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All sources NASA NTRS DOE OSTI

DOE OSTI2021

Comparative Studies of Optoelectronic Properties, Structures, and Surface Morphologies for Phosphorus-Doped Poly-Si/SiOx Passivating Contacts

We investigated and compared optoelectronic properties, crystallographic structures, and nanoscale surface morphologies of ex-situ phosphorus-doped polycrystalline silicon (poly-Si)/SiO x passivating contacts, formed by different deposition methods (sputtering, plasma-enhanced chemical vapour deposition (PECVD), and low-pressure chemical vapour deposition (LPCVD)). Across all these deposition technologies, a similar trend is observed: higher diffusion temperatures yield films that are more crystalline but have rougher surface morphologies due to bigger surface crystal grains. Also, the recrystallization process of the as-deposited Si films starts from the SiO x interface, rather than from the film surface and bulk. However, there are some distinct differences among these technologies. Firstly, the LPCVD method yields the roughest surface and smallest degree of crystallinity on finished poly-Si films. In contrast, the PECVD method has the smoothest surface for both as-deposited Si and annealed poly-Si films. Secondly, as-deposited sputtered and PECVD Si films contain only an amorphous phase whereas as-deposited LPCVD films has already had some crystalline phase. Thirdly, the LPCVD phosphorus in-diffusion into the substrate depends strongly on the initial film thickness, whereas for the other two methods it is weakly dependent on thickness.

crystallographic structures↗

NASA NTRS2017

Estimating Surface Soil Moisture from SMAP Observations Using a Neural Network Technique

A Neural Network (NN) algorithm was developed to estimate global surface soil moisture for April 2015 to March 2017 with a 2-3 day repeat frequency using passive microwave observations from the Soil Moisture Active Passive (SMAP) satellite, surface soil temperatures from the NASA Goddard Earth Observing System Model version 5 (GEOS-5) land modeling system, and Moderate Resolution Imaging Spectroradiometer-based vegetation water content. The NN was trained on GEOS-5 soil moisture target data, making the NN estimates consistent with the GEOS-5 climatology, such that they may ultimately be assimilated into this model without further bias correction. Evaluated against in situ soil moisture measurements, the average unbiased root mean square error (ubRMSE), correlation and anomaly correlation of the NN retrievals were 0.037 m(exp. 3)m(exp. -3), 0.70 and 0.66, respectively, against SMAP core validation site measurements and 0.026 m(exp. 3)m(exp. -3), 0.58 and 0.48, respectively, against International Soil Moisture Network (ISMN) measurements. At the core validation sites, the NN retrievals have a significantly higher skill than the GEOS-5 model estimates and a slightly lower correlation skill than the SMAP Level-2 Passive (L2P) product. The feasibility of the NN method was reflected by a lower ubRMSE compared to the L2P retrievals as well as a higher skill when ancillary parameters in physically-based retrievals were uncertain. Against ISMN measurements, the skill of the two retrieval products was more comparable. A triple collocation analysis against Advanced Microwave Scanning Radiometer 2 (AMSR2) and Advanced Scatterometer (ASCAT) soil moisture retrievals showed that the NN and L2P retrieval errors have a similar spatial distribution, but the NN retrieval errors are generally lower in densely vegetated regions and transition zones.

Soil Moisture Remote Sensing↗

DOE OSTI2022

High grain boundary recombination velocity in polycrystalline metal halide perovskites

Understanding carrier recombination processes in metal halide perovskites is fundamentally important to further improving the efficiency of perovskite solar cells, yet the accurate recombination velocity at grain boundaries (GBs) has not been determined. Here, we report the determination of carrier recombination velocities at GBs (S GB ) of polycrystalline perovskites by mapping the transient photoluminescence pattern change induced by the nonradiative recombination of carriers at GBs. Charge recombination at GBs is revealed to be even stronger than at surfaces of unpassivated films, with average S GB reaching 2200 to 3300 cm/s. Regular surface treatments do not passivate GBs because of the absence of contact at GBs. We find a surface treatment using tributyl(methyl)phosphonium dimethyl phosphate that can penetrate into GBs by partially dissolving GBs and converting it into one-dimensional perovskites. It reduces the average S GB by four times, with the lowest SGB of 410 cm/s, which is comparable to surface recombination velocities after passivation.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Effect of Surface Texture on Pinhole Formation in SiO x -Based Passivated Contacts for High-Performance Silicon Solar Cells

High-efficiency silicon solar cells rely on some form of passivating contact structure to reduce recombination losses at the crystalline silicon surface and losses at the metal/Si contact interface. One such structure is polycrystalline silicon (poly-Si) on oxide, where heavily doped poly-Si is deposited on a SiO x layer grown directly on the crystalline silicon (c-Si) wafer. Depending on the thickness of the SiO x layer, the charge carriers can cross this layer by tunneling (<2 nm SiO x thickness) or by direct conduction through disruptions in the SiOx, often referred to as pinholes, in thicker SiO x layers (>2 nm). In this work, we study structures with tunneling- or pinhole-like SiO x contacts grown on pyramidally textured c-Si wafers and expose variations in the SiOx layer properties related to surface morphology using electron-beam-induced current (EBIC) imaging. Using EBIC, we identify and mark regions with potential pinholes in the SiO x layer. We further perform high-resolution transmission electron microscopy on the same areas, thus allowing us to directly correlate locally enhanced carrier collection with variations in the structure of the SiO x layer. Our results show that the pinholes in the SiO x layer preferentially form in different locations based on the annealing conditions used to form the device. With greater understanding of these processes and by controlling the surface texture geometry, there is potential to control the size and spatial distribution of oxide disruptions in silicon solar cells with poly-Si on oxide-type contacts; usually, this is a random phenomenon on polished or planar surfaces. Such control will enable us to consistently produce high-efficiency devices with low recombination currents and low junction resistances using this contact structure.

14 SOLAR ENERGY↗

DOE OSTI2022

Nanoscale Mg-Depleted Layers Slow Carbonation of Forsterite (Mg 2 SiO 4 ) When Water Is Limited

Passivation of silicate surfaces by accumulated reaction products is an obstacle to efficient CO 2 mineralization. In this study, we investigate a unique passivation effect during the carbonation of the basalt mineral forsterite (Mg 2 SiO 4 ) in humid supercritical CO 2 (50 °C, 90 bar). Using in situ high-pressure infrared spectroscopy, we demonstrate that dissolution of forsterite into a thin water film slows significantly after reaction for ˜24 h, even under far-from-equilibrium conditions. Further, 29 Si magic angle spinning nuclear magnetic resonance spectroscopy detects a highly polymerized amorphous silica at this stage. On the basis of transmission electron microscopy and energy dispersive X-ray spectroscopy, we show that the silica is present as a Mg-depleted layer that is just 2–3 nm thick on the reacted forsterite particles. The decrease in the level of forsterite dissolution in the presence of an extraordinarily thin Mg-depleted layer can be strongly linked to properties of the thin fluid film at the surface, highlighting the importance of water during mineral carbonation. This study furthers our understanding of silicate mineral carbonation under select low-water, humidified fluid conditions relevant to basaltic geologic reservoirs, recovery of critical elements by carbonation of mafic ores, and sequestration of atmospheric CO 2 by enhanced rock weathering.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Gas-phase surface modification to control catalyst structure and yields in methane dehydroaromatization

Methane dehydroaromatization (MDA) is a promising approach for direct methane transformation to aromatics and hydrogen. The benchmark catalyst Mo/H-ZSM-5 struggles to find commercial adoption because of thermodynamically-limited yields and rapid coking on Brønsted acid and molybdenum carbide species, especially on zeolite external surfaces. Here, gas-phase atomic layer deposition (ALD) overcoats H-ZSM-5 external surfaces with SiO 2 or Al 2 O 3 . NH 3 -TPD, HRTEM, and textural properties show that these overcoats exclusively passivate zeolite external surfaces. Under MDA conditions, SiO 2 gives softer coke and increases cumulative benzene yields by 25%, while Al 2 O 3 strongly decreases yields. H 2 -TPR and UV-visible and Raman spectroscopy show how the overcoats redisperse the MoO x precatalysts, especially over multiple deactivation and isothermal oxidative regeneration cycles. Combined with 27 Al-MAS NMR, MoO x redistribution and dealumination are seen as the causes of long-term deactivation over multiple regeneration cycles, and this process continues to occur regardless of the overcoat. Altogether, the deposition of a small amount of silica on the outer surface of Mo/H-ZSM-5 reduces the formation of hard coke, which could be regenerated by milder methods such as hydrogen treatment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1964

Discussion of the General Electric proposal to develop a computer program to select thermal coatings for passive temperature control of satellites

The General Electric Company, Missiles and Space Division, submitted/a proposal to NASA for the development of an IBM 7094 computer program which would select the exterior surface coatings for passively controlling spacecraft temperatures. G. E. claims that the "trial and error" procedures currently used can be accomplished more rationally and can therefore be programmed for a digital computer. In the ASME paper, 63-HT-41, which was presented at the ASME-AIChE Heat Transfer Conference at Boston in August, 1963, Costello, Harper, and Cline, described the procedures that have been used at G. E. to develop a coating selection program subject to the following restrictions: 1. Steady-state conditions prevail, 2. Heat transfer occurs by radiation only, 3. Temperatures are optimized at only one interior point in the spacecraft, an d 4. Only the solar absorptance of the external coatings is varied to optimize temperature. The emittance must remain constant at initially specified values. General Electric proposes to develop a generalized program in three steps: 1. The program would vary both solar absorptance and hemispherical emittance to obtain the optimum coating patterns; 2. Temperatures would be optimized at more than one interior point; and 3. The equations would be modified to account for both conduction and radiation heat transfer. In the development of the general program, the scope would be restricted to steady-state heat transfer. Since the thermal designs of most spacecraft are based primarily on nearly equilibrium conditions, the proposed program could have wide application. An obvious extension of the proposed program would be to account for transient temperatures.

IBM 7090 COMPUTER↗

DOE OSTI2020

Phase stabilization and oxidation of a continuous composition spread multi-principal element (AlFeNiTiVZr) 1-x Cr x alloy

Multi-Principal Element Alloys (MPEA) have been hypothesized to maintain a stable single alloy phase and resist corrosion at high temperatures, which are desirable in various functional applications, including material of turbine blades. However, studies into oxidation resistant alloys have been constrained to individual MPEA systems or a limited selection of compositions within those systems. Here, High-Throughput Experimental (HTE) techniques were utilized to rapidly assess phase stability and resistance to oxidation of an (AlFeNiTiVZr) 1-x Cr x continuous composition spread (CCS) thin-film alloy system. High-throughput synchrotron diffraction and Raman spectroscopy were used to identify phases, especially high symmetry structures and oxides, as a function of annealing time and composition. The formation of two distinct phase regions, R 1 and R 2 , across the CCS was observed. One of these phase regions, R 2 , exhibited a stable high symmetry BCC-like phase at Cr concentrations greater than 25.4 at%, and grew a passivating mixed metal surface oxide; whereas, the R 1 phase region, decomposed on oxidation to multiple oxides and reacted with the substrate to form silicides. The passivating mixed metal oxide layer appears to prevent destabilization of the (AlFeNiTiVZr) 1-x Cr x MPEA BCC solid solution. Furthermore, at longer annealing times the passivating phase was seen only above 29.2 at% Cr. High Cr-doped (AlFeNiTiVZr) 1-x Cr x appear to be a good candidate for high temperature, oxidation-resistant structural alloys.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Evaluating the roles of electrolyte components on the passivation of silicon anodes

A protocol was recently developed to compare calendar life using a constant potential while monitoring the electrical current required to maintain the potential. Here, this calendar life protocol is used with electrolyte formulations containing various mole fractions of ethylene carbonate (EC), ethyl methyl carbonate (EMC), and LiPF 6 to elucidate the role each component plays in passivation for high silicon anodes. Together, EC and LiPF 6 lead to higher currents, and thus poorer passivation, whereas EMC acts as a spectator. The variation of the components' mole fraction also changes the solid-electrolyte interphase (SEI) composition, as measured by x-ray photoelectron spectroscopy. Importantly, higher LiPF 6 content leads to increased LiF as well as increased current, indicating that higher LiF content does not enhance the passivation of the silicon surface. Finding that EC did not yield a passivating SEI, instead ethylene sulfite, sulfolane, and propylene carbonate (PC) were used in place of EC. Using ethylene sulfite and sulfolane resulted in poorer passivation compared to EC, whereas PC resulted in superior passivation. As a result, the superior passivation may be related to more stable lithium-solvent complexes.

25 ENERGY STORAGE↗

DOE OSTI2021

Catalytic open-circuit passivation by thin metal oxide films of p-Si anodes in aqueous alkaline electrolytes

Ni and NiO x -based protective thin films are shown to catalyze the oxidation of Si in the presence of O 2 in strongly alkaline KOH(aq) even in the absence of illumination. The O 2 in solution drove the open-circuit potential of the electrode to >0.4 V, which is positive of the Si passivation potential. The elevated electrochemical potential of the surface promoted formation of passive oxides on exposed Si regions of Si/Ni electrodes. Catalytic passivation of Si extended the durability of an np + -Si(100)/NiO x photoanode to >400 h while operating under simulated day/night cycles. In contrast, electrodes without a Ni(O x ) layer and/or without O 2 in solution displayed direct etching of the Si and corrosion pitting during non-illuminated, simulated nighttime episodes of day/night cycling. The O 2 -derived catalyzed passivation of Si using thin films can be generalized to multiple phases of NiO x as well as to materials other than Ni. Finally, relative to operation in aqueous alkaline conditions, decreasing the pH of the electrolyte decreased the dissolution rate of the protective oxide layer formed by the catalyzed passivation process, and consequently increased the durability of the photoanode, but yielded lower photoelectrode fill factors for water oxidation due to the relatively large kinetic overpotentials for the electrocatalyzed oxygen-evolution reaction at near-neutral pH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2020

Simultaneous Retrieval of Surface Roughness Parameters for Bare Soils from Combined Active-Passive Microwave SMAP Observations

An active-passive microwave retrieval algorithm for simultaneous determination of soil surface roughness parameters [vertical root-mean-square (RMS) height (s) and horizontal correlation length (l)] is presented for bare soils. The algorithm is based on active-passive microwave covariation, including the improved Integral Equation Method (I²EM), and is tested with global soil moisture active passive (SMAP) observations. The estimated retrieval results for s and l are overall consistent with values in the literature, indicating the validity of the proposed algorithm. Sensitivity analyses showed that the developed roughness retrieval algorithm is independent of permittivity for εₛ > 10 [-]. Furthermore, the physical model basis of this approach (I²EM) allows the application of different autocorrelation functions (ACF), such as Gaussian and exponential ACFs. Global roughness retrieval results confirm bare areas in deserts such as Sahara or Gobi. However, the type of ACF used within roughness parameter estimation is important. Retrieval results for the Gaussian ACF describe a rougher surface than retrieval results for the exponential ACF. No correlations were found between roughness results and the amount of precipitation or the soil texture, which could be due to the coarse spatial resolution of the SMAP data. The extension of this approach to vegetated soils is planned as an add-on study.

correlation length↗

DOE OSTI2021

Rapid Alloy Surface Engineering through Closed-Vessel Reagent Pyrolysis

For rapid surface engineering of Cr-containing alloys by low-temperature nitrocarburization, we introduce a process based on pyrolysis of solid reagents, e.g., urea, performed in an evacuated closed vessel. Upon heating to temperatures high enough for rapid diffusion of interstitial solute, but low enough to avoid second-phase precipitation, the reagent is pyrolyzed to a gas atmosphere containing molecules that (i) activate the alloy surface by stripping away the passivating Cr 2 O 3 -rich surface film (diffusion barrier) and (ii) rapidly infuse carbon and nitrogen into the alloy. We demonstrate quantitatively that this method can generate a subsurface zone with concentrated carbon and nitrogen comparable to what can be accomplished by established (e.g., gas-phase- or plasma-based) methods, but with significantly reduced processing time. As another important difference to established gas-phase processing, the interaction of gas molecules with the alloy surface can have auto-catalytic effects by altering the gas composition in a way that accelerates solute infusion by providing a high activity of HNCO. The new method lends itself to rapid experimentation with a minimum of laboratory equipment.

36 MATERIALS SCIENCE↗

NASA NTRS1992

Studies of the kinetics and mechanisms of perfluoroether reactions on iron and oxidized iron surfaces

Polymeric perfluoroalkylethers are being considered for use as lubricants in high temperature applications, but have been observed to catalytically decompose in the presence of metals. X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPD) were used to explore the decomposition of three model fluorinated ethers on clean polycrystalline iron surfaces and iron surfaces chemically modified with oxygen. Low temperature adsorption of the model fluorinated ethers on the clean, oxygen modified and oxidized iron surfaces was molecular. Thermally activated defluorination of the three model compounds was observed on the clean iron surface at remarkably low temperatures, 155 K and below, with formation of iron fluoride. Preferential C-F bond scission occurred at the terminal fluoromethoxy, CF3O, of perfluoro-1-methoxy-2-ethoxy ethane and perfluoro-1-methoxy-2-ethoxy propane and at CF3/CF2O of perfluoro-1,3-diethoxy propane. The reactivity of the clean iron toward perfluoroalkylether decomposition when compared to other metals is due to the strength of the iron fluoride bond and the strong electron donating ability of the metallic iron. Chemisorption of an oxygen overlayer lowered the reactivity of the iron surface to the adsorption and decomposition of the three model fluorinated ethers by blocking active sites on the metal surface. Incomplete coverage of the iron surface with chemisorbed oxygen results in a reaction which resembles the defluorination reaction observed on the clean iron surface. Perfluoro-1-methoxy-2-ethoxy ethane reacts on the oxidized iron surface at 138 K, through a Lewis acid assisted cleavage of the carbon oxygen bond, with preferential attack at the terminal fluoromethoxy, CF3O. The oxidized iron surface did not passivate, but became more reactive with time. Perfluoro-1-methoxy-2-ethoxy propane and perfluoro-1,3-diethoxy propane desorbed prior to the observation of decomposition on the oxidized iron surface.

Napier, Mary E.↗

NASA NTRS1999

Minority carrier device comprising a passivating layer including a Group 13 element and a chalcogenide component

A minority carrier device includes at least one junction of at least two dissimilar materials, at least one of which is a semiconductor, and a passivating layer on at least one surface of the device. The passivating layer includes a Group 13 element and a chalcogenide component. Embodiments of the minority carrier device include, for example, laser diodes, light emitting diodes, heterojunction bipolar transistors, and solar cells.

Barron, Andrew R.↗

NASA NTRS2016

Multistatic Aerosol Cloud Lidar in Space: A Theoretical Perspective

Accurate aerosol and cloud retrievals from space remain quite challenging and typically involve solving a severely ill-posed inverse scattering problem. In this Perspective, we formulate in general terms an aerosol and aerosol-cloud interaction space mission concept intended to provide detailed horizontal and vertical profiles of aerosol physical characteristics as well as identify mutually induced changes in the properties of aerosols and clouds. We argue that a natural and feasible way of addressing the ill-posedness of the inverse scattering problem while having an exquisite vertical-profiling capability is to fly a multistatic (including bistatic) lidar system. We analyze theoretically the capabilities of a formation-flying constellation of a primary satellite equipped with a conventional monostatic (backscattering) lidar and one or more additional platforms each hosting a receiver of the scattered laser light. If successfully implemented, this concept would combine the measurement capabilities of a passive multi-angle multi-spectral polarimeter with the vertical profiling capability of a lidar; address the ill-posedness of the inverse problem caused by the highly limited information content of monostatic lidar measurements; address the ill-posedness of the inverse problem caused by vertical integration and surface reflection in passive photopolarimetric measurements; relax polarization accuracy requirements; eliminate the need for exquisite radiative-transfer modeling of the atmosphere-surface system in data analyses; yield the day-and-night observation capability; provide direct characterization of ground-level aerosols as atmospheric pollutants; and yield direct measurements of polarized bidirectional surface reflectance. We demonstrate, in particular, that supplementing the conventional backscattering lidar with just one additional receiver flown in formation at a scattering angle close to 170deg can dramatically increase the information content of the measurements. Although the specific subject of this Perspective is the multistatic lidar concept, all our conclusions equally apply to a multistatic radar system intended to study from space the global distribution of cloud and precipitation characteristics.

aerosols↗

NASA NTRS1991

Passivation of high temperature superconductors

The surface of high temperature superconductors such as YBa2Cu3O(7-x) are passivated by reacting the native Y, Ba and Cu metal ions with an anion such as sulfate or oxalate to form a surface film that is impervious to water and has a solubility in water of no more than 10(exp -3) M. The passivating treatment is preferably conducted by immersing the surface in dilute aqueous acid solution since more soluble species dissolve into the solution. The treatment does not degrade the superconducting properties of the bulk material.

Vasquez, Richard P.↗

DOE OSTI2020

Surface plasmon driven near- and midinfrared photoconductivity in ligand-free ITO nanocrystal films

Semiconductor nanocrystals (NCs) offer exciting opportunities to deploy infrared optoelectronic technology in a variety of applications that are off-limits to conventional single-crystalline materials. However, the performance and stability of state-of-the-art NC-based devices strongly depend on the details of the NC surface and its passivating ligands. Here, the authors use indium tin oxide NC films stripped of organic ligands and conformally coated with Al 2 O 3 to show that absorption enabled by infrared localized surface plasmon resonances permit infrared photoconduction. For Au electrodes, these metallic NC films exhibit stable photoconductive performance over months in ambient and under electrical stress.

36 MATERIALS SCIENCE↗

NASA NTRS2012

Engineered Multifunctional Surfaces for Fluid Handling

Designs incorporating variations in capillary geometry and hydrophilic and/or antibacterial surface properties have been developed that are capable of passive gas/liquid separation and passive water flow. These designs can incorporate capillary grooves and/or surfaces arranged to create linear and circumferential capillary geometry at the micro and macro scale, radial fin configurations, micro holes and patterns, and combinations of the above. The antibacterial property of this design inhibits the growth of bacteria or the development of biofilm. The hydrophilic property reduces the water contact angle with a treated substrate such that water spreads into a thin layer atop the treated surface. These antibacterial and hydrophilic properties applied to a thermally conductive surface, combined with capillary geometry, create a novel heat exchanger capable of condensing water from a humid, two-phase water and gas flow onto the treated heat exchanger surfaces, and passively separating the condensed water from the gas flow in a reduced gravity application. The overall process to generate the antibacterial and hydrophilic properties includes multiple steps to generate the two different surface properties, and can be divided into two major steps. Step 1 uses a magnetron-based sputtering technique to implant the silver atoms into the base material. A layer of silver is built up on top of the base material. Completion of this step provides the antibacterial property. Step 2 uses a cold-plasma technique to generate the hydrophilic surface property on top of the silver layer generated in Step 1. Completion of this step provides the hydrophilic property in addition to the antibacterial property. Thermally conductive materials are fabricated and then treated to create the antibacterial and hydrophilic surface properties. The individual parts are assembled to create a condensing heat exchanger with antibacterial and hydrophilic surface properties and capillary geometry, which is capable of passive phase separation in a reduced gravity application. The plasma processes for creating antibacterial and hydrophilic surface properties are suitable for applications where water is present on an exposed surface for an extended time, such that bacteria or biofilms could form, and where there is a need to manage the water on the surface. The processes are also suitable for applications where only the hydrophilic property is needed. In particular, the processes are applicable to condensing heat exchangers (CHXs), which benefit from the antibacterial properties as well as the hydrophilic properties. Water condensing onto the control surfaces of the CHX will provide the moist conditions necessary for the growth of bacteria and the formation of biofilms. The antibacterial properties of the base layer (silver) will mitigate and prevent the growth of bacteria and formation of biofilms that would otherwise reduce the CHX performance. In addition, the hydrophilic properties reduce the water contact angle and prevent water droplets from bridging between control surfaces. Overall, the hydrophilic properties reduce the pressure drop across the CHX.

Thomas, Chris↗