Search NASA⌕ Search

SEARCH · Search NASA

Results for “average local ionization energy”

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.

8 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Impact of lanthanide ion complexation and temperature on the chemical reactivity of N , N , N ', N '-tetraoctyl diglycolamide (TODGA) with the dodecane radical cation

The impact of trivalent lanthanide ion complexation and temperature on the chemical reactivity of N,N,N',N'-tetraoctyl diglycolamide (TODGA) with the n-dodecane radical cation (RH˙+) has been measured by electron pulse radiolysis and evaluated by quantum mechanical calculations. Additionally, Arrhenius parameters were determined for the reaction of the non-complexed TODGA ligand with the RH˙ + from 10–40 °C, giving the activation energy (E a = 17.43 ± 1.64 kJ mol –1 ) and pre-exponential factor (A = (2.36 ± 0.05) × 10 13 M –1 s –1 ). The complexation of Nd(III), Gd(III), and Yb(III) ions by TODGA yielded [LnIII(TODGA)3(NO3)3] complexes that exhibited significantly increased reactivity (up to 9.3× faster) with the RH˙ + , relative to the non-complexed ligand: k([Ln III (TODGA) 3 (NO 3 ) 3 ] + RH˙ + ) = (8.99 ± 0.93) × 10 10 , (2.88 ± 0.40) × 10 10 , and (1.53 ± 0.34) × 10 10 M –1 s –1 , for Nd(III), Gd(III), and Yb(III) ions, respectively. The rate coefficient enhancement measured for these complexes exhibited a dependence on atomic number, decreasing as the lanthanide series was traversed. Preliminary reaction free energy calculations—based on a model [Ln III (TOGDA)] 3+ complex system—indicate that both electron/hole and proton transfer reactions are energetically unfavorable for complexed TODGA. Furthermore, complementary average local ionization energy calculations showed that the most reactive region of model N,N,N',N'-tetraethyl diglycolamide (TEDGA) complexes, [Ln III (TEGDA) 3 (NO 3 ) 3 ], toward electrophilic attack is for the coordinated nitrate (NO 3 – ) counter anions. Furthermore, it is possible that radical reactions with the complexed NO 3 – counter anions dominate the differences in rates seen for the [Ln III (TODGA) 3 (NO 3 ) 3 ] complexes, and are likely responsible for the reported radioprotection in the presence of TODGA complexes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Self-interaction-corrected Kohn–Sham effective potentials using the density-consistent effective potential method

Density functional theory (DFT) and beyond-DFT methods are often used in combination with photoelectron spectroscopy to obtain physical insights into the electronic structure of molecules and solids. The Kohn–Sham eigenvalues are not electron removal energies except for the highest occupied orbital. The eigenvalues of the highest occupied molecular orbitals often underestimate the electron removal or ionization energies due to the self-interaction (SI) errors in approximate density functionals. Here, we adapt and implement the density-consistent effective potential method of Kohut, Ryabinkin, and Staroverov (2014) to obtain SI-corrected local effective potentials from the SI-corrected Fermi–Löwdin orbitals and density in the Fermi–Löwdin orbital self-interaction correction scheme. The implementation is used to obtain the density of states (photoelectron spectra) and HOMO–LUMO gaps for a set of molecules and polyacenes. Good agreement with experimental values is obtained compared to a range of SI uncorrected density functional approximations.

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

Self-interaction correction schemes for non-collinear spin-density-functional theory

We extend some of the well-established self-interaction correction (SIC) schemes of density-functional theory—the Perdew–Zunger SIC and the average-density SIC—to the case of systems with noncollinear magnetism. Our proposed SIC schemes are tested on a set of molecules and metallic clusters in combination with the widely used local spin-density approximation. As expected from the collinear SIC, we show that the averaged-density SIC works well for improving ionization energies but fails to improve more subtle quantities like the dipole moments of polar molecules. We investigate the exchange-correlation magnetic field produced by our extension of the Perdew–Zunger SIC, showing that it is not aligned with the local total magnetization, thus producing an exchange-correlation torque.

Chemistry↗
DOE OSTI2023

Gamma-Ray Emission from Galaxies Hosting Molecular Outflows

Many star-forming galaxies and those hosting active galactic nuclei show evidence of massive outflows of material in a variety of phases including ionized, neutral atomic, and molecular. Molecular outflows in particular have been the focus of recent interest as they may be responsible for removing gas from the galaxy, thereby suppressing star formation. As material is ejected from the cores of galaxies, interactions of the outflowing material with the interstellar medium can accelerate cosmic rays and produce high-energy gamma rays. In this work, we search for gamma-ray emission from a sample of local galaxies known to host molecular outflows using data collected by the Fermi Large Area Telescope. We employ a stacking technique in order to search for and characterize the average gamma-ray emission properties of the sample. Gamma-ray emission is detected from the galaxies in our sample at the 4.4σ level with a power-law photon index of Γ ≈ 2 in the 1–800 GeV energy range. The emission is found to correlate with tracers of star formation activity, namely the 8–1000 μm infrared luminosity. We also find that the observed signal can be predominantly attributed to H II galaxies hosting energy-driven outflows. While we do not find evidence suggesting that the outflows are accelerating charged particles directly, galaxies with molecular outflows may produce more gamma rays than galaxies without outflows. In particular, the set consisting of gamma-ray-detected galaxies with molecular outflows are nearly perfect calorimeters and may be future targets for searches of high-energy neutrinos.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Pulse duration dependent effects of ultrafast laser induced damage on a 1030 nm multi-layer dielectric mirror for high repetition rate, high average power laser systems

High repetition rate, high peak, and average power laser systems are crucial for next-generation particle accelerators, inertial confinement fusion, and secondary particle sources. These applications demand durable laser optics, particularly interference coatings on optics lasting millions of shots at high fluence. This study focuses on designing, testing, and simulating multi-layer dielectric (MLD) mirrors for pulse durations of 260 fs, 77 fs, and 25 fs at 1030 nm wavelength and 45-degree incidence angle with p -polarization. S-on-1 laser-induced damage thresholds (LIDT) for varying pulse numbers were determined, with single-shot LIDT values of 0.98 Jcm -2 , 1.63 Jcm -2 , and 2.3 Jcm -2 for 25 fs, 77 fs, and 260 fs respectively. A strong correlation between blister shape and local fluence was observed, implying that the layer expansion in a blister depends on local fluence. We have also examined mechanisms responsible for laser-induced stress generation and energy release rates in blister formation. Damage mechanisms are further explored by finite-difference time-domain (FDTD) simulations, incorporating Keldysh strong field ionization, whose predictions were in excellent agreement with the onset of damage determined experimentally. These findings offer insights for enhancing MLD coating technology, promising more efficient and resilient laser systems for diverse scientific and industrial applications.

Noor, Mohamed Yaseen (ORCID:000000021036644X)↗
DOE OSTI2023

Average-atom model with Siegert states

In plasmas, electronic states can be well-localized bound states or itinerant free states, or something in between. In self-consistent treatments of plasma electronic structure such as the average-atom model, all states must be accurately resolved in order to achieve a converged numerical solution. Furthermore, this is a challenging numerical and algorithmic problem in large part due to the continuum of free states which is relatively expensive and difficult to resolve accurately. Siegert states are an appealing alternative. They form a complete eigenbasis with a purely discrete spectrum while still being equivalent to a representation in terms of the usual bound states and free states. However, many of their properties are unintuitive, and it is not obvious that they are suitable for self-consistent plasma electronic structure calculations. Here it is demonstrated that Siegert states can be used to accurately solve an average-atom model and offer advantages over the traditional finite-difference approach, including a concrete physical picture of pressure ionization and continuum resonances.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Potassium carbonate decomposition modeling within rotating detonation engines for direct power extraction applications

We report that recently, there has been a significant interest in detonation-based combustion systems, such as rotating detonation engines (RDE), due to potential performance advantages in propulsion and energy applications. This includes improvements in thermodynamic efficiency, inherently high gas velocities, and the possibility of achieving an increase in total pressure (i.e. pressure gain) through the combustion process. Due to approximating a constant volume combustion process, these devices also tend to exhibit extremely high local gas temperatures relative to a comparable constant pressure combustor. These advantages overlap well with desirable performance characteristics of direct power extraction (DPE) technologies, such as a magnetohydrodynamic (MHD) generator. Typically, in DPE systems hot combustion products are seeded with an easily ionizable material such as potassium carbonate (K 2 CO 3 ) in order to boost the electrical conductivity. However, due to the short gas residence times within an RDE, it was unclear whether forming an electrically conductive combustion plasma would be feasible for integration with a downstream MHD generator. A model is presented which describes the heating, decomposition, and ionization of solid K 2 CO 3 particles and aqueous solutions of K 2 CO 3 in water, for a given initial particle diameter. This model was combined with available computational fluid dynamics (CFD) data for an oxygen-methane RDE in a one-way coupled Eulerian-Lagrangian framework to predict particle trajectories and the corresponding heating, decomposition, and ionization histories. Electrical conductivities were computed using a previously developed model, and a method was proposed to determine an equivalent average electrical conductivity. Results show that particle sizes below ~30 µm are able to fully decompose before reaching the exit of the RDE. While the one-way coupled nature of the simulations precluded rigorous evaluation of the effects of seed material on detonability, a substantial temperature reduction is expected at the detonation wave front due to heating and decomposition. A preliminary comparison is presented between the RDE and an equivalent constant pressure adiabatic combustor, showing a potential performance advantage for the RDE.

42 ENGINEERING↗
DOE OSTI2022

Reionization time of the Local Group and Local-Group-like halo pairs

ABSTRACT Patchy cosmic reionization resulted in the ionizing UV background asynchronous rise across the Universe. The latter might have left imprints visible in present-day observations. Several numerical simulation-based studies show correlations between the reionization time and overdensities and object masses today. To remove the mass from the study, as it may not be the sole important parameter, this paper focuses solely on the properties of paired haloes within the same mass range as the Milky Way. For this purpose, it uses CoDaII, a fully coupled radiation hydrodynamics reionization simulation of the local Universe. This simulation holds a halo pair representing the Local Group, in addition to other pairs, sharing similar mass, mass ratio, distance separation, and isolation criteria but in other environments, alongside isolated haloes within the same mass range. Investigations of the paired halo reionization histories reveal a wide diversity although always inside-out, given our reionization model. Within this model, haloes in a close pair tend to be reionized at the same time but being in a pair does not bring to an earlier time their mean reionization. The only significant trend is found between the total energy at z = 0 of the pairs and their mean reionization time: Pairs with the smallest total energy (bound) are reionized up to 50 Myr earlier than others (unbound). Above all, this study reveals the variety of reionization histories undergone by halo pairs similar to the Local Group, that of the Local Group being far from an average one. In our model, its reionization time is ∼625 Myr against 660 ± 4 Myr (z ∼ 8.25 against 7.87 ± 0.02) on average.

79 ASTRONOMY AND ASTROPHYSICS↗