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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Diazonium-Functionalized Silicon Hybrid Photoelectrodes: Film Thickness and Composition Effects on Photoelectrochemical Behavior

Aryl diazonium electrografting is a powerful method for imparting molecular functionality onto various substrates by forming a stable carbon-surface covalent bond. While the high reactivity of the aryl radical intermediate makes this method fast and reliable, it can also lead to the formation of an insulating and disordered multilayer film. These thick films affect electrochemical performance, especially for semiconductor substrates used in photoelectrochemical applications. For this work we studied the effects of film thickness and composition by electrografting in situ-generated aminobenzene diazonium salts onto both n-type and p-type silicon electrodes at fixed potentials. Next, we attached ferrocene to the amine-terminated films and probed their (photo)­electrochemical behavior. Cyclic voltammetry measurements showed decreased electrochemical reversibility with increasing diazonium film thickness; this reversibility was restored when ferrocene was incorporated throughout the film with a layer-by-layer deposition process. Finally, we compared the behavior of dark p-type electrodes to n-type photoelectrodes and observed differences in the electrochemical reversibility that we attribute to the change in potential drop across the two interfaces.

charge transfer↗
DOE OSTI2020

Pulsed laminar falling films in vertical tubes: Maintaining a continuous liquid film with reduced film thickness

Falling-liquid-film heat transfer is important to a wide variety of industrial applications, including two-phase thermosyphons, falling-film evaporators in the food industry, heat exchangers in fuel-ethanol processing, and the chemical service industry. Particularly for laminar falling films, the heat transfer increases as the film thickness decreases, hence it is desirable to keep the films as thin as possible. This article presents a periodically-pulsed flow concept to reduce the average mass flow inside a vertical tube. The technique provides thinner films than can be achieved with continuous flow. A drainage model is adopted to predict the film thickness as a function of flow rate and location along the tube. The concept is confirmed experimentally by measuring the film thickness in real time in a circular tube using a laser-based absorption technique. A new heat-transfer-based film continuity measurement is also integrated into the optical film measurement setup. Water at ambient temperature and pressure is used for this work. Film thickness reductions of up to 60%, and liquid-film volume-flow reductions of up to 80% compared to the minimum continuous-flow film have been obtained. The time-varying film thickness profile can also be controlled to a limited extent, which may be of interest for process industries.

42 ENGINEERING↗
DOE OSTI2025

Rational Regulation of Layer‐by‐Layer Processed Active Layer via Trimer‐Induced Pre‐Swelling Strategy for Efficient and Robust Thick‐Film Organic Solar Cells

Thick-film (>300 nm) organic solar cells (OSCs) have garnered intensifying attention due to their compatibility with commercial roll-to-roll printing technology for the large-scale continuous fabrication process. However, due to the uncontrollable donor/acceptor (D/A) arrangement in thick-film condition, the restricted exciton splitting and severe carrier traps significantly impede the photovoltaic performance and operability. For this work, combined with layer-by-layer deposition technology, a twisted 3D star-shaped trimer (BTT-Out) is synthesized to develop a trimer-induced pre-swelling (TIP) strategy, where the BTT-Out is incorporated into the buried D18 donor layer to enable the fabrication of thick-film OSCs. The integrated approach characterizations reveal that the exceptional configuration and spontaneous self-organization behavior of BTT-Out trimer could pre-swell the D18 network to facilitate the acceptor's infiltration and accelerate the formation of D/A interfaces. This enhancement triggers the elevated polarons formation with amplified hole-transfer kinetics, which is essential for the augmented exciton splitting efficiency. Furthermore, the regulated swelling process can initiate the favorable self-assembly of L8-BO acceptors, which would ameliorate carrier transport channels and mitigate carrier traps. As a result, the TIP-modified thin-film OSC devices achieve the champion performance of 20.3% (thin-film) and 18.8% (thick-film) with upgraded stability, among one of the highest performances reported of thick-film OSCs.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Effects of film thickness on electrochemical properties of nanoscale polyethylenedioxythiophene (PEDOT) thin films grown by oxidative molecular layer deposition (oMLD)

Poly(3,4-ethylene dioxythiophene) (PEDOT) has a high theoretical charge storage capacity, making it of interest for electrochemical applications including energy storage and water desalination. Nanoscale thin films of PEDOT are particularly attractive for these applications to enable faster charging. Recent work has demonstrated that nanoscale thin films of PEDOT can be formed using sequential gas-phase exposures via oxidative molecular layer deposition, or oMLD, which provides advantages in conformality and uniformity on high aspect ratio substrates over other deposition techniques. But to date, the electrochemical properties of these oMLD PEDOT thin films have not been well-characterized. In this work, we examine the electrochemical properties of 5–100 nm thick PEDOT films formed using 20–175 oMLD deposition cycles. We find that film thickness of oMLD PEDOT films affects the orientation of ordered domains leading to a substantial change in charge storage capacity. Interestingly, we observe a minimum in charge storage capacity for an oMLD PEDOT film thickness of ~30 nm (60 oMLD cycles at 150 °C), coinciding with the highest degree of face-on oriented PEDOT domains as measured using grazing incidence wide angle X-ray scattering (GIWAXS). Thinner and thicker oMLD PEDOT films exhibit higher fractions of oblique (off-angle) orientations and corresponding increases in charge capacity of up to 120 mA h g -1 . Electrochemical measurements suggest that higher charge capacity in films with mixed domain orientation arise from the facile transport of ions from the liquid electrolyte into the PEDOT layer. Greater exposure of the electrolyte to PEDOT domain edges is posited to facilitate faster ion transport in these mixed domain films. In conclusion, these insights will inform future design of PEDOT coated high-aspect ratio structures for electrochemical energy storage and water treatment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Film Thickness and Composition Effects in Symmetric Ternary Block Copolymer/Homopolymer Blend Films: Domain Spacing and Orientation

We report thickness and homopolymer molar mass dependencies in thin film blends of a compositionally symmetric 75 kg/mol lamellar polystyrene-block-poly(methyl methacrylate) diblock copolymer (PS-b-PMMA) with near-equal volume fractions of PS and PMMA homopolymers on “neutral” surfaces that promote a vertical domain orientation. PS and PMMA homopolymers with equal molar masses of 1, 3, and 22 kg/mol are blended in a 1:1 mass ratio. To efficiently explore this parameter space, we prepared combinatorial samples with gradient homopolymer concentrations using electrospray deposition (ESD) and gradient film thicknesses using flow coating; these samples were subsequently characterized by grazing-incidence small-angle X-ray scattering and scanning electron microscopy, respectively. Our results demonstrate that the added homopolymers increase or reduce domain spacings with respect to the neat (unblended) block copolymer depending on their molar masses, in line with previous reports; a simple heuristic to estimate the domain scaling in ternary blends based on the homopolymer molar mass agrees well with data for the thinnest blend films studied here. More surprisingly, we observe that the measured domain spacing in blends also depends on film thickness, with thicker films exhibiting larger domain spacings than thinner films at the same homopolymer concentration. Furthermore, thickness gradients at fixed homopolymer concentrations reveal a change in lamellae orientation from vertical to horizontal as film thickness is increased beyond the nominal lamellar domain spacing. Coarse-grained molecular dynamics simulations indicate that this change in orientation is induced by homopolymer segregation to film surfaces. Finally, tying these effects together, we hypothesize that the observed dependence of domain spacing on film thickness is a consequence of changes in the vertical homopolymer composition profile in thicker films during lamellae reorientation and the conformational asymmetry between PMMA and PS segments.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Determination of film thicknesses of metal oxides prepared by atomic layer deposition on SBA-15

ZrO 2 and CeO 2 films were grown in SBA-15 by Atomic Layer Deposition (ALD) to loadings of 0.92 g oxide/g SBA-15. Scanning Transmission Electron Microscopy (STEM) with Energy Dispersive Spectra (EDS) showed that the oxides grew uniformly inside the mesopores. Film thicknesses were then analyzed as a function of the number of ALD cycles using three methods: 1) mass changes assuming bulk densities for the films; 2) changes in pore size from Barret-Joyner-Halenda (BJH) analysis with N 2 adsorption isotherms; and 3) small-angle X-ray scattering (SAXS). Film thicknesses assuming bulk densities were between 6 and 8 times smaller than those obtained from BJH analysis. SAXS analysis gave film thicknesses that were approximately twice that obtained from bulk densities. Here, possible explanations of the discrepancies between these methods are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Development of 4.0 μm thick film REBCO tapes with length over 10 m by Ohmic heating technique

High-temperature superconducting REBCO (RE-(Gd,Y)Ba 2 Cu 3 O 7-δ ) coated conductor has an immense potential to enable magnetic fields above 20 T because of its high current-carrying capacity, high irreversibility field, and good mechanical properties. Advanced metal organic chemical vapor deposition (A-MOCVD) reactor with ohmic heating has been developed to grow long-length, thick film REBCO tapes in a single pass with superior in-field performance. Multiple long-length 5% Zr doped REBCO tapes with film thickness ranging from 1-4 µm have been produced in an A-MOCVD reactor. The critical current density (J c ) of these conductors has been examined by scanning hall probe microscopy. REBCO coated conductors with ~4 µm thickness exhibit magnetization J c >1.5 MA/cm 2 at 65 K, 1.5 T and 5.4 MA/cm 2 at 4.2 K, 13 T. As a result, the microstructure, out-of-plane and in-plane texture of REBCO coated conductors are also presented.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

High‐Performance Green Thick‐Film Ternary Organic Solar Cells Enabled by Crystallinity Regulation

Abstract The power conversion efficiency (PCE) of organic solar cells (OSCs) has reached high values of over 19%. However, most of the high‐efficiency OSCs are fabricated by spin‐coating with toxic solvents and the optimal photoactive layer thickness is limited to 100 nm, limiting practical development of OSCs. It is a great challenge to obtain ideal morphology for high‐efficiency thick‐film OSCs when using non‐halogenated solvents due to the unfavorable film formation kinetics. Herein, high‐efficiency ternary thick‐film (300 nm) OSCs with PCE of 15.4% based on PM6:BTR‐Cl:CH1007 are fabricated by hot slot‐die coating using non‐halogenated solvent (o‐xylene) in the air. Compared to PM6:BTR‐Cl:Y6 blends, the stronger pre‐aggregation of CH1007 in solution induces the earlier aggregation of CH1007 molecules and longer aggregation time, and thus results in high and balanced crystallinity of donors and acceptor in CH1007‐based ternary film, which led to high‐carrier mobility and suppressed charge recombination. The ternary strategy is further used to fabricate high‐efficiency, thick‐film, large‐area, and flexible devices processed from non‐halogenated solvents, paving the way for industrial development of OSCs.

Chemistry↗
DOE OSTI2021

High-speed impact of micron-sized diesel drop trains—Splashing dynamics, secondary droplet formation, and effects of pre-existing film thickness

This work investigates surface impingement of monodispersed diesel drop trains using computational simulations. The three-dimensional simulations include high-speed impact of micrometer-sized fuel drops onto initially dry and wetted stainless steel substrates. The drop size and impact velocity are representative of fuel injection conditions in internal combustion engines (ICEs). The drop trains serve as a simplified representation of fuel spray. To accurately capture the film that naturally develops on initially dry substrates, a dynamic diesel-stainless steel contact angle model was developed using experiments of single drop impact under ICE representative temperature. Simulations are presented for a highly splashing case and the effects of a pre-existing film on splashing dynamics were investigated, including the temporal evolution of splashed mass and film thickness. It was concluded that for thin films, the effect of pre-existing film thickness is less significant than in single drop impingement. Secondary droplet characterization was performed on simulation results, leading to instantaneous and time-averaged distributions of secondary droplet size, velocity magnitude, and trajectory angle. It was found that for each drop impingement, approximately 58% of the splashed mass is from the impinging drop itself, while the remainder of the splashed mass is composed of film liquid. From a high resolution case, details of secondary droplet formation are observed and three distinct phases of secondary droplet formation are identified. The detailed analysis of drop train impingement under engine-relevant conditions serves as a first step toward a robust understanding of fuel impingement and the development of cleaner and more efficient ICEs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Computational Analysis of Water Film Thickness During Rain Events for Assessing Hydroplaning Risk Part 2: Rough Road Surfaces

Hydroplaning occurs when a water film forms on a road during a rain event and vehicles are traveling at a speed that does not provide sufficient time for the tires to push the water film out of the tire path. Under these conditions, the tire loses contact with the road and the driver may lose control over the vehicle. The present study is a part of a multiyear research effort aimed at gaining a better understanding of the factors that contribute to hydroplaning risk in order to minimize the occurrence of hydroplaning accidents. Three-dimensional computational fluid dynamics (CFD) analysis was used to investigate the water film thickness on multilane roads, one of the key parameters in evaluating hydroplaning risk. In the first part of the study, water films forming on wide roadways, i.e. multilane highways with 2, 4, and 6 lanes per side, were analyzed, with varying cross slope, longitudinal slope, and rainfall rate. Roadways with and without curbs and drainage were included in the analysis. The analysis in the first part was limited to nearly smooth asphalt or concrete surfaces because the maximum roughness height that can be specified in a CFD model using wall functions to determine shear stress at the road surface boundary is one half the thickness of computational cell layer adjacent to the boundary and the need to resolve the vertical velocity distribution in a thin water film requires cell layers that are a fraction of a millimeter thick. In this part of the study, the analysis was extended to consider the influence of pavement roughness over a range extending up 3.6 mm on the development of water film thickness. Various methods of modeling roughness were investigated and are presented: the roughness height model, a meshed-out geometry of the macrotexture of the pavement, and a porous region model. The computational results were analyzed and compared with experimental measurements performed by Gallaway et al.

42 ENGINEERING↗
DOE OSTI2020

Computational Analysis of Water Film Thickness During Rain Events for Assessing Hydroplaning Risk, Part 1: Nearly Smooth Road Surfaces

In the research work reported here, both two- and three-dimensional computational fluid dynamics (CFD) analysis was used to investigate modern road geometries that were not frequently encountered in the latter half of the 20th century but are much more common today. The relation of newer road geometries to the water film thickness that develops on travel lanes was a major focus of this work.

42 ENGINEERING↗
DOE OSTI2022

High Temperature Thick Film Sensor Development Based on Refractory Oxide Semiconductors

Solid-state, high-temperature sensing devices are required for accurate temperature, strain/stress, and failure monitoring for a range of advanced manufacturing, transportation, and military applications. High temperature conditions limit sensing strategies, where typically traditional metal and semiconductor materials are unstable, and the sensing options are limited to optical spectroscopy methods. In addition, strategies to embed the sensors directly within active components and protective thermal refractory are of interest that permit near-environment sensing which is not possible with the traditional electronic materials and components. Rare-earth chromite semiconductors exhibit some properties of interest for high temperature sensing technologies, such as: high microstructure and chemical stability, relatively high electronic conductivity at high temperatures, and relative thermal expansion coefficient matching to refractory thermal protective insulation (such as high-zirconia and -alumina ceramics). In this work, n-type and p-type doped lanthanum chromites compositions were computationally modelled and prepared, and the electrical, thermoelectric, and thermomechanical properties were measured for the obtained material systems. A few compositions were then processed into thick film health and temperature sensors and tested at high temperatures. To establish relative stability under harsh environment conditions, post- mortem microstructure and chemical composition was characterized after extended and cycle testing at high temperatures.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2020

High frequency lithium niobate film-thickness-mode optomechanical resonator

High-frequency optomechanical resonators are in demand as transduction devices to bridge microwave and optical fields. Thin-film lithium niobate is a promising platform for implementing high-frequency optomechanics for its low optical loss and strong piezoelectric coefficients. However, its strong piezoelectricity is also known to introduce excess phonon loss. Here, we present lithium niobate optomechanical resonators with film-thickness-mode mechanical resonances up to 5.2 GHz, reaching the operating frequency regime of superconducting qubits. By engineering the mechanical anchor to minimize the phonon loss, we achieve a high quality factor up to 12 500 at cryogenic temperatures and, hence, a frequency-quality factor product of 6.6 × 10 13 . Our system also features interference between piezo-optomechanical and electro-optic modulation. A theoretical model is derived to analyze these two effects and their interference.

42 ENGINEERING↗
DOE OSTI2021

Chiral Spin Textures in Amorphous Iron–Germanium Thick Films

Topological solitary fields, such as magnetic and polar skyrmions, are envisioned to revolutionize microelectronics. These configurations have been stabilized in solid-state materials with a global inversion symmetry breaking, which translates in magnetic materials into a vector spin exchange known as the Dzyaloshinskii-Moriya interaction (DMI), as well as spin chirality selection and isotropic solitons. This work reports experimental evidence of 3D chiral spin textures, such as helical spins and skyrmions with different chirality and topological charge, stabilized in amorphous Fe-Ge thick films. Overall, these results demonstrate that structurally and chemically disordered materials with a random DMI can resemble inversion symmetry broken systems with similar magnetic properties, moments, and states. Disordered systems are distinguished from systems with global inversion symmetry breaking by their degenerate spin chirality that allows for forming isotropic and anisotropic topological spin textures at remanence, while offering greater flexibility in materials synthesis, voltage, and strain manipulation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magnetic Materials: Chiral Spin Textures in Amorphous Iron–Germanium Thick Films (Adv. Mater. 8/2021)

Topological solitary fields, such as magnetic and polar skyrmions, are envisioned to revolutionize microelectronics. These configurations have been stabilized in solid-state materials with a global inversion symmetry breaking, which translates in magnetic materials into a vector spin exchange known as the Dzyaloshinskii–Moriya interaction (DMI), as well as spin chirality selection and isotropic solitons. This work reports experimental evidence of 3D chiral spin textures, such as helical spins and skyrmions with different chirality and topological charge, stabilized in amorphous Fe–Ge thick films. These results demonstrate that structurally and chemically disordered materials with a random DMI can resemble inversion symmetry broken systems with similar magnetic properties, moments, and states. In conclusion, disordered systems are distinguished from systems with global inversion symmetry breaking by their degenerate spin chirality that allows for forming isotropic and anisotropic topological spin textures at remanence, while offering greater flexibility in materials synthesis, voltage, and strain manipulation.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Fabrication of Black Body Grids by Thick Film Printing for Quantitative Neutron Imaging

Neutron imaging offers deep penetration through many high-Z materials while also having high sensitivity to certain low-Z isotopes such as 1H, 6Li, and 10B. This unique combination of properties has made neutron imaging an attractive tool for a wide range of material science and engineering applications. However, measurements made by neutron imaging or tomography are generally qualitative in nature due to the inability of detectors to discriminate between neutrons which have been transmitted through the sample and neutrons which are scattered by the sample or within the detector. Recent works have demonstrated that deploying a grid of small black bodies (BBs) in front of the sample can allow for the scattered neutrons to be measured at the BB locations and subsequently subtracted from the total measured intensity to yield a quantitative transmission measurement. While this method can be very effective, factors such as the scale and composition of the sample, the beam divergence, and the resolution and construction of the detector may require optimization of the grid design to remove all measurement biases within a given experimental setup. Therefore, it is desirable to have a method by which BB grids may be rapidly and inexpensively produced such that they can easily be tailored to specific applications. In this work, we present a method for fabricating BB patterns by thick film printing of Gd2O3 and evaluate the performance with variation in feature size and number of print layers with cold and thermal neutrons.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Growth of High-Performance 4-5μm Thick Film REBCO Tapes Doped With Hafnium Using Advanced MOCVD

Advanced metal organic chemical vapor deposition technique (A-MOCVD) was used to grow 4-5 µm thick REBa 2 Cu 3 O 7–δ (REBCO, RE = rare earth) films, doped with 5% and 15% Hf. Thick REBCO films doped with 5% Hf exhibit self-field critical current density (J c ) over 1.8 MA/cm 2 at 77 K and 3 MA/cm 2 at 65 K, 1.5 T. Increasing the Hf content to 15% resulted in J c above 9 MA/cm 2 at 20 K, 9 T. The effect of (Ba+Hf)/Cu content in Hf-added (5 and 15 mol.%) REBCO films on the critical current density at 77 K, 0 T, c-axis lattice parameter and out-of- plane texture has been studied. In addition to growth of thick film REBCO tapes with superior performance, the A-MOCVD reactor has been used to quadruple the precursor-to-film conversion efficiency above 45%. Furthermore, this achievement has a first order impact in lowering the cost of REBCO tapes made by A-MOCVD.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗