Quasiparticle band structure and excitonic optical response in V 2 O 5 bulk and monolayer
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Garcia, Claudio (ORCID:0009000077503536)↗
SEARCH · Engineering Papers
Results for “Wave potential 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.
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Control-Affine Schrödinger Bridge and Generalized Bohm Potential
From a stochastic control perspective, the Schrödinger bridge is a density-valued continuous curve parameterized by time that connects a given pair of initial and terminal probability densities via minimum effort controlled Brownian motion. The control-affine Schrödinger bridge extends this idea to a generic control-affine Itô diffusion, possibly with an additive state cost. Here, in this letter, we recast the necessary conditions of optimality for the control-affine Schrödinger bridge problem as a two point boundary value problem for a quantum mechanical Schrödinger PDE with complex potential. This complex-valued potential is a generalization of the real-valued Bohm potential in quantum mechanics. Our derived potential is akin to the optical potential in nuclear physics where the real part of the potential encodes elastic scattering (transmission of wave function), and the imaginary part encodes inelastic scattering (absorption of wave function). The key takeaway is that the process noise that drives the evolution of probability densities induces an absorbing medium in the evolution of wave function. These results make new connections between control theory and non-equilibrium statistical mechanics through the lens of quantum mechanics.
Markov processes↗
Ab initio determination of mode coupling in HSSH - The torsional splitting in the first excited S-S stretching state
A mechanism for the enhanced splitting detected in the millimeter-wave rotational spectra of the first excited S-S stretching state of HSSH (disulfane) has been studied. The mechanism, which involves a potential coupling between the first excited S-S stretching state and excited torsional states, has been investigated in part by the use of ab initio theory. Based on an ab initio potential surface, coupling matrix elements have been calculated, and the amount of splitting has then been estimated by second-order perturbation theory. The result, while not in quantitative agreement with the measured splitting, lends plausibility to the assumed mechanism.
Herbst, Eric↗
A time-dependent wave packet approach to atom-diatom reactive collision probabilities - Theory and application to the H + H2(J = 0) system
This paper describes a new approach to the study of atom-diatom reactive collisions in three dimensions employing wave packets and the time-dependent Schroedinger equation. The method uses a projection operator approach to couple the inelastic and reactive portions of the total wave function and optical potentials to circumvent the necessity of using product arrangement coordinates. Reactive transition probabilities are calculated from the state resolved flux of the wave packet as it leaves the interaction region in the direction of the reactive arrangement channel. The present approach is used to obtain such vibrationally resolved probabilities for the three-dimensional H + H2 (J = 0) hydrogen exchange reaction, using a body-fixed system of coordinates.
Neuhauser, Daniel↗
Exact two-body expansion of the many-particle wave function
Progress toward the solution of the strongly correlated electron problem has been stymied by the exponential complexity of the wave function. Previous work established an exact two-body exponential product expansion for the ground-state wave function. By developing a reduced density-matrix analog of Dalgarno-Lewis perturbation theory, we prove here that (i) the two-body exponential product expansion is rapidly and globally convergent with each operator representing an order of a renormalized perturbation theory, (ii) the energy of the expansion converges quadratically near the solution, and (iii) the expansion is exact for both ground and excited states. The two-body expansion offers a reduced parametrization of the many-particle wave function as well as the two-particle reduced density matrix with potential applications on both conventional and quantum computers for the study of strongly correlated quantum systems. In this work, we demonstrate the result with the exact solution of the contracted Schrödinger equation for the molecular chains H 4 and H 5 .
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
High-frequency techniques for RCS prediction of plate geometries
Given here are hard polarization diffraction coefficients for the special case of a wedge that is coated with a lossy dielectric on one face and is perfectly conducting on the other face. Expressions for plane-wave incidence, far-field observation; for cylindrical-wave incidence, far-field observation; and for plane-wave incidence, near-field observation are presented for regular diffractions. In addition, terms for surface-wave and surface-wave transition fields are presented. These expressions are derived from the Uniform Theory of Diffraction (UTD) coefficients for a generalized impedance wedge and are simplified for rapid calculation for the case of one perfectly conducting face. Results from a first-order model for a coated, rectangular plate are examined; and potential problems in extending this modeling approach to more complicated coated structures are identified.
Balanis, Constantine A.↗
Multireference Methods for Chemistry and Materials Science: Automated Active Spaces, Efficient Dynamic Correlation, and Extended Systems
While multiconfigurational approaches have long been relegated to expert practitioners working on a case-by-case basis, recent developments have increasingly made these methods more routine and applicable to broader sets of systems. This article outlines the state-of-the-art in multiconfigurational approaches, with an emphasis on moving from delicate hand-selected pathways through configuration space toward more robust and efficient approaches to treating a host of challenging chemical systems accurately. First, we overview recent work in automated active-space selection, which has enabled increasingly large-scale applications of multireference methods to modeling vertical excitations and reactivity. Second, we highlight the increasingly efficient methods for recovering correlation energy beyond the active space, as headlined by extensions of pair-density functional theory and its role in accurate and efficient treatment of excited-state dynamics and its utilization to train machine-learned potentials. Finally, we highlight recent efforts to treat extended systems that until recently have lied beyond the traditional limits of active-space methods, giving center stage to product-form wave functions of the localized active space family of methods that allow for the computation of multiconfigurational band structures. These recent advancements point to a broader use of multireference approaches for high-impact chemical and materials science applications.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Pt-Assisted Carbon Remediation of Mo2C Materials for CO Disproportionation
Using the CO disproportionation (Boudouard) reaction as a probe reaction, an in-depth analysis of temperature-programmed pulse response data shows that the addition of Pt to Mo2C mitigates deactivation of Mo active sites by acting as a carbon collector. CO2 production on Mo2C and Pt/Mo2C materials is dependent on both the activation energy and the CO surface concentration. Detailed plane-wave density functional theory calculations of the CO adsorption and disproportion reactions on Mo2C-supported Pt nanoparticles (NPs) are reported. The Mo2C was modeled by the ß-Mo2C (100) surface, and the Pt/Mo2C interface was modeled by the addition of 12 Pt atoms to the Mo2C (100) surface (12Pt@Mo2C). The potential energy surfaces of the Boudouard reaction were calculated on pure Mo2C, 12Pt@Mo2C, and Pt (111) surfaces. CO dissociation readily occurs on the Mo2C (100) surface, but not on the Pt (111) surface, with the former being exothermic and the latter being endothermic. At the Pt/Mo2C interface, CO dissociation is still exothermic, but with a larger energy barrier. The Boudouard reaction takes place on the Mo2C region, where CO2 is formed from a surface O atom dissociated from one CO molecule in reaction with another CO molecule, leaving one C atom on the surface. C adsorption is preferential on the Pt site in comparison to the Mo site. The supported Pt domains can collect the remaining C atoms, facilitating further CO2 formation on the active Mo sites. A Bader charge analysis shows that the surface metal-carbon bond is a mixture of covalent and ionic bonds, whereas the surface metal-oxygen bond is ionic. Electron localization function (ELF) and partial charge density calculations agree well with the Bader charge analysis. These computational results are consistent with experimental observations of the interaction of CO with Mo2C nanotube supported Pt domains in the transient regime under far from equilibrium conditions. The Boudouard reaction is an important side reaction, and the unexpected role found for Pt as a carbon collector, with Mo serving as a disproportionation site, provides a unique vantage point for understanding carbon and coke formation on catalytic materials.
Pt-assisted carbon remediation, Pt/Mo2C interface,↗
Basic elements for simulations of standard-model physics with quantum annealers: Multigrid and clock states
Here, we explore the potential of D-Wave's quantum annealers for computing some of the basic components required for quantum simulations of standard model physics. By implementing a basic multigrid (including “zooming”) and specializing Feynman-clock algorithms, D-Wave's Advantage is used to study harmonic and anharmonic oscillators relevant for lattice scalar field theories and effective field theories, the time evolution of a single plaquette of SU(3) Yang-Mills lattice gauge field theory, and the dynamics of flavor entanglement in four-neutrino systems.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Impact Tsunami Calculations: Hydrodynamical Simulations vs. Linear Theory
Tsunamis generated by the impacts of asteroids and comets into the Earth oceans are widely recognized as a potential catastrophic hazard to the Earth s population. Our general conclusion is that linear theory is a reasonably accurate guide to behavior of tsunamis generated by impactors of moderate size, where the initial transient impact cavity is of moderate depth compared to the ocean depth. This is particularly the case for long wavelength waves that propagate fastest and would reach coastlines first. Such tsunamis would be generated in the open ocean by impactors of 300 meters in diameter, which might be expected to strike the Earth once every few thousand years, on the average. Larger impactors produce cavities deep enough to reach the ocean floor; even here, linear theory is applicable if the starting point is chosen at a later phase in the calculation when the impact crater has slumped back to produce a cavity of moderate depth and slope.
Korycansky, E.↗
A Preliminary ZEUS Lightning Location Error Analysis Using a Modified Retrieval Theory
The ZEUS long-range VLF arrival time difference lightning detection network now covers both Europe and Africa, and there are plans for further expansion into the western hemisphere. In order to fully optimize and assess ZEUS lightning location retrieval errors and to determine the best placement of future receivers expected to be added to the network, a software package is being developed jointly between the NASA Marshall Space Flight Center (MSFC) and the University of Nevada Las Vegas (UNLV). The software package, called the ZEUS Error Analysis for Lightning (ZEAL), will be used to obtain global scale lightning location retrieval error maps using both a Monte Carlo approach and chi-squared curvature matrix theory. At the core of ZEAL will be an implementation of an Iterative Oblate (IO) lightning location retrieval method recently developed at MSFC. The IO method will be appropriately modified to account for variable wave propagation speed, and the new retrieval results will be compared with the current ZEUS retrieval algorithm to assess potential improvements. In this preliminary ZEAL work effort, we defined 5000 source locations evenly distributed across the Earth. We then used the existing (as well as potential future ZEUS sites) to simulate arrival time data between source and ZEUS site. A total of 100 sources were considered at each of the 5000 locations, and timing errors were selected from a normal distribution having a mean of 0 seconds and a standard deviation of 20 microseconds. This simulated "noisy" dataset was analyzed using the IO algorithm to estimate source locations. The exact locations were compared with the retrieved locations, and the results are summarized via several color-coded "error maps."
Elander, Valjean↗
Boosting the Oxygen Reduction Performance via Tuning the Synergy between Metal Core and Oxide Shell of Metal−Organic Frameworks‐Derived Co@CoO x
Abstract Co core@Co oxide shell (Co@CoO x ) catalysts represent a large family with promising oxygen reduction reaction (ORR) catalytic activity. However, inadequate understanding of Co@CoO x synergy prohibits further pursuit of catalytic performance enhancement. Herein, a Co zeolitic−imidazolate framework was converted into metallic Co, followed by controlled air treatment to form Co@CoO x . The composition and structure evolution as a function of air treatment temperature were studied thoroughly through conventional and synchrotron (both ex‐situ and in‐situ) characterizations, confirming the coexistence of CoO and Co 3 O 4 in the shell. The optimal catalyst showed an ORR half‐wave potential of 0.87 V (vs. RHE) in an alkaline half‐cell and delivered high discharge capacity in an aprotic Li−O 2 battery (7,124 mAh g Cat+C −1 ) and an aqueous Zn−air battery (694 mAh g Zn −1 ) with good performance retention after durability test. Modeling simulation and density functional theory calculation confirmed the charge donation from metal core to oxide shell and shed light on new insights of how metal@metal oxide synergy impacted the ORR via tuning the charge conductivity, oxygen affinity and intermediate transfer pathway. This work opens up a venue to boost ORR catalytic activity from an interfacial synergy perspective.
Wang, Hao↗
Accelerating Embedding Potential Optimization by Reconstructing the Pseudo-Valence Electron Density
Density functional embedding theory (DFET) enables use of electronic structure methods with higher accuracy than density functional theory in a local region, with applications thus far ranging from (photo/electro)catalysis to reactions in solution. DFET partitions a large collection of atoms into smaller groups that interact via a shared embedding (interaction) potential V emb , determined via functional optimization. The optimized effective potential (OEP) process used to optimize V emb is time-consuming and becomes a computational bottleneck due to sharp, oscillating features of V emb near nuclei. Here, similar to pseudopotential theory, by reconstructing electron densities used in the OEP process from smoother pseudo-valence-only (PVO) electron densities as proxies for total densities of the full system and subsystems, we can retain accuracy in the embedded electronic structure calculations while potentially reducing the overhead of V emb construction, within the projector augmented-wave (PAW) formalism. We explore three different chemical reactions as exemplars to test PVO–DFET, namely, H 2 dissociative adsorption on a Cu(111) surface, H 2 O adsorption on a Pt(111) surface, and aqueous [Ca 2+ –SO 4 2– ] ion-pair formation. The PVO approximation works well for all three systems with minimal loss of accuracy (∼10–70 meV error relative to the original exact-derivative (ED) approach) while accelerating V emb generation for the Cu and Pt systems respectively by 20× and 5×. Given proper numerical convergence parameters, the spatial distributions of differences between PVO- and ED-based V emb outside the core regions are small, explaining the exceptional agreement between the two approaches. Finally, we anticipate that this more efficient PVO–DFET approximation will be useful whenever computation of V emb is much more expensive than subsequent embedded high-level electron correlation calculations.
approximation↗
On the stability of the boundary layer on a transonic swept wing
Both incompressible and compressible linear stability theory are applied to the three-dimensional compressible boundary layer on a particular transonic sweptback wing of infinite span. A spatial stability theory is used which identifies the growth direction with the real part of the complex angle of the group velocity. It is found that in the forward, but not the rear, crossflow instability region, the maximum amplification rates of the steady disturbances may be calculated to within about 10% by the incompressible stability theory. There is little difference between the sixth and eighth-order compressible theories. The maximum amplification rate of the steady disturbances at any chordwise station is closely related to the maximum crossflow at that station independent of the Reynolds number. For other than crossflow instability, there can be large differences between the incompressible and compressible theories, both as to the amplification rate and the angle of the wavenumber vector for maximum instability. Amplitude ratios of individual wave components are obtained by integrating the spatial amplification rate along the growth direction subject to the constraint that the wavenumber vector is irrotational. This procedure yields steady disturbances aligned with the local potential flow direction whose wavelengths are nearly independent of downstream distance.
Mack, L. M.↗
The terminal area simulation system. Volume 1: Theoretical formulation
A three-dimensional numerical cloud model was developed for the general purpose of studying convective phenomena. The model utilizes a time splitting integration procedure in the numerical solution of the compressible nonhydrostatic primitive equations. Turbulence closure is achieved by a conventional first-order diagnostic approximation. Open lateral boundaries are incorporated which minimize wave reflection and which do not induce domain-wide mass trends. Microphysical processes are governed by prognostic equations for potential temperature water vapor, cloud droplets, ice crystals, rain, snow, and hail. Microphysical interactions are computed by numerous Orville-type parameterizations. A diagnostic surface boundary layer is parameterized assuming Monin-Obukhov similarity theory. The governing equation set is approximated on a staggered three-dimensional grid with quadratic-conservative central space differencing. Time differencing is approximated by the second-order Adams-Bashforth method. The vertical grid spacing may be either linear or stretched. The model domain may translate along with a convective cell, even at variable speeds.
Proctor, F. H.↗
Two applications of potential vorticity thinking
The phenomena of dissipative destabilization of external Rossby waves and the acceleration of the zonal mean jet during baroclinic life cycles are described in terms of potential vorticity. The main principle of the potential temperature variations at rigid boundaries have the same effect on the interior flow as do sheets of potential vorticity located just within the boundaries. It is noted that the potential vorticity theory is useful for understanding the dynamical behavior of meterological phenomena.
Robinson, Walter A.↗
Sources of mesoscale variability of gravity waves. I - Topographic excitation. II - Frontal, convective, and jet stream excitation
The effect of topography as a source of mesoscale variability was investigated using aircraft measurements of winds and temperature collected during the Global Atmospheric Sampling Program, with results showing marked increases in the variance of zonal and meridional wind speeds and of potential temperature over rough terrain. In addition, four cases of mesoscale variance enhancements of horizontal velocity and temperature due to frontal activity, nonfrontal convection, and wind shear were studied. The implications of these episodic enhancements of variances for the vertical transports of energy and momentum are considered in the framework of the gravity wave theory.
Nastrom, Gregory D.↗
Application of First-Principles-Based Artificial Neural Network Potentials to Multiscale-Shock Dynamics Simulations on Solid Materials
The use of artificial neural network (ANN) potentials trained with first-principles calculations has emerged as a promising approach for molecular dynamics (MD) simulations encompassing large space and time scales while retaining first-principles accuracy. To date, however, the application of ANN-MD has been limited to near-equilibrium processes. Here we combine first-principles-trained ANN-MD with multiscale shock theory (MSST) to successfully describe far-from-equilibrium shock phenomena. Overall, our ANN-MSST-MD approach describes shock-wave propagation in solids with first-principles accuracy but a 5000 times shorter computing time. Accordingly, ANN-MD-MSST was able to resolve fine, long-time elastic deformation at low shock speed, which was impossible with first-principles MD because of the high computational cost. This work thus lays a foundation of ANN-MD simulation to study a wide range of far-from-equilibrium processes.
36 MATERIALS SCIENCE↗