Nanophononic materials are characterized by a periodic nanostructuration, which may lead to coherent scattering of phonons, enabling interference and resulting in modified phonon dispersions. We have used the extreme ultraviolet transient grating technique to measure phonon frequencies and lifetimes in a low-roughness nanoporous phononic membrane of SiN at wavelengths between 50 and 100 nm, comparable to the nanostructure lengthscale. Surprisingly, phonon frequencies are only slightly modified upon nanostructuration, while phonon lifetime is strongly reduced.
View Article and Find Full Text PDFHigh-Entropy Alloys (HEAs) are a new family of crystalline random alloys with four or more elements in a simple unit cell, at the forefront of materials research for their exceptional mechanical properties. Their strong chemical disorder leads to mass and force-constant fluctuations which are expected to strongly reduce phonon lifetime, responsible for thermal transport, similarly to glasses. Still, the long range order would associate HEAs to crystals with a complex disordered unit cell.
View Article and Find Full Text PDFNanophononic materials have recently arisen as a promising way for controlling heat transport, mirroring the results in macroscopic phononic materials for sound transmission, filtering and attenuation applications. Here we present a Finite Element numerical simulation of the transient propagation of an acoustic Wave-Packet in a 2D nanophononic material, which allows to identify the effect of the nanostructuration on the acoustic attenuation length and thus on the transport regime for the vibrational energy. Assuming elastic behavior in the matrix and in the inclusions, we find that the rigidity contrast between them not only tunes the apparent attenuation length of the wave packet along its main trajectory, but gives rise to different behaviours, from weak to strong scattering, and waves pinning.
View Article and Find Full Text PDFIn this work we present a molecular dynamics investigation of thermal transport in a silica-gallium nitride nanocomposite. A surprising enhancement of the thermal conductivity for crystalline volume fractions larger than 5% is found, which cannot be predicted by an effective medium approach, not even including percolation effects, the model systematically leading to an underestimation of the effective thermal conductivity. The behavior can instead be reproduced if an effective volume fraction twice larger than the real one is assumed, which translates into a percolation effect surprisingly stronger than the usual one.
View Article and Find Full Text PDFAs ultrastable metallic glasses (UMGs) are promising candidates to solve the stability issues of conventional metallic glasses, their study is of exceptional interest. By means of x-ray photon correlation spectroscopy, we have investigated the stability of UMGs at the atomic level. We find a clear signature of ultrastability at the atomic level that results in slower relaxation dynamics of UMGs with respect to conventional (rapidly quenched) metallic glasses, and in a peculiar acceleration of the dynamics by near T_{g} annealing.
View Article and Find Full Text PDFEngineering lattice thermal conductivity requires to control the heat carried by atomic vibration waves, the phonons. The key parameter for quantifying it is the phonon lifetime, limiting the travelling distance, whose determination is however at the limits of instrumental capabilities. Here, we show the achievement of a direct quantitative measurement of phonon lifetimes in a single crystal of the clathrate BaGeAu, renowned for its puzzling 'glass-like' thermal conductivity.
View Article and Find Full Text PDFWe report a study on charge-neutral crystal-field (dd) excitations in NiO as a function of applied pressure up to 55 GPa, using resonant inelastic x-ray scattering spectroscopy at the Ni K edge. We find distinct signatures of the pressure-induced modifications to the 3d orbital energies as a function of pressure. These modifications are experimentally evidenced by a subtle splitting of the dd-excitation resonance energies.
View Article and Find Full Text PDFWe present an extended investigation of phase I of carbon dioxide by x-ray diffraction and spectroscopic techniques at simultaneous high pressure and high temperature, up to 12 GPa and 800 K. Based on the present and literature data, we show that a Mie-Grüneisen-Debye model reproduces within experimental uncertainties the equation of state of CO(2) over the entire range of stability of phase I. Using infrared and Raman spectroscopy, we have determined the frequencies of the zone-center lattice modes as a function of pressure and temperature.
View Article and Find Full Text PDFWe report the oxygen K-edge spectra of ices Ih, VI, VII, and VIII measured with X-ray Raman scattering. The pre-edge and main-edge contributions increase strongly with density, even though the hydrogen bond arrangements are very similar in these phases. While the near-edge spectral features in water and ice have often been linked to hydrogen bonding, we show that the spectral changes in the phases studied here can be quantitatively related to structural changes in the second coordination shell.
View Article and Find Full Text PDFThe existence of "intermediate bonding states" in solid CO2, separating the low-pressure molecular phases from the high-pressure polymeric forms, has been the matter of a long-standing debate. Here we determine the structure of CO2-IV using x-ray diffraction of single crystals grown inside a diamond anvil cell at 11.7 GPa and 830 K.
View Article and Find Full Text PDFJ Synchrotron Radiat
November 2009
The current status of phonon-dispersion studies at high pressure using very high energy resolution inelastic X-ray scattering is discussed. A brief description of the instrumental apparatus is given, together with an illustration of the high-pressure facilities available at the IXS beamlines ID16 and ID28 of the ESRF. Some selected examples of recent studies on crystalline and liquid samples in a diamond anvil cell are then presented.
View Article and Find Full Text PDFWe report on an inelastic x-ray scattering investigation of the high frequency dynamics of liquid cesium at 493 K and 1 GPa, which corresponds to a density 23% higher than that at the room pressure melting point. The analysis of the spectra, performed within the framework of the memory function approach suggests the existence of two different relaxation processes, i.e.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
March 2009
On the macroscopic scale, the wavelengths of sound waves in glasses are large enough that the details of the disordered microscopic structure are usually irrelevant, and the medium can be considered as a continuum. On decreasing the wavelength this approximation must of course fail at one point. We show here that this takes place unexpectedly on the mesoscopic scale characteristic of the medium range order of glasses, where it still works well for the corresponding crystalline phases.
View Article and Find Full Text PDFWe present an extensive analysis of the proposed relationship [T. Scopigno et al., Science 302, 849 (2003)] between the fragility of glass-forming liquids and the nonergodicity factor as measured by inelastic x-ray scattering.
View Article and Find Full Text PDFWe report the observation of a roughening transition in carbon dioxide along the melting line of phase I, which we call reverse as faceting appears with increasing temperature. The characteristics of the transition are discussed in light of modern theories of roughening and the causes of its reverse behavior investigated. We propose that high temperature faceting is related to a pressure-induced increase of the surface stiffness.
View Article and Find Full Text PDFThe melting curve and fluid equation of state of carbon dioxide have been determined under high pressure in a resistively heated diamond anvil cell. The melting line was determined from room temperature up to 11.1+/-0.
View Article and Find Full Text PDFHigh-temperature IR absorption spectra of solid CO2 in phases II and IV were measured in a resistive heated diamond anvil cell up to 30 GPa. The spectral structures of the bending mode, observed in high quality thin crystalline samples, and of the IR lattice phonons, measured for the first time between 80 and 640 K, are discussed using group theory arguments. According to this analysis the claimed bent molecular geometry of CO2 in phase IV can be unambiguously ruled out.
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