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Results for “CONFIGURATION INTERACTION”

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.

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At least 865 records · Page 48
All sourcesNASA NTRSDOE OSTI
NASA NTRS2004

Numerical Investigation of Dual-Mode Scramjet Combustor with Large Upstream Interaction

Dual-mode scramjet combustor configuration with significant upstream interaction is investigated numerically, The possibility of scaling the domain to accelerate the convergence and reduce the computational time is explored. The supersonic combustor configuration was selected to provide an understanding of key features of upstream interaction and to identify physical and numerical issues relating to modeling of dual-mode configurations. The numerical analysis was performed with vitiated air at freestream Math number of 2.5 using hydrogen as the sonic injectant. Results are presented for two-dimensional models and a three-dimensional jet-to-jet symmetric geometry. Comparisons are made with experimental results. Two-dimensional and three-dimensional results show substantial oblique shock train reaching upstream of the fuel injectors. Flow characteristics slow numerical convergence, while the upstream interaction slowly increases with further iterations. As the flow field develops, the symmetric assumption breaks down. A large separation zone develops and extends further upstream of the step. This asymmetric flow structure is not seen in the experimental data. Results obtained using a sub-scale domain (both two-dimensional and three-dimensional) qualitatively recover the flow physics obtained from full-scale simulations. All results show that numerical modeling using a scaled geometry provides good agreement with full-scale numerical results and experimental results for this configuration. This study supports the argument that numerical scaling is useful in simulating dual-mode scramjet combustor flowfields and could provide an excellent convergence acceleration technique for dual-mode simulations.

Mohieldin, T. O.↗
DOE OSTI2021

Geometry and dynamics of passive scalar structures in compressible turbulent mixing

We present a structure-based numerical analysis of passive scalar mixing in decaying homogeneous isotropic turbulence (DHIT) and shock-turbulence interaction canonical configurations. The analysis focuses on the temporal evolution of ensembles of passive scalar structures, initialized as spheres of different sizes relative to the Taylor microscale. An algorithm is introduced to track the evolution of each individual structure and the interactions with other structures in the ensemble, relating changes in the surface geometry and the underlying physical processes (turbulent transport, scalar dissipation, and shock compression). The tracking algorithm is applied to datasets from shock-capturing direct numerical simulations of DHIT, with Taylor microscale Reynolds number Re λ =40 and turbulence Mach number M t =0.2 ⁠, and STI cases in which the turbulence is processed by a shock wave at Mach numbers M = 1.5 and 3.0. Temporal surface convolution increases for initially larger structures, resulting in a higher probability of locally hyperbolic geometries where breakup into smaller structures occurs. Shock-induced deformation of the structures amplifies breakup processes, enhancing mixing, particularly for larger structures. Mixing enhancement by the shock is manifested as an amplification of the surface-averaged scalar gradient, which increases for initially larger structures. The alignment between the scalar gradient and the most extensional strain-rate eigendirection on the scalar isosurfaces also increases across the shock. Larger magnitudes of the scalar gradient and its alignment with the most compressive strain-rate eigendirection correlate with flatter surface regions. Shock-induced structure compression increases the area coverage of flat regions, where the amplification of scalar gradient is localized.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1995

The global heliosphere: A parametric study

As the Pioneer 10 and 11 and Voyager 1 and 2 spacecraft continue their penetration into the outer heliosphere, more attention has been focused on the nature of the solar wind interaction with the Very Local Interstellar Medium (VLISM). Since the initial pioneering concepts of Davis in 1955 and Parker in the early 1960's both in situ and remote measurements have led to various constraints that do not fit well into a coherent picture. To provide a context for these various observable constraints, we have adapted an explicitly time-dependent, explicitly three-dimensional magnetohydrodynamic (MHD) code to simulate the dependence of the heliospheric configuration and interaction with the VLISM on the properties of the external medium. The code also allows us to study temporal variations brought about by both short- and long-term changes in the solar wind and/or VLISM properties. We will discuss some of the initial results from this new effort and implications for the distances inferred to the termination shock and heliopause boundary. In particular, we will consider the effect of the Very Local Interstellar Magnetic Field (VLIMF) on the configuration and compare it with inferences from observations of outer heliosphere cosmic rays and the Very Low Frequency (VLF) outer heliospheric radio emissions.

McNutt, R. L., Jr.↗
NASA NTRS2013

NO PLIF Visualizations of the Orion Capsule in LENS-I

Planar laser-induced fluorescence (PLIF) of nitric oxide (NO) was used to visualize the interaction of reaction-control-system (RCS) jet flows in the wake of a hypersonic capsule reentry vehicle. The tests were performed at the Calspan University at Buffalo Research Center's (CUBRC) LENS-I reflected shock tunnel facility. This was the first application of PLIF to study RCS jets in a large-scale pulsed hypersonic facility. The LENS-I facility allowed RCS jet flows to be studied while varying the flow enthalpy, Reynolds number, angle of attack and jet configuration. The interaction of pitch and roll jets with the flowfield was investigated. Additionally, thin film sensors were used to monitor heat transfer on the surface of the model to detect any localized heating resulting from the firing of the RCS jets. Tests were conducted with the model held at angles of attack of 18deg and 22deg. The nominal Mach number in all tests was 8, while Reynolds number based on model diameter ranged from 2.2x10(exp 6) - 1.5x10(exp 7). Images were processed using the Virtual Diagnostics Interface (ViDI) system developed at NASA Langley Research Center to provide a three-dimensional display of the experimental data.

Combs, C.↗
DOE OSTI2018

Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles

A density functional theory parameterized lattice gas cluster expansion of oxygen on an Fe(100) surface is developed in the presence and absence of an applied positive and negative external electric field, characterizing the heterogeneity in oxygen's surface distribution and the effect of an external electric field on the lateral interactions between the adsorbates. We show that the presence of a negative electric field tends to weaken both attractive and repulsive interactions while the positive electric field tends to strengthen these interactions, altering surface distributions and ground state configurations. Since lateral interactions have been shown to play a critical role in defining catalytic behavior, the application of an applied electric field has the potential to be a useful tool in adjusting critical chemical properties of Fe-based hydrodeoxygenation catalysts, by decreasing the repulsive interactions between the adspecies in the presence of a negative field and thereby mitigating the formation of an oxide.

Bray, Jacob E.↗
NASA NTRS1989

Feasibility study of vortex interaction control on a chine forebody/delta wing configuration at high angles of attack

The feasibility of controlling vortex interactions or merger on a blended chine forebody and delta wing configuration was experimentally investigated. Low-speed wind tunnel diagnostics using smoke visualizations and wing upper-surface pressure measurements were performed on a generic 60 deg delta and chine forebody model, to assess chine modifications and leading edge flaps. Both techniques were shown to promote uncoupled vortex flows at high angles of attack and sideslip, with significant influence on the wing flow field, indicating potential for alleviating adverse high-alpha characteristics of blended chine swept wing configurations.

Rao, Dhanvada M.↗
DOE OSTI2022

Piecewise interaction picture density matrix quantum Monte Carlo

The density matrix quantum Monte Carlo (DMQMC) set of methods stochastically samples the exact N-body density matrix for interacting electrons at finite temperature. We introduce a simple modification to the interaction picture DMQMC (IP-DMQMC) method that overcomes the limitation of only sampling one inverse temperature point at a time, instead allowing for the sampling of a temperature range within a single calculation, thereby reducing the computational cost. At the target inverse temperature, instead of ending the simulation, we incorporate a change of picture away from the interaction picture. The resulting equations of motion have piecewise functions and use the interaction picture in the first phase of a simulation, followed by the application of the Bloch equation once the target inverse temperature is reached. We find that the performance of this method is similar to or better than the DMQMC and IP-DMQMC algorithms in a variety of molecular test systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2022

The Turning Point of the Aerosol Era

Over the CMIP6 historical period (1850–2014), aerosols provided the largest negative forcing compared to all other climate forcings via their ability to absorb or scatter solar radiation and alter clouds. Aerosols played an important role in counterbalancing warming by greenhouse gases (GHGs). Here we study aerosol forcing trends in the CMIP6 simulations of the NASA Goddard Institute for Space Studies (GISS) ocean-atmosphere ModelE version 2.1 (GISS-E2.1-G) using a fully coupled atmospheric composition configuration, including interactive gas-phase chemistry, and either an aerosol microphysical (MATRIX) or a mass-based aerosol (OMA) module. Simulations of the CMIP6 historical period are analyzed as well as four Shared Socioeconomic Pathway (SSP) future scenarios for 2015–2100: SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5. The main conclusion of this study is that aerosol forcing in the GISS model has reached its turning point, switching from globally increasing to a decreasing trend in the first decade of the 21st century. This result is robust, independent of which aerosol module or SSP scenario is used. Non-linear aerosol-cloud interactions dominate as a forcing agent over aerosol-radiation interactions. Aerosols' ability to counterbalance GHG forcing on the global scale is today at a level comparable to that at the beginning of the last century. In the 1980s, the decade of largest global aerosol loads, aerosols balanced up to 80% of GHG forcing. As a consequence, global warming of the last decades, which is primarily driven by greenhouse gases, has been augmented by the effect of decreasing aerosol cooling in our model. By the end of this century, following the SSP scenarios, aerosols will only counterbalance 0%–20% of GHG forcing, depending on model and on scenario.

Aerosol forcing↗
DOE OSTI2016

Relativistic MR-MP energy levels: Low-lying states in the Mg isoelectronic sequence

The relativistic Multi-Reference Møller–Plesset (MR-MP) many-body perturbation theory was applied to calculate the energies of all excited states within the 3s3p, 3p{sup 2}, 3s3d, 3p3d and 3d{sup 2} configurations for every ion of the Mg isoelectronic sequence (Z=12−100). The results are compared with previous calculations and available experimental data. The MR-MP excitation energies agree with experiment typically within 100 ppm over a wide range of Z, particularly for mid- and high-range Z. Experimental data for highly charged ions in this isoelectronic sequence are limited and the complete and accurate dataset presented here is expected to ease the identification process upon measurements.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Spectroscopic and computational investigations of organometallic complexation of group 12 transition metals by methanobactins from Methylocystis sp. SB2

Methanotrophic bacteria catalyze the aerobic oxidation of methane to methanol using Cu-containing enzymes, thereby exerting a modulating influence on the global methane cycle. To facilitate the acquisition of Cu ions, some methanotrophic bacteria secrete small modified peptides known as “methanobactins,” which strongly bind Cu and function as an extracellular Cu recruitment relay, analogous to siderophores and Fe. In addition to Cu, methanobactins form complexes with other late transition metals, including the Group 12 transition metals Zn, Cd, and Hg, although the interplay among solution-phase configurations, metal interactions, and the spectroscopic signatures of methanobactin-metal complexes remains ambiguous. In this study, the complexation of Zn, Cd, and Hg by methanobactin from Methylocystis sp. strain SB2 was studied using a combination of absorbance, fluorescence, extended x-ray absorption fine structure (EXAFS) spectroscopy, and time-dependent density functional theory (TD-DFT) calculations. We report changes in sample absorbance and fluorescence spectral dynamics, which occur on a wide range of experimental timescales and characterize a clear stoichiometric complexation dependence. Mercury L3-edge EXAFS and TD-DFT calculations suggest a linear model for Hg--S coordination, and TD-DFT suggests a tetrahedral model for Zn 2+ and Cd 2+ . We observed an enhancement in the fluorescence of methanobactin upon interaction with transition metals and propose a mechanism of complexation-hindered isomerization drawing inspiration from the wild-type Green Fluorescent Protein active site. Collectively, our results represent the first combined computational and experimental spectroscopy study of methanobactins and shed new light on molecular interactions and dynamics that characterize complexes of methanobactins with Group 12 transition metals.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Spectroscopy and electronic structure of the low-energy states of ThN

The electronic spectrum of ThN over the range 19,600–21,200 cm -1 is remarkably congested, showing at least twenty vibronic bands originating from the ground state zero-point level. Rotationally resolved spectra for eleven of these bands have been examined to probe the underlying reasons for the dense manifold of states. Dispersed fluorescence spectra and fluorescence decay lifetimes were measured to provide addition insights. Our experimental measurements were complemented by electronic structure calculations for the low-energy doublet and quartet states. The ab initio calculations yielded a density of excited states that was consistent with the congested spectrum. These states were derived from the formal configurations Th 3+ (6d)N 3- , Th 2+ (7s 2 )N 2- (2p 5 ) and Th 2+ (7s6d)N 2 -(2p 5 ). The calculations indicated that the rotational and vibrational constants would be characteristic of the electronic configurations. This prediction was not borne out by the experimental data, suggesting that the full range of inter-configurational state interactions were not captured by the computational model.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Electron Transfer Pathways Facilitating U(VI) Reduction by Fe(II) on Al- vs Fe-Oxides

This study continues mechanistic development of heterogeneous electron transfer (ET) pathways at mineral surfaces in aquatic environments that enable the reduction U(VI) by surface-associated Fe(II). Using computational molecular simulation within the framework of Marcus Theory, our findings highlight the importance of the configurations and interaction of the electron donor and acceptor species with the substrate, with respect to influencing its electronic structure and thereby the ability of semiconducting minerals to facilitate ET. U(VI) reduction by surface-associated Fe(II) (adsorbed or structurally incorporated into the lattice) on an insulating, corundum (001) surface (α-Al2O3) occurs when proximal inner-sphere (IS) surface complexes are formed, such that ET occurs through a combination of direct exchange (i.e., Fe d- and U f-orbitals overlap through space) and superexchange via intervening surface oxygen atoms. U(VI) reduction by coadsorbed Fe(II) on the isostructural semiconducting hematite (α-Fe2O3) basal surface requires either their direct electronic interaction (e.g., IS complexation) or mediation of this interaction indirectly through the surface via an intrasurface pathway. Conceptually possible longer-range ET by charge-hopping through surface Fe atoms was investigated to determine whether this indirect pathway is competitive with direct ET. The calculations show that energy barriers are large for this conduction-based pathway; interfacial ET into the hematite surface is endothermic (+80.1 kJ/mol) and comprises the rate-limiting step (10–6 s–1). The presence of the IS adsorbates appears to weaken the electronic coupling between underlying Fe ions within the surface, resulting in slower intra-surface ET (10–5 s–1) than expected in the bulk basal plane. Our findings lay out first insights into donor-acceptor communication via a charge-hopping pathway through the surface for heterogeneous reduction of U(VI) by Fe(II) and help provide a basis for experimental interrogation of this important process at mineral-water interfaces.

Taylor, S. D.↗
DOE OSTI2015

The influence of intruder states in even-even Po isotopes

We study the role of intruder states and shape coexistence in the even-even {sup 190–206}Po isotopes, through an interacting boson model with configuration mixing calculation. We analyzed the results in the light of known systematics on various observable in the Pb region, paying special attention to the unperturbed energy systematics and quadrupole deformation. We find that shape coexistence in the Po isotopes behaves in very much the same way as in the Pt isotopes, i.e., it is somehow hidden, contrary to the situation in the Pb and the Hg isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Singlet-paired coupled cluster theory for open shells

Restricted single-reference coupled cluster theory truncated to single and double excitations accurately describes weakly correlated systems, but often breaks down in the presence of static or strong correlation. Good coupled cluster energies in the presence of degeneracies can be obtained by using a symmetry-broken reference, such as unrestricted Hartree-Fock, but at the cost of good quantum numbers. A large body of work has shown that modifying the coupled cluster ansatz allows for the treatment of strong correlation within a single-reference, symmetry-adapted framework. The recently introduced singlet-paired coupled cluster doubles (CCD0) method is one such model, which recovers correct behavior for strong correlation without requiring symmetry breaking in the reference. In this, we extend singlet-paired coupled cluster for application to open shells via restricted open-shell singlet-paired coupled cluster singles and doubles (ROCCSD0). The ROCCSD0 approach retains the benefits of standard coupled cluster theory and recovers correct behavior for strongly correlated, open-shell systems using a spin-preserving ROHF reference.

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

Matrix product operators, matrix product states, and ab initio density matrix renormalization group algorithms

Current descriptions of the ab initio density matrix renormalization group (DMRG) algorithm use two superficially different languages: an older language of the renormalization group and renormalized operators, and a more recent language of matrix product states and matrix product operators. The same algorithm can appear dramatically different when written in the two different vocabularies. Here, we carefully describe the translation between the two languages in several contexts. First, we describe how to efficiently implement the ab initio DMRG sweep using a matrix product operator based code, and the equivalence to the original renormalized operator implementation. Next we describe how to implement the general matrix product operator/matrix product state algebra within a pure renormalized operator-based DMRG code. Finally, we discuss two improvements of the ab initio DMRG sweep algorithm motivated by matrix product operator language: Hamiltonian compression, and a sum over operators representation that allows for perfect computational parallelism. The connections and correspondences described here serve to link the future developments with the past and are important in the efficient implementation of continuing advances in ab initio DMRG and related algorithms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Projected coupled cluster theory

Coupled cluster theory is the method of choice for weakly correlated systems. But in the strongly correlated regime, it faces a symmetry dilemma, where it either completely fails to describe the system or has to artificially break certain symmetries. On the other hand, projected Hartree-Fock theory captures the essential physics of many kinds of strong correlations via symmetry breaking and restoration. Here, we combine and try to retain the merits of these two methods by applying symmetry projection to broken symmetry coupled cluster wave functions. The non-orthogonal nature of states resulting from the application of symmetry projection operators furnishes particle-hole excitations to all orders, thus creating an obstacle for the exact evaluation of overlaps. Here we provide a solution via a disentanglement framework theory that can be approximated rigorously and systematically. Results of projected coupled cluster theory are presented for molecules and the Hubbard model, showing that spin projection significantly improves unrestricted coupled cluster theory while restoring good quantum numbers. The energy of projected coupled cluster theory reduces to the unprojected one in the thermodynamic limit, albeit at a much slower rate than projected Hartree-Fock.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

QMCPACK: Advances in the development, efficiency, and application of auxiliary field and real-space variational and diffusion quantum Monte Carlo

We review recent advances in the capabilities of the open source ab initio Quantum Monte Carlo (QMC) package QMCPACK and the workflow tool Nexus used for greater efficiency and reproducibility. The auxiliary field QMC (AFQMC) implementation has been greatly expanded to include k-point symmetries, tensor-hypercontraction, and accelerated graphical processing unit (GPU) support. These scaling and memory reductions greatly increase the number of orbitals that can practically be included in AFQMC calculations, increasing the accuracy. Advances in real space methods include techniques for accurate computation of bandgaps and for systematically improving the nodal surface of ground state wavefunctions. Results of these calculations can be used to validate application of more approximate electronic structure methods, including GW and density functional based techniques. To provide an improved foundation for these calculations, we utilize a new set of correlation-consistent effective core potentials (pseudopotentials) that are more accurate than previous sets; these can also be applied in quantum-chemical and other many-body applications, not only QMC. These advances increase the efficiency, accuracy, and range of properties that can be studied in both molecules and materials with QMC and QMCPACK.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗