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Author(s): Luis A. Zepeda-Ruiz [1]; Alexander Stukowski [2]; Tomas Oppelstrup [1]; Vasily V. Bulatov (corresponding author) [1] Ordinarily, the strength and plasticity properties of a metal are defined by dislocations--line [...]

We detail the estimation of activation energies and quantum nuclear vibrational tunneling effects for hydrogen diffusion in PuO 2 based on Density Functional Theory calculations and a quantum double well approximation. We find that results are relatively insensitive to choice of exchange correlation functional. In addition, the representation of spin in the system and use of an extended Hubbard U correction has only a small effect on hydrogen point defect formation energies when the PuO 2 lattice is held fixed at the experimental density. We then compute approximate activation energies for transitions between hydrogen interstitial sites seeded by a semi-empirical quantum model and determine the quantum tunneling enhancement relative to classical kinetic rates. Our model indicates that diffusion rates in H/PuO 2 systems could be enhanced by more than one order of magnitude at ambient conditions and that these effects persist at high temperature. The method we propose here can be used as a fast screening tool for assessing possible quantum nuclear vibrational effects in any number of condensed phase materials and surfaces, where hydrogen hopping tends to follow well defined minimum energy pathways. [ABSTRACT FROM AUTHOR]

Several molecular dynamics (MD) simulations are employed to explain the characterization of sputtering products obtained during the graphite exposure to deuterium amorphous carbon layers. The results show that the energy distribution for the physically sputtered single C atoms is almost consistent with the commonly used Thompson distribution and the assumed cosine distribution function.

A comprehensive, quantitative analysis that combines a hierarchical theoretical approach with experimental measurements is presented of the deformation behavior of coherently strained InAs/GaAs(111)A heteroepitaxial systems. The experimental measurements are found to be in excellent agreement with the calculated lattice interplanar distances and the corresponding strain fields in the thin mechanically unconstrained substrates considered in the theoretical analysis.

Direct molecular dynamics simulation of atomic deposition under realistic conditions is notoriously challenging because of the wide range of time scales that must be captured. Numerous simulation approaches have been proposed to address the problem, often requiring a compromise between model fidelity, algorithmic complexity, and computational efficiency. Coarse projective integration, an example application of the "equation-free" framework, offers an attractive balance between these constraints. Here, periodically applied, short atomistic simulations are employed to compute time derivatives of slowly evolving coarse variables that are then used to numerically integrate differential equations over relatively large time intervals. A key obstacle to the application of this technique in realistic settings is the "lifting" operation in which a valid atomistic configuration is recreated from knowledge of the coarse variables. Using Ge deposition on amorphous SiO2 substrates as an example application, we present a scheme for lifting realistic atomistic configurations comprised of collections of Ge islands on amorphous SiO2 using only a few measures of the island size distribution. The approach is shown to provide accurate initial configurations to restart molecular dynamics simulations at arbitrary points in time, enabling the application of coarse projective integration for this morphologically complex system. [ABSTRACT FROM AUTHOR]

The ability to predict the behavior of point defects in metals, particularly interstitial defects, is central to accurate modeling of the microstructural evolution in environments with high radiation fluxes. Existing interatomic potentials of embedded atom method type predict disparate stable interstitial defect configurations in vanadium. This is not surprising since accurate first-principles interstitial data were not available when these potentials were fitted. In order to provide the input information required to fit a vanadium potential appropriate for radiation damage studies, we perform a series of first-principles calculations on six different interstitial geometries and vacancies. These calculations identify the 〈111〉 dumbbell as the most stable interstitial with a formation energy of approximately 3.1 eV, at variance with predictions based upon existing potentials. Our potential is of Finnis-Sinclair type and is fitted exactly to the experimental equilibrium lattice parameter, cohesive energy, elastic constants and a calculated unrelaxed vacancy formation energy. Two additional potential parameters were used to obtain the best fit to the set of interstitial formation energies determined from the first-principles calculations. The resulting potential was found to accurately predict both the magnitude and ordering of the formation energies of six interstitial configurations and the unrelaxed vacancy ground state, in addition to accurately describing the migration characteristics of the stable interstitial and vacancy. This vanadium potential is capable of describing the point defect properties appropriate for radiation damage simulations as well as for simulations of more common crystal and simple defect properties. [ABSTRACT FROM AUTHOR]

Molecular dynamics simulations are performed to examine the effects of ion beams in selecting MgO island orientations during ion beam assisted deposition. Sputter yields are determined as a function of ion beam orientation for MgO islands of different sizes. While channeling does occur in small islands, the difference in sputter yields between channeling and nonchanneling orientations is much smaller in small islands than in larger islands or a continuous film. The ion beam is capable of disrupting the entire island structure at small island sizes, while channeling dependent sputtering occurs at larger island size. Since less sputtering occurs for channeling orientations, the ion beam produces an orientation-dependent island growth rate. This leads to island orientation-dependent nucleation rates. A new analytical model parameterized using the molecular dynamics sputter yield data is developed which predicts how growth conditions affect these island-orientation nucleation rates. Based upon these simulations and model results, we suggest a strategy to efficiently grow thin, highly textured MgO films. [ABSTRACT FROM AUTHOR]

Analyzes the energetics, interfacial stability, strain fields and film surface morphology in semiconductor heteroepitaxy. Application of continuum elasticity theory and atomistic simulations in the analysis; Computation of critical film thicknesses; Description of the atomistic simulation results; Results and discussion.

We present and evaluate a semiempirical particle-based model of electrophoretic deposition using extensive mesoscale simulations. We analyze particle configurations in order to observe how colloids accumulate at the electrode and arrange into deposits. In agreement with existing continuum models, the thickness of the deposit increases linearly in time during deposition. Resulting colloidal deposits exhibit a transition between highly ordered and bulk disordered regions that can give rise to an appreciable density gradient under certain simulated conditions. The overall volume fraction increases and falls within a narrow range as the driving force due to the electric field increases and repulsive intercolloidal interactions decrease. We postulate ordering and stacking within the initial layer(s) dramatically impacts the microstructure of the deposits. We find a combination of parameters, i.e., electric field and suspension properties, whose interplay enhances colloidal ordering beyond the commonly known approach of only reducing the driving force. [ABSTRACT FROM AUTHOR]

We develop and evaluate a semi-empirical particle-based model of electrophoresis using extensive mesoscale simulations. We parameterize the model using only measurable quantities from a broad set of colloidal suspensions with properties that span the experimentally relevant regime. With sufficient sampling, simulated diffusivities and electrophoretic velocities match predictions of the ubiquitous Stokes-Einstein and Henry equations, respectively. This agreement holds for non-polar and aqueous solvents or ionic liquid colloidal suspensions under a wide range of applied electric fields. [ABSTRACT FROM AUTHOR]

A systematic theoretical analysis is presented of the combined effects of substrate compliance and film compositional grading on the relaxation of strain due to lattice mismatch in layer-by-layer semiconductor heteroepitaxy. The analysis is based on a combination of continuum elasticity theory and a novel atomistic simulation approach for modeling structural and compositional relaxation in layer-by-layer heteroepitaxial systems. Results are presented for InAs epitaxy on GaAs(1 1 1)A compliant substrates with some marginal film compositional grading that consists of one monolayer of In0.50Ga0.50As grown on the substrate surface prior to InAs growth. A parametric study is carried out over a wide range of substrate thicknesses. Interfacial stability with respect to misfit dislocation formation, the dependence on substrate thickness of a thermodynamic critical film thickness, and the completion of the coherent-to-semicoherent interfacial transition are examined in detail. In addition, the structural characteristics and compositional distribution of the corresponding semicoherent interfaces, the associated strain fields, as well as the film surface morphological characteristics are analyzed. Most importantly, the role of segregation at defects of a semicoherent interface in the thermodynamics of layer-by-layer heteroepitaxial growth is demonstrated. Our study shows that systematic combination of the mechanical behavior of thin compliant substrates with grading of the epitaxial film composition provides a very promising engineering strategy for strain relaxation in heteroepitaxy. [Copyright &y& Elsevier]

A systematic study is presented of interfacial stability and strain relaxation through misfit dislocation formation in III–V semiconductor layer-by-layer heteroepitaxy. A multiscale modeling strategy is developed that links continuum elasticity theory with atomistic structural relaxation and Monte Carlo simulations using a valence force field description of interatomic interactions. Results are presented for the energetics of the transition from a coherent to a semicoherent film/substrate interface consisting of a misfit dislocation network, the semicoherent interface structures, the associated strain fields, and the film surface morphological characteristics for InAs epitaxy on GaAs(1 1 1)A. The capability of continuum elasticity theory to provide a satisfactory description of the atomistic simulation results is discussed. In addition, using thin compliant substrates and grading the composition of the deposited film are demonstrated to have beneficial effects on film strain relaxation. Furthermore, the dynamics of strain relaxation is analyzed based on a phenomenological mean-field theoretical framework. Our theoretical results are in very good agreement with our experimental measurements on InAs/GaAs(1 1 1)A samples for films grown by molecular beam epitaxy on thick and thin GaAs buffer layers. [Copyright &y& Elsevier]

The relation between stress evolution and surface morphology during deposition of sputtered films is examined by combining kinetic Monte Carlo simulations and stress measurements. We find that the surface morphology is susceptible to an instability, which transforms from layer-by-layer growth to the formation of pillarlike columns. The gaps between these columns prevent complete densification and can lead to a network of pores in the layer. We propose that the formation of this structure changes the stress in the growing layers from compressive to tensile. [ABSTRACT FROM AUTHOR]

We employ molecular dynamics simulations of defect-free nanopillars with realistic cylindrical geometries to obtain an atomic-level picture of their deformation behavior under compression. We find that dislocations are nucleated in the two outermost surface layers. Furthermore, plastic yield depends crucially on the particular arrangement of steps and facets at the surface of the nanopillars. We show that different facet orientations can differ dramatically in their response to external stresses. Freestanding nanopillars exhibit a highly nonuniform distribution of stresses along their height. This causes an elastic deformation that leads to a barrel-like shape attained by the nanopillars under compression. The stress concentration at the center of the pillars due to barreling causes dislocations to preferentially nucleate in this region. [ABSTRACT FROM AUTHOR]

We report the results of a theoretical analysis for the kinetics of strain relaxation in Si1-xGex thin films grown epitaxially on Si(100) substrates. The analysis is based on a properly parametrized dislocation mean-field theoretical model describing plastic deformation dynamics due to threading dislocation propagation and addresses strain relaxation kinetics during both epitaxial growth and thermal annealing, including post-implantation annealing. Theoretical predictions for strain relaxation as a function of film thickness in Si0.80Ge0.20/Si(100) samples annealed after epitaxial growth either unimplanted or after He ion implantation are in excellent agreement with experimental measurements [J. Cai et al., J. Appl. Phys. 95, 5347 (2004)]. [ABSTRACT FROM AUTHOR]

We apply a hybrid Monte Carlo-molecular dynamics code to the study of grain boundary motion upon annealing of pure Cu and Cu with low concentrations of Fe. The hybrid simulations account for segregation and precipitation of the low solubility Fe, together with curvature-driven grain boundary motion. Grain boundaries in two different systems, a Σ7+U-shaped half-loop grain and a nanocrystalline sample, were found to be pinned in the presence of Fe concentrations exceeding 3%. [ABSTRACT FROM AUTHOR]

Molecular dynamics simulations are performed to study the fundamental role of the ion beam in determining the in-plane texture of <100> oriented (out-of-plane) MgO films during ion beam assisted deposition (IBAD). Sputter yields are determined as a function of in-plane orientation for Ar ion beams. The minimum sputter yield exists at an ion beam orientation corresponding to the MgO <110> direction. The finite width of the sputter yield minimum is attributable to two main factors: (i) only a fraction of the incident ions are oriented to travel directly down the center of the channel and (ii) ions that are not exactly parallel to the channeling direction may channel. While the simulations imply that it is possible to in-plane orient {001} MgO films using IBAD, there are fundamental limitations on the degree of ordering that can be achieved. © 2001 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Examines the surface morphology of indium films by scanning tunneling microscopy. Vertical surface displacement on the films; Atomistic simulations within a valence force field model; Misfit dislocation network at the semicoherent interface.

A phenomenological mean-field theory is presented for the kinetics of strain relaxation due to misfit dislocation generation in the strained-layer growth of epitaxial semiconductor films on thin compliant substrates. The theory provides a generalized dislocation kinetic framework by coupling the mechanics of an epitaxial film on a compliant substrate with a well-known description of plastic deformation dynamics in semiconductor crystals. The theoretical results reproduce successfully recent experimental data for strain relaxation in the InAs/GaAs(110) heteroepitaxial system. © 1998 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Interfacial stability and the morphology of the epitaxial film surface have been studied in InAs/GaAs(111)A heteroepitaxy based on atomistic simulations and scanning tunneling microscopy. Effects of buffer layer thickness were examined by analyzing two heteroepitaxial systems consisting of thin and thick GaAs buffer layers. In both cases, one monolayer of In[sub 0.50]Ga[sub 0.50]As is grown initially on the buffer layer prior to InAs growth. Our results indicate that film compositional grading and the resulting segregation of In atoms at defects in the semicoherent interface can be used effectively in conjunction with the mechanical compliance of thin buffer layers to delay the completion of the coherent-to-semicoherent interfacial transition. © 2000 American Institute of Physics. [ABSTRACT FROM AUTHOR]

The mechanical behavior of thin buffer layers for InAs/GaAs(111)A heteroepitaxy has been investigated by x-ray diffraction (XRD). XRD θ-2θ spectra are presented for the (220) reflection for two monolayers (MLs) of InAs deposited on GaAs buffer layers of both 20 ML and 150 nm (≅ 460 ML) in thickness. For the thicker buffer layer, the XRD spectrum exhibits a single, symmetric peak at a reflected angle corresponding to the bulk GaAs lattice parameter, while for the thinner one it exhibits asymmetry around the GaAs substrate reflection with the spectrum tailing to lower angle. This indicates that the thin buffer layer possesses a distribution of interlayer distances in the [220] direction that are larger than that of the GaAs substrate. The XRD data agree very well with theoretical calculations in which the thin GaAs buffer layer is modeled as unconstrained at its base. Our results provide direct evidence that thin GaAs buffer layers behave mechanically similarly to compliant substrates. © 2000 American Institute of Physics. [ABSTRACT FROM AUTHOR]

The article presents information on the requirement of the Monte Carlo algorithm for the purpose of studying the atomistic simulations of the precipitation in the alloys. The transmutation of the simulations of the multicomponent systems is allowed by the semi-grand-canonical ensemble. Information on the study of the precipitation of copper in the nanocrystalline iron through the algorithm is also presented.

Recent nanomechanical tests on submicron metal columns and wires have revealed a dramatic increase in yield strength with decreasing sample size. Here, we demonstrate that nanoporous metal foams can be envisioned as a three-dimensional network of ultrahigh-strength nanowires, thus bringing together two seemingly conflicting properties: high strength and high porosity. Specifically, we characterized the size-dependent mechanical properties of nanoporous gold using a combination of nanoindentation, column microcompression, and molecular dynamics simulations. We find that nanoporous gold can be as strong as bulk Au, despite being a highly porous material, and that the ligaments in nanoporous gold approach the theoretical yield strength of Au.