David L. Olmsted

Atomistic simulations of dislocation mobility in Al, Ni and Al/Mg alloys

Dislocation velocities and mobilities are studied using molecular dynamics simulations for edge and screw dislocations in pure aluminium and nickel, and edge dislocations in Al-2.5%Mg and Al-5.0%Mg random substitutional alloys using EAM potentials. In the pure materials, the velocities of all dislocations are close to linear with the ratio of (applied stress)/(temperature) at low velocities consistent with phonon drag models, and quantitative agreement with the experiment is obtained for the mobility in Al. At higher velocities, different behaviour is observed. The edge dislocation velocity remains dependent solely on (applied stress)/(temperature) up to approximately 1.0 MPa K(-1), and approaches a plateau velocity that is lower than the smallest forbidden speed predicted by continuum models. In contrast, above a velocity around half of the smallest continuum wave speed, the screw dislocation damping has a contribution dependent solely on stress with a functional form close to that predicted by a radiation damping model of Eshelby. At the highest applied stresses, there are several regimes of nearly constant (transonic) velocity separated by velocity gaps in the vicinity of forbidden velocities; various modes of dislocation disintegration and destabilization were also encountered in this regime. In the alloy systems, there is a temperature- and concentration-dependent pinning regime where the velocity drops sharply below the pure metal velocity. Above the pinning regime but at moderate stresses, the velocity is again linear in (applied stress)/(temperature) but with a lower mobility than in the pure metal.

Evaluation of the constant potential method in simulating electric double-layer capacitors

A major challenge in the molecular simulation of electric double layer capacitors (EDLCs) is the choice of an appropriate model for the electrode. Typically, in such simulations the electrode surface is modeled using a uniform fixed charge on each of the electrode atoms, which ignores the electrode response to local charge fluctuations in the electrolyte solution. In this work, we evaluate and compare this Fixed Charge Method (FCM) with the more realistic Constant Potential Method (CPM), [S. K. Reed et al., J. Chem. Phys. 126, 084704 (2007)], in which the electrode charges fluctuate in order to maintain constant electric potential in each electrode. For this comparison, we utilize a simplified LiClO4-acetonitrile/graphite EDLC. At low potential difference (ΔΨ ⩽ 2u2009V), the two methods yield essentially identical results for ion and solvent density profiles; however, significant differences appear at higher ΔΨ. At ΔΨ ⩾ 4u2009V, the CPM ion density profiles show significant enhancement (over FCM) of inner-sphere adsorbed Li(+) ions very close to the electrode surface. The ability of the CPM electrode to respond to local charge fluctuations in the electrolyte is seen to significantly lower the energy (and barrier) for the approach of Li(+) ions to the electrode surface.

Structural disjoining potential for grain-boundary premelting and grain coalescence from molecular-dynamics simulations

We describe a molecular-dynamics framework for the direct calculation of the short-ranged structural forces underlying grain-boundary premelting and grain coalescence in solidification. The method is applied in a comparative study of (i) a Sigma9115120 degrees twist and (ii) a Sigma9110{411} symmetric tilt boundary in a classical embedded-atom model of elemental Ni. Although both boundaries feature highly disordered structures near the melting point, the nature of the temperature dependence of the width of the disordered regions in these boundaries is qualitatively different. The former boundary displays behavior consistent with a logarithmically diverging premelted layer thickness as the melting temperature is approached from below, while the latter displays behavior featuring a finite grain-boundary width at the melting point. It is demonstrated that both types of behavior can be quantitatively described within a sharp-interface thermodynamic formalism involving a width-dependent interfacial free energy, referred to as the disjoining potential. The disjoining potential for boundary (i) is calculated to display a monotonic exponential dependence on width, while that of boundary (ii) features a weak attractive minimum. The results of this work are discussed in relation to recent simulation and theoretical studies of the thermodynamic forces underlying grain-boundary premelting.

Lattice resistance and Peierls stress in finite size atomistic dislocation simulations

Atomistic computations of the Peierls stress in fcc metals are relatively scarce. By way of contrast, there are many more atomistic computations for bcc metals, as well as mixed discrete-continuum computations of the Peierls-Nabarro type for fcc metals. One of the reasons for this is the low Peierls stresses in fcc metals. Because atomistic computations of the Peierls stress take place in finite simulation cells, image forces caused by boundaries must either be relaxed or corrected for if system size-independent results are to be obtained. One of the approaches that has been developed for treating such boundary forces is by computing them directly and subsequently subtracting their effects, as developed in (Shenoy V B and Phillips R 1997 Phil. Mag. A 76 367). That work was primarily analytic, and limited to screw dislocations and special symmetric geometries. We extend that work to edge and mixed dislocations, and to arbitrary two-dimensional geometries, through a numerical finite element computation. We also describe a method for estimating the boundary forces directly on the basis of atomistic calculations. We apply these methods to the numerical measurement of the Peierls stress and lattice resistance curves for a model aluminium (fcc) system using an embedded-atom potential.

Modelling diffusion in crystals under high internal stress gradients

Diffusion of vacancies and impurities in metals is important in many processes occurring in structural materials. This diffusion often takes place in the presence of spatially rapidly varying stresses. Diffusion under stress is frequently modelled by local approximations to the vacancy formation and diffusion activation enthalpies which are linear in the stress, in order to account for its dependence on the local stress state and its gradient. Here, more accurate local approximations to the vacancy formation and diffusion activation enthalpies, and the simulation methods needed to implement them, are introduced. The accuracy of both these approximations and the linear approximations are assessed via comparison to full atomistic studies for the problem of vacancies around a Lomer dislocation in Aluminium. Results show that the local and linear approximations for the vacancy formation enthalpy and diffusion activation enthalpy are accurate to within 0.05 eV outside a radius of about 13 A (local) and 17 A (linear) from the centre of the dislocation core or, more generally, for a strain gradient of roughly up to 6 × 10^6 m^-1 and 3 × 10^6 m^-1, respectively. These results provide a basis for the development of multiscale models of diffusion under highly non-uniform stress.

Science at the interface : grain boundaries in nanocrystalline metals.

Interfaces are a critical determinant of the full range of materials properties, especially at the nanoscale. Computational and experimental methods developed a comprehensive understanding of nanograin evolution based on a fundamental understanding of internal interfaces in nanocrystalline nickel. It has recently been shown that nanocrystals with a bi-modal grain-size distribution possess a unique combination of high-strength, ductility and wear-resistance. We performed a combined experimental and theoretical investigation of the structure and motion of internal interfaces in nanograined metal and the resulting grain evolution. The properties of grain boundaries are computed for an unprecedented range of boundaries. The presence of roughening transitions in grain boundaries is explored and related to dramatic changes in boundary mobility. Experimental observations show that abnormal grain growth in nanograined materials is unlike conventional scale material in both the level of defects and the formation of unfavored phases. Molecular dynamics simulations address the origins of some of these phenomena.