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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 631 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Implementation of Perdew–Zunger self-interaction correction in real space using Fermi–Löwdin orbitals

Most widely used density functional approximations suffer from self-interaction error, which can be corrected using the Perdew–Zunger (PZ) self-interaction correction (SIC). We implement the recently proposed size-extensive formulation of PZ-SIC using Fermi–Löwdin Orbitals (FLOs) in real space, which is amenable to systematic convergence and large-scale parallelization. Here, we verify the new formulation within the generalized Slater scheme by computing atomization energies and ionization potentials of selected molecules and comparing to those obtained by existing FLOSIC implementations in Gaussian based codes. The results show good agreement between the two formulations, with new real-space results somewhat closer to experiment on average for the systems considered. We also obtain the ionization potentials and atomization energies by scaling down the Slater statistical average of SIC potentials. The results show that scaling down the average SIC potential improves both atomization energies and ionization potentials, bringing them closer to experiment. Finally, we verify the present formulation by calculating the barrier heights of chemical reactions in the BH6 dataset, where significant improvements are obtained relative to Gaussian based FLOSIC results.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Guiding center and gyrokinetic orbit theory for large electric field gradients and strong shear flows

The guiding center and gyrokinetic theory of magnetized particle motion is extended to the regime of large electric field gradients perpendicular to the magnetic field. A gradient in the electric field directly modifies the oscillation frequency and causes the Larmor orbits to deform from circular to elliptical trajectories. In order to retain a good adiabatic invariant, there can only be strong dependence on a single coordinate at lowest order, so that resonances do not generate chaotic motion that destroys the invariant. When the gradient across magnetic flux surfaces is dominant, the guiding center drift velocity becomes anisotropic in response to external forces and additional curvature drifts must be included. The electric polarization density remains gyrotropic, but both the polarization and magnetization are modified by the change in gyrofrequency. The theory can be applied to shear flows that are even stronger than those observed in the edge transport barrier of a high-performance tokamak (H-mode) pedestal, even if the toroidal field is as small as or even smaller than the poloidal field. Yet, the theory retains a mathematical form that is similar to the standard case and can readily be implemented within existing simulation tools.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Domain wall-magnetic tunnel junction spin–orbit torque devices and circuits for in-memory computing

There are pressing problems with traditional computing, especially for accomplishing data-intensive and real-time tasks, that motivate the development of in-memory computing devices to both store information and perform computation. Magnetic tunnel junction memory elements can be used for computation by manipulating a domain wall, a transition region between magnetic domains, but the experimental study of such devices has been limited by high current densities and low tunnel magnetoresistance. Here, we study prototypes of three-terminal domain wall-magnetic tunnel junction in-memory computing devices that can address data processing bottlenecks and resolve these challenges by using perpendicular magnetic anisotropy, spin–orbit torque switching, and an optimized lithography process to produce average device tunnel magnetoresistance TMR = 171% and average resistance-area product RA = 29 Ω μm2, close to the RA of the unpatterned film. Device initialization variation in switching voltage is shown to be curtailed to 7%–10% by controlling the domain wall initial position, which we show corresponds to 90%–96% accuracy in a domain wall-magnetic tunnel junction full adder simulation. Repeatability of writing and resetting the device is shown. A circuit shows an inverter operation between two devices, showing that a voltage window is large enough, compared to the variation noise, to repeatably operate a domain wall-magnetic tunnel junction circuit. These results make strides in using magnetic tunnel junctions and domain walls for in-memory and neuromorphic computing applications.

Alamdar, Mahshid (ORCID:0000000221732935)↗
DOE OSTI2021

Strongly heat-assisted spin–orbit torque switching of a ferrimagnetic insulator

Ferrimagnetic insulators promise low-power and high-speed spintronic applications, thanks to their insulating nature and fast dynamics near compensation points. In a ferrimagnetic insulator/heavy metal heterostructure, we investigate field- and current-induced magnetization switching at various temperatures and observe distinct magnetization switching behaviors owing to spin-orbit torque (SOT) and heating effect. We have realized SOT switching across the magnetization compensation temperature and discovered that the SOT switching is strongly heat-assisted: the temperature is always above the compensation temperature while the SOT switching happens in our case. Moreover, we show that the SOT efficiency is strongly magnetization-dependent by characterizing the current dependence of SOT efficiency and explaining the anomalous SOT switching back phenomena in the presence of a titled external field. Our results reveal the critical role of Joule heating on the dynamics of magnetic insulators and pave the way for the application of spintronic devices based on magnetic insulators.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ion beam etching dependence of spin-orbit torque memory devices with switching current densities reduced by Hf interlayers

We report on the fabrication of nanoscale, three-terminal in-plane spin–orbit torque switching devices with low switching current densities. Critical parameters in the fabrication process, including the ion beam etching angle and time, were optimized to avoid fabrication defects and improve device yield. Measurements of the magnetic field and current-induced switching behavior of the tunnel junctions demonstrate a sensitivity to the nanopillar aspect ratio, which dictates the nanopillars’ anisotropy and thermal stability. Additionally, we show that the current density required for switching can be reduced and the device thermal stability increased by inserting Hf interlayers into the heterostructure. Micromagnetic simulations are generally consistent with the experimentally observed switching behavior, suggesting an increase in the interfacial perpendicular anisotropy at the CoFeB/MgO interface and the reduction in the Dzyaloshinskii–Moriya interaction at the W/CoFeB interface by the Hf interlayers.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Fermi–Löwdin orbital self-interaction correction of adsorption energies on transition metal ions

Density functional theory (DFT)-based descriptions of the adsorption of small molecules on transition metal ions are prone to self-interaction errors. Here, we show that such errors lead to a large over-estimation of adsorption energies of small molecules on Cu + , Zn + , Zn 2+ , and Mn + in local spin density approximation (LSDA) and Perdew, Burke, Ernzerhof (PBE) generalized gradient approximation calculations compared to reference values computed using the coupled-cluster with single, doubles, and perturbative triple excitations method. These errors are significantly reduced by removing self-interaction using the Perdew–Zunger self-interaction correction (PZ-SIC) in the Fermi–Löwdin Orbital (FLO) SIC framework. In the case of FLO-PBE, typical errors are reduced to less than 0.1 eV. Furthermore, analysis of the results using DFT energies evaluated on self-interaction-corrected densities [DFT(@FLO)] indicates that the density-driven contributions to the FLO-DFT adsorption energy corrections are roughly the same size in DFT = LSDA and PBE, but the total corrections due to removing self-interaction are larger in LSDA.

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

Nuclear–electronic orbital approach to quantization of protons in periodic electronic structure calculations

The nuclear–electronic orbital (NEO) method is a well-established approach for treating nuclei quantum mechanically in molecular systems beyond the usual Born–Oppenheimer approximation. In this work, we present a strategy to implement the NEO method for periodic electronic structure calculations, particularly focused on multicomponent density functional theory (DFT). The NEO-DFT method is implemented in an all-electron electronic structure code, FHI-aims, using a combination of analytical and numerical integration techniques as well as a resolution of the identity scheme to enhance computational efficiency. After validating this implementation, proof-of-concept applications are presented to illustrate the effects of quantized protons on the physical properties of extended systems, such as two-dimensional materials and liquid–semiconductor interfaces. Specifically, periodic NEO-DFT calculations are performed for a trans-polyacetylene chain, a hydrogen boride sheet, and a titanium oxide–water interface. The zero-point energy effects of the protons as well as electron–proton correlation are shown to noticeably impact the density of states and band structures for these systems. These developments provide a foundation for the application of multicomponent DFT to a wide range of other extended condensed matter systems.

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

Molecular dipole moment learning via rotationally equivariant derivative kernels in molecular-orbital-based machine learning

This study extends the accurate and transferable molecular-orbital-based machine learning (MOB-ML) approach to modeling the contribution of electron correlation to dipole moments at the cost of Hartree–Fock computations. A MOB pairwise decomposition of the correlation part of the dipole moment is applied, and these pair dipole moments could be further regressed as a universal function of MOs. The dipole MOB features consist of the energy MOB features and their responses to electric fields. An interpretable and rotationally equivariant derivative kernel for Gaussian process regression (GPR) is introduced to learn the dipole moment more efficiently. The proposed problem setup, feature design, and ML algorithm are shown to provide highly accurate models for both dipole moments and energies on water and 14 small molecules. To demonstrate the ability of MOB-ML to function as generalized density-matrix functionals for molecular dipole moments and energies of organic molecules, we further apply the proposed MOB-ML approach to train and test the molecules from the QM9 dataset. The application of local scalable GPR with Gaussian mixture model unsupervised clustering GPR scales up MOB-ML to a large-data regime while retaining the prediction accuracy. In addition, compared with the literature results, MOB-ML provides the best test mean absolute errors of 4.21 mD and 0.045 kcal/mol for dipole moment and energy models, respectively, when training on 110 000 QM9 molecules. The excellent transferability of the resulting QM9 models is also illustrated by the accurate predictions for four different series of peptides.

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

Molecular-orbital-based machine learning for open-shell and multi-reference systems with kernel addition Gaussian process regression

We introduce a novel machine learning strategy, kernel addition Gaussian process regression (KA-GPR), in molecular-orbital-based machine learning (MOB-ML) to learn the total correlation energies of general electronic structure theories for closed- and open-shell systems by introducing a machine learning strategy. The learning efficiency of MOB-ML(KA-GPR) is the same as the original MOB-ML method for the smallest criegee molecule, which is a closed-shell molecule with multi-reference characters. In addition, the prediction accuracies of different small free radicals could reach the chemical accuracy of 1 kcal/mol by training on one example structure. Accurate potential energy surfaces for the H10 chain (closed-shell) and water OH bond dissociation (open-shell) could also be generated by MOB-ML(KA-GPR). To explore the breadth of chemical systems that KA-GPR can describe, we further apply MOB-ML to accurately predict the large benchmark datasets for closed- (QM9, QM7b-T, and GDB-13-T) and open-shell (QMSpin) molecules.

Chemistry↗
DOE OSTI2022

Electronic states and transitions of PrO and PrO + probed by threshold ionization spectroscopy and spin–orbit multiconfiguration perturbation theory

The precise ionization energy of praseodymium oxide (PrO) seeded in supersonic molecular beams is measured with mass-analyzed threshold ionization (MATI) spectroscopy. Here, a total of 33 spin–orbit (SO) states of PrO and 23 SO states of PrO + are predicted by second-order multiconfigurational quasi-degenerate perturbation (MCQDPT2) theory. Electronic transitions from four low-energy SO levels of the neutral molecule to the ground state of the singly charged cation are identified by combining the MATI spectroscopic measurements with the MCQDPT2 calculations. The precise ionization energy is used to reassess the ionization energies and the reaction enthalpies of the Pr + O → PrO + + e – chemi-ionization reaction reported in the literature. An empirical formula that uses atomic electronic parameters is proposed to predict the ionization energies of lanthanide monoxides, and the empirical calculations match well with available precise experimental measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Tailoring light-induced charge transfer and intersystem crossing in FeCO using time-dependent spin–orbit configuration interaction

Real-time (RT) electronic structure methods provide a natural framework for describing light–matter interactions in arbitrary time-dependent electromagnetic fields (EMF). Optically induced excited state transitions are of particular interest, which require tuned EMF to drive population transfer to and from the specific state(s) of interest. Intersystem crossing, or spin-flip, may be driven through shaped EMF or laser pulses. These transitions can result in long-lived “spin-trapped” excited states, which are especially useful for materials requiring charge separation or protracted excited state lifetimes. Time-dependent configuration interaction (TDCI) is unique among RT methods in that it may be implemented in a basis of eigenstates, allowing for rapid propagation of the time-dependent Schrödinger equation. The recent spin–orbit TDCI (TD-SOCI) enables a real-time description of spin-flip dynamics in an arbitrary EMF and, therefore, provides an ideal framework for rational pulse design. The present study explores the mechanism of multiple spin-flip pathways for a model transition metal complex, FeCO, using shaped pulses designed to drive controlled intersystem crossing and charge transfer. These results show that extremely tunable excited state dynamics can be achieved by considering the dipole transition matrix elements between the states of interest.

Chemistry↗
DOE OSTI2024

Coherent spin wave excitation with radio-frequency spin–orbit torque

Spin waves, collective perturbations of magnetic moments, are both fundamental probes for magnetic physics and promising candidates for energy-efficient signal processing and computation. Traditionally, coherent propagating spin waves have been generated by radio frequency (RF) inductive Oersted fields from current-carrying electrodes. An alternative mechanism, spin–orbit torque (SOT), offers more localized excitation through interfacial spin accumulation but has been mostly limited to DC to kHz frequencies. SOT driven by RF currents, with potentially enhanced pumping efficiency and unique spin dynamics, remains largely unexplored, especially in magnetic insulators. Here, we conduct a comprehensive theoretical and computational investigation into the generation of coherent spin waves via RF-SOT in the prototypical yttrium iron garnet. We characterize the excitation of forward volume, backward volume, and surface modes in both linear and nonlinear regimes, employing single and interdigitated electrode configurations. We reveal and explain several unique and surprising features of RF-SOT compared to inductive excitation, including higher efficiency, distinct mode selectivity, and directional symmetry, a ~ $3π/4$ phase offset, reduced anharmonic distortion in the nonlinear regime, and the absence of second harmonic generation. These insights position RF-SOT as a promising new mechanism for future magnonic and spintronic applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Lagrangian formulation of nuclear–electronic orbital Ehrenfest dynamics with real-time TDDFT for extended periodic systems

Here, we present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear–electronic orbital (NEO) theory and real-time time-dependent density functional theory for extended periodic systems. In addition to a quantum dynamical treatment of electrons and selected protons, this approach allows for the classical movement of all other nuclei to be taken into account in simulations of condensed matter systems. Furthermore, we introduce a Lagrangian formulation for the traveling proton basis approach and propose new schemes to enhance its application for extended periodic systems. Validation and proof-of-principle applications are performed on electronically excited proton transfer in the o-hydroxybenzaldehyde molecule with explicit solvating water molecules. These simulations demonstrate the importance of solvation dynamics and a quantum treatment of transferring protons. This work broadens the applicability of the NEO Ehrenfest dynamics approach for studying complex heterogeneous systems in the condensed phase.

Calculus of variations↗
DOE OSTI2025

Energy conservation in real-time nuclear–electronic orbital Ehrenfest dynamics

Real-time nuclear–electronic orbital Ehrenfest (RT-NEO-Ehrenfest) dynamics methods provide a first-principles approach for describing nonadiabatic molecular processes with nuclear quantum effects. For an efficient description of proton transfer within RT-NEO-Ehrenfest dynamics, the basis function center associated with the quantum proton can be allowed to move classically. Here, this traveling proton basis (TPB) approach effectively captures proton quantum dynamics, although its energy conservation behavior is not yet fully satisfactory. Two recently proposed TPB approaches, in principle, conserve the extended energy, which includes both the system energy and the kinetic energy associated with the proton basis function center. Herein, a thermostatted TPB approach is proposed to improve the conservation of the system energy, excluding the kinetic energy associated with the proton basis function center. In this approach, the quantum proton dynamics are modulated by dynamically rescaling the proton momentum operator to maintain the system energy conservation. With the excited-state intramolecular proton transfer of o-hydroxybenzaldehyde as an example, this approach is shown to significantly improve the system energy conservation while preserving the accuracy of the quantum proton dynamics as achieved in the original TPB approach.

Ehrenfest dynamics↗
DOE OSTI2025

Constrained nuclear–electronic orbital method for periodic density functional theory: Application to H 2 chemisorption on Si(001) surfaces

The nuclear–electronic orbital (NEO) method provides a powerful computational framework for incorporating nuclear quantum effects (NQE) in electronic structure calculations beyond the Born–Oppenheimer approximation. By incorporating additional constraints to the position operator on quantum particles like protons, the NEO method enables calculation of effective potential that accounts for NQE. Here, in this work, we present a new constrained NEO (cNEO) formulation for density functional theory (cNEO-DFT) calculations in the context of extended periodic systems. Using the nudged elastic band method, we discuss an application of the cNEO-DFT approach to studying the adsorption of a hydrogen molecule on the Si(001) surfaces. The calculation shows how NQE impacts the reaction energetics. The proton density changes are computed along the reaction pathways. This work demonstrates the capability of the new cNEO-DFT method to study a wide range of chemical processes, such as surface reactions where the quantum nature of light atoms like protons is non-negligible.

Chemical processes↗
DOE OSTI2024

Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La 1.65 Eu 0.2 Sr 0.15 CuO 4

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump–probe time-resolved resonant X-ray scattering on the (0 0 1) Bragg peak at the Cu L 3 and O K resonances, we investigate nonequilibrium dynamics of Q a = Q b = 0 nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La 1.65 Eu 0.2 Sr 0.15 CuO 4 . The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2 p and Cu 3 d states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Nonstatistical Behavior of the Photoionization of Spin-Orbit Doublets

The photoionization branching ratios of spin-orbit doublets are studied both experimentally and theoretically at energies several keV above threshold. The results show significant relativistic effects for Ar 2p in the autoionizing region below the 1s threshold, and large many-body effects for Xe 3d and 4d in the vicinity of the L-shell thresholds. The branching ratios in Xe are also found to vary significantly over very broad multi-keV energy regions both above and below the inner-shell thresholds. In addition, the Ar 2p study confirms experimentally the decades-old theoretical prediction that the nonresonant branching ratio does not approach the statistical (nonrelativistic) value, and, in fact, progressively diverges from statistical with increasing photon energy.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Voltage and cathode emission mechanisms of a magnetized, constricted, orbiting plasma in helium 6.7–850 Pa

Abstract We present a semiquantitative description of several important properties of a magnetized cold-cathode plasma in helium over a wide pressure range 6.7–850 Pa. We focus on the ‘constricted orbiting’ mode where the plasma attaches to the cathode as a moving ‘dot’ and the voltage and rate of cathode erosion are both unusually low. We propose that the low plasma voltage and observed motion of the plasma adjacent to the cathode can be attributed to field emission as the source of electrons from the cathode, a process that is aided by the charging of an oxide film by ions. We find that the observed dependence of plasma voltage on pressure is consistent with the assumption that the axial electric field must increase in regions of strong crossed magnetic field to maintain current continuity.

Physics↗