaS$_2$, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photo-induced I-CDW phase then develops through a nucleation/growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a non-conservative order parameter.

cond-mat.str-el

Ultrafast evolution and transient phases of the prototype out-of-equilibrium Mott-Hubbard material V2O3

The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. Here we present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V2O3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A1g coherent phonon. This configuration is in stark contrast with the thermally accessible ones - the A1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned.

cond-mat.str-el

Pressure-induced phonon freezing in the ZnSeS II-VI mixed crystal: phonon-polaritons and ab initio calculations

Near-forward Raman scattering combined with ab initio phonon and bond length calculations is used to study the phonon-polariton transverse optical modes (with mixed electrical and mechanical character) of the II-VI ZnSeS mixed crystal under pressure. The goal of the study is to determine the pressure dependence of the poorly resolved percolation-type Zn-S Raman doublet of the three oscillator [1(Zn-Se),2(Zn-S)] ZnSe68S32 mixed crystal, which exhibits a phase transition at approximately the same pressure as its two end compounds (~14 GPa, zincblende-to-rocksalt), as determined by high-pressure x-ray diffraction. We find that the intensity of the lower Zn-S sub-mode of ZnSe68S32, due to Zn-S bonds vibrating in their own (S-like) environment, decreases under pressure (Raman scattering), whereas its frequency progressively converges onto that of the upper Zn- S sub-mode, due to Zn-S vibrations in the foreign (Se-like) environment (ab initio calculations). Ultimately, only the latter sub-mode survives. A similar phonon freezing was earlier evidenced with the well-resolved percolation-type Be-Se doublet of ZnBeSe [Pradhan et al. Phys. Rev. B 81, 115207 (2010)], that exhibits a large contrast in the pressure-induced structural transitions of its end compounds. We deduce that the above collapse and convergence process is intrinsic to the percolation doublet of a short bond under pressure, at least in a ZnSe-based mixed crystal, and not due to any pressure-induced structural transition.

cond-mat.mtrl-sci

Charge and Spin Density Waves observed through their spatial fluctuations by coherent and simultaneous X-ray diffraction

Spatial uctuations of spin density wave (SDW) and charge density wave (CDW) in chromium have been compared by combining coherent and simultaneous X-ray diffraction experiments. Despite their close relationship, spatial fluctuations of the spin and of the charge density waves display a very different behavior: the satellite reflection associated to the charge density displays speckles while the spin one displays an impressive long-range order. This observation is hardly compatible with the commonly accepted magneto-elastic origin of CDW in chromium and is more consistent with a purely electronic scenario where CDW is the second harmonic of SDW. A BCS model taking into account a second order nesting predicts correctly the existence of a CDW and explains why the CDW is more sensitive to punctual defects.

cond-mat.str-el

Evolution of the electronic structure of a Mott system across its phase diagram: an X-ray absorption spectroscopy study of (V(1-x)Crx)2O3

V2O3 is an archetypal system for the study of correlation induced, Mott-Hubbard metal-insulator transitions. Despite decades of extensive investigations, the accurate description of its electronic properties remains an open problem in the physics of strongly correlated materials, also because of the lack of detailed experimental data on its electronic structure over the whole phase diagram. We present here a high resolution X-ray absorption spectroscopy study at the V K-edge of (V(1-x)Crx)2O3 to probe its electronic structure as a function of temperature, doping and pressure, providing an accurate picture of the electronic changes over the whole phase diagram. We also discuss the relevance of the parallel evolution of the lattice parameters, determined with X-ray diffraction. This allows us to draw two conclusions of general interest: first, the transition under pressure presents peculiar properties, related to a more continuous evolution of the lattice and electronic structure; second, the lattice mismatch is a good parameter describing the strength of the first order transition, and is consequently related to the tendency of the system towards the coexistence of different phases. Our results show that the evolution of the electronic structure while approaching a phase transition, and not only while crossing it, is also a key element to unveil the underlying physical mechanisms of Mott materials .

cond-mat.str-el

A Microscopic View on the Mott transition in Chromium-doped V2O3

V2O3 is the prototype system for the Mott transition, one of the most fundamental phenomena of electronic correlation. Temperature, doping or pressure induce a metal to insulator transition (MIT) between a paramagnetic metal (PM) and a paramagnetic insulator (PI). This or related MITs have a high technological potential, among others for intelligent windows and field effect transistors. However the spatial scale on which such transitions develop is not known in spite of their importance for research and applications. Here we unveil for the first time the MIT in Cr-doped V2O3 with submicron lateral resolution: with decreasing temperature, microscopic domains become metallic and coexist with an insulating background. This explains why the associated PM phase is actually a poor metal. The phase separation can be associated with a thermodynamic instability near the transition. This instability is reduced by pressure which drives a genuine Mott transition to an eventually homogeneous metallic state.

cond-mat.str-el

A coherent way to image dislocations

The use of coherent x-ray beams has been greatly developing for the past decades. They are now used by a wide scientific community to study biological materials, phase transitions in crystalline materials, soft matter, magnetism, strained structures, or nano-objects. Different kinds of measurements can be carried out: x-ray photon correlation spectroscopy allowing studying dynamics in soft and hard matter, and coherent diffraction imaging enabling to reconstruct the shape and strain of some objects by using methods such as holography or ptychography. In this article, we show that coherent x-ray diffraction (CXRD) brings a new insight in another scientific field: the detection of single phase defects in bulk materials. Extended phase objects such as dislocations embedded in the bulk are usually probed by electron microscopy or X-ray topography. However, electron microscopy is restricted to thin samples, and x-ray topography is resolution-limited. We show here that CXRD brings much more accurate information about dislocation lines (DLs) in bulk samples and opens a route for a better understanding of the fine structure of the core of bulk dislocations.

cond-mat.mtrl-sci

Spin density wave dislocation in chromium probed by coherent x-ray diffraction

We report on the study of a magnetic dislocation in pure chromium. Coherent x-ray diffraction profiles obtained on the incommensurate Spin Density Wave (SDW) reflection are consistent with the presence of a dislocation of the magnetic order, embedded at a few micrometers from the surface of the sample. Beyond the specific case of magnetic dislocations in chromium, this work may open up a new method for the study of magnetic defects embedded in the bulk.

cond-mat.str-el

Combining high pressure and coherent diffraction: a first feasibility test

We present a first experiment combining high pression and coherent X-ray diffraction. By using a dedicated diamond anvil cell, we show that the degree of coherence of the X-ray beam is preserved when the X-ray beam passes through the diamond cell. This observation opens the possibility of studying the dynamics of slow fluctuations under high pressure.

cond-mat.other

Coherent scattering from silicon mocrystal surface

Using coherent x-ray scattering, we evidenced atomic step roughness at the [111] vicinal surface of a silicon monocrystal of 0.05 degree miscut. Close to the (1/2 1/2 1/2) anti-Bragg position of the reciprocal space which is particularly sensitive to the [111] surface, the truncation rod exhibits a contrasted speckle pattern that merges into a single peak closer to the (111) Bragg peak of the bulk. The elongated shape of the speckles along the[111] direction confirms the monoatomic step sensibility of the technique. This experiment opens the way towards studies of step dynamics on crystalline surfaces.

cond-mat.mtrl-sci

Observation of correlations up to the micrometer scale in sliding charge-density waves

High-resolution coherent x-ray diffraction experiment has been performed on the charge density wave (CDW) system K$_{0.3}$MoO$_3$. The $2k_F$ satellite reflection associated with the CDW has been measured with respect to external dc currents. In the sliding regime, the $2k_F$ satellite reflection displays secondary satellites along the chain axis which corresponds to correlations up to the micrometer scale. This super long range order is 1500 times larger than the CDW period itself. This new type of electronic correlation seems inherent to the collective dynamics of electrons in charge density wave systems. Several scenarios are discussed.

cond-mat.str-el

The SrTiO$_3$ displacive transition revisited by Coherent X-ray Diffraction

We present a Coherent X-ray Diffraction study of the antiferrodistortive displacive transition of SrTiO$_3$, a prototypical example of a phase transition for which the critical fluctuations exhibit two length scales and two time scales. From the microbeam x-ray coherent diffraction patterns, we show that the broad (short-length scale) and the narrow (long-length scale) components can be spatially disentangled, due to 100 $\mu$m-scale spatial variations of the latter. Moreover, both components exhibit a speckle pattern, which is static on a $\sim$10 mn time-scale. This gives evidence that the narrow component corresponds to static ordered domains. We interpret the speckles in the broad component as due to a very slow dynamical process, corresponding to the well-known \emph{central} peak seen in inelastic neutron scattering.

cond-mat.mtrl-sci

Structural aspects of the metal-insulator transition in BaVS3

A sequence of structural transitions occurring in the quasi-one-dimensional (1D) 3d1 system BaVS3 at low temperature was investigated by high resolution synchrotron X-ray diffraction. The orthorhombic Cmc21 structure of the intermediate-temperature (70K<T<240K) phase was confirmed. A model for the low-T (T<70K) k=(1 0 1/2)O superstructure (with Im symmetry) is proposed and refined. The formation of the superstructure is associated with the stabilization of a mixed bond order / charge density wave.

cond-mat.str-el

X-Ray Study of the Density Wave Instability of alpha-(BEDT-TTF)2MHg(SCN)4 with M=K and Rb

We present an X-ray diffraction study of the quasi-2D conductors a-(BEDTTTF)2MHg(SCN), with M=K and Rb. They exhibit a phase transition of the density wave type at TDW=8-10K and 12-13K respectively, evidenced by magnetoresistivity, specific heat, NMR and Hall constant measurements. The structural study shows the presence of satellite reflections already at ambient temperature. The related modulation is incommensurate with multiple harmonics. For some of the compounds studied, the intensity of the satellite reflections strongly increases below TDW. According to Fermi surface (FS) calculations, the wave vector of the structural modulation achieves a quite good nesting of the global FS. This suggests a coupling of the modulation with the electronic degrees of freedom leading to a charge density wave ground state.

cond-mat.str-el

X-ray anomalous scattering investigations on the charge order in $\alpha^\prime$-NaV$_2$O$_5$

Anomalous x-ray diffraction studies show that the charge ordering in $\alpha^\prime$-NaV$_2$O$_5$ is of zig-zag type in all vanadium ladders. We have found that there are two models of the stacking of layers along \emph{c-}direction, each of them consisting of 2 degenerated patterns, and that the experimental data is well reproduced if the 2 patterns appears simultaneously. We believe that the low temperature structure contains stacking faults separating regions corresponding to the four possible patterns.

cond-mat.str-el

Friedel Oscillations and Charge-density Waves Pinning in Quasi-one-dimensional Conductors: An X-ray Access

We present an x-ray diffraction study of the Vanadium-doped blue bronze K0.3(Mo0.972V0.028)O3. At low temperature, we have observed both an intensity asymmetry of the +-2kF satellite reflections relative to the pure compound, and a profile asymmetry of each satellite reflections. We show that the profile asymmetry is due to Friedel oscillation around the V substituant and that the intensity asymmetry is related to the charge density wave (CDW) pinning. These two effects, intensity and profile asymmetries, gives for the first time access to the local properties of CDW in disordered systems, including the pinning and even the phase shift of FOs.

cond-mat