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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 577 records · Page 32
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Formation of Large Polysulfide Complexes during the Lithium-Sulfur Battery Discharge

Sulfur cathodes have much larger capacities than transition-metal-oxide cathodes used in commercial lithium-ion batteries but suffer from unsatisfactory capacity retention and long-term cyclability. Capacity degradation originates from soluble lithium polysulfides gradually diffusing into the electrolyte. Understanding of the formation and dynamics of soluble polysulfides during the discharging process at the atomic level remains elusive, which limits further development of lithium-sulfur (Li-S) batteries. Here we report first-principles molecular dynamics simulations and density functional calculations, through which the discharging products of Li-S batteries are studied. We find that, in addition to simple Li2Sn (1 n 8) clusters generated from single cyclooctasulfur (S8) rings, large Li-S clusters form by collectively coupling several different rings to minimize the total energy. At high lithium concentration, a Li-S network forms at the sulfur surfaces. The results can explain the formation of the soluble Li-S complex, such as Li2S8, Li2S6, and Li2S4, and the insoluble Li2S2 and Li2S structures. In addition, we show that the presence of oxygen impurities in graphene, particularly oxygen atoms bonded to vacancies and edges, may stabilize the lithium polysulfides that may otherwise diffuse into the electrolyte.

Wang, Bin↗
DOE OSTI2015

Strong enhancement of surface diffusion by nonlinear surface acoustic waves

The phenomenon of acoustic activation of surface diffusion is investigated in a combined computational and experimental study. The ability of pulsed laser-generated surface acoustic waves (SAWs) to enhance the mobility of small atomic clusters is demonstrated by directly tracking, with fluorescence microscopy, individual Au 8 clusters moving on a (111) silicon substrate. In this work, a 19-fold increase in the effective diffusion coefficient is measured in room temperature experiments in the presence of SAWs generated by nanosecond pulse laser irradiation at a 100 Hz repetition rate. A strong enhancement of cluster mobility by SAWs is also observed in large-scale molecular dynamics simulations of surface diffusion of small atomic clusters. The analysis of the computational results demonstrates that the nonlinear sharpening of SAWs and the corresponding enrichment of the SAW spectra by high frequency harmonics which are capable of dynamic coupling to the cluster vibrations are responsible for the efficient acoustic activation of surface mobility in the simulations. The increase in the effective diffusion coefficient is proportional to the number of the SAW pulses passing through the diffusion region per unit time and a dramatic 4500-fold diffusion enhancement (corresponds to an equivalent temperature increase by ~10 3 K ) is predicted in the simulations for 15 GHz SAWs. The ability of SAWs to affect atomic-level surface processes has far-reaching implications for the design of new techniques where the acoustic energy serves as an effective substitution for thermal activation in applications where heating must be avoided or rapid switching of surface conditions is required.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Direct Measurement of Anharmonic Decay Channels of a Coherent Phonon

In this paper, we report channel-resolved measurements of the anharmonic coupling of the coherent ${A}_{1g}$ phonon in photoexcited bismuth to pairs of high wave vector acoustic phonons. The decay of a coherent phonon can be understood as a parametric resonance process whereby the atomic displacement periodically modulates the frequency of a broad continuum of modes. This coupling drives temporal oscillations in the phonon mean-square displacements at the ${A}_{1g}$ frequency that are observed across the Brillouin zone by femtosecond x-ray diffuse scattering. Finally, we extract anharmonic coupling constants between the ${A}_{1g}$ and several representative decay channels that are within an order of magnitude of density functional perturbation theory calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Evidence of Extreme Ultraviolet Superfluorescence in Xenon

We present a comprehensive experimental and theoretical study on superfluorescence in the extreme ultraviolet wavelength regime. Focusing a free-electron laser pulse in a cell filled with Xe gas, the medium is quasi-instantaneously population inverted by 4d-shell ionization on the giant resonance followed by Auger decay. On the timescale of ~10 ps to ~100 ps (depending on parameters) a macroscopic polarization builds up in the medium, resulting in superfluorescent emission of several Xe lines in the forward direction. As the number of emitters in the system is increased by either raising the pressure or the pump-pulse energy, the emission yield grows exponentially over four orders of magnitude and reaches saturation. With increasing yield, we observe line broadening, a manifestation of superfluorescence in the spectral domain. Here, our novel theoretical approach, based on a full quantum treatment of the atomic system and the irradiated field, shows quantitative agreement with the experiment and supports our interpretation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Surface preparation method for investigating the three-dimensional electronic structure of perovskite nickelates

The investigation of the electronic structures on perovskite oxides using surface-sensitive spectroscopy techniques is often hindered by their “uncleavable” nature, typically requiring expensive and complex in situ experimental setups that integrate the capabilities of sample synthesis and spectroscopy measurement under ultrahigh vacuum condition. Here, we address this challenge by developing an ozone-annealing process that yields atomically flat surfaces on perovskite oxide thin films, making them suitable for high-resolution angle-resolved photoemission spectroscopy measurements. Using this method, we present a three-dimensional electronic structure study of Nd 1−𝑥 ⁢Sr 𝑥 ⁢NiO 3 (𝑥=0 and 0.175) thin films with unprecedented accuracy. The experimentally determined low-energy fermiology exhibits quantitative agreements with two-band tight-binding simulations, which is further validated by first-principles calculations considering the material's actual crystal structure. This work provides an accessible approach for ex situ ARPES measurements on perovskite oxides and other strongly correlated oxides, including the recently discovered high-𝑇 c nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Optical laser systems at the Linac Coherent Light Source

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump–probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump–probe experiments to be performed at LCLS.

42 ENGINEERING↗
DOE OSTI2014

Fluorocarbon assisted atomic layer etching of SiO{sub 2} using cyclic Ar/C{sub 4}F{sub 8} plasma

The authors demonstrate atomic layer etching of SiO{sub 2} using a steady-state Ar plasma, periodic injection of a defined number of C{sub 4}F{sub 8} molecules, and synchronized plasma-based Ar{sup +} ion bombardment. C{sub 4}F{sub 8} injection enables control of the deposited fluorocarbon (FC) layer thickness in the one to several Ångstrom range and chemical modification of the SiO{sub 2} surface. For low energy Ar{sup +} ion bombardment conditions, the physical sputter rate of SiO{sub 2} vanishes, whereas SiO{sub 2} can be etched when FC reactants are present at the surface. The authors have measured for the first time the temporal variation of the chemically enhanced etch rate of SiO{sub 2} for Ar{sup +} ion energies below 30 eV as a function of fluorocarbon surface coverage. This approach enables controlled removal of Ångstrom-thick SiO{sub 2} layers. Our results demonstrate that development of atomic layer etching processes even for complex materials is feasible.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Influence of dosing sequence and film thickness on structure and resistivity of Al-ZnO films grown by atomic layer deposition

Aluminum-doped zinc oxide (AZO) films were deposited onto amorphous silica substrates using an atomic layer deposition process with diethyl zinc (DEZ), trimethyl aluminum (TMA), and deionized water at 200 °C. Three different Al doping sequences were used at a ZnO:Al ratio of 11:1 within the films. A minimum film resistivity of 1.6 × 10{sup −3} Ω cm was produced using sequential dosing of DEZ, TMA, DEZ, followed by H{sub 2}O for the Al doping step. This “ZAZW” sequence yielded an AZO film resistivity that is independent of film thickness, crystallographic texture, and grain size, as determined by high resolution x-ray diffraction (XRD). A pseudo-Voigt analysis method yields values for grain sizes that are smaller than those calculated using other XRD methods. Anisotropic grain sizes or variations in crystallographic texture have minimal influence on film resistivity, which suggests that factors other than film texture, such as intragrain scattering, may be important in influencing film resistivity.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Effect of substrate pretreatments on the atomic layer deposited Al{sub 2}O{sub 3} passivation quality

The authors show here that the passivation quality of Al{sub 2}O{sub 3} is highly sensitive to the surface condition prior to the atomic layer deposition, affecting especially the thermal stability of the film. Pretreatments like diluted HCl bath or preheating at 200 °C both improved significantly the passivation quality and thermal stability of the films. In addition, the authors observed that a thin chemical SiO{sub 2} layer resulting from diluted HCl solves the blistering problem often encountered in H{sub 2}O based atomic layer deposited process. Finally, the authors show that the chemical oxide protects the surface from contaminants, enabling long storage times in a dirty ambient between the cleaning and the film deposition.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Atmospheric pressure plasma enhanced spatial ALD of silver

The authors have investigated the growth of thin silver films using a unique combination of atmospheric process elements: spatial atomic layer deposition and an atmospheric pressure surface dielectric barrier discharge plasma source. Silver films were grown on top of Si substrates with good purity as revealed by resistivity values as low as 18 μΩ cm and C- and F-levels below detection limits of energy dispersive x-ray analysis. The growth of the silver films starts through the nucleation of islands that subsequently coalesce. The authors show that the surface island morphology is dependent on surface diffusion, which can be controlled by temperature within the deposition temperature range of 100–120 °C.

42 ENGINEERING↗
DOE OSTI2016

Ultraviolet optical properties of aluminum fluoride thin films deposited by atomic layer deposition

Aluminum fluoride (AlF{sub 3}) is a low refractive index material with promising optical applications for ultraviolet (UV) wavelengths. An atomic layer deposition process using trimethylaluminum and anhydrous hydrogen fluoride has been developed for the deposition of AlF{sub 3} at substrate temperatures between 100 and 200 °C. This low temperature process has resulted in thin films with UV-optical properties that have been characterized by ellipsometric and reflection/transmission measurements at wavelengths down to 200 nm. The optical loss for 93 nm thick films deposited at 100 °C was measured to be less than 0.2% from visible wavelengths down to 200 nm, and additional microstructural characterization demonstrates that the films are amorphous with moderate tensile stress of 42–105 MPa as deposited on silicon substrates. X-ray photoelectron spectroscopy analysis shows no signature of residual aluminum oxide components making these films good candidates for a variety of applications at even shorter UV wavelengths.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Asymmetric photoenzymatic incorporation of fluorinated motifs into olefins

Enzymes capable of assimilating fluorinated feedstocks are scarce. This situation poses a challenge for the biosynthesis of fluorinated compounds used in pharmaceuticals, agrochemicals, and materials. We developed a photoenzymatic hydrofluoroalkylation that integrates fluorinated motifs into olefins. The photoinduced promiscuity of flavin-dependent ene-reductases enables the generation of carbon-centered radicals from iodinated fluoroalkanes, which are directed by the photoenzyme to engage enantioselectively with olefins. This approach facilitates stereocontrol through interaction between a singular fluorinated unit and the enzyme, securing high enantioselectivity at β, γ, or δ positions of fluorinated groups through enzymatic hydrogen atom transfer—a process that is notably challenging with conventional chemocatalysis. Furthermore, this work advances enzymatic strategies for integrating fluorinated chemical feedstocks and opens avenues for asymmetric synthesis of fluorinated compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Algorithm for solving the linear Cauchy problem for large systems of ordinary differential equations with the use of parallel computations

An algorithm for solving the linear Cauchy problem for large systems of ordinary differential equations is presented. The algorithm for systems of first-order differential equations is implemented in the EDELWEISS code with the possibility of parallel computations on supercomputers employing the MPI (Message Passing Interface) standard for the data exchange between parallel processes. The solution is represented by a series of orthogonal polynomials on the interval [0, 1]. The algorithm is characterized by simplicity and the possibility to solve nonlinear problems with a correction of the operator in accordance with the solution obtained in the previous iterative process.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Application of Quantum Scattering Theory in Calculation of the Simplest Chemical Reactions (Dissociative Attachment, Dissociation, and Recombination)

Several parameters (cross section, reaction rate, etc.) of various processes in laser, atomic, and chemical physics are calculated using quantum scattering theory for a system of a few particles. Results of the study of electronic and atomic collisions with diatomic molecules and collisions of diatomic molecules in excited rovibrational states are discussed. Several approximations needed for calculations of real physical systems consisting of several bodies are analyzed. Such approximations can be used for simulation of direct reactions and reactions that yield intermediate transient complexes. Calculated cross sections of electronic and atomic collisions with diatomic molecules and collisions of diatomic molecules are compared with experimental data and results of alternative calculations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Damage Pseudo Cross Section Generator

This software is a python script for generating group damage pseudo-cross-sections for specific elements, and tabulating them in forms useful to python or to office-open workbooks (xlsx). The damage pseudo-cross-section is needed for calculating how much neutron radiation damage a structural material receives in a reactor measured in displacements per atom (DPA). The process of generating these pseudo-cross-sections is laborious as it requires running the nuclear data processing code, NJOY, for hundreds of isotopes, and then post-processing the data. This also allows many opportunities for human error to be involved. This script eliminates these problems by fully automating the process.

Gale, MicahD.↗
DOE OSTI2024

Shadow of a laser beam

Light, being massless, casts no shadow; under ordinary circumstances, photons pass right through each other unimpeded. Here, we demonstrate a laser beam acting like an object — the beam casts a shadow upon a surface when the beam is illuminated by another light source. We observe a regular shadow in the sense it can be seen by the naked eye, it follows the contours of the surface it falls on, and it follows the position and shape of the object (the laser beam). Specifically, we use a nonlinear optical process involving four atomic levels of ruby. We are able to control the intensity of a transmitted laser beam by applying another perpendicular laser beam. We experimentally measure the dependence of the contrast of the shadow on the power of the laser beam, finding a maximum of approximately 22%, similar to that of a shadow of a tree on a sunny day. We provide a theoretical model that predicts the contrast of the shadow. This work opens new possibilities for fabrication, imaging, and illumination.

47 OTHER INSTRUMENTATION↗
DOE OSTI2016

Study of Volumetrically Heated Ultra-High Energy Density Plasmas

Heating dense matter to millions of degrees is important for applications, but requires complex and expensive methods. The major goal of the project was to demonstrate using a compact laser the creation of a new ultra-high energy density plasma regime characterized by simultaneous extremely high temperature and high density, and to study it combining experimental measurements and advanced simulations. We have demonstrated that trapping of intense femtosecond laser pulses deep within ordered nanowire arrays can heat near solid density matter into a new ultra hot plasma regime. Extreme electron densities, and temperatures of several tens of million degrees were achieved using laser pulses of only 0.5 J energy from a compact laser. Our x-ray spectra and simulations showed that extremely highly ionized plasma volumes several micrometers in depth are generated by irradiation of gold and Nickel nanowire arrays with femtosecond laser pulses of relativistic intensities. We obtained extraordinarily high degrees of ionization (e.g. we peeled 52 electrons from gold atoms, and up to 26 electrons from nickel atoms). In the process we generated Gigabar pressures only exceeded in the central hot spot of highly compressed thermonuclear fusion plasmas.. The plasma created after the dissolved wires expand, collide, and thermalize, is computed to have a thermal energy density of 0.3 GJ cm -3 and a pressure of 1-2 Gigabar. These are pressures only exceeded in highly compressed thermonuclear fusion plasmas. Scaling these results to higher laser intensities promises to create plasmas with temperatures and pressures exceeding those in the center of the sun.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Investigation of Plasmas Having Complex, Dynamic Evolving Morphology

Three different types of plasmas have been investigated using both experimental and theoretical methods. The first type of plasma is dense, highly ionized, governed by magnetohydrodynamics, and highly dynamic. This plasma is relevant to solar coronal loops, astrophysical jets, and other situations where strong magnetic forces act on the plasma. A well-diagnosed laboratory experiment creates a magnetohydrodynamically driven highly collimated plasma jet. This jet undergoes a kink instability such that it rapidly develops a corkscrew shape. The kink causes lateral acceleration of the jet, and this lateral acceleration drives a Rayleigh-Taylor instability that in turn chokes the current flowing in the jet and causes a magnetic reconnection. The magnetic reconnection causes electron and ion heating as well as emission of whistler waves. This entire sequence of events has been observed, measured in detail, and related to theoretical models. The second type of plasma is a transient rf-produced plasma used as a seed plasma for the magnetohydrodynamic experiments described above. Detailed atomic physics ionization processes have been investigated and modeled. The third type of plasma that has been studied is a dusty plasma where the dust particles are spontaneously growing ice grains. The rapid growth of the ice grains to large size and their highly ordered alignment has been investigated as well as collective motion of the ice grains, including well-defined flows on the surface of nested toroids. In addition to the experimental work described above, several related theoretical models have been developed, most notably a model showing how a complex interaction between gravity and magnetic fields on extremely weakly ionized plasma in an accretion disk provides an electric power source that can drive astrophysical jets associated with the accretion disk. Eighteen papers reporting this work have been published in a wide variety of journals.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗