arXiv subjects

T. Scopigno

Publications and source records attributed to T. Scopigno.

At least 19 recordsLinked to original sources

arXiv2019

Tracking the connection between disorder and energy landscape in glasses using geologically hyperaged amber

Fossil amber offers the unique opportunity of investigating an amorphous material which has been exploring its energy landscape for more than 110 Myears of natural aging. By applying different x-ray scattering methods to amber before and after annealing the sample to erase its thermal history, we identify a link between the potential energy landscape and the structural and vibrational properties of glasses. We find that hyperaging induces a depletion of the vibrational density of states in the THz region, also ruling the sound dispersion and attenuation properties of the corresponding acoustic waves. Critically, this is accompanied by a densification with structural implications different in nature from that caused by hydrostatic compression. Our results, rationalized within the framework of fluctuating elasticity theory, reveal how upon approaching the bottom of the potential energy landscape (9% decrease in the fictive temperature $T_f$) the elastic matrix becomes increasingly less disordered (6%) and longer-range correlated (22%).

cond-mat.dis-nn↗

arXiv2019

Coherent anti-Stokes Raman Spectroscopy of single and multi-layer graphene

We report stimulated Raman spectroscopy of the G phonon in both single and multi-layer graphene, through Coherent anti-Stokes Raman Scattering (CARS). The signal generated by the third order nonlinearity is dominated by a vibrationally non-resonant background (NVRB), which obscures the Raman lineshape. We demonstrate that the vibrationally resonant CARS peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the NVRB. We model the observed spectra, taking into account the electronically resonant nature of both CARS and NVRB. We show that CARS can be used for graphene imaging with vibrational sensitivity.

cond-mat.mes-hall↗

arXiv2018

Raman spectroscopy of graphene under ultrafast laser excitation

The equilibrium optical phonons of graphene are well characterized in terms of anharmonicity and electron-phonon interactions, however their non-equilibrium properties in the presence of hot charge carriers are still not fully explored. Here we study the Raman spectrum of graphene under ultrafast laser excitation with 3ps pulses, which trade off between impulsive stimulation and spectral resolution. We localize energy into hot carriers, generating non-equilibrium temperatures in the ~1700-3100K range, far exceeding that of the phonon bath, while simultaneously detecting the Raman response. The linewidth of both G and 2D peaks show an increase as function of the electronic temperature. We explain this as a result of the Dirac cones' broadening and electron-phonon scattering in the highly excited transient regime, important for the emerging field of graphene-based photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2015

Probing equilibrium glass flow up to exapoise viscosities

Glasses are out-of-equilibrium systems aging under the crystallization threat. During ordinary glass formation, the atomic diffusion slows down rendering its experimental investigation impractically long, to the extent that a timescale divergence is taken for granted by many. We circumvent here these limitations, taking advantage of a wide family of glasses rapidly obtained by physical vapor deposition directly into the solid state, endowed with different "ages" rivaling those reached by standard cooling and waiting for millennia. Isothermally probing the mechanical response of each of these glasses, we infer a correspondence with viscosity along the equilibrium line, up to exapoise values. We find a dependence of the elastic modulus on the glass age, which, traced back to temperature steepness index of the viscosity, tears down one of the cornerstones of several glass transition theories: the dynamical divergence. Critically, our results suggest that the conventional wisdom picture of a glass ceasing to flow at finite temperature could be wrong.

cond-mat.dis-nn↗

arXiv2015

Heat capacity of liquids: A hydrodynamic approach

We study autocorrelation functions of energy, heat and entropy densities obtained by molecular dynamics simulations of supercritical Ar and compare them with the predictions of the hydrodynamic theory. It is shown that the predicted by the hydrodynamic theory single-exponential shape of the entropy density autocorrelation functions is perfectly reproduced for small wave numbers by the molecular dynamics simulations and permits the calculation of the wavenumber-dependent specific heat at constant pressure. The estimated wavenumber-dependent specific heats at constant volume and pressure, $C_{v}(k)$ and $C_{p}(k)$, are shown to be in the long-wavelength limit in good agreement with the macroscopic experimental values of $C_{v}$ and $C_{p}$ for the studied thermodynamic points of supercritical Ar.

cond-mat.soft↗

arXiv2013

Acoustic-like dynamics of amorphous drugs in the THz regime

The high frequency dynamics of Indomethacin and Celecoxib glasses has been investigated by inelastic x-ray scattering, accessing a momentum-energy region still unexplored in amorphous pharmaceuticals. We find evidence of phonon-like acoustic dynamics, and determine the THz behavior of sound velocity and acoustic attenuation. Connections with ordinary sound propagation are discussed, along with the relation between fast and slow degrees of freedom as represented by non-ergodicity factor and kinetic fragility, respectively.

cond-mat.dis-nn↗

arXiv2012

Optimally shaped narrowband pulses for Femtosecond Stimulated Raman Spectroscopy in the range 330-750 nm

Spectral compression of femtosecond pulses by second harmonic generation in the presence of substantial group velocity dispersion provides a convenient source of narrowband Raman pump pulses for femtosecond stimulated Raman spectroscopy (FSRS). We discuss here a simple and efficient modification that dramatically increases the versatility of the second harmonic spectral compression technique. Adding a spectral filter following second harmonic generation produces narrowband pulses with a superior temporal profile. This simple modification i) increases the Raman gain for a given pulse energy, ii) improves the spectral resolution, iii) suppresses coherent oscillations associated with slowly dephasing vibrations, and iv) extends the useful tunable range to at least 330-750 nm.

physics.optics↗

arXiv2008

High frequency dynamics in liquid nickel: an IXS study

Owing to their large relatively thermal conductivity, peculiar, non-hydrodynamic features are expected to characterize the acoustic-like 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 non conductive fluids are observed. Implications for high frequency transport properties in metallic fluids are discussed.

cond-mat.dis-nn↗

arXiv2007

Vibrational excitations in systems with correlated disorder

We investigate a $d$-dimensional model ($d$ = 2,3) for sound waves in a disordered environment, in which the local fluctuations of the elastic modulus are spatially correlated with a certain correlation length. The model is solved analytically by means of a field-theoretical effective-medium theory (self-consistent Born approximation) and numerically on a square lattice. As in the uncorrelated case the theory predicts an enhancement of the density of states over Debye's $ω^{d-1}$ law (``boson peak'') as a result of disorder. This anomay becomes reinforced for increasing correlation length $ξ$. The theory predicts that $ξ$ times the width of the Brillouin line should be a universal function of $ξ$ times the wavenumber. Such a scaling is found in the 2d simulation data, so that they can be represented in a universal plot. In the low-wavenumber regime, where the lattice structure is irrelevant there is excellent agreement between the simulation at small disorder. At larger disorder the continuum theory deviates from the lattice simulation data. It is argued that this is due to an instability of the model with stronger disorder.

cond-mat.dis-nn↗

arXiv2007

Acoustic attenuation in glasses and its relation with the boson peak

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 ($Ω_k)$ and width ($Γ_k$), as well as the density of vibrational states ($g(ω)$), in disordered systems. As a result, we give a firm theoretical ground to the ubiquitous $k^2$ dependence of $Γ_k$ observed in glasses. Moreover, we derive a quantitative relation between the excess of the density of states (the boson peak) and $Γ_k$, 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.

cond-mat.mtrl-sci↗

arXiv2006

High Frequency dynamics in metallic glasses

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.

cond-mat.dis-nn↗

arXiv2005

Hard sphere-like dynamics in a non hard sphere liquid

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.

cond-mat.dis-nn↗

arXiv2004

Landscapes and Fragilities

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.

cond-mat.stat-mech↗

arXiv2004

Evidence of anomalous dispersion of the generalized sound velocity in glasses

The dynamic structure factor, S(Q,w), of vitreous silica, has been measured by inelastic X-ray scattering in the exchanged wavevector (Q) region Q=4-16.5 nm-1 and up to energies hw=115 meV in the Stokes side. The unprecedented statistical accuracy in such an extended energy range allows to accurately determine the longitudinal current spectra, and the energies of the vibrational excitations. The simultaneous observation of two excitations in the acoustic region, and the persistence of propagating sound waves up to Q values comparable with the (pseudo-)Brillouin zone edge, allow to observe a positive dispersion in the generalized sound velocity that, around Q=5 nm-1, varies from 6500 to 9000 m/s: this phenomenon was never experimentally observed in a glass.

cond-mat.dis-nn↗

arXiv2004

Collective dynamics in molten potassium: an Inelastic X-ray Scattering study

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 $1<Q<3$ nm$^{-1}$, which marks the departure from the isothermal value. We point out how this phenomenology is the consequence of a microscopic relaxation process that, in turn, can be traced back to the presence of ''instantaneous'' disorder, rather than to the crossover from a liquid to solid-like response.

cond-mat.dis-nn↗

arXiv2003

High frequency dynamics in a monatomic glass

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 $1.5<Q<12.5$ nm$^{-1}$, helping to clarify a previous contradiction between experimental and numerical results. The sound velocity shows a positive dispersion, exceeding the hydrodynamic value by $\approx$ 10% at $Q<3.5$ nm$^{-1}$. The $Q^2$ dependence of the sound attenuation $Γ(Q)$, reported for other glasses, is found to be the low-$Q$ limit of a more general $Γ(Q) \propto Ω(Q)^2$ law which applies also to the higher $Q$ region, where $Ω(Q)\propto Q$ no longer holds.

cond-mat.dis-nn↗

arXiv2003

A spectroscopic cell for fast pressure jumps across the glass transition line

We present a new experimental protocol for the spectroscopic study of the dynamics of glasses in the aging regime induced by sudden pressure jumps (crunches) across the glass transition line. The sample, initially in the liquid state, is suddenly brought in the glassy state, and therefore out of equilibrium, in a four-window optical crunch cell which is able to perform pressure jumps of 3 kbar in a time interval of ~10 ms. The main advantages of this setup with respect to previous pressure-jump systems is that the pressure jump is induced through a pressure transmitting fluid mechanically coupled to the sample stage through a deformable membrane, thus avoiding any flow of the sample itself in the pressure network and allowing to deal with highly viscous materials. The dynamics of the sample during the aging regime is investigated by Brillouin Light Scattering (BLS). For this purpose the crunch cell is used in conjunction with a high resolution double monochromator equipped with a CCD detector. This system is able to record a full spectrum of a typical glass forming material in a single 1 s shot. As an example we present the study of the evolution toward equilibrium of the infinite frequency longitudinal elastic modulus (M_infinity) of a low molecular weight polymer (Poly(bisphenol A-co-epichlorohydrin), glycidyl end capped). The observed time evolution of M_infinity, well represented by a single stretched exponential, is interpreted within the framework of the Tool-Narayanaswamy theory.

cond-mat.dis-nn↗

arXiv2002

High frequency acoustic modes in liquid gallium at the melting point

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.

cond-mat.dis-nn↗