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At least 1,315 records · Page 73
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Defect analysis in low temperature atomic layer deposited Al{sub 2}O{sub 3} and physical vapor deposited SiO barrier films and combination of both to achieve high quality moisture barriers

Al{sub 2}O{sub 3} [20 nm, atomic layer deposition (ALD)] and SiO films' [25 nm, physical vacuum deposition (PVD)] single barriers as well as hybrid barriers of the Al{sub 2}O{sub 3}/SiO or SiO/Al{sub 2}O{sub 3} have been deposited onto single 100 nm thick tris-(8-hydroxyquinoline) aluminum (AlQ{sub 3}) organic films made onto silicon wafers. The defects in the different barrier layers could be easily observed as nonfluorescent AlQ{sub 3} black spots, under ultraviolet light on the different systems stored into accelerated aging conditions (85 °C/85% RH, ∼2000 h). It has been observed that all devices containing an Al{sub 2}O{sub 3} layer present a lag time τ from which defect densities of the different systems start to increase significantly. This is coherent with the supposed pinhole-free nature of fresh, ALD-deposited, Al{sub 2}O{sub 3} films. For t > τ, the number of defect grows linearly with storage time. For devices with the single Al{sub 2}O{sub 3} barrier layer, τ has been estimated to be 64 h. For t > τ, the defect occurrence rate has been calculated to be 0.268/cm{sup 2}/h. Then, a total failure of fluorescence of the AlQ{sub 3} film appears between 520 and 670 h, indicating that the Al{sub 2}O{sub 3} barrier has been totally degraded by the hot moisture. Interestingly, the device with the hybrid barrier SiO/Al{sub 2}O{sub 3} shows the same characteristics as the device with the single Al{sub 2}O{sub 3} barrier (τ = 59 h; 0.246/cm{sup 2}/h for t > τ), indicating that Al{sub 2}O{sub 3} ALD is the factor that limits the performance of the barrier system when it is directly exposed to moisture condensation. At the end of the storage period (1410 h), the defect density for the system with the hybrid SiO/Al{sub 2}O{sub 3} barrier is 120/cm{sup 2}. The best sequence has been obtained when Al{sub 2}O{sub 3} is passivated by the SiO layer (Al{sub 2}O{sub 3}/SiO). In that case, a large lag time of 795 h and a very low defect growth rate of 0.032/cm{sup 2}/h (t > τ) have been measured. At the end of the storage test (2003 h), the defect density remains very low, i.e., only 50/cm{sup 2}. On the other hand, the device with the single PVD-deposited SiO barrier layer shows no significant lag time (τ ∼ 0), and the number of defects grows linearly from initial time with a high occurrence rate of 0.517/cm{sup 2}/h. This is coherent with the pinhole-full nature of fresh, PVD-deposited, SiO films. At intermediate times, a second regime shows a lower defect occurrence rate of 0.062/cm{sup 2}/h. At a longer time span (t > 1200 h), the SiO barrier begins to degrade, and a localized crystallization onto the oxide surface, giving rise to new defects (occurrence rate 0.461/cm{sup 2}/h), could be observed. At the end of the test (2003 h), single SiO films show a very high defect density of 600/cm{sup 2}. Interestingly, the SiO surface in the Al{sub 2}O{sub 3}/SiO device does not appeared crystallized at a high time span, suggesting that the crystallization observed on the SiO surface in the AlQ{sub 3}/SiO device rather originates into the AlQ{sub 3} layer, due to high humidity ingress on the organic layer through SiO pinholes. This has been confirmed by atomic force microscopy surface imaging of the AlQ{sub 3}/SiO surface showing a central hole in the crystallization zone with a 60 nm depth, deeper than SiO thickness (25 nm). Using the organic AlQ{sub 3} sensor, the different observations made in this work give a quantitative comparison of defects' occurrence and growth in ALD-deposited versus PVD-deposited oxide films, as well as in their combination PVD/ALD and ALD/PVD.

42 ENGINEERING↗
DOE OSTI2014

Spin transport in epitaxial magnetic manganite/ruthenate heterostructures with an LaMnO{sub 3} layer

Epitaxial La{sub 0.7}Sr{sub 0.3}MnO{sub 3}/LaMnO{sub 3}/SrRuO{sub 3} (LSMO/LMO/SRO) heterostructures with an LMO layer 0–35 nm thick are grown by laser ablation on an NdGaO{sub 3} substrate at a high temperature. X-ray diffraction and transmission electron microscopy demonstrate sharp interfaces and epitaxial growth of the LSMO and SRO layers in the heterostructures at an LMO layer thickness of 0–35 nm. SQUID measurements of the magnetic moment of the heterostructures with an LMO layer and the data obtained with reflectometry of polarized neutrons show that the manganite LMO layer is a ferromagnet at a temperature below 150 K and strongly affects the magnetic moment of the heterostructures at low temperatures. The magnetoresistance of the mesostructure created from the heterostructure using lithography and ion etching decreases with increasing LMO layer thickness and weakly depends on the direction of an applied magnetic field. If the LMP layer is absent, a negative magnetoresistance is detected; it is likely to be caused by a negative magnetization of the SRO layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Ohmic Contacts to CVD Diamond with Boron-Doped Delta Layers

Various methods for the formation of ohmic contacts to boron-doped δ layers in CVD-diamond epitaxial structures are investigated. In the first variant, an additional thin heavily doped layer was formed on the diamond surface to which an ohmic contact is formed. Then, the surface p{sup +} layer between the contact pads is etched out; therefore, the current in the structure flows only through a buried δ layer. In the second approach, the doped diamond selectively grows in the contact windows under a metallic mask after preliminary etching of the undoped diamond layer (cap) up to the δ layer. In this case, the heavily doped p{sup +} layer forms an end contact to the δ layer. These two variants differ in terms of the conditions of applicability, the complexity of the manufacturing technology, the value of the contact resistance, and can be used to solve problems in which it is necessary to have a different quality of the contacts, such as the formation of transistor structures or test cells for measuring physical characteristics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Catalyst Layer Resistance and Utilization in PEM Electrolysis

Improving utilization, performance, and stability of low iridium (Ir)-loaded anodes is a key goal to enable widespread adoption of polymer electrolyte membrane water electrolysis (PEMWE) for clean hydrogen production. A potential limitation is high ionic or electronic resistance of the anode catalyst layer, which leads to poor catalyst utilization, increased voltage losses, and high local overpotentials that can accelerate degradation. While catalyst layer resistance is relatively well-understood in fuel cells and other porous electrode systems, characterization of these effects is not as well established in PEMWE research. Here we present in-situ methods for measuring catalyst layer resistance in electrolysis cells using a non-faradaic H 2 /H 2 O condition as well as methods for calculating the associated voltage losses. These methods are applied to anode catalyst layers based on IrO 2 nanoparticles as well as dispersed nano-structured thin film (NSTF) Ir catalysts. Trends with anode catalyst loading and interactions between the porous transport layer and catalyst layer are investigated for IrO 2 anodes. Post-mortem microscopic analysis of durability-tested anodes is also presented, showing uneven degradation of the catalyst layer caused by catalyst layer resistance.

08 HYDROGEN↗
DOE OSTI2020

Modeling Arctic boundary layer cloud streets at grey-zone resolutions

To better understand how model resolution affects the formation of Arctic boundary layer clouds, we investigated the influence of grid spacing on simulating cloud streets that occurred near Utqiagvik (formerly Barrow), Alaska on 2 May 2013 and were observed by the Moderate Resolution Imaging Spectroradiometer (MODIS). The Weather Research and Forecasting model was used to simulate the clouds using nested domains with increasingly fine resolution ranging from a horizontal grid spacing of 27 km in the boundary-layer-parameterized mesoscale domain to a grid spacing of 0.111 km in the large-eddy-permitting domain. We investigated the model-simulated mesoscale environment, horizontal and vertical cloud structures, boundary layer stability, and cloud properties, all of which were subsequently used to interpret the observed roll-cloud case. Increasing model resolution led to a transition from a more buoyant boundary layer to a more shear-driven turbulent boundary layer. The clouds were stratiform-like in the mesoscale domain, but as the model resolution increased, roll-like structures, aligned along the wind field, appeared with ever smaller wavelengths. A stronger vertical water vapor gradient occurred above the cloud layers with decreasing grid spacing. With fixed model grid spacing at 0.333 km, changing the model configuration from a boundary layer parameterization to a large-eddy-permitting scheme produced a more shear-driven and less unstable environment, a stronger vertical water vapor gradient below the cloud layers, and the wavelengths of the rolls decreased slightly. In this study, only the large-eddy-permitting simulation with gird spacing of 0.111 km was sufficient to model the observed roll clouds.

Lai, Hui-Wen↗
DOE OSTI2017

Effect of TiO 2 particle size and layer thickness on mesoscopic perovskite solar cells

Mesoporous TiO 2 (mp-TiO 2 ) layers are commonly used as electron transport layers in perovskite solar cells, which help to extract electrons from the perovskite light-absorbing layer and transport them to the electrodes. We investigated the effects of the layer thickness of mp-TiO 2 and particle size of TiO 2 on photovoltaic properties, in terms of the surface area of the mp-layer and the interfacial areas of the TiO 2 nanoparticles in the mp-layer. Various mp-TiO 2 layers with thicknesses of 150, 250, and 400 nm and particle sizes of 25 nm and 41 nm were prepared to compare the photovoltaic properties of such layer-containing perovskite solar cells. Time-resolved photoluminescence decay and impedance studies showed that interfacial resistance as well as perovskite-to-TiO 2 charge injection are important factors affecting photovoltaic performance. The deterioration of the photovoltaic parameters with increasing TiO 2 /TiO 2 interfacial area also confirms that the interfacial series resistance that arises from these connections should be reduced to enhance the performance of mesoscopic perovskite solar cells.

14 SOLAR ENERGY↗
DOE OSTI2022

Explicitly antisymmetrized neural network layers for variational Monte Carlo simulation

The combination of neural networks and quantum Monte Carlo methods has arisen as a promising path forward for highly accurate electronic structure calculations. Previous proposals have combined equivariant neural network layers with a final antisymmetric layer in order to satisfy the antisymmetry requirements of the electronic wavefunction. However, to date it is unclear if one can represent antisymmetric functions of physical interest, and it is difficult to precisely measure the expressiveness of the antisymmetric layer. Here, this work attempts to address this problem by introducing explicitly antisymmetrized universal neural network layers. This approach has a computational cost which increases factorially with respect to the system size, but we are nonetheless able to apply it to small systems to better understand how the structure of the antisymmetric layer affects its performance. We first introduce a generic antisymmetric (GA) neural network layer, which we use to replace the entire antisymmetric layer of the highly accurate ansatz known as the FermiNet. We demonstrate that the resulting FermiNet-GA architecture can yield effectively the exact ground state energy for small atoms and molecules. We then consider a factorized antisymmetric (FA) layer which more directly generalizes the FermiNet by replacing the products of determinants with products of antisymmetrized neural networks. We find, interestingly, that the resulting FermiNet-FA architecture does not significantly outperform the FermiNet. This strongly suggests that the sum of products of antisymmetries is a key limiting aspect of the FermiNet architecture. To explore this further, we investigate a slight modification of the FermiNet, called the full determinant mode, which replaces each product of determinants with a single combined determinant. We find that the full single-determinant FermiNet closes a large part of the gap between the standard single-determinant FermiNet and FermiNet-GA on small atomic and molecular problems. Surprisingly, on the nitrogen molecule at a dissociating bond length of 4.0 Bohr, the full single-determinant FermiNet can outperform the largest standard FermiNet calculation with 64 determinants.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2026

Experiments and simulations on the Richtmyer-Meshkov instability with a thin intermediate layer

Experiments and simulations of the Richtmyer-Meshkov instability (RMI) in two- and three-layer configurations are presented. The two-layer case utilizes a light-over-heavy configuration and consists of air as the light gas and sulfur hexafluoride (SF 6 ) as the heavy gas. The three-layer case utilizes a light-intermediate-heavy configuration, with helium (He) as the light gas, air as the intermediate gas, and SF 6 as the heavy gas. Statistically significant differences in the mixing layer width of the lower interface are not observed between the two cases. This differs from the experiments of Schalles et al., where a small, though statistically significant, difference in mixing layer growth was observed between the two- and three-layer cases with a nominally two-dimensional, single mode perturbation. Notably, the perturbations on the lower interface in the present work do not grow large enough to significantly interact with the upper interface during the duration of the experiments. In conclusion, this suggests that the differences in mixing layer growth observed by Schalles et al. may be due to interactions of the perturbations on one interface with the other interface rather than being inherent to the three-layer problem.

42 ENGINEERING↗
DOE OSTI2017

Structural and chemical evolution of the CdS:O window layer during individual CdTe solar cell processing steps

Oxygenated cadmium sulfide (CdS:O) is often used as the n-type window layer in high-performance CdTe heterojunction solar cells. The as-deposited layer prepared by reactive sputtering is XRD amorphous, with a bulk composition of CdS0.8O1.2. Recently it was shown that this layer undergoes significant transformation during device fabrication, but the roles of the individual high temperature processing steps was unclear. In this work high resolution transmission electron microscopy coupled to elemental analysis was used to understand the evolution of the heterojunction region through the individual high temperature fabrication steps of CdTe deposition, CdCl2 activation, and back contact activation. It is found that during CdTe deposition by close spaced sublimation at 600 degrees C the CdS:O film undergoes recrystallization, accompanied by a significant (~30%) reduction in thickness. It is observed that oxygen segregates during this step, forming a bi-layer morphology consisting of nanocrystalline CdS adjacent to the tin oxide contact and an oxygen-rich layer adjacent to the CdTe absorber. This bilayer structure is then lost during the 400 degrees C CdCl2 treatment where the film transforms into a heterogeneous structure with cadmium sulfate clusters distributed randomly throughout the window layer. The thickness of window layer remains essentially unchanged after CdCl2 treatment, but a ~25 nm graded interfacial layer between CdTe and the window region is formed. Finally, the rapid thermal processing step used to activate the back contact was found to have a negligible impact on the structure or composition of the heterojunction region.

14 SOLAR ENERGY↗
DOE OSTI2024

Effect of layer bending on montmorillonite hydration and structure from molecular simulation

Conceptual models of smectite hydration include planar (flat) clay layers that undergo stepwise expansion as successive monolayers of water molecules fill the interlayer regions. However, X-ray diffraction (XRD) studies indicate the presence of interstratified hydration states, suggesting non-uniform interlayer hydration in smectites. Additionally, recent theoretical studies have shown that clay layers can adopt bent configurations over nanometer-scale lateral dimensions with minimal effect on mechanical properties. Therefore, in this study we used molecular simulations to evaluate structural properties and water adsorption isotherms for montmorillonite models composed of bent clay layers in mixed hydration states. Results are compared with models consisting of planar clay layers with interstratified hydration states (e.g. 1W–2W). The small degree of bending in these models (up to 1.5 Å of vertical displacement over a 1.3 nm lateral dimension) had little or no effect on bond lengths and angle distributions within the clay layers. Except for models that included dry states, porosities and simulated water adsorption isotherms were nearly identical for bent or flat clay layers with the same averaged layer spacing. Similar agreement was seen with Na- and Ca-exchanged clays. In conclusion, while the small bent models did not retain their configurations during unconstrained molecular dynamics simulation with flexible clay layers, we show that bent structures are stable at much larger length scales by simulating a 41.6×7.1 nm 2 system that included dehydrated and hydrated regions in the same interlayer.

58 GEOSCIENCES↗
DOE OSTI2022

Destabilization of binary mixing layer in supercritical conditions

Compressible mixing layer instabilities are of importance to a wide range of environmental and industrial applications. Past studies have focused on either ideal-gas or real-fluid thermodynamic regimes of single-species mixing layers. However, mixing layers of binary mixtures at supercritical conditions, commonly encountered in fuel injection systems, introduce additional complexities due to the added compositional degree-of-freedom. Moreover, the effect of strong variations in thermodynamic response functions across the Widom line on the binary mixing layer stability remains poorly understood. Thus, the objective of this study is to examine the coupling between the hydrodynamic instability and the real-fluid thermodynamics across the Widom line and its effects on the overall binary mixing layer dynamics. To this end, we develop a linear stability analysis of the full binary-species compressible transport equations coupled with the PC-SAFT equation of state. Analysis shows the existence of a novel instability mechanism that arises from juxtapositioning of the Widom-line transition and the hydrodynamic inflection point. This novel thermodynamically induced instability mechanism has the net effect of destabilizing the binary mixing layer at lowering supercritical conditions towards the critical pressure point. This is in contrast to previous stability analyses of supercritical single-species mixing layers, where increasing pressure destabilizes the flow due to its effect on reducing the density stratification. The discovered thermodynamically induced instability mechanism of binary mixing flows highlights the need for an extension of classical instability criteria to incorporate the effect of strong variations in the thermodynamic response functions across the Widom line on mixing layer instability.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Capacitive Energy Extraction by Few-Layer Graphene Electrodes

Capacitive double-layer expansion is a promising technology to harvest energy arising from the salinity difference between freshwater and seawater. Its optimal performance requires a careful selection of the operation potentials and electrode materials. While carbonaceous materials such as graphene and various forms of activated carbons are routinely used as the electrodes, there is little knowledge on how the quantum capacitance and the electric double-layer (EDL) capacitance, which are on the same order of magnitude, affect the capacitive performance. Toward understanding that from a theoretical perspective, here we study the capacitive energy extraction with graphene electrodes as a function of the number of graphene layers. The classical density functional theory is joined with the electronic density functional theory to obtain the EDL and the quantum capacitance, respectively. The theoretical results show that the quantum capacitance contribution plays a dominant role in extracting energy using the single-layer graphene, but its effect diminishes as the number of graphene layers increases. The overall extracted energy is dominated by the EDL contribution beyond about four graphene layers. Electrodes with more graphene layers are able to extract more energy at low charging potential. Here, because many porous carbons have nanopores with stacked graphene layers, our theoretical predictions are useful to identify optimal operation parameters for capacitive energy extraction with porous electrodes of different wall thickness.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Less is More: Improved Thermal Stability and Plasmonic Response in Au Films via the Use of SubNanometer Ti Adhesion Layers

The use of a metallic adhesion layer is known to increase the thermo-mechanical stability of Au thin films against solid-state dewetting, but in turn results in damping of the plasmonic response, reducing their utility in applications such as heat-assisted magnetic recording (HAMR). In this work, 50 nm Au films with Ti adhesion layers ranging in thickness from 0 to 5 nm were fabricated, and their thermal stability, electrical resistivity, and plasmonic response were measured. Subnanometer adhesion layers are demonstrated to significantly increase the stability of the thin films against dewetting at elevated temperatures (>200 °C), compared to more commonly used adhesion layer thicknesses that are in the range of 2-5 nm. For adhesion layers thicker than 1 nm, the diffusion of excess Ti through Au grain boundaries and subsequent oxidation was determined to result in degradation of the film. This mechanism was confirmed using transmission electron microscopy and X-ray photoelectron spectroscopy on annealed 0.5 and 5 nm adhesion layer samples. The superiority of subnanometer adhesion layers was further demonstrated through measurements of the surface-plasmon polariton resonance; those with thinner adhesion layers possessed both a stronger and spectrally sharper resonance. Furthermore, these results have relevance beyond HAMR to all Ti/Au systems operating at elevated temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Cloud‐Surface Coupling Alters the Morning Transition From Stable to Unstable Boundary Layer

Abstract Due to surface heating, the morning boundary layer transits from stable to neutral or convective conditions, exerting critical influences on low tropospheric thermodynamics. Low clouds closely interact with the boundary layer development, yet their interactions bear considerable uncertainties. Our study reveals that cloud‐surface coupling alters the morning transition from stable to unstable boundary layer and thus notably affects the diurnal variation of the boundary layer. Specifically, due to the reduction in surface fluxes, decoupled clouds can delay the process of eroding nocturnal inversion by 0.8‐hr and even prevent the transition of the boundary layer from happening for 12% of decoupled cases, keeping the boundary layer in a stable state during the noontime. On the other hand, when clouds are coupled with the surface, cloud‐top radiative cooling can directly cool the upper boundary layer to facilitate sub‐cloud convection, leading to an unstable boundary layer in the earlier morning.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Unveiling the operation mechanism of layered perovskite solar cells

Layered perovskites have been shown to improve the stability of perovskite solar cells while its operation mechanism remains unclear. Here we investigate the process for the conversion of light to electrical current in high performance layered perovskite solar cells by examining its real morphology. The layered perovskite films in this study are found to be a mixture of layered and three dimensional (3D)-like phases with phase separations at micrometer and nanometer scale in both vertical and lateral directions. This phase separation is explained by the surface initiated crystallization process and the competition of the crystallization between 3D-like and layered perovskites. We further propose that the working mechanisms of the layered perovskite solar cells involve energy transfer from layered to 3D-like perovskite network. The impact of morphology on efficiency and stability of the hot-cast layered perovskite solar cells are also discussed to provide guidelines for the future improvement.

14 SOLAR ENERGY↗
DOE OSTI2021

Layer number dependent ferroelasticity in 2D Ruddlesden–Popper organic-inorganic hybrid perovskites

Ferroelasticity represents material domains possessing spontaneous strain that can be switched by external stress. Three-dimensional perovskites like methylammonium lead iodide are determined to be ferroelastic. Layered perovskites have been applied in optoelectronic devices with outstanding performance. However, the understanding of lattice strain and ferroelasticity in layered perovskites is still lacking. Here, using the in-situ observation of switching domains in layered perovskite single crystals under external strain, we discover the evidence of ferroelasticity in layered perovskites with layer number more than one, while the perovskites with single octahedra layer do not show ferroelasticity. Density functional theory calculation shows that ferroelasticity in layered perovskites originates from the distortion of inorganic octahedra resulting from the rotation of aspherical methylammonium cations. The absence of methylammonium cations in single layer perovskite accounts for the lack of ferroelasticity. These ferroelastic domains do not induce non-radiative recombination or reduce the photoluminescence quantum yield.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Emergence of antiferromagnetic correlations and Kondolike features in a model for infinite layer nickelates

We report a determinant quantum Monte Carlo study of a two-band model, inspired by infinite-layer nickelates, focusing on the influence of interlayer hybridization between $3d_{x^{2}-y^{2}}$ orbitals derived from Ni (or Ni and O) in one layer and rare-earth (R) 5d orbitals in the other layer, hereafter the Ni and R layers, respectively. For a filling with one electron shared between the two layers on average, interlayer hybridization leads to “self-doped" holes in the Ni layer and the absence of antiferromagnetic ordering, but rather the appearance of spin-density and charge-density stripe-like states. As the interlayer hybridization increases, both the Ni and R layers develop antiferromagnetic correlations, even though either layer individually remains away from half-filling. For hybridization within an intermediate range, roughly comparable to the intralayer nearest-neighbor hopping t Ni , the model develops signatures of Kondo-like physics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

High-throughput manufacturing of epitaxial membranes from a single wafer by 2D materials-based layer transfer process

Layer transfer techniques have been extensively explored for semiconductor device fabrication as a path to reduce costs and to form heterogeneously integrated devices. These techniques entail isolating epitaxial layers from an expensive donor wafer to form freestanding membranes. However, current layer transfer processes are still low-throughput and too expensive to be commercially suitable. Here we report a high-throughput layer transfer technique that can produce multiple compound semiconductor membranes from a single wafer. We directly grow two-dimensional (2D) materials on III–N and III–V substrates using epitaxy tools, which enables a scheme comprised of multiple alternating layers of 2D materials and epilayers that can be formed by a single growth run. Each epilayer in the multistack structure is then harvested by layer-by-layer mechanical exfoliation, producing multiple freestanding membranes from a single wafer without involving time-consuming processes such as sacrificial layer etching or wafer polishing. Moreover, atomic-precision exfoliation at the 2D interface allows for the recycling of the wafers for subsequent membrane production, with the potential for greatly reducing the manufacturing cost.

77 NANOSCIENCE AND NANOTECHNOLOGY↗