Search NASA⌕ Search

SEARCH · Search NASA

Results for “atomic processes”

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 739 records · Page 41
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Early stage oxynitridation process of Si(001) surface by NO gas: Reactive molecular dynamics simulation study

Initial stage of oxynitridation process of Si substrate is of crucial importance in fabricating the ultrathin gate dielectric layer of high quality in advanced MOSFET devices. The oxynitridation reaction on a relaxed Si(001) surface is investigated via reactive molecular dynamics (MD) simulation. A total of 1120 events of a single nitric oxide (NO) molecule reaction at temperatures ranging from 300 to 1000 K are statistically analyzed. The observed reaction kinetics are consistent with the previous experimental or calculation results, which show the viability of the reactive MD technique to study the NO dissociation reaction on Si. We suggest the reaction pathway for NO dissociation that is characterized by the inter-dimer bridge of a NO molecule as the intermediate state prior to NO dissociation. Although the energy of the inter-dimer bridge is higher than that of the intra-dimer one, our suggestion is supported by the ab initio nudged elastic band calculations showing that the energy barrier for the inter-dimer bridge formation is much lower. The growth mechanism of an ultrathin Si oxynitride layer is also investigated via consecutive NO reactions simulation. The simulation reveals the mechanism of self-limiting reaction at low temperature and the time evolution of the depth profile of N and O atoms depending on the process temperature, which would guide to optimize the oxynitridation process condition.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Probing the Effects of Dimethyl Aluminum Isopropoxide Surface Reaction Byproducts on Atomic Layer Deposition Nucleation

Atomic layer deposition (ALD) processes that leverage a myriad of metal–organic and complementary reactant combinations have been identified to realize precise and conformal thin film growth. However, the effects of the ALD reaction byproducts on nucleation and growth mechanisms are rarely considered. Site-selective ALD processes provide an opportunity for the detailed investigation of uniform surface sites with atomistic accuracy. Intentional pretreatment with a known ALD reaction byproduct – isopropanol – enables a significant improvement in the nucleation rate reproducibility of dimethylaluminum isopropoxide and water ALD on rutile TiO 2 (110). In situ spectroscopic ellipsometry reveals a partially reversible byproduct binding that is site-selective for TiO 2 (110) surface oxygen vacancies. First-principles calculations reveal surface site-specific thermodynamics for adsorption of isopropanol and water that may influence ALD nucleation. In conclusion, the sensitivity of site-selective ALD motivates consideration of secondary surface reactions when designing precision deposition processes, including area- or site-selective ALD reactions.

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

Low temperature atomic layer deposition of PbO 2 for electrochemical applications

A low temperature atomic layer deposition (ALD) process for PbO 2 was developed using bis(1-dimethylamino-2-methyl-2-propanolate)lead(II), Pb(DMAMP) 2 , and O 3 as the reactants, with a high growth rate of 2.6 Å/cycle. PbO 2 readily reduces under low oxygen partial pressures at moderate temperatures making it challenging to deposit ALD PbO 2 from Pb 2+ precursors. However, thin films deposited with this process showed small crystalline grains of α-PbO 2 and β-PbO 2 , without signs of reduced PbO x phases. The ALD PbO 2 thin films show the high electrical conductivity characteristic of bulk PbO 2 . In situ measurements of ALD PbO 2 film conductivity during growth suggest a reaction mechanism by which sub-surface oxygen mobility contributes to the growth of resistive PbO or PbO x during the Pb(DMAMP) 2 surface reaction step, which is only fully oxidized from Pb 2+ to Pb 4+ during the O 3 reaction step. These films were electrochemically reduced to PbSO 4 in H 2 SO 4 and then reoxidized to PbO 2 , demonstrating their suitability for use as an electrode material for fundamental battery research and other electrochemical applications.

atomic layer deposition↗
DOE OSTI2012

Efficient laser-induced 6-8 keV x-ray production from iron oxide aerogel and foil-lined cavity targets

The performance of new iron-based laser-driven x-ray sources has been tested at the OMEGA laser facility for production of x rays in the 6.5-8.5 keV range. Two types of targets were experimentally investigated: low-density iron oxide aerogels (density 6-16 mg/cm{sup 3}) and stainless steel foil-lined cavity targets (steel thickness 1-5 {mu}m). The targets were irradiated by 40 beams of the OMEGA laser (500 J/beam, 1 ns pulse, wavelength 351 nm). All targets showed good coupling with the laser, with <5% of the incident laser light backscattered by the resulting plasma in all cases (typically <2.5%). The aerogel targets produced T{sub e}=2 to 3 keV, n{sub e}=0.12-0.2 critical density plasmas yielding a 40%-60% laser-to-x-ray total conversion efficiency (CE) (1.2%-3% in the Fe K-shell range). The foil cavity targets produced T{sub e}{approx} 2 keV, n{sub e}{approx} 0.15 critical density plasmas yielding a 60%-75% conversion efficiency (1.6%-2.2% in the Fe K-shell range). Time-resolved images illustrate that the volumetric heating of low-density aerogels allow them to emit a higher K-shell x-ray yield even though they contain fewer Fe atoms. However, their challenging fabrication process leads to a larger shot-to-shot variation than cavity targets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2013

Reversible Single Spin Control of Individual Magnetic Molecule by Hydrogen Atom Adsorption

The reversible control of a single spin of an atom or a molecule is of great interest in Kondo physics and a potential application in spin based electronics. Here we demonstrate that the Kondo resonance of manganese phthalocyanine molecules on a Au(111) substrate have been reversibly switched off and on via a robust route through attachment and detachment of single hydrogen atom to the magnetic core of the molecule. As further revealed by density functional theory calculations, even though the total number of electrons of the Mn ion remains almost the same in the process, gaining one single hydrogen atom leads to redistribution of charges within 3d orbitals with a reduction of the molecular spin state from S 5 3/2 to S 5 1 that directly contributes to the Kondo resonance disappearance. This process is reversed by a local voltage pulse or thermal annealing to desorb the hydrogen atom.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Mesoscopic transport and interferometry with wave packets of ultracold atoms: Effects of quantum coherence and interactions

We propose a way to simulate mesoscopic transport processes with counterpropagating wave packets of ultracold atoms in quasi-one-dimensional (1D) waveguides and show quantitative agreement with analytical results. The method allows the study of a broad range of transport processes at the level of individual modes, not possible in electronic systems. Typically suppressed effects of quantum coherence become manifest, along with the effects of tunable interactions, which can be used to develop a simpler type of sensitive atom interferometer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Atomic layer deposition of zirconium oxide thin films

In this work, we studied an atomic layer deposition (ALD) process of ZrO 2 with the precursors of tetrakis(dimethylamido)zirconium(IV) and water. We investigated the growth characteristics and mechanism of the ALD ZrO 2 in the temperature range of 50–275 °C. Furthermore, the evolutions of film thickness and morphology were studied and discussed. It was found that the growth rate of ZrO2 decreased almost linearly with the increasing temperature from ~1.81 Å/cycle at 50 °C to ~0.8 Å/cycle at 225 °C. Interestingly, it was revealed that the growth of ZrO 2 films ceased after a certain number of ALD cycles at a temperature higher than 250 °C. Additionally, we also verified that the crystallinity of ZrO 2 evolved with deposition temperature from amorphous to crystalline phase. In addition, the wettability of ZrO 2 films was studied, showing a hydrophobic nature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Effects of the local structure dependence of evaporation fields on field evaporation behavior

Accurate three dimensional reconstructions of atomic positions and full quantification of the information contained in atom probe microscopy data rely on understanding the physical processes taking place during field evaporation of atoms from needle-shaped specimens. However, the modeling framework for atom probe microscopy has only limited quantitative justification. Building on the continuum field models previously developed, we introduce a more physical approach with the selection of evaporation events based on density functional theory calculations. This model reproduces key features observed experimentally in terms of sequence of evaporation, evaporation maps, and depth resolution, and provides insights into the physical limit for spatial resolution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

KLL dielectronic recombination resonant strengths of He-like up to O-like tungsten ions

Dielectronic recombination (DR) is an important process in hot plasma physics as well as in atomic structure and collision theory. This work reports the studies of the KLL DR resonance strengths of He-, Li-, Be-, B-, C-, N-, and O-like tungsten ions, through both experiment and calculation. The experimental resonance strengths were determined within uncertainty below 11% at the Shanghai electron beam ion trap by employing a fast electron beam-energy scanning technique. A fully relativistic configuration interaction method implemented in the flexible atomic code was employed to calculate DR process and also radiative recombination (RR). The consideration of the interference effect between DR and RR was revealed to be necessary to determine the resonance strength.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Single Metal Atom Catalysts Prepared by Diluted Atomic Layer Deposition

The scalable and facile preparation of single-atom catalysts remains a critical challenge. Here, in this study, we introduce diluted atomic layer deposition (DALD), a unique approach for synthesizing supported metal catalysts with precisely tunable loadings. Unlike conventional metal deposition by ALD which uses pure metal precursors, DALD employs a diluted precursor mixture, combining organometallic precursors with the corresponding free ligand in controlled ratios. The method enables precise control over metal loadings, allowing the synthesis of structures ranging from nanoparticles to isolated single atoms, as exemplified by Ir, Rh, and Pt on high-surface-area γ-Al 2 O 3 . With its inherent simplicity and exceptional efficiency in metal precursor utilization, DALD represents a highly scalable strategy, unlocking opportunities for integrating single-atom catalysts into industrial processes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

The Role of SnO2 Processing on Ionic Distribution in Double-Cation-Double Halide Perovskites

Moving toward a future of efficient, accessible, and less carbon-reliant energy devices has been at the forefront of energy research innovations for the past 30 years. Metal-halide perovskite (MHP) thin films have gained significant attention due to their flexibility of device applications and tunable capabilities for improving power conversion efficiency. Serving as a gateway to optimize device performance, consideration must be given to chemical synthesis processing techniques. Therefore, how does common substrate processing techniques influence the behavior of MHP phenomena such as ion migration and strain? Here, we demonstrate how a hybrid approach of chemical bath deposition (CBD) and nanoparticle SnO2 substrate processing significantly improves the performance of (FAPbI3)0.97(MAPbBr3)0.03 by reducing micro-strain in the SnO2 lattice, allowing distribution of K+ from K-Cl treatment of substrates to passivate defects formed at the interface and produce higher current in light and dark environments. X-ray diffraction reveals differences in lattice strain behavior with respect to SnO2 substrate processing methods. Through use of conductive atomic force microscopy (c-AFM), conductivity is measured spatially with MHP morphology, showing higher generation of current in both light and dark conditions for films with hybrid processing. Additionally, time-of-flight secondary ionization mass spectrometry (ToF-SIMS) observed the distribution of K+ at the perovskite/SnO2 interface, indicating K+ passivation of defects to improve the power conversion efficiency (PCE) and device stability. We show how understanding the role of ion distribution at the SnO2 and perovskite interface can help reduce the creating of defects and promote a more efficient MHP device.

conductive atomic force microscopy↗
DOE OSTI2020

Plasma enhanced atomic layer deposition of thin film Li 1+x Mn 2-x O 4 for realization of all solid-state 3D lithium-ion microbatteries

Here, the plasma enhanced atomic layer deposition (PEALD) process for MnO 2 was demonstrated, exhibiting self-limiting growth as well as stable composition and stable growth rate over a temperature window of 205–265 °C. The PEALD process for MnO 2 was combined with the thermal ALD process for LiOH to synthesize Li 1+x Mn 2-x O 4 thin film cathodes, where the stoichiometry was effectively controlled to allow for crystallization in the electrochemically active spinel phase. A 3D nanostructure consisting of an Li 1+x Mn 2-x O 4 cathode layer, ALD Li x Al y Si z O solid electrolyte, and SiGe nanowire anode was fabricated and characterized via TEM. The Li 1+x Mn 2-x O 4 thin films maintained 66% of the areal capacity upon a 100× increase in the rate (4–360 μ A cm -2 ) as well as 97% capacity retention over 100 cycles at ~5C. The ALD Li 1+x Mn 2-x O 4 thin films exhibited a volumetric capacity of 52 μ Ah cm -2 μ m -1 at a C-rate of ~0.5C and, coupled with the high operating voltage (4.0 V), offer some of best areal energy densities for ALD thin film cathodes, making it a viable material for integration with 3D lithium-ion microbatteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Template-free vapor-phase growth of patrónite by atomic layer deposition

Despite challenges to control stoichiometry in the vanadium-sulfur system, template-free growth of patrónite, VS 4 , thin films is demonstrated for the first time. A novel atomic layer deposition (ALD) process enables the growth of phase pure films and the study of electrical and vibrational properties of the quasi-one-dimensional (1D) transition metal sulfide. Self-limiting surface chemistry during ALD of VS4 is established via in situ quartz crystal microbalance and quadrupole mass spectrometry between 150 to 200 °C. The V precursor, unconventionally, sheds all organic components in the first half-cycle, while the H 2 S half-cycle generates the disulfide dimer moiety, S 2 -2 , and oxidizes V 3+ to V 4+ . X-ray analysis establishes VS 4 crystallinity and phase purity, as well as a self-limiting growth rate of 0.33 Å/cy, modest roughness (2.4 nm) and expected density (2.7g/cm 3 ). Phase pure films enable a new assignment of vibrational modes and corresponding Raman activity of VS4 that is corroborated by density functional theory (DFT) calculations. Lastly, at elevated growth temperatures, a change in the surface mechanism provides a synthetic route to a second vanadium-sulfur phase, V 2 S 3 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Strong-field physics in three-dimensional topological insulators

We investigate theoretically the strong-field regime of light-matter interactions in the topological-insulator class of quantum materials. In particular, we focus on the process of nonperturbative high-order harmonic generation from the paradigmatic three-dimensional topological insulator bismuth selenide (Bi 2 Se 3 ) subjected to intense midinfrared laser fields. We analyze the contributions from the spin-orbit-coupled bulk states and the topological surface bands separately and reveal a major difference in how their harmonic yields depend on the ellipticity of the laser field. Furthermore, bulk harmonics show a monotonic decrease in their yield as the ellipticity increases, in a manner reminiscent of high harmonic generation in gaseous media. However, the surface contribution exhibits a highly nontrivial dependence, culminating with a maximum for circularly polarized fields. We attribute the observed anomalous behavior to (i) the enhanced amplitude and the circular pattern of the interband dipole and the Berry connections in the vicinity of the Dirac point and (ii) the influence of the higher-order, hexagonal warping terms in the Hamiltonian, which are responsible for the hexagonal deformation of the energy surface at higher momenta. The latter are associated directly with spin-orbit-coupling parameters. Our results thus establish the sensitivity of strong-field-driven high harmonic emission to the topology of the band structure as well as to the manifestations of spin-orbit interaction.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Predicting Complex Relaxation Processes in Metallic Glass

Relaxation processes significantly influence the properties of glass materials. However, understanding their specific origins is difficult; even more challenging is to forecast them theoretically. In this study, using microseconds molecular dynamics simulations together with an accurate many-body interaction potential, we predict that an Al 90 Sm 10 metallic glass would have complex relaxation behaviors: In addition to the main (α) relaxation, the glass (i) shows a pronounced secondary (β) relaxation at cryogenic temperatures and (ii) exhibits an anomalous relaxation process (α 2 ) accompanying α relaxation. Both of the predictions are verified by experiments. Computational simulations reveal the microscopic origins of relaxation processes: while the pronounced β relaxation is attributed to the abundance of stringlike cooperative atomic rearrangements, the anomalous α 2 process is found to correlate with the decoupling of the faster motions of Al with slower Sm atoms. The combination of simulations and experiments represents a first glimpse of what may become a predictive routine and integral step for glass physics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Atomic operations in a large scale distributed computing network

Techniques for executing an atomic command in a distributed computing network are provided. A core cluster, including a plurality of processing cores that do not natively issue atomic commands to the distributed computing network, is coupled to a translation unit. To issue an atomic command, a core requests a location in the translation unit to write an opcode and operands for the atomic command. The translation unit identifies a location (a “window”) that is not in use by another atomic command and indicates the location to the processing core. The processing core writes the opcode and operands into the window and indicates to the translation unit that the atomic command is ready. The translation generates an atomic command and issues the command to the distributed computing network for execution. After execution, the distributed computing network provides a response to the translation unit, which provides that response to the core.

Lackey, Jr., Stanley A.↗
DOE OSTI2017

Exploration of Turbulent Atomization Mechanisms for Diesel Spray Simulations

The atomization and initial spray formation processes in direct injection engines are not well understood due to the experimental and computational challenges associated with resolving these processes. Although different physical mechanisms, such as aerodynamic-induced instabilities and nozzle-generated turbulence and cavitation, have been proposed in the literature to describe these processes, direct validation of the theoretical basis of these models under engine-relevant conditions has not been possible to date. Recent developments in droplet sizing measurement techniques offer a new opportunity to evaluate droplet size distributions formed in the central and peripheral regions of the spray. There is therefore a need to understand how these measurements might be utilized to validate unobservable physics in the near nozzle-region. To address this need, we conduct a computational study using 3D CFD simulations in CONVERGE to explore the relationship between the selected primary atomization model and droplet sizes formed in the central and peripheral regions of the spray. Two existing primary atomization models from the literature are studied to characterize the influence of competing aerodynamics and turbulence mechanisms on the spray formation process. We develop and implement a new hybrid primary atomization model to evaluate the influence of the assumed turbulent scaling on the predicted spray structure. Local sensitivity analysis is performed over a wide range of ambient densities, injection pressures and nozzle diameters to compare the response of predicted droplet sizes in different regions of the spray to changes in injection and ambient conditions. Comparison of the predicted spray structure among the three spray models and against available measurements helps identify a set of experimental conditions and measurements that are needed to inform the development of improved atomization and spray breakup models.

33 ADVANCED PROPULSION SYSTEMS↗