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Ultrafast reactions activated by light absorption are governed by multidimensional excited-state (ES) potential energy surfaces (PESs), which describe how the molecular potential varies with the nuclear coordinates. ES PESs ad-hoc displaced with respect to the ground state can drive subtle structural rearrangements, accompanying molecular biological activity and regulating physical/chemical properties. Such displacements are encoded in the Franck-Condon overlap integrals, which in turn determine the resonant Raman response. Conventional spectroscopic approaches only access their absolute value, and hence cannot determine the sense of ES displacements. Here, we introduce a two-color broadband impulsive Raman experimental scheme, to directly measure complex Raman excitation profiles along desired normal modes. The key to achieve this task is in the signal linear dependence on the Frank-Condon overlaps, brought about by non-degenerate resonant probe and off-resonant pump pulses, which ultimately enables time-domain sensitivity to the phase of the stimulated vibrational coherences. Our results provide the tool to determine the magnitude and the sensed direction of ES displacements, unambiguously relating them to the ground state eigenvectors reference frame.

Spontaneous Raman spectroscopy is a powerful characterization tool for graphene research. Its extension to the coherent regime, despite the large nonlinear third-order susceptibility of graphene, has so far proven challenging. Due to its gapless nature, several interfering electronic and phononic transitions concur to generate its optical response, preventing to retrieve spectral profiles analogous to those of spontaneous Raman. Here we report stimulated Raman spectroscopy of the G-phonon in single and multi-layer graphene, through coherent anti-Stokes Raman Scattering. The nonlinear signal is dominated by a vibrationally non-resonant background, obscuring the Raman lineshape. We demonstrate that the vibrationally resonant coherent anti-Stokes Raman Scattering peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the vibrationally non-resonant background. We model the spectra, taking into account the electronically resonant nature of both. We show how coherent anti-Stokes Raman Scattering can be used for graphene imaging with vibrational sensitivity., Coherent anti-Stokes Raman Scattering (CARS) accesses the vibrational properties of a material via nonlinear four-wave mixing (FWM); CARS in graphene has not been observed to date despite its high nonlinear third-order susceptibility. Here, the authors devised a FWM scheme to perform stimulated Raman spectroscopy in single and multi-layer graphene through CARS.

Monitoring the interactions between electronic and vibrational degrees of freedom in molecules is critical to our understanding of their structural dynamics. This is typically hampered by the lack of spectroscopic probes able to detect different energy scales with high temporal and frequency resolution. Coherent Raman spectroscopy can combine the capabilities of multidimensional spectroscopy with structural sensitivity at ultrafast timescales. Here, we develop a three-color-based 2D impulsive stimulated Raman technique that can selectively probe vibrational mode couplings between different active sites in molecules by taking advantage of resonance Raman enhancement. Three temporally delayed pulses generate nuclear wave packets whose evolution reports on the underlying potential energy surface, which we decipher using a diagrammatic approach enabling us to assign the origin of the spectroscopic signatures. We benchmark the method by revealing vibronic couplings in the ultrafast dynamics following photoexcitation of the green fluorescent protein.

Electronic properties and lattice vibrations are supposed to be strongly correlated in metal-halide perovskites, due to the "soft" fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultra-fast photoexcitation is necessary for understanding the optoelectronic behaviour of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal ground and excited state vibrational modes of methylammonium lead-bromide perovskite. We observe a coherent phonon at 106 cm-1 (13 meV), pertaining to the inorganic octahedral, which is peculiar of the electronic excited state and generated via displacive excitation mechanism. This indicates the formation of a new geometry, reached after a quarter of the phonon period T/4=80 fs, and fully equilibrated within the phonon lifetime of about 1 ps. Our observations unambiguously prove that this mode drives the crystalline distortion occurring upon carrier generation, implying the presence of polaronic effects., 8 pages, 2 figures

Author(s): Batignani, G; Pontecorvo, E; Bossini, D; Ferrante, C; Fumero, G; Cerullo, G; Mukamel, S; Scopigno, T | Abstract: Illuminating a magnetic material with femtosecond laser pulses induces complex ultrafast dynamical processes. The resulting optically detectable response usually contains contributions from both the optical properties and the magnetic degrees of freedom. Disentangling all the different components concurring to the generation of the total signal is a major challenge of contemporary experimental solid-state physics. Here, this problem is tackled, addressing the purely optical, nonmagnetic artifacts on the time resolved two-magnon stimulated Raman spectrum of an antiferromagnet, rationalizing the recent observation on the exchange energy modification upon photo-excitation. It is demonstrated how the genuine dynamics of the magnetic eigenmode can be disentangled from the nonlinear optical effects, generated by cross phase modulation, on the femtosecond timescale. The introduced approach can be extended for the investigation of l100nfs dynamic processes by means of coherent Ramannscattering.

© the Owner Societies 2015. We introduce a general theoretical description of non resonant impulsive femtosecond stimulated Raman spectroscopy in a multimode harmonic model. In this technique an ultrashort actinic pulse creates coherences of low frequency modes and is followed by a paired narrowband Raman pulse and a broadband probe pulse. Using closed-time-path-loop (CTPL) diagrams, the response on both the red and the blue sides of the broadband pulse with respect to the narrowband Raman pulse is calculated, the process couples high and low frequency modes, which share the same ground state. The transmitted intensity oscillates between the red and the blue side, while the total number of photons is conserved. The total energy of the probe signal is periodically modulated in time by the coherence created in the low frequency modes.

The experimental results relevant for the understanding of the microscopic dynamics in liquid metals are reviewed, with special regards to the ones achieved in the last two decades. Inelastic Neutron Scattering played a major role since the development of neutron facilities in the sixties. The last ten years, however, saw the development of third generation radiation sources, which opened the possibility of performing Inelastic Scattering with X rays, thus disclosing previously unaccessible energy-momentum regions. The purely coherent response of X rays, moreover, combined with the mixed coherent/incoherent response typical of neutron scattering, provides enormous potentialities to disentangle aspects related to the collectivity of motion from the single particle dynamics. If the last twenty years saw major experimental developments, on the theoretical side fresh ideas came up to the side of the most traditional and established theories. Beside the raw experimental results, therefore, we review models and theoretical approaches for the description of microscopic dynamics over different length-scales, from the hydrodynamic region down to the single particle regime, walking the perilous and sometimes uncharted path of the generalized hydrodynamics extension. Approaches peculiar of conductive systems, based on the ionic plasma theory, are also considered, as well as kinetic and mode coupling theory applied to hard sphere systems, which turn out to mimic with remarkable detail the atomic dynamics of liquid metals. Finally, cutting edges issues and open problems, such as the ultimate origin of the anomalous acoustic dispersion or the relevance of transport properties of a conductive systems in ruling the ionic dynamic structure factor are discussed., 53 pages, 41 figures, to appear in "The Review of Modern Physics". Tentatively scheduled for July issue

Acoustics dynamics of the molecular glass-former indomethacin (IMC) have been investigated by Brillouin light scattering (BLS) at GHz frequencies. Elastic response of the system has been tracked from the melting temperature down to the glass transition through the supercooled liquid. Both the structural arrest and the vibrational dynamics are described by modeling the experimentally determined dynamic structure factor within the framework of the Langevin equation, through a simplified choice of memory function which allows one to determine sound velocity and the acoustic attenuation coefficient as a function of temperature. The density fluctuation spectra in the glassy phase, as probed by BLS, are compared with time-domain results from photoacoustics experiments. The arising scenario is discussed in the context of current literature reporting inelastic X-ray scattering and BLS in platelet geometry. The link between the probed elastic properties and the non-ergodicity factor of the glass phase is finally scrutinized.

New inelastic X-ray scattering experiments have been performed on liquid lithium in a wide wavevector range. With respect to the previous measurements, the instrumental resolution, improved up to 1.5 meV, allows to accurately investigate the dynamical processes determining the observed shape of the the dynamic structure factor, $S(Q,\omega)$. A detailed analysis of the lineshapes shows the co-existence of relaxation processes with both a slow and a fast characteristic timescales, and therefore that pictures of the relaxation mechanisms based on a simple viscoelastic model must be abandoned., Comment: 5 pages, 4 .PS figures

The sound attenuation in the THz region is studied down to T 16 K in glassy glycerol by inelastic x-ray scattering. At striking variance with the decrease found below 100 K in the GHz data, the attenuation in the THz range does not show any T dependence. This result (i) indicates the presence of two different attenuation mechanisms, active, respectively, in the high- and low-frequency limits, (ii) demonstrates the nondynamic origin of the attenuation of THz sound waves, and confirms a similar conclusion obtained in SiO2 glass by molecular dynamics, and (iii) supports the low-frequency attenuation mechanism proposed by Fabian and Allen [ Phys. Rev. Lett. 82, 1478 (1999)].

We present new inelastic X-ray scattering data for the dynamic structure factor S(Q, ω) of liquid lithium collected at two different temperatures (T = 475K and T = 600K) and in a wide range of exchanged wave-vectors (Q = 1 nm−1 to Q=110nm−1). The analysed Q range covers the transition from collective to single-particle regimes. The spectra have been put on an absolute scale using its first sum rules, and the result obtained has been tested on diffraction data and novel molecular dynamie results. A relaxation fingerprint is observed at low wave-vectors (the so-called positive dispersion of the apparent sound speed), while at higher Q the single particle behaviour gradually emerges.

Exact relation for contributions to heat capacity of liquids is obtained from hydrodynamic theory. It is shown from analysis of the long-wavelength limit of heat density autocorrelation functions that the heat capacity of simple liquids is represented as a sum of two contributions due to “phonon-like” collective excitations and heat relaxation. The ratio of both contributions being the analogy of Landau-Placzek ratio for heat processes depends on the specific heats ratio. The theory of heat density autocorrelation functions in liquids is verified by computer simulations. Molecular dynamics simulations for six liquids having the ratio of specific heats γ in the range 1.1–2.3, were used for evaluation of the heat density autocorrelation functions and predicted Landau-Placzek ratio for heat processes. The dependence of contributions from collective excitations and heat relaxation process to specific heat on γ is shown to be in excellent agreement with the theory.

The lack of long-range structural order in amorphous solids induces well known thermodynamic anomalies, which are the manifestation of distinct peculiarities in the vibrational spectrum. Although the impact of such anomalies vanishes in the long wavelength, elastic continuum limit, it dominates at length scales comparable to interatomic distances, implying an intermediate transition regime still poorly understood. Here we report a study of such mesoscopic domains by means of a broadband version of picosecond photo-acoustics, developed to coherently generate and detect hypersonic sound waves in the sub-THz region with unprecedented sampling efficiency. We identify a temperature-dependent fractal v3/2 frequency behaviour of the sound attenuation, pointing to the presence of marginally stable regions and a transition between the two above mentioned limits. The essential features of this behaviour are captured by a theoretical approach based on random spatial variation of the shear modulus, including anharmonic interactions., Characterizing the acoustic dynamics of glasses at mesoscopic wavelengths is challenging. Here, Ferrante et al. use the broadband picosecond acoustics technique to study attenuation at such length scales, where they find temperature-dependent, fractal frequency behaviour.

Density-driven phase transformations are a known phenomenon in liquids. Pressure-driven transitions from an open low-density to a higher-density close-packed structure were observed for a number of systems. Here, we show a less intuitive, inverse behavior. We investigated the electronic, atomic, and dynamic structures of liquid Rb along an isothermal line at 573 K, at 1.2-27.4 GPa, by means of ab initio molecular dynamics simulations and inelastic x-ray scattering experiments. The excellent agreement of the simulations with experimental data performed up to 6.6 GPa validates the overall approach. Above 12.5 GPa, the breakdown of the nearly-free-electron model drives a transition of the pure liquid metal towards a less metallic, denser liquid, whose first coordination shell is less compact. Our study unveils the interplay between electronic, structural, and dynamic degrees of freedom along this liquid-liquid phase transition. In view of its electronic nature, we believe that this behavior is general for the first group elements, thus shedding new light into the high-pressure properties of alkali metals.

Molecular dynamics (MD) simulations of the glass-former 2Ca(NO(3))(2·3KNO(3), CKN, were performed as a function of temperature at pressures 0.1 MPa, 0.5 GPa, 1.0 GPa, and 2.0 GPa. Diffusion coefficient, relaxation time of the intermediate scattering function, and anion reorientational time were obtained as a function of temperature and densitiy ρ. These dynamical properties of CKN scale as ρ(γ)∕T with a common value γ = 1.8 ± 0.1. The scaling parameter γ is consistent with the exponent of the repulsive part of an effective intermolecular potential for the repulsion between the atoms at shortest distance in the equilibrium structure of liquid CKN, Ca(2+), and oxygen atoms of NO(3)(-). Correlation between potential energy and virial is obeyed for the short-range terms of the potential function, but not for the whole potential including coulombic interactions. Decoupling of diffusion coefficient and reorientational relaxation time from relaxation time take place at a given ρ(γ)∕T value, i.e., breakdown of Stokes-Einstein and Debye-Stokes-Einstein equations result from combined thermal and volume effects. The MD results agree with correlations proposed between long-time relaxation and short-time dynamics, lnτ ∝ 1∕u(2), where the mean square displacementu(2)concerns a time window of 10.0 ps. It has been found thatu(2)scales as ρ(γ)∕T above and below the glass transition temperature, so that thermodynamic scaling of liquid dynamics can be thought as a consequence of theories relating short- and long-time dynamics, and the more fundamental scaling concerns short-time dynamical properties.

International audience; Liquid and amorphous metals are an outstanding example of systems combining great relevance in both industrial applications and basic science. They find broad technological application, ranging from the production of industrial coatings (walls of refinery cokers, drill pipes for oil drilling) to medical equipment (reconstructive devices, surgical blades) or high-performance sporting goods. Most metallic materials, indeed, need to be refined in the molten state before being manufactured. Liquid metals, in particular the monoatomic ones, have long been recognized as the prototype of simple liquids, in the sense that they encompass most of the physical properties of real fluids without the complications which may be present in a particular system. Until the sixties the understanding of the physical properties of liquid metals proceeded rather slowly. It was John Ziman, indeed, who first developed a theory for the electron transport in liquid metals in 1961, and subsequently several experimental and theoretical studies were presented at the first Liquid Metals International Conference held in Brookhaven in 1966 (see, for example, refs. [1-3]). From the experimental point of view, the 1950s saw major efforts related to the development of neutron scattering facilities, which constitute a unique probe in accessing the microscopic structure and dynamics in condensed matter and, in particular, in the liquid and amorphous state. A further experimental breakthrough, however, has happened in the last twenty years when X-rays generated by synchrotron radiation facilities could be used as a probe for structure and dynamics in frequency and wavelength regions similar to those explored by neutrons. Concerning the nature of the dynamical structure in liquid and amorphous metals, in the last two decades many theoretical and experimental groups have switched their studies to researching effects due to non-hydrodynamic processes in liquids, i.e. collective processes which cannot be predicted by ordinary hydrodynamics. Examples of such non-hydrodynamic propagating excitations are shear waves, the famous "fast sound" [4] in binary liquids with disparate masses, or charge waves in ionic melts [5], while the most obvious non-hydrodynamic relaxation process is structural

In contrast to crystalline solids in which structural order governs dynamics and thermodynamics, the lack of long-range periodicity in amorphous materials is responsible for several anomalies. Although the relation between these anomalies and the 'bulk structure' is generally understood, the surface structure and the corresponding vibrational spectrum of amorphous solids is practically an unexplored theme. In this study, we resolve the differences in vibrational dynamics and atomic structure between bulk and surface (top 5 nm) atoms of amorphous selenium. We combine experimental (grazing incidence inelastic X-ray scattering) and computational (ab initio and semiempirical molecular orbital theoretical calculations) methods to scrutinize a variety of possible structural models. We find that a high concentration of particular types of 'coordination defects' in the surface layer is responsible for the observed differences. Resolving the structure of amorphous surfaces is, for example, important for understanding nanoparticles' properties where the surface-to-bulk ratio has a crucial role.

According to textbook definitions1, there exists no physical observable able to distinguish a liquid from a gas beyond the critical point, and hence only a single fluid phase is defined. There are, however, some thermophysical quantities, having maxima that define a line emanating from the critical point, named 'the Widom line'2 in the case of the constant-pressure specific heat. We determined the velocity of nanometric acoustic waves in supercritical fluid argon at high pressures by inelastic X-ray scattering and molecular dynamics simulations. Our study reveals a sharp transition on crossing the Widom line demonstrating how the supercritical region is actually divided into two regions that, although not connected by a first-order singularity, can be identified by different dynamical regimes: gas-like and liquid-like, reminiscent of the subcritical domains. These findings will pave the way to a deeper understanding of hot dense fluids, which are of paramount importance in fundamental and applied sciences.

The approach of generalized collective modes is applied to the study of dispersion curves of collective excitations along isothermal lines of supercritical pure Lennard-Jones fluid. An effect of structural relaxation and other nonhydrodynamic relaxation processes on the dispersion law is discussed. A simple analytical expression for the dispersion law in the long-wavelength region of acoustic excitations is obtained within a three-variable viscoelastic model of generalized hydrodynamics. It is shown that the deviation from the linear dependence in the long-wavelength region can be either "positive" or "negative" depending on the ratio between the high-frequency (elastic) and isothermal speed of sound. An effect of thermal fluctuations on positive and negative dispersion is estimated from the analytical solution of a five-variable thermoviscoelastic model that generalizes the results of the viscoelastic treatment. Numerical results are reported for a Lennard-Jones supercritical fluid along two isothermal lines T(*)=1.71,4.78 with different densities and discussed along the theoretical expressions derived.

Molecular dynamics simulations of the glass-forming liquid 2Ca(NO3)2.3KNO3 (CKN) were performed from high temperature liquid states down to low temperature glassy states at six different pressures from 10(-4) to 5.0 GPa. The temperature dependence of the structural relaxation time indicates that the fragility of liquid CKN changes with pressure. In line with recent proposal [Scopigno et al., Science 302, 849 (2003)], the change on liquid fragility is followed by a proportional change of the nonergodicity factor of the corresponding glass at low temperature.

Owing to their large relatively thermal conductivity, peculiar, nonhydrodynamic features are expected to characterize the acousticlike excitations observed in liquid metals. We report here an experimental study of collective modes in molten nickel, a case of exceptional geophysical interest for its relevance in earth interior science. Our result shed light on previously reported contrasting evidences: In the explored energy-momentum region, no deviation from the generalized hydrodynamic picture describing nonconductive fluids is observed. Implications for high frequency transport properties in metallic fluids are discussed. (C) 2008 American Institute of Physics.

Developing a novel experimental technique, we applied photon correlation spectroscopy using infrared radiation in liquid sulfur around ${T}_{\ensuremath{\lambda}}$, i.e., in the temperature range where an abrupt increase in viscosity by 4 orders of magnitude is observed upon heating within few degrees. This allowed us---overcoming photoinduced and absorption effects at visible wavelengths---to reveal a chain relaxation process with characteristic time in the millisecond range. These results do rehabilitate the validity of the Maxwell relation in sulfur from an apparent failure, allowing rationalizing of the mechanical and thermodynamic behavior of this system within a viscoelastic scenario.

A theory for the vibrational dynamics in disordered solids [W. Schirmacher, Europhys. Lett. {\bf 73}, 892 (2006)], based on the random spatial variation of the shear modulus, has been applied to determine the wavevector ($k$) dependence of the Brillouin peak position ($\Omega_k)$ and width ($\Gamma_k$), as well as the density of vibrational states ($g(\omega)$), in disordered systems. As a result, we give a firm theoretical ground to the ubiquitous $k^2$ dependence of $\Gamma_k$ observed in glasses. Moreover, we derive a quantitative relation between the excess of the density of states (the boson peak) and $\Gamma_k$, two quantities that were not considered related before. The successful comparison of this relation with the outcome of experiments and numerical simulations gives further support to the theory., Comment: To appear on PRL

A Comment on the Letter by B. Ruffl\'e et al., Phys. Rev. Lett. 96, 045502 (2006). The authors of the Letter offer a Reply.

Unlike phonons in crystals, the collective excitations in liquids cannot be treated as propagation of harmonic displacements of atoms around stable local energy minima. The viscoelasticity of liquids, reflected in transition from the adiabatic to elastic high-frequency speed of sound and in absence of the long-wavelength transverse excitations, results in dispersions of longitudinal (L) and transverse (T) collective excitations essentially different from the typical phonon ones. Practically, nothing is known about the effect of high pressure on the dispersion of collective excitations in liquids, which causes strong changes in liquid structure. Here dispersions of L and T collective excitations in liquid Li in the range of pressures up to 186 GPa were studied by ab initio simulations. Two methodologies for dispersion calculations were used: direct estimation from the peak positions of the L/T current spectral functions and simulation-based calculations of wavenumber-dependent collective eigenmodes. It is found that at ambient pressure, the longitudinal and transverse dynamics are well separated, while at high pressures, the transverse current spectral functions, density of vibrational states, and dispersions of collective excitations yield evidence of two types of propagating modes that contribute strongly to transverse dynamics. Emergence of the unusually high-frequency transverse modes gives evidence of the breakdown of a regular viscoelastic theory of transverse dynamics, which is based on coupling of a single transverse propagating mode with shear relaxation. The explanation of the observed high-frequency shift above the viscoelastic value is given by the presence of another branch of collective excitations. With the pressure increasing, coupling between the two types of collective excitations is rationalized within a proposed extended viscoelastic model of transverse dynamics.

The high frequency dynamics of fluid oxygen have been investigated by Inelastic X-ray Scattering. In spite of the markedly supercritical conditions ($T\approx 2 T_c$, $P>10^2 P_c$), the sound velocity exceeds the hydrodynamic value of about 20%, a feature which is the fingerprint of liquid-like dynamics. The comparison of the present results with literature data obtained in several fluids allow us to identify the extrapolation of the liquid vapor-coexistence line in the ($P/P_c$, $T/T_c$) plane as the relevant edge between liquid- and gas-like dynamics. More interestingly, this extrapolation is very close to the non metal-metal transition in hot dense fluids, at pressure and temperature values as obtained by shock wave experiments. This result points to the existence of a connection between structural modifications and transport properties in dense fluids., 4 pages, 3 figures, accepted by Phys. Rev. Lett

Using Inelastic X-ray Scattering we studied the collective dynamics of the glassy alloy Ni$_{33}$Zr$_{67}$ in the first pseudo Brillouin zone, an energy-momentum region still unexplored in metallic glasses. We determine key properties such as the momentum transfer dependence of the sound velocity and of the acoustic damping, discussing the results in the general context of recently proposed pictures for acoustic dynamics in glasses. Specifically, we demonstrate the existence in this strong glass of well defined (in the Ioffe Regel sense) acoustic-like excitations well above the Boson Peak energy., 4 pages, 4 .eps figures, accepted in Phys. Rev. Lett

The collective dynamics of liquid Gallium close to the melting point has been studied using Inelastic X-ray Scattering to probe lengthscales smaller than the size of the first coordination shell. %(momentum transfers, $Q$, $>$15 nm$^{-1}$). Although the structural properties of this partially covalent liquid strongly deviate from a simple hard-sphere model, the dynamics, as reflected in the quasi-elastic scattering, are beautifully described within the framework of the extended heat mode approximation of Enskog's kinetic theory, analytically derived for a hard spheres system. The present work demonstrates the applicability of Enskog's theory to non hard- sphere and non simple liquids., 5 pages, 2 figures, accepted in Phys. Rev. Lett

The concept of fragility provides a possibility to rank different supercooled liquids on the basis of the temperature dependence of dynamic and/or thermodynamic quantities. We recall here the definitions of kinetic and thermodynamic fragility proposed in the last years and discuss their interrelations. At the same time we analyze some recently introduced models for the statistical properties of the potential energy landscape. Building on the Adam-Gibbs relation, which connects structural relaxation times to configurational entropy, we analyze the relation between statistical properties of the landscape and fragility. We call attention to the fact that the knowledge of number, energy depth and shape of the basins of the potential energy landscape may not be sufficient for predicting fragility. Finally, we discuss two different possibilities for generating strong behavior., 17 pages, 10 figures; accepted version, minor corrections

The high frequency collective dynamics of molten potassium has been investigated by inelastic x-ray scattering, disclosing an energy/momentum transfer region unreachable by previous neutron scattering experiments (INS). We find that a two-step relaxation scenario, similar to that found in other liquid metals, applies to liquid potassium. In particular, we show how the sound velocity determined by INS experiments, exceeding the hydrodynamic value by $\approx 30 %$, is the higher limit of a speed up, located in the momentum region $1, Comment: 7 pages, 5 .eps figures. To appear in J. Chem. Phys

The high frequency dynamics of glassy Selenium has been studied by Inelastic X-ray Scattering at beamline BL35XU (SPring-8). The high quality of the data allows one to pinpoint the existence of a dispersing acoustic mode for wavevectors ($Q$) of $1.5, Comment: Phys. Rev. Lett. (Accepted)

Inelastic X-ray Scattering measurements of the dynamics structure factor have bene performed on vitreous Beryllium Fluoride ({\it v-}BeF$_2$) at $T$=297 K in the momentum transfer, $Q$, range $Q$=1.5$\div$10 nm$^{-1}$. We find evidence of well defined high frequency acoustic modes. The energy position and linewidth of the excitations disperse with $Q$ as $\propto Q$ and $\propto Q^2$, respectively up to about one half of the first maximum of the static structure factor. Their magnitude compare favorably with low-frequency sound velocity and absorption data. The results indicate worth mentioning similarities of the high frequency collective dynamics of different network forming glasses such as {\it v-}B$_2$O$_3$ and {\it v-}SiO$_2$., Comment: 17 pages, 5 .ps figs

The microscopic dynamics in liquid gallium (l-Ga) at melting (T=315 K) has been studied by inelastic x-ray scattering. We demonstrate the existence of collective acoustic-like modes up to wave-vectors above one half of the first maximum of the static structure factor, at variance with earlier results from inelastic neutron scattering data [F.J. Bermejo et al. Phys. Rev. E 49, 3133 (1994)]. Despite the structural (an extremely rich polymorphism and rather complex phase diagram) and electronic (mixed valence) peculiarity of l-Ga, its collective dynamics is strikingly similar to the one of Van der Walls and alkali metals liquids. This result speaks in favor of the universality of the short time dynamics in monatomic liquids rather than of system-specific dynamics., LaTex format, 11 pages, 4 EncapsulatedPostScript figures

The dynamical structure factor (S(Q,E)) of vitreous silica has been measured by Inelastic X-ray Scattering varying the exchanged wavevector (Q) at fixed exchanged energy (E) - an experimental procedure that, contrary to the usual one at constant Q, provides spectra with much better identified inelastic features. This allows the first direct evidence of Brillouin peaks in the S(Q,E) of SiO_2 at energies above the Boson Peak (BP) energy, a finding that excludes the possibility that the BP marks the transition from propagating to localised dynamics in glasses., 4 pages, 3 Postscript figures. To appear in Physical Review Letters

The dynamic structure factor, S(Q,E), of liquid lithium (T=475 K) has been determined by inelastic x-ray scattering (IXS) in the momentum transfer region (Q = 1.4-110 nm-1). These data allow to observe how, in a simple liquid, a phonon-like collective mode evolves towards the single particle dynamics. As a function of Q, one finds: i) at low Q's, a sound mode with a positive dispersion of the sound velocity, ii) at intermediate Q's, excitations whose energy oscillates similarly to phonons in the crystal Brillouin zones, and iii) at high Q's, the S(Q,E) approaches a Gaussian shape, indicating that the single particle dynamics has been reached., Comment: 3 pages and 5 figures

A relaxation process, with the associated phenomenology of sound attenuation and sound velocity dispersion, is found in a simulated harmonic Lennard-Jones glass. We propose to identify this process with the so called microscopic (or instantaneous) relaxation process observed in real glasses and supercooled liquids. A model based on the memory function approach accounts for the observation, and allows to relate to each others: 1) the characteristic time and strength of this process, 2) the low frequency limit of the dynamic structure factor of the glass, and 3) the high frequency sound attenuation coefficient, with its observed quadratic dependence on the momentum transfer., 11 pages, 3 figures

Coherent inelastic neutron and light (Raman and Brillouin) scattering measurements are repbrted on silica xerogels over a wide range of densities and temperatures. Raman scattering results show the presence of a boson peak at temperatures where the quasielastic contribution is negligible. The boson peak of xerogels is at a frequency around 35cm−1 and has a shape similar to that of melted silica. At lower frequencies (7–16cm−1) another bump is visible in the Raman scattering, believed to be connected to the presence of the pores and its frequency connected to their mean sizes. This important result seems to indicate that the disorder introduced by the presence of the pores does not influence very much the density of states in the frequency range of the boson peak. A comparison is made between the Q dependence of the elastic and inelastic structure factors as a function of sample density and temperature. The absence of a peak in the inelastic structure factor for the Q value corresponding to the fi...

New temperature dependent inelastic x-ray (IXS) and Raman (RS) scattering data are compared to each other and with existing inelastic neutron scattering data in vitreous silica (v-SiO_2), in the 300 - 1775 K region. The IXS data show collective propagating excitations up to Q=3.5 nm^-1. The temperature behaviour of the excitations at Q=1.6 nm^-1 matches that of the boson peak found in INS and RS. This supports the acoustic origin of the excess of vibrational states giving rise to the boson peak in this glass., 10 pages and 4 figures

The collective dynamics of a simple metal (lithium) have been numerically investigated by molecular dynamics and normal mode analysis. A generalized hydrodynamic framework allowed us to describe the system in different thermodynamic phases by the same model based on two relaxation processes. At the melting point we find good agreement with recent inelastic X-ray scattering results, while below the melting point, and ultimately in the glassy state, we find evidences of a “harmonie” relaxation as recently found in Lennard-Jones systems.

We propose an explanation for the quadratic dependence on the momentum $Q$, of the broadening of the acoustic excitation peak recently found in the study of the dynamic structure factor of many real and simulated glasses. We ascribe the observed $Q^2$ law to the spatial fluctuations of the local wavelength of the collective vibrational modes, in turn produced by the dishomegeneity of the inter-particle elastic constants. This explanation is analitically shown to hold for 1-dimensional disordered chains and satisfatorily numerically tested in both 1 and 3 dimensions.