Pressure-induced isostructural phase transition of metal-doped silicon clathrates

We propose an atomistic model for the pressure-induced isostructural phase transition of metal-doped silicon clathrates, Ba8Si46 and K8Si46, that has been observed at 14 GPa and 23 GPa, respectively. The model explains successfully the equation of state, transition pressure, change of Raman spectra and dependence on the doped cations as well as the effects of substituting Si(6c) atoms with noble metals.Comment: 5 pages, two coumn, 5 figures. See http://www.iitaka.org/down.html for more informatio

Stability, Adsorption and Diffusion of CH4, CO2 and H2 in Clathrate Hydrates

We present a study of the adsorption and diffusion of CH4, CO2 and H2 molecules in clathrate hydrates using ab initio van der Waals density functional formalism [Dion et al. Phys. Rev. Lett. 92, 246401 (2004)]. We find that the adsorption energy is dominated by van der Waals interactions and that, without them, gas hydrates would not be stable. We calculate the maximum adsorption capacity as well as the maximum hydrocarbon size that can be adsorbed.The relaxation of the host lattice is essential for a good description of the diffusion activation energies, which are estimated to be of the order of 0.2, 0.4, and 1.0 eV for H2, CO2, and CH4, respectively.Comment: 4 pages, 4 figures, 3 table

Adaptive Multidimensional Integration Based on Rank-1 Lattices

Quasi-Monte Carlo methods are used for numerically integrating multivariate functions. However, the error bounds for these methods typically rely on a priori knowledge of some semi-norm of the integrand, not on the sampled function values. In this article, we propose an error bound based on the discrete Fourier coefficients of the integrand. If these Fourier coefficients decay more quickly, the integrand has less fine scale structure, and the accuracy is higher. We focus on rank-1 lattices because they are a commonly used quasi-Monte Carlo design and because their algebraic structure facilitates an error analysis based on a Fourier decomposition of the integrand. This leads to a guaranteed adaptive cubature algorithm with computational cost $O(mb^m)$, where $b$ is some fixed prime number and $b^m$ is the number of data points

Force and energy dissipation variations in non-contact atomic force spectroscopy on composite carbon nanotube systems

UHV dynamic force and energy dissipation spectroscopy in non-contact atomic force microscopy were used to probe specific interactions with composite systems formed by encapsulating inorganic compounds inside single-walled carbon nanotubes. It is found that forces due to nano-scale van der Waals interaction can be made to decrease by combining an Ag core and a carbon nanotube shell in the Ag@SWNT system. This specific behaviour was attributed to a significantly different effective dielectric function compared to the individual constituents, evaluated using a simple core-shell optical model. Energy dissipation measurements showed that by filling dissipation increases, explained here by softening of C-C bonds resulting in a more deformable nanotube cage. Thus, filled and unfilled nanotubes can be discriminated based on force and dissipation measurements. These findings have two different implications for potential applications: tuning the effective optical properties and tuning the interaction force for molecular absorption by appropriately choosing the filling with respect to the nanotube.Comment: 22 pages, 6 figure

On the thermodynamic stability and structural transition of clathrate hydrates

Gas mixtures of methane and ethane form structure II clathrate hydrates despite the fact that each of pure methane and pure ethane gases forms the structure I hydrate. Optimization of the interaction potential parameters for methane and ethane is attempted so as to reproduce the dissociation pressures of each simple hydrate containing either methane or ethane alone. An account for the structural transitions between type I and type II hydrates upon changing the mole fraction of the gas mixture is given on the basis of the van der Waals and Platteeuw theory with these optimized potentials. Cage occupancies of the two kinds of hydrates are also calculated as functions of the mole fraction at the dissociation pressure and at a fixed pressure well above the dissociation pressure

The Nystrom plus Correction Method for Solving Bound State Equations in Momentum Space

A new method is presented for solving the momentum-space Schrodinger equation with a linear potential. The Lande-subtracted momentum space integral equation can be transformed into a matrix equation by the Nystrom method. The method produces only approximate eigenvalues in the cases of singular potentials such as the linear potential. The eigenvalues generated by the Nystrom method can be improved by calculating the numerical errors and adding the appropriate corrections. The end results are more accurate eigenvalues than those generated by the basis function method. The method is also shown to work for a relativistic equation such as the Thompson equation.Comment: Revtex, 21 pages, 4 tables, to be published in Physical Review

Growth and Structure of Stochastic Sequences

We introduce a class of stochastic integer sequences. In these sequences, every element is a sum of two previous elements, at least one of which is chosen randomly. The interplay between randomness and memory underlying these sequences leads to a wide variety of behaviors ranging from stretched exponential to log-normal to algebraic growth. Interestingly, the set of all possible sequence values has an intricate structure.Comment: 4 pages, 4 figure

CASSIS: The Cornell Atlas of Spitzer/Infrared Spectrograph Sources. II. High-resolution observations

The Infrared Spectrograph (IRS) on board the Spitzer Space Telescope observed about 15,000 objects during the cryogenic mission lifetime. Observations provided low-resolution (R~60-127) spectra over ~5-38um and high-resolution (R~600) spectra over ~10-37um. The Cornell Atlas of Spitzer/IRS Sources (CASSIS) was created to provide publishable quality spectra to the community. Low-resolution spectra have been available in CASSIS since 2011, and we present here the addition of the high-resolution spectra. The high-resolution observations represent approximately one third of all staring observations performed with the IRS instrument. While low-resolution observations are adapted to faint objects and/or broad spectral features (e.g., dust continuum, molecular bands), high-resolution observations allow more accurate measurements of narrow features (e.g., ionic emission lines) as well as a better sampling of the spectral profile of various features. Given the narrow aperture of the two high-resolution modules, cosmic ray hits and spurious features usually plague the spectra. Our pipeline is designed to minimize these effects through various improvements. A super sampled point-spread function was created in order to enable the optimal extraction in addition to the full aperture extraction. The pipeline selects the best extraction method based on the spatial extent of the object. For unresolved sources, the optimal extraction provides a significant improvement in signal-to-noise ratio over a full aperture extraction. We have developed several techniques for optimal extraction, including a differential method that eliminates low-level rogue pixels (even when no dedicated background observation was performed). The updated CASSIS repository now includes all the spectra ever taken by the IRS, with the exception of mapping observations