Numerical studies of the vibrational isocoordinate rule in chalcogenide glasses

Many properties of alloyed chalcogenide glasses can be closely correlated with the average coordination of these compounds. This is the case, for example, of the ultrasonic constants, dilatometric softening temperature and the vibrational densities of states. What is striking, however, is that these properties are nevertheless almost independent of the composition at given average coordination. Here, we report on some numerical verification of this experimental rule as applied to vibrational density of states.Comment: 7 pages, including 3 figure

Evolution of the potential-energy surface of amorphous silicon

The link between the energy surface of bulk systems and their dynamical properties is generally difficult to establish. Using the activation-relaxation technique (ART nouveau), we follow the change in the barrier distribution of a model of amorphous silicon as a function of the degree of relaxation. We find that while the barrier-height distribution, calculated from the initial minimum, is a unique function that depends only on the level of distribution, the reverse-barrier height distribution, calculated from the final state, is independent of the relaxation, following a different function. Moreover, the resulting gained or released energy distribution is a simple convolution of these two distributions indicating that the activation and relaxation parts of a the elementary relaxation mechanism are completely independent. This characterized energy landscape can be used to explain nano-calorimetry measurements.Comment: 5 pages, 4 figure

The Kinetic Activation-Relaxation Technique: A Powerful Off-lattice On-the-fly Kinetic Monte Carlo Algorithm

Many materials science phenomena, such as growth and self-organisation, are dominated by activated diffusion processes and occur on timescales that are well beyond the reach of standard-molecular dynamics simulations. Kinetic Monte Carlo (KMC) schemes make it possible to overcome this limitation and achieve experimental timescales. However, most KMC approaches proceed by discretizing the problem in space in order to identify, from the outset, a fixed set of barriers that are used throughout the simulations, limiting the range of problems that can be addressed. Here, we propose a more flexible approach -- the kinetic activation-relaxation technique (k-ART) -- which lifts these constraints. Our method is based on an off-lattice, self-learning, on-the-fly identification and evaluation of activation barriers using ART and a topological description of events. The validity and power of the method are demonstrated through the study of vacancy diffusion in crystalline silicon.Comment: 5 pages, 4 figure

Traveling through potential energy landscapes of disordered materials: the activation-relaxation technique

A detailed description of the activation-relaxation technique (ART) is presented. This method defines events in the configurational energy landscape of disordered materials, such as a-Si, glasses and polymers, in a two-step process: first, a configuration is activated from a local minimum to a nearby saddle-point; next, the configuration is relaxed to a new minimum; this allows for jumps over energy barriers much higher than what can be reached with standard techniques. Such events can serve as basic steps in equilibrium and kinetic Monte Carlo schemes.Comment: 7 pages, 2 postscript figure

Event-based relaxation of continuous disordered systems

A computational approach is presented to obtain energy-minimized structures in glassy materials. This approach, the activation-relaxation technique (ART), achieves its efficiency by focusing on significant changes in the microscopic structure (events). The application of ART is illustrated with two examples: the structure of amorphous silicon, and the structure of Ni80P20, a metallic glass.Comment: 4 pages, revtex, epsf.sty, 3 figure

Structural, electronic, and dynamical properties of amorphous gallium arsenide: a comparison between two topological models

We present a detailed study of the effect of local chemical ordering on the structural, electronic, and dynamical properties of amorphous gallium arsenide. Using the recently-proposed ``activation-relaxation technique'' and empirical potentials, we have constructed two 216-atom tetrahedral continuous random networks with different topological properties, which were further relaxed using tight-binding molecular dynamics. The first network corresponds to the traditional, amorphous, Polk-type, network, randomly decorated with Ga and As atoms. The second is an amorphous structure with a minimum of wrong (homopolar) bonds, and therefore a minimum of odd-membered atomic rings, and thus corresponds to the Connell-Temkin model. By comparing the structural, electronic, and dynamical properties of these two models, we show that the Connell-Temkin network is energetically favored over Polk, but that most properties are little affected by the differences in topology. We conclude that most indirect experimental evidence for the presence (or absence) of wrong bonds is much weaker than previously believed and that only direct structural measurements, i.e., of such quantities as partial radial distribution functions, can provide quantitative information on these defects in a-GaAs.Comment: 10 pages, 7 ps figures with eps

Short synthesis of oxetane and azetidine 3-Aryl-3-carboxylic acid derivatives by selective Furan oxidative cleavage

4-Membered rings remain under explored motifs despite offering attractive physicochemical properties for medicinal chemistry. Arylacetic acids bearing oxetanes, azetidines and cyclobutanes are prepared in two steps: a catalytic Friedel–Crafts reaction from 4-membered ring alcohol substrates, followed by mild oxidative cleavage. The suitability of the products as building blocks is reflected in their facile purification and amenability to derivatization. Examples include heteroaromatics and aryltriflates, as well as oxetane-derived profen drug analogues and a new endomorphin derivative containing an azetidine amino acid residue

Accuracy and Efficiency of a Coupled Neutronics and Thermal Hydraulics Model

The accuracy requirements for modern nuclear reactor simulation are steadily increasing due to the cost and regulation of relevant experimental facilities. Because of the increase in the cost of experiments and the decrease in the cost of simulation, simulation will play a much larger role in the design and licensing of new nuclear reactors. Fortunately as the work load of simulation increases, there are better physics models, new numerical techniques, and more powerful computer hardware that will enable modern simulation codes to handle the larger workload. This manuscript will discuss a numerical method where the six equations of two-phase flow, the solid conduction equations, and the two equations that describe neutron diffusion and precursor concentration are solved together in a tightly coupled, nonlinear fashion for a simplified model of a nuclear reactor core. This approach has two important advantages. The first advantage is a higher level of accuracy. Because the equations are solved together in a single nonlinear system, the solution is more accurate than the traditional “operator split” approach where the two-phase flow equations are solved first, the heat conduction is solved second and the neutron diffusion is solved third, limiting the temporal accuracy to 1st order because the nonlinear coupling between the physics is handled explicitly. The second advantage of the method described in this manuscript is that the time step control in the fully implicit system can be based on the timescale of the solution rather than a stability-based time step restriction like the material Courant. Results are presented from a simulated control rod movement and a rod ejection that address temporal accuracy for the fully coupled solution and demonstrate how the fastest timescale of the problem can change between the state variables of neutronics, conduction and two-phase flow during the course of a transient

Extended Forward Sensitivity Analysis for Uncertainty Quantification

Verification and validation (V&V) are playing more important roles to quantify uncertainties and realize high fidelity simulations in engineering system analyses, such as transients happened in a complex nuclear reactor system. Traditional V&V in the reactor system analysis focused more on the validation part or did not differentiate verification and validation. The traditional approach to uncertainty quantification is based on a 'black box' approach. The simulation tool is treated as an unknown signal generator, a distribution of inputs according to assumed probability density functions is sent in and the distribution of the outputs is measured and correlated back to the original input distribution. The 'black box' method mixes numerical errors with all other uncertainties. It is also not efficient to perform sensitivity analysis. Contrary to the 'black box' method, a more efficient sensitivity approach can take advantage of intimate knowledge of the simulation code. In these types of approaches equations for the propagation of uncertainty are constructed and the sensitivities are directly solved for as variables in the simulation. This paper presents the forward sensitivity analysis as a method to help uncertainty qualification. By including time step and potentially spatial step as special sensitivity parameters, the forward sensitivity method is extended as one method to quantify numerical errors. Note that by integrating local truncation errors over the whole system through the forward sensitivity analysis process, the generated time step and spatial step sensitivity information reflect global numerical errors. The discretization errors can be systematically compared against uncertainties due to other physical parameters. This extension makes the forward sensitivity method a much more powerful tool to help uncertainty qualification. By knowing the relative sensitivity of time and space steps with other interested physical parameters, the simulation is allowed to run at optimized time and space steps without affecting the confidence of the physical parameter sensitivity results. The time and space steps forward sensitivity analysis method can also replace the traditional time step and grid convergence study with much less computational cost. Several well defined benchmark problems with manufactured solutions are utilized to demonstrate the extended forward sensitivity analysis method. All the physical solutions, parameter sensitivity solutions, even the time step sensitivity in one case, have analytical forms, which allows the verification to be performed in the strictest sense