Search NASA⌕ Search

SEARCH · Search NASA

Results for “Electronic wave function”

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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

X-ray Excitation Triggers Ytterbium Anomalous Emission in CaF 2 :Yb but Not in SrF 2 :Yb

Materials that luminesce after excitation with ionizing radiation are extensively applied in physics, medicine, security, and industry. Lanthanide dopants are known to trigger crystal scintillation through their fast d–f emissions; the same is true for other important applications as lasers or phosphors for lighting. However, this ability can be seriously compromised by unwanted anomalous emissions often found with the most common lanthanide activators. We report high-resolution X-ray-excited optical (IR to UV) luminescence spectra of CaF 2 :Yb and SrF 2 :Yb samples excited at 8949 eV and 80 K. Ionizing radiation excites the known anomalous emission of ytterbium in the CaF 2 host but not in the SrF 2 host. Wave function-based ab initio calculations of host-to-dopant electron transfer and Yb 2+ /Yb 3+ intervalence charge transfer explain the difference. Furthermore, the model also explains the lack of anomalous emission in Yb-doped SrF 2 excited by VUV radiation.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Excitation variance matching with limited configuration interaction expansions in variational Monte Carlo

In the regime where traditional approaches to electronic structure cannot afford to achieve accurate energy differences via exhaustive wave function flexibility, rigorous approaches to balancing different states’ accuracies become desirable. As a direct measure of a wave function’s accuracy, the energy variance offers one route to achieving such a balance. Here, we develop and test a variance matching approach for predicting excitation energies within the context of variational Monte Carlo and selective configuration interaction. In a series of tests on small but difficult molecules, we demonstrate that the approach it is effective at delivering accurate excitation energies when the wave function is far from the exhaustive flexibility limit. Results in C3, where we combine this approach with variational Monte Carlo orbital optimization, are especially encouraging.

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

Covalency in Fe 2 O 3 and FeO: Consequences for XPS satellite intensity

The covalent character of the interaction between the metal cation and the oxygen ligands has been examined for two Fe oxides with different nominal oxidation states, Fe(II)O, and Fe(III) 2 O 3 . The covalent character is examined for the initial, ground state configuration and for the ionic states involving the removal of a shallow core, Fe 3p, and a deep core, Fe 2p, electron. The covalency is assessed based on novel theoretical analyses of wave functions for the various cases. It is found that the covalency is considerably different for different oxidation states and for different ionized and non-ionized configurations. The changes in covalency for the ions are shown to be responsible for important changes in relaxation energies for X-Ray Photoelectron Spectroscopy (XPS) spectra and in the intensity lost from main XPS peaks to shake satellites. While these consequences are not observables themselves, they are important for the interpretation of the XPS spectra, in particular, for efforts to extract stoichiometries of these iron oxides from XPS data. This is a finding likely applicable across various 3d transition metal oxide materials.

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

Band structure and Fermi surface nesting in LaSb 2

Here we use high-resolution angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) to investigate the electronic structure of the charge density wave (CDW) system LaSb 2 . This compound is among an interesting group of materials that manifests both a CDW transition and lower temperature superconductivity. We find the DFT calculations to be in good agreement with our ARPES data. The Fermi surface of LaSb 2 consists of two small hole pockets close to Γ and four larger pockets near the Brillouin zone boundary. The key features of the Fermi surface do not vary significantly with temperature. A saddle point is present at -0.19 eV below the Fermi level at Γ. Saddle points in the band structure have more pronounced effects on materials properties when they are located closer to the Fermi level, making doped LaSb 2 compounds a potential interesting subject of future research. Multiple peaks are present in the generalized, electronic susceptibility calculations, indicating the presence of three possible nesting vectors. We were not able to detect any signatures of the CDW transition at 355 K down to the lowest temperature of 7 K, pointing to the subtle nature of this transition. This is unusual, given that such a high transition temperature is expected to be associated with the presence of a large CDW gap. This is confirmed through investigation of the Fermi surface and through analysis of momentum distribution curves. It is possible that changes are subtle and occur below current sensitivity of our measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Datasets for Custom-trained Machine-learning Interatomic Potentials: Nitric Acid Aqueous Solution

This dataset was generated using an iterative active learning strategy with the ArcaNN software package (https://github.com/arcann-chem/arcann_training) to train machine-learning interatomic potentials (MLIPs) for aqueous nitric acid. Each active-learning cycle consisted of three stages: (1) training, (2) exploration, and (3) labeling. The initial training set comprised approximately 800 randomly selected configurations from a previous study by Lewis et al. (https://doi.org/10.1021/jp205510q), which investigated nitric acid solutions at 2, 3, 4, and 5 mol/L. For all configurations, single-point calculations of atomic forces and total energies were performed at the quantum density functional theory BLYP-D2 and PBE-D3 levels of theory using the CP2K Quickstep module. Valence electrons were treated explicitly, while core electrons on all atoms were represented by norm-conserving Goedecker–Teter–Hutter (GTH) pseudopotentials. Long-range dispersion interactions were accounted for using Grimme dispersion corrections. Wave functions were expanded in a mixed Gaussian-and-plane-wave scheme using TZV2P-MOLOPT basis sets for all elements and an 800 Ry auxiliary plane-wave cutoff for the electron density. Self-consistent field convergence was accelerated using orbital transformation and Direct Inversion in the Iterative Subspace, with a convergence threshold of 10^{-6}. All single-point calculations were carried out in periodic orthorhombic cells whose dimensions match those of the molecular configurations sampled from earlier trajectories. The CELL_REF keyword in CP2K was used to define a fixed reference cell, ensuring consistency in the reference data used for MLIP training, particularly when cell fluctuations are present in NpT simulations. The resulting high-fidelity energies and forces constitute the ground-truth labels used to train the MLIPs contained in this dataset.

Dinpajooh, Mohammadhasan [Pacific Northwest Nation↗
DOE OSTI2018

Mn{sub Ga} Acceptor Center in GaAs (Review)

The model of the Mn{sub Ga} acceptor in GaAs in which initial ground state of a coupled hole Γ{sub 8} is changed due to the antiferromagnetic exchange interaction with five 3d electrons of the Mn core is described. The acceptor energy spectrum and the wave functions of its states and also their changes under action of deformations, electric and magnetic fields are considered. Expressions are presented for the description of various properties of isolated Mn{sub Ga} acceptors in GaAs, and the data of some experiments (changes in the Mn{sub Ga}{sup 0} luminescence and absorption spectra and polarization under uniaxial pressures and in magnetic field, EPR spectra, temperature dependence of the magnetic susceptibility, circular polarization of photoluminescence during excitation by polarized light in magnetic field, etc.) are analyzed. It is demonstrated that, in some cases, it is necessary to take into account the existence of random electric and strain fields splitting the acceptor states in the crystal. The analysis results show that this model agrees well with most of the experimental results. The exchange interaction constant is in the range of 3–5 meV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

1D PIC-DSMC analysis of a high-pressure nanosecond pulse discharge breakdown in helium

Kinetic simulations of plasma phenomena during and after formation of the conductive plasma channel of a nanosecond pulse discharge are analyzed and compared to existing experimental measurements. Particle-in-cell with direct simulation Monte Carlo collisions (PIC-DSMC) modeling is used to analyze a discharge in helium at 200 Torr and 300 K over a 1 cm gap. The analysis focuses on physics that would not be reproduced by fluid models commonly used at this high number density and collisionality, specifically non-local and stochastic phenomena. Similar analysis could be used to improve the predictive capability of lower fidelity or reduced order models. First, the modeling results compare favorably with experimental measurements of electron number density, temperature, and 1D electron energy distribution function at the same conditions. Second, it is shown that the ionization wave propagates in a stochastic, stepwise manner, dependent on rare, random ionization events ahead of the ionization wave when the ionization fraction in front of the ionization wave is very low, analagous to the stochastic branching of streamers in 3D. Third, analysis shows high-energy runaway electrons accelerated in the cathode layer produce electron densities in the negative glow region over an order of magnitude above those in the positive column. Finally, future work to develop reduced order models of these two phenomena would improve the accuracy of fluid plasma models without the cost of PIC-DSMC simulations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Charge-Density-Wave Thin-Film Devices Printed with Chemically Exfoliated 1T-TaS 2 Ink

In this work, we report on the preparation of inks containing fillers derived from quasi-two-dimensional charge-density-wave materials, their application for inkjet printing, and the evaluation of their electronic properties in printed thin-film form. The inks were prepared by liquid-phase exfoliation of CVT-grown 1T-TaS 2 crystals to produce fillers with nm-scale thickness and μm-scale lateral dimensions. Exfoliated 1T-TaS 2 was dispersed in a mixture of isopropyl alcohol and ethylene glycol to allow fine-tuning of filler particles thermophysical properties for inkjet printing. The temperature-dependent electrical and current fluctuation measurements of printed thin films demonstrated that the charge-density-wave properties of 1T-TaS 2 are preserved after processing. The functionality of the printed thin-film devices can be defined by the nearly commensurate to the commensurate charge-density-wave phase transition of individual exfoliated 1T-TaS 2 filler particles rather than by electron-hopping transport between them. The obtained results are important for the development of printed electronics with diverse functionality achieved by the incorporation of quasi-two-dimensional van der Waals quantum materials.

1T-TaS2↗
DOE OSTI2018

Investigation of Transport Properties of Some Superconductor Nickel-Based Antiperovskite XNNi{sub 3} (X = Mg, Al, Cu, Zn, Ga, Ag, Cd, In, Sn, Sb, Pt and Pb)

We report, in this work, a theoretical study of electronic and transport (thermoelectric) properties of some superconductor nickel-based antiperovskite XNNi{sub 3} (X = Mg, Al, Cu, Zn, Ga, Ag, Cd, In, Sn, Sb, Pt and Pb) using first-principles calculations with the full-potential linearized augmented plane wave (FPLAPW) method based on the density functional theory (DFT) as implemented in the WIEN2k package. Electronic properties are calculated and show that the studied materials are of metallic type which is in good agreement with experimental data. The Seebeck coefficient, thermal conductivity, electrical conductivity and figure of merit were reported. The results obtained show that the zinc (Zn) and silver (Ag) materials are characterized by a high value of the figure of merit at room temperature (300 K) which is respectively 0.86 and 1.02 in a p-type region. In the case of the transition metals, the maximum values of S increase in going from the Pt atom to the Zn atom and then decrease for the Cd atom. Furthermore, the Wiedemann–Franz law which states that the ratio of thermal to electrical conductivity for metals is constant is well verified in this work. The electric conductivity values are almost invariant with the temperature except for the case of MgNNi{sub 3} and AgNNi{sub 3} compounds in which it increases with T slightly. So, the superconducting materials based on silver and zinc are the best for the thermoelectric applications at room temperature due to the very important value of the factor of merit and the Seebeck coefficient obtained.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Shake-up and shake-off spectra in the electron capture decay of atomic $^7$Be

The most stringent laboratory-based experimental limits on the existence of sub-MeV sterile neutrinos are currently set by decay spectroscopy of radioactive $^7$Be embedded into superconducting sensors. The systematic uncertainties are dominated by the modeling of the electron shake-up and shake-off spectra that are not based on state-of-the-art atomic theory and do not include electron correlations or relativistic effects. We have used the multiconfiguration Dirac-Fock formalism to obtain correlated wavefunctions ab initio and compute all single and double shake processes in the electron capture decay of atomic $^7$Be. The simulations can explain some but not all of the observed spectral features, likely because the wave functions are modified by the Ta sensor material that the $^7$Be is embedded into. The new models also show that the L/K electron capture ratio of $^7$Be in Ta has previously been slightly underestimated revising the previous value of 0.070(7) to a new value of 0.0756(20).

Atomic Physics (physics.atom-ph)↗
DOE OSTI2024

Intermittency, bursty turbulence, and ion and electron phase-space holes formation in collisionless current-carrying plasmas

In the previous studies of nonlinear saturation of the Buneman instability caused by high electron drift velocity relative to ions, the phase-space holes and the plateau on the electron velocity distribution function were identified as features of the saturation stage of instability [notably in the paper by Omura et al., J. Geophys. Res. 108, 1197 (2003)]. We have performed a much longer simulation of the Buneman instability and observed a secondary instability. This secondary instability generates fast electron-acoustic waves. By analyzing the phase-space plot of ions and electrons, we show that the fast electron heating and the formation of the plateau of electron velocity distribution function are not due to the quasi-linear diffusion but due to the nonlinear interaction of ion- and electron-acoustic solitary waves (phase-space holes) by exchange of trapped electrons in each wave. We also report the details on the intermittent and bursty nature of turbulence driven by this instability.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Andreev Reflection and Klein Tunneling in High-Temperature Superconductor-Graphene Junctions

Scattering processes in quantum materials emerge as resonances in electronic transport, including confined modes, Andreev states, and Yu-Shiba-Rusinov states. However, in most instances, these resonances are driven by a single scattering mechanism. Here, in this paper, we show the appearance of resonances due to the combination of two simultaneous scattering mechanisms, one from superconductivity and the other from graphene p-n junctions. These resonances stem from Andreev reflection and Klein tunneling that occur at two different interfaces of a hole-doped region of graphene formed at the boundary with superconducting graphene due to proximity effects from Bi 2 Sr 2 Ca 1 Cu 2 O 8+δ . The resonances persist with gating from p + -p and p-n configurations. The suppression of the oscillation amplitude above the bias energy which is comparable to the induced superconducting gap indicates the contribution from Andreev reflection. Our experimental measurements are supported by quantum transport calculations in such interfaces, leading to analogous resonances. Our results put forward a hybrid scattering mechanism in graphene–high-temperature superconductor heterojunctions of potential impact for graphene-based Josephson junctions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Electronic structure of NdO via slow photoelectron velocity-map imaging spectroscopy of NdO –

Electronically excited NdO is a possible product of the chemistry associated with the release of Nd into the ionosphere, and emission from these states may contribute to the observations following such experiments. To better characterize the energetics and spectroscopy of NdO, we report a combined experimental and theoretical study using slow photoelectron velocity-map imaging spectroscopy of cryogenically cooled NdO – anions (cryo-SEVI) supplemented by wave function-based quantum-chemical calculations. Using cryo-SEVI, we measure the electron affinity of NdO to be 1.0091(7) eV and resolve numerous transitions to low-lying electronic and vibrational states of NdO that are assigned with the aid of the electronic structure calculations. Additionally, temperature-dependent data suggest contributions from the (2)4.5 state of NdO – residing 2350 cm –1 above the ground anion state. Finally, photodetachment to higher-lying excited states of NdO is also reported, which may help to clarify observations from prior release experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Shake loss intensities in x-ray photoelectron spectroscopy: Theory, experiment, and atomic composition accuracy for MgO and related compounds

The relative intensities of XPS core levels, scaled by their photoionization cross sections, are regularly used to determine sample atomic composition. Cross sections, however, give the intensity to all possible final states for the core ionizations, not just to the main peak. This includes all intrinsic satellite structure (shake states and, for open shell systems, the different ionic multiplets). In practice, for solids, this is usually experimentally impossible to determine accurately because such a satellite structure sits on the inelastically scattered electron background and cannot be easily separated. Therefore, usually, only the intensity of the main peak is used. This limits the ultimate possible accuracy of XPS composition determination. The purpose of the present paper is to examine the contributions that a theoretical analysis of losses of intensity can make to improve quantitation. For an MgO single crystal, we show that the correct stoichiometry of 1:1 can be recovered using the theoretical analysis of the experimental MgO peak ratio intensities. For materials with a sufficient bandgap for the XPS main peaks to be separated from the scattered background, the intensity of main peaks can often be accurately determined. Thus, if one uses theory to calculate that fraction of the total intensity lost from a main peak into all its satellite structure, the intensity of just main peaks could then be used to more accurately determine relative atom % composition. This work tests this approach using a single crystal MgO (50% Mg, 50% O) standard. Ab initio electronic structure theory of representative MgO clusters is used to determine Hartree–Fock wave functions for the ground state and final ionized states corresponding to the main Mg 2p and O1s XPS peaks of the oxide. The sudden approximation, SA, is used to determine the fractional losses from these main peaks to shake satellites, which is found to be greater for O1s than Mg2p. This results in predicted “apparent composition” for stoichiometric MgO of 55.2% Mg, 44.8% O instead of the true 50% Mg, 50% O. Equivalent theory for CaO results in a predicted apparent Ca value of 53.4%. Experimentally, using Mg2s or 2p intensity ratio to O1s, we find values between 52.2% and 56.0% Mg using two crystals and four different instrument electron pass energies. The average value of the measurements is 54.5% Mg when corrected for the presence of an adventitious carbon overlayer and slight surface hydroxide. Though this agreement with theory may be somewhat fortuitous, given the potential experimental errors, which are fully discussed, it is similar to that in our earlier study on LiF. We also present preliminary experimental data on Mg(OH) 2 and MgSO 4 , which show a similar trend of apparently higher than 50% Mg, but we have no theory values. We are not yet able to experimentally test for validation of the difference between apparent composition for MgO (55.2% Mg) and CaO (53.4% Ca), owing to significant carbonate formation at the surface of the single crystal CaO. Here, an important conclusion is that the theoretical determination of shake losses, obtained with ab initio wavefunctions and the SA, is likely to be a useful way to calibrate the accuracy and reliability of compositions obtained from XPS intensities and merits further study.

47 OTHER INSTRUMENTATION↗
DOE OSTI2017

Generation of auroral kilometric radiation by a finite-size source in a dipole magnetic field. Part II

Propagation and amplification of extraordinary electromagnetic waves in a dipole magnetic field in a narrow 3D plasma cavity in which a weakly relativistic electron beam propagates along the magnetic field in the direction of the gradient of the magnetic field strength is investigated. The domain of wave vectors at the starting point for which the wave amplification factors at the output of the density cavity reach their maximum values is found, and the amplification factor as a function of the wave frequency is determined. It is shown that the longitudinal velocity of fast electrons, which enables generation of waves in a broader frequency range, plays an important role in the formation of the spectrum of the auroral kilometric radiation (AKR). In this case, waves with the largest amplification factors at the output of the cavity have frequencies exceeding the cutoff frequency of the background plasma at the wave generation altitude. The global inhomogeneity of the magnetic field and plasma density, which governs the residence time of the waves in the amplification region, plays a key role in the formation of the AKR spectrum. It is shown that this time is the main factor determining the energy of the waves emerging from the source.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Revealing quasi-excitations in the low-density homogeneous electron gas with model exchange–correlation kernels

Time-dependent density functional theory within the linear response regime provides a solid mathematical framework to capture excitations. The accuracy of the theory, however, largely depends on the approximations for the exchange–correlation (xc) kernels. Away from the long-wavelength (or q = 0 short wave-vector) and zero-frequency (ω = 0) limit, the correlation contribution to the kernel becomes more relevant and dominant over exchange. The dielectric function, in principle, can encompass xc effects relevant to describe low-density physics. Furthermore, besides collective plasmon excitations, the dielectric function can reveal collective electron–hole excitations, often dubbed “ghost excitons.” Besides collective excitons, the physics of the low-density regime is rich, as exemplified by a static charge-density wave that was recently found for r s > 69, and was shown to be associated with softening of the plasmon mode. These excitations are seen to be present in much higher density 2D homogeneous electron gases of r s ≳ 4. Here, in this work, we perform a thorough analysis with xc model kernels for excitations of various nature. The uniform electron gas, as a useful model of real metallic systems, is used as a platform for our analysis. We highlight the relevance of exact constraints as we display and explain screening and excitations in the low-density region.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electronic properties of ThC − and ThC

The present study investigates the properties of low-lying states of ThC − and ThC using correlated wave function theories. To this end, we employed multireference calculations and various coupled-cluster approaches in combination with large correlation-consistent basis sets. These methods were applied to examine potential energy curves (PECs), electron configurations, energetics, spectroscopic constants, and spin–orbit coupling effects for 9 states of ThC − and 18 states of ThC. The ground states of ThC − and ThC were identified as single-reference 2 Σ + 1/2 (I) and $^3Σ^+_{0^-} (\textrm{I})$, respectively. Electron detachment from the 7s orbital of the Th center in ThC − [ 2 Σ + (I); 1σ 2 2σ1 3 σ2 1 π 4 ] yields ThC [ 3 Σ + (I); 1σ 2 2σ 1 3σ 1 1π 4 ]. The calculated adiabatic detachment energy (ADE) and vertical detachment energy (VDE) for this process are 1.591 and 1.604 eV, respectively. Furthermore, the dissociation energy (D 0 ) of ThC [$^3Σ^+_{0^-} (\textrm{I})$] is predicted to be 5.099 eV. The standard enthalpy of formation, $ΔH^{°}_{\textrm{f}}$ (298 K), of ThC is estimated to be 822.52 ± 6 kJ mol −1 .

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Real-Time Time-Dependent Electronic Structure Theory

Real-time electronic structure methods provide an unprecedented view of electron dynamics and ultrafast spectroscopy on the atto- and femtosecond time scale with vast potential to yield new insights into the electronic behavior of molecules and materials. Here, we discuss the fundamental theory underlying various real-time electronic structure methods as well as advantages and disadvantages of each. We give an overview of the numerical techniques that are widely used for real-time propagation of the quantum electron dynamics with an emphasis on Gaussian basis set methods. We also showcase many of the chemical applications and scientific advances made by using real-time electronic structure calculations and provide an outlook of possible new directions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗