Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

Fast parallel algorithms for short-range molecular dynamics

The support plays an important role for supported metal catalysts by positioning itself as a macromolecular ligand, which conditions the nature of the active site and contributes indirectly but also sometimes directly to the reactivity. Metal species such as nanoparticles, clusters, or single atoms can be deposited on carbon materials for various catalytic reactions. All the carbon materials used as catalyst support constitute a large family of compounds that can vary both at textural and at structural levels. Today, the recent developments of well-controlled synthesis methodologies, advanced characterization techniques, and modeling tools allow one to correlate the relationships between metal/support/reactant at the molecular level. Based on these considerations, in this Review article, we wish to provide some answers to the question "How and why anchoring metal nanoparticles, clusters, or single atoms on carbon materials for catalysis?". To do this, we will rely on both experimental and theoretical studies. We will first analyze what sites are available on the surface of a carbon support for the anchoring of the active phase. Then, we will describe some important effects in catalysis inherent to the presence of a carbon-type support (metal-support interaction, confinement, spillover, and surface functional group effects). These effects will be commented on by putting into perspective catalytic results obtained in numerous reactions of thermal catalysis, electrocatalysis, or photocatalysis.

A Theory/Experience Description of Support Effects in Carbon-Supported Catalysts.

A theory is developed which allows one to discuss the stability of multiply-twinned particles and to calculate critical sizes for stable and quasi-stable states. An icosahedral particle is essentially stable for r ≦ r i w * , quasi-stable for r i w * r i t 0 where r is an edge length of the particle, while a decahedral particle is not essentially stable but quasi-stable for r ≦ r d t 0 and unstable for r > r d t 0 . The critical sizes r i w * , r i t 0 and r d t 0 are formulated as functions of the specific surface energy γ h k l , the twin boundary energy γ t , the elastic strain energy W and the adhesive energy γ a to the substrate. Calculated critical diameters 2 r i w * ,2 r i t 0 and 2 r d t 0 for the particles grown in free space for several elements range between 15.5A and 106.8A, between 109.8A and 486.1A and between 725A and 3961A, respectively. These values are in good agreement with experimental results.

Stability of Multiply-Twinned Particles

At the nanoscale, the investigation of structural features becomes fundamental as we can establish relationships between cluster geometries and their physicochemical properties. The peculiarity lies in the variety of shapes often unusual and far from any geometrical and crystallographic intuition clusters can assume. In this respect, we should treat and consider nanoparticles as a new form of matter. Nanoparticle structures depend on their size, chemical composition, ordering, as well as external conditions e.g. synthesis method, pressure, temperature, support. On top of that, at finite temperatures nanoparticles can fluctuate among different structures, opening new and exciting horizons for the design of optimal nanoparticles for advanced applications. This article aims to overview geometrical features of transition metal clusters and of their various rearrangements.

Structural properties of sub-nanometer metallic clusters.

Defect Electrocatalysts and Alkaline Electrolyte Membranes in Solid-State Zinc–Air Batteries: Recent Advances, Challenges, and Future Perspectives

On the nature of the structural transitions between anti-Mackay stacking, chiral stacking and their thermal stability in AgCu nanoalloys

Novel structural motifs: Chiral AgCu nanoalloys with chiral Cu core

Strain variation within a nanoparticle plays a crucial role in tuning its properties. High Resolution Transmission Electron Microscopy (HRTEM) images of a nanoparticle supported on amorphous carbon film are used to determine the strain variation. Experimental measurements in this present study on a single crystalline silver nanoparticle exhibited an unexpected high strain variation. Generally, the influence of carbon film is not accounted for during interpretation of measured strain variation. However, experimental observations raise the question whether the supporting carbon film alters the measured strain variation. In order to address this, strain variation within a simulated Ag nanoparticle supported on an amorphous carbon is measured with varying film thicknesses. The results show that supporting carbon film thickness introduces an artefact leading to more strain variation than what is present within an unsupported nanoparticle. Moreover, the variation increases with increasing supporting carbon film thickness. This effect is more pronounced in a thinner nanoparticle. Without considering this influence, the interpretation of strain within a nanoparticle may introduce severe errors which in turn will affect the tunability of desirable properties for different applications. Since strain measurement depends on the accuracy of the atomic position, the interpretation of any result using the atomic position from HRTEM images of a nanoparticle should consider the influence of supporting film.

Influence of supporting amorphous carbon film thickness on measured strain variation within a nanoparticle.

In AgCu nanoalloys a size-dependent transition to the chiral stacking from the anti-Mackay stacking has been predicted previously. This trend is explained by considering the interplay between the core-shell energetics. Results indicate that the energy changes in the Ag shell alone is not sufficient to explain the stability of the chiral stacking and the energy changes in the Cu core also need to be considered. In addition to this, thermally induced transition to chiral stacking was observed at sizes where anti-Mackay stacking is energetically favourable. On transition to the chiral stacking, the Ag-Ag, Ag-Cu and Cu-Cu bond lengths change significantly. These observations are also applicable for AgCu nanoalloys with incomplete Ag shells.

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Manoj Settem

Papers

On the nature of the structural transitions between anti-Mackay stacking, chiral stacking and their thermal stability in AgCu nanoalloys

Novel structural motifs: Chiral AgCu nanoalloys with chiral Cu core

Influence of supporting amorphous carbon film thickness on measured strain variation within a nanoparticle.

Role of core-shell energetics on anti-Mackay, chiral stacking in AgCu nanoalloys and thermally induced transition to chiral stacking.

On the effect of relative stabilities of FCC-like and HCP-like atoms on structure of FCC silver nanoclusters