Search NASA⌕ Search

SEARCH · Search NASA

Results for “surface perturbation theory”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Adjoint-based constant-mass partial derivatives

In transport theory, adjoint-based partial derivatives with respect to mass density are constant-volume derivatives. Likewise, adjoint-based partial derivatives with respect to surface locations (i.e., internal interface locations and the outer system boundary) are constant-density derivatives. This study derives the constant-mass partial derivative of a response with respect to an internal interface location or the outer system boundary and the constant-mass partial derivative of a response with respect to the mass density of a region. Numerical results are given for a multiregion two-dimensional (r-z) cylinder for three very different responses: the uncollided gamma-ray flux at an external detector point, k eff of the system, and the total neutron leakage. Finally, results from the derived formulas compare extremely well with direct perturbation calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Second order classical perturbation theory for atom surface scattering: Analysis of asymmetry in the angular distribution

A second order classical perturbation theory is developed and applied to elastic atom corrugated surface scattering. The resulting theory accounts for experimentally observed asymmetry in the final angular distributions. These include qualitative features, such as reduction of the asymmetry in the intensity of the rainbow peaks with increased incidence energy as well as the asymmetry in the location of the rainbow peaks with respect to the specular scattering angle. The theory is especially applicable to “soft” corrugated potentials. Expressions for the angular distribution are derived for the exponential repulsive and Morse potential models. The theory is implemented numerically to a simplified model of the scattering of an Ar atom from a LiF(100) surface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Second order classical perturbation theory for the sticking probability of heavy atoms scattered on surfaces

A second order classical perturbation theory is developed to calculate the sticking probability of a particle scattered from an uncorrugated thermal surface. An analytic expression for the temperature dependent energy loss of the particle to the surface is derived by employing a one-dimensional generalized Langevin equation. The surface temperature reduces the energy loss, since the thermal surface transfers energy to the particle. Using a Gaussian energy loss kernel and the multiple collision theory of Fan and Manson [J. Chem. Phys. 130, 064703 (2009)], enables the determination of the fraction of particles trapped on the surface after subsequent momentum reversals of the colliding particle. This then leads to an estimate of the trapping probability. The theory is tested for the model scattering of Ar on a LiF(100) surface. Comparison with numerical simulations shows excellent agreement of the analytical theory with simulations, provided that the energy loss is determined by the second order perturbation theory.

36 MATERIALS SCIENCE↗
DOE OSTI2015

High precision quantum-chemical treatment of adsorption: Benchmarking physisorption of molecular hydrogen on graphane

A multilevel hierarchical ab initio protocol for calculating adsorption on non-conducting surfaces is presented. It employs fully periodic treatment, which reaches local Møller-Plesset perturbation theory of second order (MP2) with correction for the basis set incompleteness via the local F12 technique. Post-MP2 corrections are calculated using finite clusters. That includes the coupled cluster treatment in the local and canonical frameworks (up to perturbative quadruples) and correlated core (with MP2). Using this protocol, the potential surface of hydrogen molecules adsorbed on graphane was computed. According to the calculations, hydrogen molecules are adsorbed on graphane in a perpendicular to the surface orientation with the minimum of the potential surface of around −3.6 kJ/mol located at the distance of 3.85 Å between the bond center of the hydrogen molecule and the mid-plane of graphane. The adsorption sites along the path from the downward-pointing carbon to the ring center of the graphane are energetically virtually equally preferable, which can enable nearly free translations of hydrogen molecules along these paths. Consequently, the hydrogen molecules on graphane most likely form a non-commensurate monolayer. The analysis of the remaining errors reveals a very high accuracy of the computed potential surface with an error bar of a few tenths of a kJ/mol. The obtained results are a high-precision benchmark for further theoretical and experimental studies of hydrogen molecules interacting with graphane.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Effect of chaos on plasma filament dynamics and turbulence in the scrape-off layer

Naturally occurring error fields as well as resonant magnetic perturbations applied for stability control are known to cause magnetic field-line chaos in the scrape-off layer (SOL) region of tokamaks. Here, 2D simulations with the BOUT++ simulation framework are used to investigate the effect of the field-line chaos on the SOL and in particular on its width and peak particle flux. The chaos enters the SOL dynamics only through the connection length, which is evaluated using a Poincaré map. The variation of experimentally relevant quantities, such as the SOL gradient length scale and the intermittency of the particle flux in the SOL, is described as a function of the strength of the magnetic perturbation. It is found that the effect of the chaos is to broaden the profile of the sheath-loss coefficient, which is proportional to the inverse connection length. That is, the SOL transport in a chaotic field is equivalent to that in a model where the sheath-loss coefficient is replaced by its average over the unperturbed flux surfaces. The model does not include the effects of chaotic features other than the parallel connection length.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

Delineating the magnetic field line escape pattern and stickiness in a poloidally diverted tokamak

We analyze a Hamiltonian model with five wire loops that delineates magnetic surfaces of tokamaks with poloidal divertor. Non-axisymmetric magnetic perturbations are added by external coils, similar to the correction coils that have been installed or designed in present tokamaks. To show the influence of magnetic perturbations on the field line escape, we integrate numerically the field line differential equations and obtain the footprints and deposition patterns on the divertor plate. Moreover, we show that the homoclinic tangle describes the deposition patterns in the divertor plate, agreeing with results observed in sophisticated simulation codes. Additionally, we show that while chaotic lines escape to the divertor plates, some of them are trapped, for many toroidal turns, in complex structures around magnetic islands, embedded in the chaotic region, giving rise to stickiness evidences characteristic of chaotic Hamiltonian systems. Finally, we introduce a random collisional term to the field line mapping to investigate stickiness alterations due to particle collisions. Within this model, we conclude that, even reduced by collisions, the observed trapping still influences the field line transport. The results obtained for our numerical estimations indicate that the reported trapping may affect the transport in present tokamaks.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Vibrational energies for HFCO using a neural network sum of exponentials potential energy surface

A six-dimensional potential energy surface (PES) for formyl fluoride (HFCO) is fit in a sum-of-products form using neural network exponential fitting functions. The ab initio data upon which the fit is based were computed at the explicitly correlated coupled cluster with single, double, and perturbative triple excitations [CCSD(T)-F12]/cc-pVTZ-F12 level of theory. The PES fit is accurate (RMSE = 10 cm{sup −1}) up to 10 000 cm{sup −1} above the zero point energy and covers most of the experimentally measured IR data. The PES is validated by computing vibrational energies for both HFCO and deuterated formyl fluoride (DFCO) using block improved relaxation with the multi-configuration time dependent Hartree approach. The frequencies of the fundamental modes, and all other vibrational states up to 5000 cm{sup −1} above the zero-point energy, are more accurate than those obtained from the previous MP2-based PES. The vibrational frequencies obtained on the PES are compared to anharmonic frequencies at the MP2/aug-cc-pVTZ and CCSD(T)/aug-cc-pVTZ levels of theory obtained using second-order vibrational perturbation theory. The new PES will be useful for quantum dynamics simulations for both HFCO and DFCO, e.g., studies of intramolecular vibrational redistribution leading to unimolecular dissociation and its laser control.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

The interaction between hexagonal boron nitride and water from first principles

The use of hexagonal boron nitride (h-BN) in microfluidic and nanofluidic applications requires a fundamental understanding of the interaction between water and the h-BN surface. A crucial component of the interaction is the binding energy, which is sensitive to the treatment of electron correlation. In this work, we use state of the art quantum Monte Carlo and quantum chemistry techniques to compute the binding energy. Compared to high-level many-body theory, we found that the second-order Møller-Plesset perturbation theory captures the interaction accurately and can thus be used to develop force field parameters between h-BN and water for use in atomic scale simulations. On the contrary, density functional theory with standard dispersion corrections tends to overestimate the binding energy by approximately 75%.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2013

The 'virtual density' principle of neutronics: Toward rapid computation of reactivity effects in practical core distortion scenarios

Fast reactor core reactivities are sensitive to geometric distortions arising from three distinct phenomena: (1) irradiation swelling of fuel throughout core lifetime, (2) thermal expansion of fuel during transients, and (3) mechanical oscillations during seismic events. Performing comprehensive reactivity analysis of these distortions requires methods for rapidly computing a multitude of minute reactivity changes. Thus, we introduce the 'virtual density' principle of neutronics as a new perturbation technique to achieve this rapid computation. This new method obviates many of the most challenging aspects of conventional geometric perturbation theory. Essentially, this 'virtual density' principle converts geometric perturbations into equivalent material density perturbations (either isotropic or anisotropic), which are highly accurate and comparatively simple to evaluate. While traditional boundary perturbation theory employs surface integrals, the 'virtual density' principle employs equivalent volume integrals. We introduce and validate this method in three subsequent stages: (1) isotropic 'virtual density', (2) anisotropic 'virtual density' for whole cores, and (3) anisotropic 'virtual density' for interior zones within cores. We numerically demonstrate its accuracy for 2-D core flowering scenarios. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2015

Investigation of finite-size effects in chemical bonding of AuPd nanoalloys

In this paper, the size-dependent changes in energetic, vibrational, and electronic properties of C–O gas molecule interacting with surface Pd atom of a variety of AuPd nanoalloy structures are investigated by means of first principles calculations. The variation in C–O adsorption energies, C–O vibration frequencies (ν{sub C−O}), and Pd d-bond centers (ε{sub d}) on a series of non-supported Au{sub n−1}–Pd{sub 1} nanoparticles (with n varying from 13 to 147) and on two semi-finite surfaces are inspected with cluster size. We demonstrate for the first time that, with small AuPd bimetallic three-dimensional clusters as TOh{sub 38}, one can reach cluster size convergence even for such a sensitive observable as the adsorption energy on a metal surface. Indeed, the results show that the adsorbate-induced perturbation is extremely local and it only concerns the isolated Pd interacting with the reactive gas molecule. Except for 13 atom clusters, in which molecular behaviour is predominant, no finite-size effects are observed for surface Pd atom substituted in AuPd free nanoclusters above 38 atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Detection of the adsorption of water monolayers through the ion oscillation frequency in the magnesium oxide lattice by means of low energy electron diffraction

We investigate the variation of the oscillation frequency of the Mg{sup 2+} and O{sup 2−} ions in the magnesium oxide lattice due to the interactions of the surface with water monolayers by means of Low Energy Electron Diffraction. Our key result is a new technique to determine the adsorbate vibrations produced by the water monolayers on the surface lattice as a consequence of their change in the surface Debye temperature and its chemical shift. The latter was systematically investigated for different annealing times and for a constant external thermal perturbation in the range of 110–300 K in order to accomplish adsorption or desorption of water monolayers in the surface lattice.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Long-range spatial correlations in the turbulent edge plasma of the L-2M stellarator

Long-range spatial correlations in the turbulent plasma of the L-2M stellarator were revealed experimentally, and their relation to the geometry of magnetic surfaces was analyzed (Plasma Phys. Control. Fusion 50, 045001 (2008)). The operation modes of the facility in which fast transport transitions in plasma are possible were studied. Upon these transitions, the turbulence level is found to decrease substantially. It is shown that long-range spatial correlations are typical of relatively narrow frequency ranges. In particular, before a transport transition, such frequency ranges are f ∼ 30–40 kHz and f ∼ 1–3 kHz. After the transition, long-range spatial correlations in the frequency range of f ∼ 30–40 kHz disappear due to a significant decrease in the turbulence level in this frequency range. At the same time, correlations in the low frequency range are retained and new correlations at frequencies of f ∼ 6-12 kHz occur. It is found that global electromagnetic oscillations in the frequency range of f ∼ 1–3 kHz are related to the m/n = 0/0 perturbation and its toroidal satellites (here, m and n are the poloidal and toroidal mode numbers, respectively). It is also shown that, after the transport transition, a three-dimensional localized electromagnetic mode at the frequency of the geodesic acoustic mode governed by the average magnetic field curvature is excited. At higher frequencies typical of a geodesic acoustic mode related to the three-dimensional curvature of the magnetic field, no long-range spatial correlations were observed both before and after the transport transition.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Surface states in a 3D topological insulator: The role of hexagonal warping and curvature

We explore a combined effect of hexagonal warping and a finite effective mass on both the tunneling density of electronic surface states and the structure of Landau levels of 3D topological insulators. We find the increasing warping to transform the square-root van Hove singularity into a logarithmic one. For moderate warping, an additional logarithmic singularity and a jump in the tunneling density of surface states appear. By combining the perturbation theory and the WKB approximation, we calculate the Landau levels in the presence of hexagonal warping. We predict that due to the degeneracy removal, the evolution of Landau levels in the magnetic field is drastically modified.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Semiclassical multi-phonon theory for atom-surface scattering: Application to the Cu(111) system

The semiclassical perturbation theory of Hubbard and Miller [J. Chem. Phys. 80, 5827 (1984)] is further developed to include the full multi-phonon transitions in atom-surface scattering. A practically applicable expression is developed for the angular scattering distribution by utilising a discretized bath of oscillators, instead of the continuum limit. At sufficiently low surface temperature good agreement is found between the present multi-phonon theory and the previous one-, and two-phonon theory derived in the continuum limit in our previous study [Daon, Pollak, and Miret-Artés, J. Chem. Phys. 137, 201103 (2012)]. The theory is applied to the measured angular distributions of Ne, Ar, and Kr scattered from a Cu(111) surface. We find that the present multi-phonon theory substantially improves the agreement between experiment and theory, especially at the higher surface temperatures. This provides evidence for the importance of multi-phonon transitions in determining the angular distribution as the surface temperature is increased.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Post-Hartree-Fock studies of the He/Mg(0001) interaction: Anti-corrugation, screening, and pairwise additivity

The adsorption of noble gases on metallic surfaces represents a paradigmatic case of van-der-Waals (vdW) interaction due to the role of screening effects on the corrugation of the interaction potential [J. L. F. Da Silva et al., Phys. Rev. Lett. 90, 066104 (2003)]. The extremely small adsorption energy of He atoms on the Mg(0001) surface (below 3 meV) and the delocalized nature and mobility of the surface electrons make the He/Mg(0001) system particularly challenging, even for state-of-the-art vdW-corrected density functional-based (vdW-DFT) approaches [M. P. de Lara-Castells et al., J. Chem. Phys. 143, 194701 (2015)]. In this work, we meet this challenge by applying two different procedures. First, the dispersion-corrected second-order Möller-Plesset perturbation theory (MP2C) approach is adopted, using bare metal clusters of increasing size. Second, the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)] is applied at coupled cluster singles and doubles and perturbative triples level, using embedded cluster models of the metal surface. Both approaches provide clear evidences of the anti-corrugation of the interaction potential: the He atom prefers on-top sites, instead of the expected hollow sites. This is interpreted as a signature of the screening of the He atom by the metal for the on-top configuration. The strong screening in the metal is clearly reflected in the relative contribution of successively deeper surface layers to the main dispersion contribution. Aimed to assist future dynamical simulations, a pairwise potential model for the He/surface interaction as a sum of effective He–Mg pair potentials is also presented, as an improvement of the approximation using isolated He–Mg pairs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Electronic structure of an anticancer drug DC81 and its interaction with DNA base pairs

The drug, 8-Hydroxy-7-methoxy-pyrrolo-[2,1-c][1,4] benzodiazepine-5-one, commonly christened as DC81 belongs to the pyrrolo-[2,1-c][1,4]benzodiazepine (PBDs) family. It is a member of the group of naturally occurring antitumour antibiotics produced by various Streptomyces species. The antitumour activity of DC81 is attributed to its sequence specific interaction with G-C rich DNA region in particular, for Pu-G-Pu motifs. In the present paper, physico-chemical properties DC81 have been carried out using an ab-initio method, HF/6-31G(d,p) with GAMESS program. MEP, HOMO and LUMO surfaces have been scanned. Ionization potential, electron affinity, electronegativity, global hardness and softness of the drug have been calculated. Further, drug-DNA interactions have been examined using modified second order perturbation theory along with multicentred-multipole expansion technique. Results have been discussed in the light of other theoretical and experimental observations. Efforts have been made to elucidate the binding patterns and thereby biological properties of the drug.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Dynamic Instability of Solid Surfaces under Load

The mechanism of dynamic instability of a solid surface under a load, determined by perturbations of the electron density and the change in the interatomic interaction, is considered. This instability is manifested upon the excitation of dynamic displacements of atoms in the surface layer, which can lead to formation of finite-lifetime structures in the form of waves with a large amplitude. Such structures were earlier observed experimentally on a stretched germanium (111) surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗