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

Nanocrystals are fundamental to modern science and technology. Mastery over the shape of a nanocrystal enables control of its properties and enhancement of its usefulness for a given application. Our aim is to present a comprehensive review of current research activities that center on the shape-controlled synthesis of metal nanocrystals. We begin with a brief introduction to nucleation and growth within the context of metal nanocrystal synthesis, followed by a discussion of the possible shapes that a metal nanocrystal might take under different conditions. We then focus on a variety of experimental parameters that have been explored to manipulate the nucleation and growth of metal nanocrystals in solution-phase syntheses in an effort to generate specific shapes. We then elaborate on these approaches by selecting examples in which there is already reasonable understanding for the observed shape control or at least the protocols have proven to be reproducible and controllable. Finally, we highlight a number of applications that have been enabled and/or enhanced by the shape-controlled synthesis of metal nanocrystals. We conclude this article with personal perspectives on the directions toward which future research in this field might take.

Shape‐Controlled Synthesis of Metal Nanocrystals: Simple Chemistry Meets Complex Physics?

Recent years have seen a renewed interest in the harvesting and conversion of solar energy. Among various technologies, the direct conversion of solar to chemical energy using photocatalysts has received significant attention. Although heterogeneous photocatalysts are almost exclusively semiconductors, it has been demonstrated recently that plasmonic nanostructures of noble metals (mainly silver and gold) also show significant promise. Here we review recent progress in using plasmonic metallic nanostructures in the field of photocatalysis. We focus on plasmon-enhanced water splitting on composite photocatalysts containing semiconductor and plasmonic-metal building blocks, and recently reported plasmon-mediated photocatalytic reactions on plasmonic nanostructures of noble metals. We also discuss the areas where major advancements are needed to move the field of plasmon-mediated photocatalysis forward.

Plasmonic-metal nanostructures for efficient conversion of solar to chemical energy

Nanocrystals (NCs) discussed in this Review are tiny crystals of metals, semiconductors, and magnetic material consisting of hundreds to a few thousand atoms each. Their size ranges from 2-3 to about 20 nm. What is special about this size regime that placed NCs among the hottest research topics of the last decades? The quantum mechanical coupling * To whom correspondence should be addressed. E-mail: dvtalapin@uchicago.edu. † The University of Chicago. ‡ Argonne National Lab. Chem. Rev. 2010, 110, 389–458 389

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Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications

Localized Surface Plasmon Resonance Sensors

Nanokristalle sind von grundlegender Bedeutung in der modernen Wissenschaft und Technologie. Die Eigenschaften eines Nanokristalls lassen sich uber seine Form beeinflussen und auf eine bestimmte Anwendung hin zuschneiden. Ziel dieses Aufsatzes ist es, einen umfassenden Uberblick uber den aktuellen Stand der Forschung auf dem Gebiet der formkontrollierten Synthese von Metallnanokristallen zu geben. Nach einer kurzen Einleitung uber die Prinzipien von Kristallkeimbildung und -wachstum diskutieren wir einzelne Arten von Nanokristallformen und betrachten verschiedene experimentelle Parameter, uber die die Keimbildung und das Wachstum von Metallnanokristallen in der Losungssynthese gezielt manipuliert werden kann. Wir erlautern diese Methoden anhand von Beispielen, wo zumindest ein Grundverstandnis fur die beobachtete Formkontrolle vorhanden ist. Schlieslich stellen wir Anwendungen vor, bei denen die Formkontrolle von Metallnanokristallen ein entscheidender Faktor ist, und beenden den Aufsatz mit einem personlichen Ausblick auf kunftig zu erwartende Entwicklungen auf diesem Gebiet.

Formkontrolle bei der Synthese von Metallnanokristallen: einfache Chemie, komplexe Physik?

The polyol synthesis is a popular method of preparing metal nanostructures, yet the mechanism by which metal ions are reduced is poorly understood. Using a spectrophotometric method, we show, for the first time, that heating ethylene glycol (EG) in air results in its oxidation to glycolaldehyde (GA), a reductant capable of reducing most noble metal ions. The dependence of reducing power on temperature for EG can be explained by this temperature-dependent oxidation, and the factors influencing GA production can have a profound impact on the nucleation and growth kinetics. These new findings provide critical insight into how the polyol synthesis can be used to generate metal nanostructures with well-controlled shapes. For example, with the primary reductant identified, it becomes possible to evaluate and understand its explicit role in generating nanostructures of a specific shape to the exclusion of others.

On the polyol synthesis of silver nanostructures: glycolaldehyde as a reducing agent.

The hydrodesulfurization (HDS) activity of molybdenum sulfide-based catalysts is localized to the edges of this layered solid and is, therefore, highly dependent on the technique used to prepare the material. Here, ultrasonic spray pyrolysis (USP) was used to synthesize porous, nanostructured MoS2. Low surface area powders, not useful for catalysis, are generally produced by USP. This work shows that when combined with a dissolvable template, USP is capable of producing high surface area materials. An aqueous solution of ammonium tetrathiomolybdate and colloidal silica was nebulized and pyrolyzed to give a MoS2/SiO2 composite material. Leaching with HF removed the sacrificial SiO2, resulting in a highly porous MoS2 network with surface areas as high as 250 m2/g. Cobalt-promoted MoS2 networks were also synthesized. The thiophene HDS activities of these materials were substantially higher than those of unsupported MoS2 and RuS2 standards, illustrating the enhanced dispersion of the HDS active phase achieved by this synthetic technique.

Porous MoS2 synthesized by ultrasonic spray pyrolysis.

Noble-metal nanocages comprise a novel class of nanostructures possessing hollow interiors and porous walls. They are prepared using a remarkably simple galvanic replacement reaction between solutions containing metal precursor salts and Ag nanostructures prepared through polyol reduction. The electrochemical potential difference between the two species drives the reaction, with the reduced metal depositing on the surface of the Ag nanostructure. In our most studied example, involving HAuCl4 as the metal precursor, the resultant Au is deposited epitaxially on the surface of the Ag nanocubes, adopting their underlying cubic form. Concurrent with this deposition, the interior Ag is oxidized and removed, together with alloying and dealloying, to produce hollow and, eventually, porous structures that we commonly refer to as Au nanocages. This approach is versatile, with a wide range of morphologies (e.g., nanorings, prism-shaped nanoboxes, nanotubes, and multiple-walled nanoshells or nanotubes) available upon...

Gold Nanocages: Synthesis, Properties, and Applications

The optical properties of metal nanomaterials are determined by a set of parameters that include composition, particle size and shape, overall architecture, and local environment. This Tutorial Review examines the influence of each of these factors on the localized surface plasmon resonance of colloidal metal nanoparticles. This examination is paralleled with a discussion of the advances which have enabled the synthesis of structurally defined metal nanomaterials, as these samples serve as the best platforms for elucidating the fundamental properties of plasmonic colloids. Based on the analysis of such samples, five guidelines are presented to aid the rational design and synthesis of new metal nanostructures for advanced applications in nanomedicine, energy, chemical sensing, and colloidal plasmonics in general.

Sara E. Skrabalak

Papers

Formkontrolle bei der Synthese von Metallnanokristallen: einfache Chemie, komplexe Physik?

On the polyol synthesis of silver nanostructures: glycolaldehyde as a reducing agent.

Porous MoS2 synthesized by ultrasonic spray pyrolysis.

Gold Nanocages: Synthesis, Properties, and Applications

Engineering plasmonic metal colloids through composition and structural design.