Femtosecond X-Ray Diffraction Studies of the Reversal of the Microstructural Effects of Plastic Deformation during Shock Release of Tantalum.

We have used femtosecond x-ray diffraction to study laser-shocked fiber-textured polycrystalline tantalum targets as the 37-253 GPa shock waves break out from the free surface. We extract the time and depth-dependent strain profiles within the Ta target as the rarefaction wave travels back into the bulk of the sample. In agreement with molecular dynamics simulations, the lattice rotation and the twins that are formed under shock compression are observed to be almost fully eliminated by the rarefaction process.

Effect of wetting on nucleation and growth of D2 in confinement.

We have performed a computational study to determine how the wetting of liquid deuterium to the walls of the material influences nucleation. We present the development of a pair-wise interatomic potential that includes zero-point motion of molecular deuterium. Deuterium is used in this study because of its importance to inertial confinement fusion and the potential to generate a superfluid state if the solidification can be suppressed. Our simulations show that wetting dominates undercooling compared to the pore geometries. We observe a transition from heterogeneous nucleation at the confining wall to homogeneous nucleation at the bulk of the liquid (and intermediate cases) as the interaction with the confining wall changes from perfect wetting to non-wetting. When nucleation is heterogeneous, the temperature needed for solidification changes by 4 K with decreasing deuterium-wall interaction, but it remains independent (and equal to the one from bulk samples) when homogeneous nucleation dominates. We find that growth and quality of the resulting microstructure also depends on the magnitude of liquid deuterium-wall interaction strength.

Extraction of effective solid-liquid interfacial free energies for full 3D solid crystallites from equilibrium MD simulations.

Molecular dynamics simulations of an embedded atom copper system in the isobaric-isenthalpic ensemble are used to study the effective solid-liquid interfacial free energy of quasi-spherical solid crystals within a liquid. This is within the larger context of molecular dynamics simulations of this system undergoing solidification, where single individually prepared crystallites of different sizes grow until they reach a thermodynamically stable final state. The resulting equilibrium shapes possess the full structural details expected for solids with weakly anisotropic surface free energies (in these cases, ∼5% radial flattening and rounded [111] octahedral faces). The simplifying assumption of sphericity and perfect isotropy leads to an effective interfacial free energy as appearing in the Gibbs-Thomson equation, which we determine to be ∼177 erg/cm2, roughly independent of crystal size for radii in the 50-250 Šrange. This quantity may be used in atomistically informed models of solidification kinetics for this system.

In situ X-ray diffraction measurement of shock-wave-driven twinning and lattice dynamics.

Pressure-driven shock waves in solid materials can cause extreme damage and deformation. Understanding this deformation and the associated defects that are created in the material is crucial in the study of a wide range of phenomena, including planetary formation and asteroid impact sites, the formation of interstellar dust clouds, ballistic penetrators, spacecraft shielding and ductility in high-performance ceramics. At the lattice level, the basic mechanisms of plastic deformation are twinning (whereby crystallites with a mirror-image lattice form) and slip (whereby lattice dislocations are generated and move), but determining which of these mechanisms is active during deformation is challenging. Experiments that characterized lattice defects have typically examined the microstructure of samples after deformation, and so are complicated by post-shock annealing and reverberations. In addition, measurements have been limited to relatively modest pressures (less than 100 gigapascals). In situ X-ray diffraction experiments can provide insights into the dynamic behaviour of materials, but have only recently been applied to plasticity during shock compression and have yet to provide detailed insight into competing deformation mechanisms. Here we present X-ray diffraction experiments with femtosecond resolution that capture in situ, lattice-level information on the microstructural processes that drive shock-wave-driven deformation. To demonstrate this method we shock-compress the body-centred-cubic material tantalum-an important material for high-energy-density physics owing to its high shock impedance and high X-ray opacity. Tantalum is also a material for which previous shock compression simulations and experiments have provided conflicting information about the dominant deformation mechanism. Our experiments reveal twinning and related lattice rotation occurring on the timescale of tens of picoseconds. In addition, despite the common association between twinning and strong shocks, we find a transition from twinning to dislocation-slip-dominated plasticity at high pressure (more than 150 gigapascals), a regime that recovery experiments cannot accurately access. The techniques demonstrated here will be useful for studying shock waves and other high-strain-rate phenomena, as well as a broad range of processes induced by plasticity.

Are nanoporous materials radiation resistant?

The key to perfect radiation endurance is perfect recovery. Since surfaces are perfect sinks for defects, a porous material with a high surface to volume ratio has the potential to be extremely radiation tolerant, provided it is morphologically stable in a radiation environment. Experiments and computer simulations on nanoscale gold foams reported here show the existence of a window in the parameter space where foams are radiation tolerant. We analyze these results in terms of a model for the irradiation response that quantitatively locates such window that appears to be the consequence of the combined effect of two length scales dependent on the irradiation conditions: (i) foams with ligament diameters below a minimum value display ligament melting and breaking, together with compaction increasing with dose (this value is typically ∼5 nm for primary knock on atoms (PKA) of ∼15 keV in Au), while (ii) foams with ligament diameters above a maximum value show bulk behavior, that is, damage accumulation (few hundred nanometers for the PKA's energy and dose rate used in this study). In between these dimensions, (i.e., ∼100 nm in Au), defect migration to the ligament surface happens faster than the time between cascades, ensuring radiation resistance for a given dose-rate. We conclude that foams can be tailored to become radiation tolerant.

Surface-chemistry-driven actuation in nanoporous gold.

Although actuation in biological systems is exclusively powered by chemical energy, this concept has not been realized in man-made actuator technologies, as these rely on generating heat or electricity first. Here, we demonstrate that surface-chemistry-driven actuation can be realized in high-surface-area materials such as nanoporous gold. For example, we achieve reversible strain amplitudes of the order of a few tenths of a per cent by alternating exposure of nanoporous Au to ozone and carbon monoxide. The effect can be explained by adsorbate-induced changes of the surface stress, and can be used to convert chemical energy directly into a mechanical response, thus opening the door to surface-chemistry-driven actuator and sensor technologies.

Vapor pressure and sublimation rate of molecular crystals: role of internal degrees of freedom.

It is a common practice to approximate the desorption rate of atoms from crystal surfaces with an expression of the form nueff exp(-DeltaE/kBT), where DeltaE is an activation barrier to desorb and nueff is an effective vibrational frequency approximately 10(12) s(-1). For molecular solids, however, such an approximation can lead to a many orders of magnitude underestimation of vapor pressure and sublimation rates due to neglected contributions from molecular internal degrees of freedom. Here, we develop a simple working formula that yields good estimates for a general molecular (or atomic) solid and illustrate the approach by computing equilibrium vapor pressure of three different molecular solids and an atomic solid, as well as the desorption rate of a foreign (inhibitor) molecule from the surface of a molecular solid.