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At least 1,621 records · Page 90
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

The effect of bond coating surface modification on the performance of atmospheric plasma spray thermal barrier coatings

Asperities in atmospheric plasma sprayed (APS) CoNiCrAlY bond coatings were observed to rapidly form spinel-type oxides growing into the APS yttria-stabilized zirconia (YSZ) top coating during isothermal exposures. To minimize these transient oxides, bond coatings were either lightly or heavily modified to remove asperities, prior to top coating deposition. After a 100 h isothermal exposure at 1100 °C in dry air, modified regions formed a thin, Al-rich thermally grown oxide (TGO) scale while unmodified regions formed Cr- and Ni-rich transient oxide. However, in 1-h furnace cycle testing (FCT) at 1100 °C, the modified bond coatings showed a reduced average lifetime compared to the specimens with unmodified bond coatings. The benefit of asperities may be to geometrically inhibit crack propagation, but the volume of transient oxide formed may also densify the adjacent YSZ and further inhibit cracking.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Engineering of niobium surfaces through accelerated neutral atom beam technology for quantum applications

A major roadblock to scalable quantum computing is phase decoherence and energy relaxation caused by qubits interacting with defect-related two-level systems (TLSs). Native oxides present on the surfaces of superconducting metals used in quantum devices are acknowledged to be a source of TLS that decrease qubit coherence times. Reducing microwave loss by “surface engineering” (i.e., replacing the uncontrolled native oxide of superconducting metals with a thin, stable surface with predictable characteristics) can be a key enabler for pushing performance forward with devices of higher intrinsic quality factor. In this work, we present a novel approach to replace the native oxide of niobium (typically formed in an uncontrolled fashion when its pristine surface is exposed to air) with an engineered oxide, using a room-temperature process that leverages accelerated neutral atom beam (ANAB) technology at 300 mm wafer scale. This ANAB is composed of a mixture of argon and oxygen, with tunable energy per atom, which is rastered across the wafer surface. The ANAB-engineered Nb-oxide thickness was found to vary from 2 to 6 nm depending on ANAB process parameters. The modeling of variable-energy x-ray photoelectron spectroscopy data confirms the thickness and compositional control of Nb surface oxide by the ANAB process. Furthermore, these results correlate well with those from transmission electron microscopy and x-ray reflectometry. Since ANAB is broadly applicable to material surfaces, the present study indicates its promise for modification of the surfaces of superconducting quantum circuits to achieve longer coherence times.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Organic-semiconducting hybrid solar cell

The embodiment of this invention lies on experimental evidence of photoconductivity activity of a hybrid solar cell, organic/chalcogenide. The device is made of thin layers of conductive indium-tin-oxide (ITO) on glass with a 100 nm layer of chalcogenide molybdenum di-sulfide (MoS 2 ) and a thin layer of about ˜50 nm of complex organic compound assembled at room temperature. The device was tested to conventional electrical transport measurements in the regime of −1V to 1V under electromagnetic radiation simulator at 100 mW/cm 2 . Results indicate solar conversion efficiency of 2.48% and current density of 6.35 mA/cm 2 .

14 SOLAR ENERGY↗
DOE OSTI2022

Atomic layer deposition of lithium zirconium oxides for the improved performance of lithium-ion batteries

Recently there has been increasing interest to develop lithium-containing films as solid-state electrolytes or surface coatings for lithium-ion batteries (LIBs) and related systems. Here, in this study, we for the first time investigated the thin film growth of lithium zirconium oxides (Li x Zr y O or LZOs) through combining two individual atomic layer deposition (ALD) processes of ZrO 2 and LiOH, i.e., sub-ALD of ZrO 2 and LiOH. We revealed that the hygroscopic nature of the LiOH component has a big impact on the growth of LZOs. We found that an increased temperature to 225 °C was more effective than an elongated purge to mitigate the adverse effects of physisorbed H 2 O. We further discovered that, during the resultant LZO super-ALD processes, the growth of sub-ALD LiOH has been promoted while the growth of sub-ALD ZrO 2 has been inhibited. In this study, a suite of instruments has been applied to characterize the LZO super-ALD processes and the resultant LZO films, including in situ quartz crystal microbalance (QCM), scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM), atomic force microscopy (AFM), synchrotron-based X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Furthermore, we applied the resulting LZO films over LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) cathodes in LIBs and demonstrated that the LZO coating films could evidently improve the lithium-ion insertion and extraction rates of the NMC622 electrodes up to 3.4 and 2.6 times, respectively. The LZO-coated NMC622 cathodes exhibited much better performance than the uncoated NMC622 ones.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Fabrication and Characterization of Front-Illuminated Dye-Sensitized Solar Cells with Anodic Titanium Oxide Nanotubes

We have fabricated front-side illuminated dye-sensitized solar cells (DSSCs) with a thin film of vertically oriented TiO2 nanotubes used as the negative electrode. The TiO2 nanotube film was formed by anodizing a metallic titanium thin film that was deposited on a transparent conductive oxide (TCO) layer with an intermediate, protective TiO2 layer.We characterized the structural and electronic properties of the formed TiO2 nanotube films. Titanium tetrachloride (TiCl4) treatment was applied on the TiO2 nanotube film to improve the performance of the DSSCs. We have investigated effects of TiCl4 treatment on the solar cell parameters of the DSSCs: short-circuit current density (ISC), open-circuit voltage (Voc), ideal factor (n), series resistance (Rs) and shunt resistance (Rsh). The parameters have been derived by analyzing measured I-V characteristic of the DSSCs on the basis of the method we have previously proposed. We demonstrate that the performance of the DSSCs is improved by TiCl4 treatment. We discuss the effects of TiCl4 treatment on the performance on the basis of the derived cell parameters.

Kojima, Ryota↗
DOE OSTI2016

Asymmetric band offsets in silicon heterojunction solar cells: Impact on device performance

Amorphous/crystalline silicon interfaces feature considerably larger valence than conduction band offsets. In this article, we analyze the impact of such band offset asymmetry on the performance of silicon heterojunction solar cells. To this end, we use silicon suboxides as passivation layers—inserted between substrate and (front or rear) contacts—since such layers enable intentionally exacerbated band-offset asymmetry. Investigating all topologically possible passivation layer permutations and focussing on light and dark current-voltage characteristics, we confirm that to avoid fill factor losses, wider-bandgap silicon oxide films (of at least several nanometer thin) should be avoided in hole-collecting contacts. As a consequence, device implementation of such films as window layers—without degraded carrier collection—demands electron collection at the front and hole collection at the rear. Furthermore, at elevated operating temperatures, once possible carrier transport barriers are overcome by thermionic (field) emission, the device performance is mainly dictated by the passivation of its surfaces. In this context, compared to the standard amorphous silicon layers, the wide-bandgap oxide layers applied here passivate remarkably better at these temperatures, which may represent an additional benefit under practical operation conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Radiative Transfer, Non-transparency, Stability Against Quench in Superconductors and Their Correlations

Radiative transfer calculations are presented for multi-filamentary BSCCO 2212 and 2223 and for thin film-coated YBaCuO 123 superconductors. A strictly radiative view allows conductor morphology of these superconductors to be interpreted as particulate or quasi-particulate objects. Problems then arising from non-regular particle shape, missing refractive indices, dependent scattering and superconductor material (diamagnetic) properties are solved in a multi-step, approximation approach. Both types of conductors are shown to be non-transparent to mid-IR radiation. Non-transparency may become critical for superconductor stability. The obtained extinction cross sections converge near the phase transition. A substantial difference of extinction properties between the superconducting and normal conducting state thus cannot be observed. As a first corollary from non-transparency, application of the additive approximation for the total thermal conductivity used in previous numerical calculations of the BSCCO and YBaCuO superconductors is confirmed. Second, within transit time intervals, the length of which depends on optical thickness, no uniform equilibrium conditions of electron pair density within the conductor cross section and near critical temperature are observed. Phase transition does not proceed uniformly, neither spatial nor temporal, and the order (succession on time scales) of local events (temperature variations, quench), in extreme cases, is completely dissolved. As another corollary, non-transparency even makes the existence of uniquely defined, physical time scales doubtful in a superconductor. The obtained results are expected to improve existing stability models and will be of practical value for future materials development.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Detection of saliva-range glucose concentrations using organic thin-film transistors

We describe the development of a glucose sensor through direct incorporation of an enzyme (glucose oxidase) into the gate of an organic thin film transistor (OTFT). We show that glucose diffusion is the key determinant of the device response time and present a mechanism of glucose sensing in these devices that involves protonic doping of the transistor channel via enzymatic oxidation of glucose. The integrated OTFT sensor is sensitive across 4 decades of glucose concentration; a range that encompasses both the blood and salivary glucose concentration levels. As such, this work acts as a proof-of-concept for low-cost printed biosensors for salivary glucose.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1988

RF surface resistance of YBa2Cu3O(7-x) thin films

The excitement engendered by the discovery of the new T sub c oxide superconductors has led to much speculation about practical applications of thin films of these materials in digital and analog electronic devices. Most of these envisioned applications involve high frequency signals for which a detailed knowledge of the surface impedance of the novel superconductors is very important. We have measured the surface resistance of thin films of YBaCuO in the frequency range 0.5 less than f less than 17 GHz using a stripline-resonator method. The stripline procedure also was used to measure the surface resistance of high quality gold and aluminum films; the resistance values obtained agree with values predicted from the measured dc resistance using the Pippard formalism for the anomalous skin effect. The YBaCuO were produced by a multilayer deposition process. The films are formed by e-beam evaporation of 24 layers of Y, Ba, and Cu. Films with the highest transition temperature were obtained using yttria-stabilized zirconia (YSZ) substrates. After deposition, the films are transferred to a furnace where they are annealed in flowing O2 at 850 C for 2h. The furnace then is turned off and allowed to cool to 100 C in about 16 h. Auger profiling of the films made by this process shows that the concentrations of Y, Ba, Cu, and O are uniform to within 1 percent throughout the thickness of the film.

Source record↗
DOE OSTI2022

Direct utilization of gaseous fuels in metal supported solid oxide fuel cells

Direct utilization and internal reforming of gaseous fuels is investigated on symmetric-architecture metal supported solid oxide fuel cells (MS-SOFCs) with thin ceramic electrolyte and scaffold backbone layers, and low cost ferritic stainless steel supports on both sides. Infiltrated Pr-oxide and Ni/samarium-doped ceria catalysts are added to the cathode and anode electrodes, respectively. Initial performance and durability is evaluated for MS-SOFCs operating with natural gas, propane, ammonia, and dimethyl ether at 700 °C. Cells for natural gas and propane utilize a novel high entropy alloy (HEA) catalyst for internal reforming with performance and degradation rates similar to H 2 (0.5W cm -2 and ~12%/100 h). In conclusion, initial testing with sulfur shows reversible degradation for levels found in natural gas and irreversible degradation for higher levels found in commercial propane. Overall, MS-SOFCs show successful fuel flexibility.

08 HYDROGEN↗
DOE OSTI2017

Investigation of Cody–Lorentz and Tauc–Lorentz Models in Characterizing Dielectric Function of (HfO{sub 2}){sub x}(ZrO{sub 2}){sub 1–x} Mixed Thin Film

In the present study, Tauc–Lorentz and Urbach tail assisted Cody–Lorentz models were intuitively derived, explained, and employed to simulate the imaginary dielectric function of the atomic layer deposited (HfO{sub 2}){sub x}(ZrO{sub 2}){sub 1–x} in the energy range of 0.7–9.3 eV. A fitting procedure is carried out using the Levenberg–Marquardt method for minimizing mean square errors. Both models support the experimental data derived by vacuum ultraviolet spectroscopic ellipsometry. For a zirconium content of 60 and 75%, a weak absorption profile is observed in the visible region and elaborately explained by the Lorentz oscillator model. In order to calculate the band gap of different compositions, Cody plots and Tauc plots are presented. The results show that the Cody–Lorentz model is more accuracy due to its exponential absorption below the band gap energy and modified density of states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Nano-engineering the material structure of preferentially oriented nano-graphitic carbon for making high-performance electrochemical micro-sensors

Direct synthesis of thin-film carbon nanomaterials on oxide-coated silicon substrates provides a viable pathway for building a dense array of miniaturized (micron-scale) electrochemical sensors with high performance. However, material synthesis generally involves many parameters, making material engineering based on trial and error highly inefficient. Here, we report a two-pronged strategy for producing engineered thin-film carbon nanomaterials that have a nano-graphitic structure. First, we introduce a variant of the metal-induced graphitization technique that generates micron-scale islands of nano-graphitic carbon materials directly on oxide-coated silicon substrates. A novel feature of our material synthesis is that, through substrate engineering, the orientation of graphitic planes within the film aligns preferentially with the silicon substrate. This feature allows us to use the Raman spectroscopy for quantifying structural properties of the sensor surface, where the electrochemical processes occur. Second, we find phenomenological models for predicting the amplitudes of the redox current and the sensor capacitance from the material structure, quantified by Raman. Our results indicate that the key to achieving high-performance micro-sensors from nano-graphitic carbon is to increase both the density of point defects and the size of the graphitic crystallites. Our study offers a viable strategy for building planar electrochemical micro-sensors with high-performance.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Unraveling the Stable Cathode Electrolyte Interface in all Solid‐State Thin‐Film Battery Operating at 5 V

Abstract Spinel‐type LiNi 0.5 Mn 1.5 O 4 (LNMO) is one of the most promising 5 V‐class cathode materials for Li‐ion batteries that can achieve high energy density and low production costs. However, in liquid electrolyte cells, the high voltage causes continuous cell degradation through the oxidative decomposition of carbonate‐based liquid electrolytes. In contrast, some solid‐state electrolytes have a wide electrochemical stability range and can withstand the required oxidative potential. In this work, a thin‐film battery consisting of an LNMO cathode with a solid lithium phosphorus oxynitride (LiPON) electrolyte is tested and their interface before and after cycling is characterized. With Li metal as the anode, this system can deliver stable performance for 600 cycles with an average Coulombic efficiency >99%. Neutron depth profiling indicates a slight overlithiated layer at the interface prior to cycling, a result that is consistent with the excess charge capacity measured during the first cycle. Cryogenic electron microscopy further reveals intimate contact between LNMO and LiPON without noticeable structure and chemical composition evolution after extended cycling, demonstrating the superior stability of LiPON against a high voltage cathode. Consequently, design guidelines are proposed for interface engineering that can accelerate the commercialization of a high voltage cell with solid or liquid electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2016

Indium tin oxide refractometer in the visible and near infrared via lossy mode and surface plasmon resonances with Kretschmann configuration

An indium tin oxide (ITO) refractometer based on the generation of lossy mode resonances (LMRs) and surface plasmon resonances (SPRs) is presented. Both LMRs and SPRs are excited, in a single setup, under grazing angle incidence with Kretschmann configuration in an ITO thin-film deposited on a glass slide. The sensing capabilities of the device are demonstrated using several solutions of glycerin and water with refractive indices ranging from 1.33 to 1.47. LMRs are excited in the visible range, from 617 nm to 682 nm under TE polarization and from 533 nm to 637 nm under TM polarization, with a maximum sensitivity of 700 nm/RIU and 1200 nm/RIU, respectively. For the SPRs, a sensing range between 1375 nm and 2494 nm with a maximum sensitivity of 8300 nm/RIU is measured under TM polarization. Experimental results are supported with numerical simulations based on a modification of the plane-wave method for a one-dimensional multilayer waveguide.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Solid-state rechargeable magnesium battery

Embodiments of a solid-state electrolyte comprising magnesium borohydride, polyethylene oxide, and optionally a Group IIA or transition metal oxide are disclosed. The solid-state electrolyte may be a thin film comprising a dispersion of magnesium borohydride and magnesium oxide nanoparticles in polyethylene oxide. Rechargeable magnesium batteries including the disclosed solid-state electrolyte may have a coulombic efficiency .gtoreq.95% and exhibit cycling stability for at least 50 cycles.

25 ENERGY STORAGE↗
DOE OSTI2014

Observation of radio frequency ring-shaped hollow cathode discharge plasma with MgO and Al electrodes for plasma processing

Various high-density plasma sources have been proposed for plasma processing. Especially, the hollow cathode discharge is one of the powerful ones. In this work, radio-frequency (RF) driven ring-shaped hollow cathode discharges with high secondary-electron emission have been investigated, using an aluminum (Al) cathode, coated or not with magnesium oxide (MgO). The thickness of MgO thin film is approximately 200 nm. The RF discharge voltage for the coated cathode is almost the same as that for the uncoated one, in a wide range of Ar gas pressure, from 5.3 to 53.2 Pa. The results reveal that the plasma density has a peak at an Ar gas pressure of 10.6 Pa for both cathodes. The plasma density for the coated cathode is about 1.5–3 times higher than that for the uncoated one, at various gas pressures. To the contrary, the electron temperature for the coated cathode is lower than temperature obtained with the uncoated cathode, at various gas pressures. Radial profiles of electron saturation current, which is proportional to plasma flux, are also examined for a wide range of gas pressure. Radial profiles of electron temperature at various axial positions are almost uniform for both cathodes so that the diffusion process due to density gradient is dominant for plasma transport. The secondary electrons emitted from the coated cathode contribute to the improvement of the plasma flux radial profile obtained using the uncoated cathode.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Thermal conductivity control by oxygen defect concentration modification in reducible oxides: The case of Pr{sub 0.1}Ce{sub 0.9}O{sub 2−δ} thin films

We demonstrate the impact on thermal conductivity of varying the concentration of oxygen vacancies and reduced cations in Pr{sub 0.1}Ce{sub 0.9}O{sub 2−δ} thin films prepared by pulsed laser deposition. The oxygen vacancy concentration is controlled by varying the oxygen partial pressure between 1 × 10{sup −4} and 1 atm at 650 °C. Corresponding changes in the oxygen non-stoichiometry (δ) are monitored by detecting the lattice parameters of the films with high-resolution X-ray diffraction, while the thermal properties are characterized by time-domain thermoreflectance measurements. The films are shown to exhibit a variation in oxygen vacancy content, and in the Pr{sup 3+}/Pr{sup 4+} ratio, corresponding to changes in δ from 0.0027 to 0.0364, leading to a reduction in the thermal conductivity from k = 6.62 ± 0.61 to 3.82 ± 0.51 W/m-K, respectively. These values agree well with those predicted by the Callaway and von Baeyer model for thermal conductivity in the presence of point imperfections. These results demonstrate the capability of controlling thermal conductivity via control of anion and cation defect concentrations in a given reducible oxide.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗