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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 811 records · Page 45
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Calculation of electron-ion temperature equilibration rates and friction coefficients in plasmas and liquid metals using quantum molecular dynamics

In this work, we discuss a method to calculate with quantum molecular dynamics simulations the rate of energy exchanges between electrons and ions in two-temperature plasmas, liquid metals, and hot solids. Promising results from this method were recently reported for various materials and physical conditions. Like other ab initio calculations, the approach offers a very useful comparison with the experimental measurements and permits an extension into conditions not covered by the experiments. The energy relaxation rate is related to the friction coefficients felt by individual ions due to their nonadiabatic interactions with electrons. Each coefficient satisfies a Kubo relation given by the time integral of the autocorrelation function of the interaction force between an ion and the electrons. These Kubo relations are evaluated using the output of quantum molecular dynamics calculations in which electrons are treated in the framework of finite-temperature density functional theory. The calculation presents difficulties that are unlike those encountered with the Kubo formulas for the electrical and thermal conductivities. In particular, the widely used Kubo-Greenwood approximation is inapplicable here. Indeed, the friction coefficients and the energy relaxation rate diverge in this approximation since it does not properly account for the electronic screening of electron-ion interactions. The inclusion of screening effects considerably complicates the calculations. We discuss the physically motivated approximations we applied to deal with these complications in order to investigate a widest range of materials and physical conditions. Unlike the standard method used for the electronic conductivities, the Kubo formulas are evaluated directly in the time domain and not in the energy domain, which spares one from needing to introduce an extraneous undetermined numerical parameter to account for the discrete character of the numerical density of states. We highlight interesting properties of the energy relaxation rate not shared by other electronic properties, in particular its self-averaging character. We then present a detailed parametric and convergence study with the numerical parameters, including the system size, the number of bands and k-points, and the physical approximations for the dielectric function and the exchange-correlation energy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Materials Dynamics

The Materials Dynamics area of leadership focuses on understanding process-structure-properties-performance (PSPP) relationships for the extreme conditions of dynamic loading. This research encompasses controlled synthesis of materials to meet dynamic performance requirements and entails computational coupling across length and time scales for three-dimensional microstructure modeling. For this leadership area, we define dynamic loading as strain rates ≥ 10 3 /s and often, high pressures. A key grand challenge of this area is to predict and measure the evolution of microstructural phases, defect structures, and electronic structure under dynamic conditions while also measuring local temperature to understand transition states. Solving this challenge will require agile, multi-dimensional data analysis and interpretation capability.

36 MATERIALS SCIENCE↗
DOE OSTI2022

2D Reconstruction of Magnetotail Electron Diffusion Region Measured by MMS

Models for collisionless magnetic reconnection in near-Earth space are distinctly characterized as 2D or 3D. In 2D kinetic models, the frozen-in law for the electron fluid is usually broken by laminar dynamics involving structures set by the electron orbit size, while in 3D models the width of the electron diffusion region is broadened by turbulent effects. We present an analysis of in situ spacecraft observations from the Earth's magnetotail of a fortuitous encounter with an active reconnection region, mapping the observations onto a 2D spatial domain. While the event likely was perturbed by low-frequency 3D dynamics, the structure of the electron diffusion region remains consistent with results from a 2D kinetic simulation. As such, the event represents a unique validation of 2D kinetic, and laminar reconnection models.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1977

Cosmic rays in a dynamical halo. I - Age and matter traversal distributions and anisotropy for nuclei. II - Electrons

Recent measurements of the mean lifetime of galactic cosmic rays (at least 10 million yr) have suggested a dynamical halo model of cosmic-ray confinement to the Galaxy. A one-dimensional version of the model is analyzed to determine the ranges of parameters required to give self-consistent values of the mean lifetime, matter traversed, anisotropy, and interstellar gamma-ray flux. It is found that the ranges of the parameters are: disk scale height of 4000-10,000 pc, average convection velocity of no more than 60 km/s, and diffusion coefficient of (3-10) by 10 to the 28th power sq cm/sec for particles with charges of the order of 10 GV. Some consequences for this model of a much shorter lifetime are also discussed. The energy spectrum and spatial distribution of electrons in the dynamical halo model are considered. A gradual steepening of the electron energy spectrum beginning at several GeV energy is found, as indicated by observations. The decrease of electron density with height in the halo depends on the particle energy and may be much steeper than that for nuclei. The models give a halo with a scale height of the order of 3 kpc for several-GeV electrons, which is shown to be consistent with radio observations.

Owens, A. J.↗
DOE OSTI2024

Exciton polaron formation and hot-carrier relaxation in rigid Dion–Jacobson-type two-dimensional perovskites

The efficiency of two-dimensional Dion–Jacobson-type materials relies on the complex interplay between electronic and lattice dynamics; however, questions remain about the functional role of exciton–phonon interactions. Here we establish the robust polaronic nature of the excitons in these materials at room temperature by combining ultrafast spectroscopy and electronic structure calculations. We show that polaronic distortion is associated with low-frequency (30–60 cm –1 ) lead iodide octahedral lattice motions. More importantly, we discover how targeted ligand modification of this two-dimensional perovskite structure manipulates exciton–phonon coupling, exciton polaron population and carrier cooling. At high excitation density, stronger exciton–phonon coupling increases the hot-carrier lifetime, forming a hot-phonon bottleneck. Furthermore, our study provides detailed insight into the exciton–phonon coupling and its role in carrier cooling in two-dimensional perovskites relevant for developing emerging hybrid semiconductor materials with tailored properties.

36 MATERIALS SCIENCE↗
NASA NTRS1990

The electron signature of parallel electric fields

Dynamics Explorer I High-Altitude Plasma Instrument electron data are presented. The electron distribution functions have characteristics expected of a region of parallel electric fields. The data are consistent with previous test-particle simulations for observations within parallel electric field regions which indicate that typical hole, bump, and loss-cone electron distributions, which contain evidence for parallel potential differences both above and below the point of observation, are not expected to occur in regions containing actual parallel electric fields.

Burch, J. L.↗
DOE OSTI2022

Tuning discharge voltage by Schottky electron barrier in P2-Na 2/3 Mg 0.205 Ni 0.1 Fe 0.05 Mn 0.645 O 2

Recently, Mg doped Na metal oxide layered cathode compounds have attracted strong interest for Na-ion battery applications. We report a new type of asymmetric phase evolution between charge and discharge is found to show much-enhanced discharge voltage in P2-Na 2/3 Mg 0.205 Ni 0.1 Fe 0.05 Mn 0.645 O 2 over the parent cathode compound. P2 solid solution is found to show an abnormal coexistence with O2-P2 two-phase reaction during discharge with simultaneous reduction of O, Ni, and Fe redoxes, distinct from the conventional P2-O2 two-phase reaction in the charge. Our analysis suggests that the P2 and O2 two-phase boundary forms a novel unidirectional Schottky barrier to impede electron and Na diffusions in discharge only, thus making the kinetically preferred P2 solid solution phase abnormally coexist with the two-phase region for high discharge voltage and low polarization. Our work demonstrates tuning dynamic evolution of electronic Schottky barrier as a new dimension for advanced kinetic design of high-performance battery cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2020

Hetero-site Double Core Ionization Energies with Sub-electronvolt Accuracy from Delta-Coupled-Cluster Calculations

Benchmark scalar-relativistic delta-coupled-cluster calculations of hetero-site double core ionization energies of small molecules containing second-row elements are reported. The present study has focused on the high-spin triplet components of two-site double core-ionized states, which are single reference in character and consistent with the use of standard coupledcluster methods. Contributions to computed double core ionization energies from electron-correlation and basis-set effects as well as corrections to the core-valence separation approximation have been analyzed. Furthermore, on the basis of systematic convergence of computational results with respect to these effects, delta-coupled-cluster calculations have been shown to be capable of providing accurate double core ionization energies with remaining errors estimated to be below 0.3 eV, and thus they are recommended for use to facilitate experimental studies of two-site double core-ionized states that are involved in X-ray pump/X-ray probe studies of electronic and molecular dynamics following inner shell ionization or excitation.

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

Efficient time-dependent orbital-free density functional theory: Semilocal adiabatic response

Orbital-free density functional theory and its time-dependent extension are efficient ab initio methods for calculating the electronic structure and dynamics of large systems. Through the calculation of the optical spectra of selected clusters, we reach three important conclusions: (1) The quality of the spectra is strongly affected by the quality of the corresponding ground-state electron density; (2) the adiabatic part of the electronic response to external perturbations can be safely evaluated at the semilocal level; and (3) the nonadiabatic, current-dependent part of the time-dependent Pauli potential is key to recover correct spectral envelopes.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Slow Auger Recombination of Trapped Excitons Enables Efficient Multiple Electron Transfer in CdS–Pt Nanorod Heterostructures

We report solar-to-fuel conversion reaction often requires multiple proton-coupled electron transfer (PCET) processes powered by the energetic electrons and/or holes generated by the absorption of multiple photons. The effective coupling of multiple electron transfer from the light absorber with the multiple PCET reactions at the catalytic center is one of the key challenges in efficient and selective conversion of solar energy to chemical fuels. In this paper, we examine the dynamics of multiple electron transfer in quantum confined CdS nanorods with a Pt tip, in which the CdS rod functions as the light absorber and the Pt tip the catalytic center. By excitation-fluence-dependent transient absorption spectroscopic measurements, we show that the multiexciton Auger recombination rate in CdS rods follows a carrier-collision model, k n A = n 2 (n – 1)/4k 2 A , with a biexciton lifetime (1/k 2 A ) of 2.0 ± 0.2 ns. In CdS–Pt nanorods, electron transfer kinetics from the CdS conduction band edge to the Pt show negligible dependence on the excitation fluence, occurring with a half-life time of 5.6 ± 0.6 ps. The efficiency of multiple exciton dissociation by multiple electron transfer to Pt decreases from 100% in biexciton states to ~41% at 22 exciton state due to the competition with Auger recombination. The half-lifetime of the n-charge separated state recombination (with n electrons in the Pt and n holes in the CdS) decreases from 10 μs in the single charge separated state to 42 ns in nine charge separated states. Our findings suggest the possibility of driving multielectron photocatalytic reactions under intense illumination and controlling product selectivity through multielectron transfer.

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

Non-Empirical and Self-Interaction Corrections for DFTB: Towards Accurate Quantum Simulations for Large Mesoscale Systems (Final Report)

This project was comprised of two complementary (but parallel) thrusts: (1) implementing massively-parallelized computing hardware (with new computational hardware that may replace GPUs) in the density functional tight binding (DFTB) approach and (2) developing new capabilities in DFTB to calculate the electronic structure and dynamics of large chemical systems. While classical molecular dynamics can handle hundreds of thousands of atoms, it cannot provide a first-principles based description of chemical systems at the quantum level. At the other extreme, conventional Kohn-Sham DFT methods can probe the true quantum mechanical nature of chemical systems; however, these methods cannot tackle the large sizes and length scales relevant to dynamics simulations of realistic systems. The DFTB formalism utilized in this project provides a viable approach for probing these large systems at a quantum mechanical level of detail. However, to utilize the DFTB approach for accurate calculations of electronic properties, it is crucial to incorporate quantum-based corrections in DFTB since exchange-correlation effects can still remain very strong in these large systems. At the same time, enhancing the computational efficiency of DFTB is also essential since optimal computational performance is required for addressing the large size scales associated with realistic chemical systems. As such, the new non-empirical corrections and computing hardware enhancements implemented in this project will enable accurate and computationally efficient approaches to directly probe electronic properties in these large, complex systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Reduction of electron-phonon coupling in warm dense iron

The electron-ion relaxation dynamics in warm dense iron were investigated by time-resolved x-ray absorption near-edge spectroscopy (XANES). A novel analysis, combining ab initio density functional theory (DFT) and two temperature model (TTM) simulations, was developed to calculate the x-ray absorption spectra as a function of delay time. Here we present experimental evidence of changes at the XAS L3 edge of iron that are consistent with the reduction of the electron-phonon coupling under warm dense matter conditions. The experimental results are in agreement with the model that takes both the electron ($T_e$) and the ion temperature ($T_i$) dependence of the thermophysical properties into consideration, while models where either constant electron-phonon coupling factor (G) or only $T_e$- dependent G are used do not agree with the observed relaxation dynamics of iron.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2003

Flywheels Upgraded for Systems Research

With the advent of high-strength composite materials and microelectronics, flywheels are becoming attractive as a means of storing electrical energy. In addition to the high energy density that flywheels provide, other advantages over conventional electrochemical batteries include long life, high reliability, high efficiency, greater operational flexibility, and higher depths of discharge. High pulse energy is another capability that flywheels can provide. These attributes are favorable for satellites as well as terrestrial energy storage applications. In addition to energy storage for satellites, the several flywheels operating concurrently can provide attitude control, thus combine two functions into one system. This translates into significant weight savings. The NASA Glenn Research Center is involved in the development of this technology for space and terrestrial applications. Glenn is well suited for this research because of its world-class expertise in power electronics design, rotor dynamics, composite material research, magnetic bearings, and motor design and control. Several Glenn organizations are working together on this program. The Structural Mechanics and Dynamics Branch is providing magnetic bearing, controls, and mechanical engineering skills. It is working with the Electrical Systems Development Branch, which has expertise in motors and generators, controls, and avionics systems. Facility support is being provided by the Space Electronic Test Engineering Branch, and the program is being managed by the Space Flight Project Branch. NASA is funding an Aerospace Flywheel Technology Development Program to design, fabricate, and test the Attitude Control/Energy Storage Experiment (ACESE). Two flywheels will be integrated onto a single power bus and run simultaneously to demonstrate a combined energy storage and 1-degree-of-freedom momentum control system. An algorithm that independently regulates direct-current bus voltage and net torque output will be experimentally demonstrated.

Jansen, Ralph H.↗
DOE OSTI2023

Dissociation dynamics of ion-pair states accessed by low-energy electron collisions

Abstract Ion-pair (IP) states are the superexcited states of the neutral molecule that dissociate as a pair of positive and negative ions. These states are generally present near the ionization continuum of the molecule. IP states can be accessed by using photoexcitation or by using the electron collision technique. Different photoexcitation techniques are widely used over the years to study the threshold (threshold IP production spectroscopy) and the dynamics (IP imaging spectroscopy) of the IP states. However, the electron collision technique is ignored over the years and only a few studies are available. In this review, we will discuss different experimental techniques to probe IP states by using electron collision and also the dynamics of the IP states that are accessed by the electron collision.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

eReaxFF force field development for BaZr 0.8 Y 0.2 O 3-δ solid oxide electrolysis cells applications

The use of solid-oxide materials in electrocatalysis applications, especially in hydrogen-evolution reactions, is promising. However, further improvements are warranted to overcome the fundamental bottlenecks to enhancing the performance of solid-oxide electrolysis cells (SOECs), which is directly linked to the more-refined fundamental understanding of complex physical and chemical phenomena and mass exchanges that take place at the surfaces and in the bulk of electrocatalysis materials. Here, we developed an eReaxFF force field for barium zirconate doped with 20 mol% of yttrium, BaZr 0.8 Y 0.2 O 3-δ (BZY20) to enable a systematic, large-length-scale, and longer-timescale atomistic simulation of solid-oxide electrocatalysis for hydrogen generation. All parameters for the eReaxFF were optimized to reproduce quantum-mechanical (QM) calculations on relevant condensed phase and cluster systems describing oxygen vacancies, vacancy migrations, electron localization, water adsorption, water splitting, and hydrogen generation on the surfaces of the BZY20 solid oxide. Using the developed force field, we performed both zero-voltage (excess electrons absent) and non-zero-voltage (excess electrons present) molecular dynamics simulations to observe water adsorption, water splitting, proton migration, oxygen-vacancy migrations, and eventual hydrogen-production reactions. Based on investigations offered in the present study, we conclude that the eReaxFF force field-based approach can enable computationally efficient simulations for electron conductivity, electron leakage, and other non-zero-voltage effects on the solid oxide materials using the explicit-electron concept. Moreover, we demonstrate how the eReaxFF force field-based atomistic-simulation approach can enhance our understanding of processes in SOEC applications and potentially other renewable-energy applications.

08 HYDROGEN↗
DOE OSTI2026

Ultrafast One-Dimensional Peierls-Distortion Dynamics in 1⁢T′−Re⁢S 2 Revealed by 4D Electron Microscopy

Rhenium disulfide (ReS 2 ), a prototypical 2D semiconductor with an anisotropic 1⁢T′ structure due to the pronounced Peierls distortion, has demonstrated great potential for polarization-dependent optoelectronics and photonics. Here, we report an ultrafast phase transition occurring within 1 ps, accompanied by a one-dimensional Peierls-distortion relaxation in 1⁢T′−ReS 2 revealed with combined 4D electron microscopy and time-dependent density functional theory calculations. Upon femtosecond laser pulse excitation, the Re-Re dimerization morphology rapidly transforms from a diamond cluster to zigzag chains and persists for several nanoseconds. Here, this ultrafast Peierls-distortion relaxation is further verified by transient changes in optical anisotropy via polarization-dependent transient absorption spectroscopy. Time-dependent density functional theory calculations attribute this novel phase transition to strong correlation between Peierls distortion and impulsive photoexcited carrier doping, predicting a transient band-gap collapse. This Letter opens up an exciting avenue for ultrafast control of Peierls-distortion-induced anisotropy and the metal-insulator transition in 1⁢T′−ReS 2 .

1T’-ReS2↗
DOE OSTI2026

Ultrafast nano-imaging and nano-spectroscopy

Ultrafast pump–probe nano-imaging combines scanning probe-based optical near-field microscopy with ultrafast spectroscopy to enable imaging with deep sub-wavelength spatial resolution, femtosecond temporal resolution and simultaneous spectral resolution. Ultrafast nano-imaging has gained increased attention for its ability to provide far-from-equilibrium excitation and excited-state contrast. With coherent and nonlinear probing, coupled electron, spin and lattice dynamics on elementary timescale and length scale can be resolved. Through nano-movies, ultrafast nano-imaging visualizes correlated quantum dynamics underlying the properties of solid-state materials, semiconductors, molecular electronic, photonic, photovoltaic and other functional materials. With nanometre spatial resolution, this method probes elementary dynamic processes across multiple length scales that are otherwise obscured in conventional ultrafast spectroscopy in which heterogeneities are spatially averaged. Furthermore, this Primer describes the theoretical background and experimental implementation of ultrafast nano-imaging; signal interpretation and modelling; representative examples and a perspective for the future development of the field.

Microscopy↗