Enhancement and anticipation of the Ioffe-Regel crossover in amorphous/nanocrystalline composites.

Nanocomposites made of crystalline nanoinclusions embedded in an amorphous matrix are at the forefront of current research for energy harvesting applications. However, the microscopic mechanisms leading alternatively to an effectively reduced or enhanced thermal transport still escape understanding. In this work, we present a molecular dynamics simulation study of model systems, where for the first time we combine a microscopic investigation of phonon dynamics with the macroscopic thermal conductivity calculation, to shed light on thermal transport in these materials. We clearly show that crystalline nanoinclusions represent a novel scattering source for vibrational waves, modifying the nature of low energy vibrations and significantly anticipating the propagative-to-diffusive crossover (Ioffe-Regel), usually located at energies of few THz in amorphous materials. Moreover, this crossover position can be tuned by changing the elastic contrast between nanoinclusions and the matrix, and anticipated by a factor as large as 10 for a harder inclusion. While the propagative contribution to thermal transport is drastically reduced, the calculated thermal conductivity is not significantly affected in the chosen system, as the diffusive contribution dominates heat transport when all phonons are thermally populated. These findings allow finally to understand the panoply of contradictory results reported on thermal transport in nanocomposites and give clear indications to the characteristics that the parent phases should have for efficiently reducing heat transport in a nanocomposite.

Influence of the electron-phonon interfacial conductance on the thermal transport at metal/dielectric interfaces.

Thermal boundary conductance at a metal-dielectric interface is a quantity of prime importance for heat management at the nanoscale. While the boundary conductance is usually ascribed to the coupling between metal phonons and dielectric phonons, in this work we examine the influence of a direct coupling between the metal electrons and the dielectric phonons. The effect of electron-phonon processes is generally believed to be resistive and tends to decrease the overall thermal boundary conductance as compared to the phonon-phonon conductance σ(p). Here, we find that the effect of a direct electron-phonon interfacial coupling σ(e) is to enhance the effective thermal conductance between the metal and the dielectric. Resistive effects turn out to be important only for thin films of metals that have a low electron-phonon coupling strength. Two approaches are explored to reach these conclusions. First, we present an analytical solution of the two-temperature model to compute the effective conductance which accounts for all the relevant energy channels, as a function of σ(e), σ(p) and the electron-phonon coupling factor G. Second, we use numerical resolution to examine the influence of σ(e) on two realistic cases: a gold film on silicon or silica substrates. We point out the implications for the interpretation of time-resolved thermoreflectance experiments.

A mesoscopic model for (de)wetting.

We present a mesoscopic model for simulating the dynamics of a non-volatile liquid on a solid substrate. The wetting properties of the solid can be tuned from complete wetting to total non-wetting. This model opens the way to study the dynamics of drops and liquid thin films at mesoscopic length scales of the order of the nanometer. As particular applications, we analyze the kinetics of spreading of a liquid drop wetting a solid substrate and the dewetting of a liquid film on a hydrophobic substrate. In all these cases, very good agreement is found between simulations and theoretical predictions.

Heterogeneous nature of the dynamics and glass transition in thin polymer films.

Recent experiments have demonstrated that the dynamics in liquids close to and below the glass transition temperature is strongly heterogeneous, on the scale of a few nanometers. We use here a model proposed recently for explaining these features, and show that the heterogeneous nature of the dynamics has important consequences when considering the dynamics of thin films. We show how the dominant relaxation time in a thin film is changed as compared to the bulk, as a function of the thickness, the interaction energy with the substrate, and the temperature. The corresponding time scales cover the so-called VFT (or WLF) regime and vary between 10(-8) s to 10(4) s typically. In the absence of interaction, our model allows for interpreting suspended films experiments, in the case of small polymers for which the data do not depend on the polymer weight. The interaction leads to an increase of T(g) for an interaction per monomer of the order of the thermal energy T. This increase saturates at the value corresponding to strongly interacting films for adsorption energies slightly larger and still of order T. In particular, we predict that the T(g) shift can be non-monotonous as a function of the film thickness, in the case of intermediate interaction strength.

Heterogeneous dynamics at the glass transition in van der Waals liquids: determination of the characteristic scale.

Recent experiments have demonstrated that the dynamics in liquids close to the glass transition temperature is strongly heterogeneous. The characteristic size of these heterogeneities has been measured to be a few nanometers at Tg. We extend here a recent model for describing the heterogeneous nature of the dynamics which allows both to derive this length scale and the right orders of magnitude of the heterogeneities of the dynamics close to the glass transition. Our model allows then to interpret quantitatively small probes diffusion experiments.