We use x-ray photon correlation spectroscopy to investigate the structural relaxation process in a metallic glass on the atomic length scale. We report evidence for a dynamical crossover between the supercooled liquid phase and the metastable glassy state, suggesting different origins of the relaxation process across the transition. Furthermore, using different cooling rates, we observe a complex hierarchy of dynamic processes characterized by distinct aging regimes. Strong analogies with the aging dynamics of soft glassy materials, such as gels and concentrated colloidal suspensions, point at stress relaxation as a universal mechanism driving the relaxation dynamics of out-of-equilibrium systems.

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. Specifically, we find that the acoustic excitations with nanometric wavelengths show the clear signature of being strongly scattered, indicating the existence of a cross-over between well-defined acoustic modes for larger wavelengths and ill-defined ones for smaller wavelengths. This cross-over region is accompanied by a softening of the sound velocity that quantitatively accounts for the excess observed in the vibrational density of states of glasses over the Debye level at energies of a few milli-electronvolts. These findings thus highlight the acoustic contribution to the well-known universal low-temperature anomalies found in the specific heat of glasses.

The propagation and damping of the acoustic excitations in vitreous silica is measured at terahertz frequencies using inelastic x-ray scattering. The apparent sound velocity shows a marked dispersion with frequency while the sound attenuation undergoes a crossover from a fourth to a second power law frequency dependence. This finding solves a recent controversy concerning the location of this crossover in vitreous silica, clarifying that it occurs at the position of the glass-characteristic excess of vibrational modes known as boson peak, and thus establishing a direct connection between boson peak and acoustic dispersion curves.

It is largely accepted that liquids are characterized by a short-range order usually corresponding to that of the solid phase at the same density. It is less clear to what extent dynamic properties of liquids and crystals can be compared. In particular, high-frequency collective excitations reminiscent of phonons in solids exist as well in liquids. They are however traditionally discussed in terms of relaxation processes characteristic of the liquid phase. We report here on a quantitative comparison of the collective excitations in liquid and polycrystalline sodium. We show that liquid sodium exhibits acoustic excitations of both longitudinal and transverse polarization at frequencies strictly related to those of the corresponding crystal. The only relevant difference between the liquid and the polycrystal appears in the broadening of the excitations: An additional disorder-induced contribution comes into play in the case of the liquid, which we show to be related to the distribution of local structures around the average one. These results establish a direct connection between structural and dynamic properties of liquids, with short-range order and overall structural disorder leaving very specific fingerprints.

Engineering 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 Ba_7.81Ge_40.67Au_5.33, renowned for its puzzling ‘glass-like’ thermal conductivity. Surprisingly, thermal transport is dominated by acoustic phonons with long lifetimes, travelling over distances of 10 to 100 nm as their wave-vector goes from 0.3 to 0.1 Å⁻¹. Considering only low-energy acoustic phonons, and their observed lifetime, leads to a calculated thermal conductivity very close to the experimental one. Our results challenge the current picture of thermal transport in clathrates, underlining the inability of state-of-the-art simulations to reproduce the experimental data, thus representing a crucial experimental input for theoretical developments.

Perfectly crystalline solids are excellent heat conductors. Prominent counterexamples are intermetallic clathrates, guest-host systems with a high potential for thermoelectric applications due to their ultralow thermal conductivities. Our combined experimental and theoretical investigation of the lattice dynamics of a particularly simple binary representative, ${\mathrm{Ba}}_8{\mathrm{Si}}_{46}$, identifies the mechanism responsible for the reduction of lattice thermal conductivity intrinsic to the perfect crystal structure. Above a critical wave vector, the purely harmonic guest-host interaction leads to a drastic transfer of spectral weight to the guest atoms, corresponding to a localization of the propagative phonons.