Toward Fully Quantum Modelling of Ultrafast Photodissociation Imaging Experiments. Treating Tunnelling in the Ab Initio Multiple Cloning Approach

We present an account of our recent effort to improve simulation of the photodissociation of small heteroaromatic molecules using the Ab Initio Multiple Cloning (AIMC) algorithm. The ultimate goal is to create a quantitative and converged technique for fully quantum simulations which treats both electrons and nuclei on a fully quantum level. We calculate and analyse the total kinetic energy release (TKER) spectra and Velocity Map Images (VMI), and compare the results directly with experimental measurements. In this work, we perform new extensive calculations using an improved AIMC algorithm that now takes into account the tunnelling of hydrogen atoms. This can play an extremely important role in photodissociation dynamics

Relativistic Images in Randall-Sundrum II Braneworld Lensing

In this paper, we explore the properties of gravitational lensing by black holes in the Randall-Sundrum II braneworld. We use numerical techniques to calculate lensing observables using the Tidal Reissner-Nordstrom (TRN) and Garriga-Tanaka metrics to examine supermassive black holes and primordial black holes. We introduce a new way tp parameterize tidal charge in the TRN metric which results in a large increase in image magnifications for braneworld primordial black holes compared to their 4 dimensional analogues. Finally, we offer a mathematical analysis that allows us to analyze the validity of the logarithmic approximation of the bending angle for any static, spherically symmetric metric. We apply this to the TRN metric and show that it is valid for any amount of tidal charge.Comment: 13 pages, 3 figures; Accepted for Publication in Physical Review

Atomic spectral-product representations of molecular electronic structure: metric matrices and atomic-product composition of molecular eigenfunctions

Recent progress is reported in development of ab initio computational methods for the electronic structures of molecules employing the many-electron eigenstates of constituent atoms in spectral-product forms. The approach provides a universal atomic-product description of the electronic structure of matter as an alternative to more commonly employed valence-bond- or molecular-orbital-based representations. The Hamiltonian matrix in this representation is seen to comprise a sum over atomic energies and a pairwise sum over Coulombic interaction terms that depend only on the separations of the individual atomic pairs. Overall electron antisymmetry can be enforced by unitary transformation when appropriate, rather than as a possibly encumbering or unnecessary global constraint. The matrix representative of the antisymmetrizer in the spectral-product basis, which is equivalent to the metric matrix of the corresponding explicitly antisymmetric basis, provides the required transformation to antisymmetric or linearly independent states after Hamiltonian evaluation. Particular attention is focused in the present report on properties of the metric matrix and on the atomic-product compositions of molecular eigenstates as described in the spectral-product representations. Illustrative calculations are reported for simple but prototypically important diatomic (H_2, CH) and triatomic (H_3, CH_2) molecules employing algorithms and computer codes devised recently for this purpose. This particular implementation of the approach combines Slater-orbital-based one- and two-electron integral evaluations, valence-bond constructions of standard tableau functions and matrices, and transformations to atomic eigenstate-product representations. The calculated metric matrices and corresponding potential energy surfaces obtained in this way elucidate a number of aspects of the spectral-product development, including the nature of closure in the representation, the general redundancy or linear dependence of its explicitly antisymmetrized form, the convergence of the apparently disparate atomic-product and explicitly antisymmetrized atomic-product forms to a common invariant subspace, and the nature of a chemical bonding descriptor provided by the atomic-product compositions of molecular eigenstates. Concluding remarks indicate additional studies in progress and the prognosis for performing atomic spectral-product calculations more generally and efficiently

Strong Gravitational Lensing by Sgr A*

In recent years, there has been increasing recognition of the potential of the galactic center as a probe of general relativity in the strong field. There is almost certainly a black hole at Sgr A* in the galactic center, and this would allow us the opportunity to probe dynamics near the exterior of the black hole. In the last decade, there has been research into extreme gravitational lensing in the galactic center. Unlike in most applications of gravitational lensing, where the bending angle is of the order of several arc seconds, very large bending angles are possible for light that closely approaches a black hole. Photons may even loop multiple times around a black hole before reaching the observer. There have been many proposals to use light's close approach to the black hole as a probe of the black hole metric. Of particular interest is the property of light lensed by the S stars orbiting in the galactic center. This paper will review some of the attempts made to study extreme lensing as well as extend the analysis of lensing by S stars. In particular, we are interested in the effect of a Reissner-Nordstrom like 1/r^2 term in the metric and how this would affect the properties of relativistic images.Comment: 13 pages, 9 figures. Submitted as invited review article for the GR19 issue of CQ

Particle breakage criteria in discrete-element modelling

Previous work by the authors, using the discrete element method (DEM) has used the octahedral shear stress within a sphere together with a Weibull distribution of strengths and a size effect on average strength, to determine whether fracture occurs or not. This leads to fractal particle size distributions and a normal compression line which are consistent with experimental data. However there is no agreement in the literature as to what the fracture criterion should be and as yet it is not clear whether other criteria could lead to the correct evolution of voids ratio and particle size distribution under increasing stress. Various possibilities for the criterion have been studied in detail here to ascertain whether these other criteria may give the correct behaviour under normal compression. The use of the major principal stress within a particle, the mean stress, and the stress calculated from the maximum contact force on a particle are each investigated as alternatives to the octahedral shear stress. Only the criterion based on the maximum contact force is shown to give behaviour observed experimentally and the simulations shed further insight into the micro mechanics of normal compression

Modifications of comet materials by the sublimation process: Results from simulation experiments

An active comet like comet Halley loses by sublimation a surface layer of the order of 1 m thickness per perihelion passage. In situ measurements show that water ice is the main constituent which contributes to the gas emission although even more volatile species (CO, NH3, CH4, CO2 etc.) have been identified. Dust particles which were embedded in the ices are carried by the sublimating gases. Measurements of the chemical composition of cometary grains indicate that they are composed of silicates of approximate chondritic composition and refractory carbonaceous material. Comet simulation experiments show that significant modifications of cometary materials occur due to sublimation process in near surface layers which have to be taken into account in order to derive the original state of the material

Theoretical Spectra and Atmospheres of Extrasolar Giant Planets

We present a comprehensive theory of the spectra and atmospheres of irradiated extrasolar giant planets. We explore the dependences on stellar type, orbital distance, cloud characteristics, planet mass, and surface gravity. Phase-averaged spectra for specific known extrasolar giant planets that span a wide range of the relevant parameters are calculated, plotted, and discussed. The connection between atmospheric composition and emergent spectrum is explored in detail. Furthermore, we calculate the effect of stellar insolation on brown dwarfs. We review a variety of representative observational techniques and programs for their potential for direct detection, in light of our theoretical expectations, and we calculate planet-to-star flux ratios as a function of wavelength. Our results suggest which spectral features are most diagnostic of giant planet atmospheres and reveal the best bands in which to image planets of whatever physical or orbital characteristics.Comment: 47 pages, plus 36 postscript figures; with minor revisions, accepted to the Astrophysical Journal, May 10, 2003 issu

Outgassing of icy bodies in the solar system - I. The sublimation of hexagonal water ice through dust layers

Our knowledge about the physical processes determining the activity of comets were mainly influenced by several extremely successful space missions, the predictions of theoretical models and the results of laboratory experiments. However, novel computer models should not be treated in isolation but should be based on experimental results. Therefore, a new experimental setup was constructed to investigate the temperature dependent sublimation properties of hexagonal water ice and the gas diffusion through a dry dust layer covering the ice surface. We show that this experimental setup is capable to reproduce known gas production rates of pure hexagonal water ice. The reduction of the gas production rate due to an additional dust layer on top of the ice surface was measured and compared to the results of another experimental setup in which the gas diffusion through dust layers at room temperature was investigated. We found that the relative permeability of the dust layer is inversely proportional to its thickness, which is also predicted by theoretical models. However, the measured absolute weakening of the gas flow was smaller than predicted by models. This lack of correspondence between model and experiment may be caused by an ill-determination of the boundary condition in the theoretical models, which further demonstrates the necessity of laboratory investigations. Furthermore, the impedance of the dust layer to the ice evaporation was found to be similar to the impedance at room temperature, which means that the temperature profile of the dust layer is not influencing the reduction of the gas production. Finally, we present the results of an extended investigation of the sublimation coefficient, which is an important factor for the description of the sublimation rate of water ice and, thus, an important value for thermophysical modeling of icy bodies in the solar system.Comment: Submitted to Icaru

Albedo and Reflection Spectra of Extrasolar Giant Planets

We generate theoretical albedo and reflection spectra for a full range of extrasolar giant planet (EGP) models, from Jovian to 51-Pegasi class objects. Our albedo modeling utilizes the latest atomic and molecular cross sections, a Mie theory treatment of extinction by condensates, a variety of particle size distributions, and an extension of the Feautrier radiative transfer method which allows for a general treatment of the scattering phase function. We find that due to qualitative similarities in the compositions and spectra of objects within each of five broad effective temperature ranges, it is natural to establish five representative EGP albedo classes: a ``Jovian'' class (T$_{\rm eff} \lesssim 150$ K; Class I) with tropospheric ammonia clouds, a ``water cloud'' class (T$_{\rm eff} \sim 250$ K; Class II) primarily affected by condensed H$_2$O, a ``clear'' class (T$_{\rm eff} \gtrsim 350$ K; Class III) which lacks clouds, and two high-temperature classes: Class IV (900 K $\lesssim$ T$_{\rm{eff}}$ $\lesssim$ 1500 K) for which alkali metal absorption predominates, and Class V (T$_{\rm{eff}}$ $\gtrsim$ 1500 K and/or low surface gravity ($\lesssim$ 10$^3$ cm s$^{-2}$)) for which a high silicate layer shields a significant fraction of the incident radiation from alkali metal and molecular absorption. The resonance lines of sodium and potassium are expected to be salient features in the reflection spectra of Class III, IV, and V objects. We derive Bond albedos and effective temperatures for the full set of known EGPs and explore the possible effects of non-equilibrium condensed products of photolysis above or within principal cloud decks. As in Jupiter, such species can lower the UV/blue albedo substantially, even if present in relatively small mixing ratios.Comment: revised LaTeX manuscript accepted to Ap.J.; also available at http://jupiter.as.arizona.edu/~burrows/paper

The effects of methanol on the trapping of volatile ice components

The evaporation of icy mantles, which have been formed on the surface of dust grains, is acknowledged to give rise to the rich chemistry that has been observed in the vicinity of hot cores and corinos. It has long been established that water ice is the dominant species within many astrophysical ices. However, other molecules found within astrophysical ices, particularly methanol, can influence the desorption of volatile species from the ice. Here we present a detailed investigation of the adsorption and desorption of methanol-containing ices, showing the effect that methanol has on the trapping and release of volatiles from model interstellar ices. OCS and CO2 have been used as probe molecules since they have been suggested to reside in water-rich and methanol-rich environments. Experiments show that methanol fundamentally changes the desorption characteristics of both OCS and CO2, leading to the observation of mainly codesorption of both species with bulk water ice for the tertiary ices and causing a lowering of the temperature of the volcano component of the desorption. In contrast, binary ices are dominated by standard volcano desorption. This observation clearly shows that codepositing astrophysically relevant impurities with water ice, such as methanol, can alter the desorption dynamics of volatiles that become trapped in the pores of the amorphous water ice during the sublimation process. Incorporating experimental data into a simple model to simulate these processes on astrophysical timescales shows that the additional methanol component releases larger amounts of OCS from the ice mantle at lower temperatures and earlier times. These results are of interest to astronomers as they can be used to model the star formation process, hence giving information about the evolution of our Universe