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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Atoms and interatomic bonding synergism inherent in molecular electronic wave functions

The chemical model of matter consists of atoms held together by bonds. The success of this model implies that the physical interactions of the electrons and nuclei in molecules combine into compound interactions that create the bonding. In the quantum mechanical description, the modified atoms in molecules and the bonding synergism are contained in the molecular electronic wave function. So far, only part of this information has been recovered from the wave function. Notably, the atoms have remained unidentified in the wave function. One reason is that conventional energy decomposition analyses formulate separate model wave functions, independent of the actual wave function, to represent “prepared atoms” and preconceived interactions and, then, intuitively catenate the parts. In the present work, the embedded modified atoms and the inherent physical synergisms between them are determined by a unified derivation entirely from the actual molecular valence space wave function. By means of a series of intrinsic orbital and configurational transformations of the wave function, the energy of formation of a molecule is additively resolved in terms of intra-atomic energy changes, interference energies, and quasi-classical, non-classical, and charge-transfer Coulombic interactions. Here, the analysis furnishes an algorithm for the quantitative resolution of the energy of formation, which enables analyses elucidating reaction energies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Chiral catalysis of nuclear fusion in molecules

At low energies, nuclear fusion is strongly affected by electron screening of the Coulomb repulsion among the fusing nuclei. It may thus be possible to catalyze nuclear fusion in molecules (i.e., to fuse specific nuclei in situ) through quantum control of electron wave functions in intense laser fields. The circularly polarized (chiral) laser field can effectively squeeze the electron wave functions, greatly enhancing the screening in the spatial region relevant for the fusion process. Here, we estimate the corresponding fusion probabilities, and find that the proposed chiral catalysis of nuclear fusion in molecules may be observable, potentially with important practical applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

GronOR: Massively Parallel and GPU-Accelerated Non-Orthogonal Configuration Interaction for Large Molecular Systems

GronOR is a program package for non-orthogonal configuration interaction calculations for an electronic wave function built in terms of anti-symmetrized products of multi-configuration molecular fragment wave functions. The two-electron integrals that have to be processed may be expressed in terms of atomic orbitals or in terms of an orbital basis determined from the molecular orbitals of the fragments. The code has been specifically designed for execution on distributed memory massively parallel and Graphics Processing Unit (GPU)-accelerated computer architectures, using an MPI+OpenACC/OpenMP programming approach. The task-based execution model used in the implementation allows for linear scaling with the number of nodes on the largest pre-exascale architectures available, provides hardware fault resiliency, and enables effective execution on systems with distinct central processing unit-only and GPU-accelerated partitions. The code interfaces with existing multi-configuration electronic structure codes that provide optimized molecular fragment orbitals, configuration interaction coefficients, and the required integrals. Algorithm and implementation details, parallel and accelerated performance benchmarks, and an analysis of the sensitivity of the accuracy of results and computational performance to thresholds used in the calculations are presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Distinguishing Elements at the Sub‐Nanometer Scale on the Surface of a High Entropy Alloy

Materials in crystalline form possess translational symmetry (TS) when the unit cell is repeated in real space with long- and short-range orders. The periodic potential in the crystal regulates the electron wave function and results in unique band structures, which further define the physical properties of the materials. Amorphous materials lack TS due to the randomization of distances and arrangements between atoms, causing the electron wave function to lack a well-defined momentum. High entropy materials provide another way to break the TS by randomizing the potential strength at periodic atomic sites. The local elemental distribution has a great impact on physical properties in high entropy materials. It is critical to distinguish elements at the sub-nanometer scale to uncover the correlations between the elemental distribution and the material properties. Here, the use of synchrotron X-ray scanning tunneling microscopy (SX-STM) with sub-nm scale resolution in identifying elements on a high entropy alloy (HEA) surface is demonstrated. By examining the elementally sensitive X-ray absorption spectra with an STM tip to enhance the spatial resolution, the elemental distribution on an HEA's surface at a sub-nm scale is extracted. In conclusion, these results open a pathway towards quantitatively understanding high entropy materials and their material properties.

36 MATERIALS SCIENCE↗
DOE OSTI2022

GronOR: Scalable and Accelerated Nonorthogonal Configuration Interaction for Molecular Fragment Wave Functions

GronOR is a program package for nonorthogonal configuration interaction calculations. Electronic wave functions are constructed in terms of antisymmetrized products of multiconfiguration molecular fragment wave functions. The computational complexity of the nonorthogonal methodologies implemented in GronOR applied to large molecular assemblies requires a design that takes full advantage of massively parallel supercomputer architectures and accelerator technologies. This work describes the implementation strategy and resulting performance characteristics. In addition to parallelization and acceleration, the software development strategy includes aspects of fault resiliency and heterogeneous computing. The program was designed for large-scale supercomputers but also runs effectively on small clusters and workstations for small molecular systems. GronOR is available as open source to the scientific community.

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

Revisiting the Hole Size in Double Helical DNA with Localized Orbital Scaling Corrections

The extent of electronic wave function delocalization for the charge carrier (electron or hole) in double helical DNA plays an important role in determining the DNA charge transfer mechanism and kinetics. The size of the charge carrier’s wave function delocalization is regulated by the solvation induced localization and the quantum delocalization among the π stacked base pairs at any instant of time. Using a newly developed localized orbital scaling correction (LOSC) density functional theory method, we accurately characterized the quantum delocalization of the hole wave function in double helical B-DNA. This approach can be used to diagnose the extent of delocalization in fluctuating DNA structures. Our studies indicate that the hole state tends to delocalize among 4 guanine–cytosine (GC) base pairs and among 3 adenine–thymine (AT) base pairs when these adjacent bases fluctuate into degeneracy. The relatively small delocalization in AT base pairs is caused by the weaker π–π interaction. This extent of delocalization has significant implications for assessing the role of coherent, incoherent, or flickering coherent carrier transport in DNA.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Full radiator-perturber interaction in computer simulations of hydrogenic spectral line broadening by plasmas

Spectral line broadening by plasmas can be computed by solving the equation of motion for the dipole of the radiating system perturbed by a fluctuating potential obtained from computer simulations. Such calculations have relied on the multipole expansion of the radiator-plasma interaction often keeping only the dipole term. With increasing density, however, higher multipoles as well as plasma perturbers overlapping the bound electron wave functions are expected to become important. For hydrogenic systems, the atomic matrix elements of the full Coulomb and screened Coulomb interactions are given by analytical formulas. Using these results, a computer simulation approach that accounts for the full radiator-plasma interaction is developed. One benefit is the removal of inherent strong collision divergences in the multipole expansion approximation. Furthermore, it yields the plasma polarization shift produced by perturbers penetrating the wave function of the radiator bound electrons. Here, the model was applied to hydrogenic argon Ly-α , Ly- β , and Ly-$\gamma$ spectral lines in a dense argon plasma at free electron densities of 10 24 or 10 25 cm ⁻3 and temperature of $800$ $eV$ relevant to plasma diagnostic techniques for inertial confinement fusion implosions.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Photoelectrochemically Self Improving Si/GaN Photocathode: Figure 4a Raw Data

Calculated formation energy of (0001 ̅) c-plane GaN surfaces. The density-functional theory (DFT) calculations were performed with the generalized gradient approximation, using the plane-wave pseudopotential quantum-ESPRESSO package. Ultrasoft pseudopotentials were used to describe the interaction between valence electrons and ionic cores, where Ga 3d electrons were explicitly treated as valence electrons. The wave functions and electronic density were expanded in a plane-wave basis set truncated at a cutoff energy of 30 Ry and 240 Ry, respectively. The surface was modeled using a repeated slab geometry using a (2×2) unit cell with a thickness of seven GaN bilayers, where the Ga-terminated bottom side was passivated by pseudo-hydrogen with charge of 1.25e. In addition, the (1010) surface was modeled using 8 GaN atomic layers with a lateral dimension of 9.57 Å x 10.38 Å. A vacuum width of at least 15.0 Å was introduced between consecutive slabs, and a k-point mesh of 5x5x1 and 2x2x1 was used to sample the surface Brillouin zone for the polar and non-polar surfaces, respectively. Calculated formation energy of (0001 ̅) c-plane GaN surfaces with different oxygen configuration within the anion and cation-rich limits: ideal GaN surfaces of c-plane and m-plane; configurations with 100% replacement of nitrogen by oxygen on the surface c-plane and m-plane; 100% replacement of nitrogen by oxygen in the subsurface bilayer c-plane and m-plane; and configurations with 50% replacement of nitrogen of the surface and subsurface bilayers by oxygens c-plane and m-plane. In both cases, the ideal surface is chosen as the reference.

photocathode↗
DOE OSTI2021

Photoelectrochemically Self Improving Si/GaN Photocathode: Figure 4b Raw Data

Calculated formation energy of (1010 ̅) m-plane GaN surfaces. The density-functional theory (DFT) calculations were performed with the generalized gradient approximation, using the plane-wave pseudopotential quantum-ESPRESSO package. Ultrasoft pseudopotentials were used to describe the interaction between valence electrons and ionic cores, where Ga 3d electrons were explicitly treated as valence electrons. The wave functions and electronic density were expanded in a plane-wave basis set truncated at a cutoff energy of 30 Ry and 240 Ry, respectively. The surface was modeled using a repeated slab geometry using a (2×2) unit cell with a thickness of seven GaN bilayers, where the Ga-terminated bottom side was passivated by pseudo-hydrogen with charge of 1.25e. In addition, the (1010) surface was modeled using 8 GaN atomic layers with a lateral dimension of 9.57 Å x 10.38 Å. A vacuum width of at least 15.0 Å was introduced between consecutive slabs, and a k-point mesh of 5x5x1 and 2x2x1 was used to sample the surface Brillouin zone for the polar and non-polar surfaces, respectively. Calculated formation energy of (1010 ̅) m-plane GaN surfaces with different oxygen configuration within the anion and cation-rich limits: ideal GaN surfaces of c-plane and m-plane; configurations with 100% replacement of nitrogen by oxygen on the surface c-plane and m-plane; 100% replacement of nitrogen by oxygen in the subsurface bilayer c-plane and m-plane; and configurations with 50% replacement of nitrogen of the surface and subsurface bilayers by oxygens c-plane and m-plane. In both cases, the ideal surface is chosen as the reference.

photocathode↗
DOE OSTI2020

Dual-cone variational calculation of the two-electron reduced density matrix

The computation of strongly correlated quantum systems is challenging because of its potentially exponential scaling in the number of electron configurations. Variational calculation of the two-electron reduced density matrix (2-RDM) without the many-electron wave function exploits the pairwise nature of the electronic Coulomb interaction to compute a lower bound on the ground-state energy with polynomial computational scaling. Recently, a dual-cone formulation of the variational 2-RDM calculation was shown to generate the ground-state energy, albeit not the 2-RDM, at a substantially reduced computational cost, especially for higher $\textit{N}$-representability conditions such as the T2 constraint. Here we generalize the dual-cone variational 2-RDM method to compute not only the ground-state energy but also the 2-RDM. The central result is that we can compute the 2-RDM from a generalization of the Hellmann-Feynman theorem. Specifically, we prove that in the Lagrangian formulation of the dual-cone optimization the 2-RDM is the Lagrange multiplier. Further, we apply the method to computing the energies and properties of strongly correlated electrons—including atomic charges, electron densities, dipole moments, and orbital occupations—in an illustrative hydrogen chain and the nitrogen-fixation catalyst FeMoco. The dual variational computation of the 2-RDM with T2 or higher N -representability conditions provides a polynomially scaling approach to strongly correlated molecules and materials with significant applications in atomic and molecular and condensed-matter chemistry and physics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Superradiance and Subradiance due to Quantum Interference of Entangled Free Electrons

When multiple quantum emitters radiate, their emission rate may be enhanced or suppressed due to collective interference in a process known as super- or subradiance. Such processes are well known to occur also in light emission from free electrons, known as coherent cathodoluminescence. Unlike atomic systems, free electrons have an unbounded energy spectrum, and, thus, all their emission mechanisms rely on electron recoil, in addition to the classical properties of the dielectric medium. To date, all experimental and theoretical studies of super- and subradiance from free electrons assumed only classical correlations between particles. However, dependence on quantum correlations, such as entanglement between free electrons, has not been studied. Recent advances in coherent shaping of free-electron wave functions motivate the investigation of such quantum regimes of super- and subradiance. In this Letter, we show how a pair of coincident path-entangled electrons can demonstrate either super- or subradiant light emission, depending on the two-particle wave function. By choosing different free-electron Bell states, the spectrum and emission pattern of the light can be reshaped, in a manner that cannot be accounted for by a classical mixed state. We show these results for light emission in any optical medium and discuss their generalization to many-body quantum states. Furthermore, our findings suggest that light emission can be sensitive to the explicit quantum state of the emitting matter wave and possibly serve as a nondestructive measurement scheme for measuring the quantum state of many-body systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Quantum Nature of Dielectric Laser Accelerators

Dielectric laser accelerators (DLAs) hold great promise for producing economic and compact on-chip radiation sources. On-chip DLAs benefit from fabrication capabilities of the silicon industry and from breakthroughs in silicon-photonic nanostructures to enhance the interaction between particles and laser fields. Seemingly unrelated recent advances in the quantum interactions of electrons and light have raised interest in the underlying classical-quantum correspondence principle at the foundations of electron acceleration. Here, we present the observation of the underlying quantum nature of DLAs: observing quantized peaks in the electron-energy spectra. Our findings demonstrate quasi-phase-matching between an electron wave function and a light wave, which also demonstrates the role of the quantum wave function in the inverse Smith-Purcell effect. We harness the capabilities of an ultrafast transmission electron microscope (UTEM) to maintain a long electron-light interaction length extending over hundreds of periods of the laser pulse, mediated by a silicon-photonic nanograting DLA. The UTEM is shown as a new platform for characterization of future DLA concepts. The results raise fundamental questions regarding the role of quantum mechanics in DLA design, and more generally about the prospects of manipulating particles’ quantum wave functions in accelerator physics.

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

Electron impact ionization in dense plasmas

Here, the distorted-wave with exchange (DWE) method is employed to evaluate electron impact ionization cross sections in dense electron–ion plasmas. Bound and continuum electron wave functions are obtained from a non-relativistic average-atom code. Plots of DWE cross sections are presented for 1s electrons in Li and Be plasmas and 2p electrons in Na and Mg plasmas. For each of these elements, cross sections are evaluated at metallic density in a range of temperatures from 10 to 100 eV and at their respective melting points. Resonances in the cross sections appear near the incident energy threshold at high temperatures. The origin of these resonances is discussed. In general, the distorted wave (DW) method without exchange is found to be a good approximation to the DWE method for electron impact ionization calculations. In the resonance region, however, exchange effects are found to be very important and cannot be neglected.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Anti-symmetric barron functions and their approximation with sums of determinants

A fundamental problem in quantum physics is to encode functions that are completely anti-symmetric under permutations of identical particles. The architecture of neural network models for the electron wave function typically comprises an equivariant component followed by a summation of determinants. The recently introduced Generic Antisymmetric (GA) block is designed to enhance the expressivity of such neural wave functions, and it was found that the 2-layer GA block achieved more accurate energies than the corresponding single-determinant FermiNet architecure, suggesting its promise as a way to improve the expressivity of neural wave functions. In this paper we show how the function expressed by the 2-layer GA block can be decomposed into a sum of determinants. We formalize this result by defining the antisymmetric Barron space as a generalized version of the 2-layer GA block and providing an appromation theorem for this function class. This result can be viewed as a negative result showing that the 2-layer GA block is not more expressive than using multiple determinants.

Abrahamsen, Nilin↗
DOE OSTI2021

Spin-texture-driven electrical transport in multi-Q antiferromagnets

Abstract Unusual magnetic textures can be stabilized in f -electron materials due to the interplay between competing magnetic interactions, complex Fermi surfaces, and crystalline anisotropy. Here we investigate CeAuSb 2 , an f -electron incommensurate antiferromagnet hosting both single- Q and double- Q spin textures as a function of magnetic fields ( H ) applied along the c axis. Experimentally, we map out the field-temperature phase diagram via electrical resistivity and thermal expansion measurements. Supported by calculations of a Kondo lattice model, we attribute the puzzling magnetoresistance enhancement in the double- Q phase to the localization of the electronic wave functions caused by the incommensurate magnetic texture.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Full configuration interaction simulations of exchange-coupled donors in silicon using multi-valley effective mass theory

Abstract Donor spins in silicon have achieved record values of coherence times and single-qubit gate fidelities. The next stage of development involves demonstrating high-fidelity two-qubit logic gates, where the most natural coupling is the exchange interaction. To aid the efficient design of scalable donor-based quantum processors, we model the two-electron wave function using a full configuration interaction method within a multi-valley effective mass theory. We exploit the high computational efficiency of our code to investigate the exchange interaction, valley population, and electron densities for two phosphorus donors in a wide range of lattice positions, orientations, and as a function of applied electric fields. The outcomes are visualized with interactive images where donor positions can be swept while watching the valley and orbital components evolve accordingly. Our results provide a physically intuitive and quantitatively accurate understanding of the placement and tuning criteria necessary to achieve high-fidelity two-qubit gates with donors in silicon.

Joecker, Benjamin (ORCID:0000000302635440)↗