Biomedical subjects

J Daniel Gezelter

Publications and source records attributed to J Daniel Gezelter.

5 recordsLinked to original sources

PubMed2006

Is the Ewald summation still necessary? Pairwise alternatives to the accepted standard for long-range electrostatics.

We investigate pairwise electrostatic interaction methods and show that there are viable computationally efficient (O(N)) alternatives to the Ewald summation for typical modern molecular simulations. These methods are extended from the damped and cutoff-neutralized Coulombic sum originally proposed by Wolf et al. [J. Chem. Phys. 110, 8255 (1999)]. One of these, the damped shifted force method, shows a remarkable ability to reproduce the energetic and dynamic characteristics exhibited by simulations employing lattice summation techniques. Comparisons were performed with this and other pairwise methods against the smooth particle-mesh Ewald summation to see how well they reproduce the energetics and dynamics of a variety of molecular simulations.

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PubMed2005

Breathing mode dynamics and elastic properties of gold nanoparticles.

We present calculations of the bulk modulus, heat capacity, and the period of the breathing mode for spherical nanoparticles following excitation by ultrafast laser pulses. The bulk modulus and heat capacities both exhibit clear transitions upon bulk melting of the particles. Equilibrium calculations of the heat capacity show that the melting transition is sharper and occurs at a lower temperature than one would observe from an ultrafast experiment. We also observe an intriguing splitting in the low-frequency spectra of the nanoparticles and analyze this splitting in terms of Lamb's classical theory of elastic spheres. We conclude that the particles either (1) melt during the observation period following laser excitation or (2) melt an outer shell while maintaining a crystalline core. Both mechanisms for melting are commensurate with our observations.

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PubMed2005

OOPSE: an object-oriented parallel simulation engine for molecular dynamics.

OOPSE is a new molecular dynamics simulation program that is capable of efficiently integrating equations of motion for atom types with orientational degrees of freedom (e.g. "sticky" atoms and point dipoles). Transition metals can also be simulated using the embedded atom method (EAM) potential included in the code. Parallel simulations are carried out using the force-based decomposition method. Simulations are specified using a very simple C-based meta-data language. A number of advanced integrators are included, and the basic integrator for orientational dynamics provides substantial improvements over older quaternion-based schemes.

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PubMed2004

On the structural and transport properties of the soft sticky dipole and related single-point water models.

The density maximum and temperature dependence of the self-diffusion constant were investigated for the soft sticky dipole (SSD) water model and two related reparametrizations of this single-point model. A combination of microcanonical and isobaric-isothermal molecular dynamics simulations was used to calculate these properties, both with and without the use of reaction field to handle long-range electrostatics. The isobaric-isothermal simulations of the melting of both ice-Ih and ice-Ic showed a density maximum near 260 K. In most cases, the use of the reaction field resulted in calculated densities which were significantly lower than experimental densities. Analysis of self-diffusion constants shows that the original SSD model captures the transport properties of experimental water very well in both the normal and supercooled liquid regimes. We also present our reparametrized versions of SSD for use both with the reaction field or without any long-range electrostatic corrections. These are called the SSD/RF and SSD/E models, respectively. These modified models were shown to maintain or improve upon the experimental agreement with the structural and transport properties that can be obtained with either the original SSD or the density-corrected version of the original model (SSD1). Additionally, a novel low-density ice structure is presented which appears to be the most stable ice structure for the entire SSD family.

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PubMed2002

Size-dependent spontaneous alloying of Au-Ag nanoparticles.

We report on systematic studies of size-dependent alloy formation of silver-coated gold nanoparticles (NPs) in aqueous solution at ambient temperature using X-ray absorption fine structure spectroscopy (XAFS). Various Au-core sizes (2.5-20 nm diameter) and Ag shell thicknesses were synthesized using radiolytic wet techniques. The equilibrium structures (alloy versus core-shell) of these NPs were determined in the suspensions. We observed remarkable size dependence in the room temperature interdiffusion of the two metals. The interdiffusion is limited to the subinterface layers of the bimetallic NPs and depends on both the core size and the total particle size. For the very small particles (< or =4.6 nm initial Au-core size), the two metals are nearly randomly distributed within the particle. However, even for these small Au-core NPs, the interdiffusion occurs primarily in the vicinity of the original interface. Features from the Ag shells do remain. For the larger particles, the boundary is maintained to within one monolayer. These results cannot be explained either by enhanced self-diffusion that results from depression of the melting point with size or by surface melting of the NPs. We propose that defects, such as vacancies, at the bimetallic interface enhance the radial migration (as well as displacement around the interface) of one metal into the other. Molecular dynamics calculations correctly predict the activation energy for diffusion of the metals in the absence of vacancies and show an enormous dependence of the rate of mixing on defect levels. They also suggest that a few percent of the interfacial lattice sites need to be vacant to explain the observed mixing.

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