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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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Atomic layer deposition and other thin film deposition techniques: from principles to film properties
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Defects in local atomic structure of ZnO films sensitized with tinto and mangrove organic dyes
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Multifunctional smart electronic skin fabricated from two-dimensional like polymer film
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Nanostructured Pr-doped Ceria (PCO) thin films as sensing electrodes in solid-electrolyte type gas sensors with enhanced toluene sensitivity
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Strong cube-textured titanium nitride conductive films directly on flexible metal substrate
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Reveal of Magnetic Domains and Tunable Supercell Structures in Two-dimensional Layered Oxide Thin Film via Differential Phase Contrast Imaging and Atomic-resolution STEM
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Reduced recombination via tunable surface fields in perovskite thin films
Here, the ability to reduce energy loss at semiconductor surfaces through passivation or surface field engineering is an essential step in the manufacturing of efficient photovoltaic (PV) and optoelectronic devices. Similarly, surface modification of emerging halide perovskites with quasi-two-dimensional (2D) heterostructures is now ubiquitous to achieve PV power conversion efficiencies (PCEs) >25%, yet a fundamental understanding to how these treatments function is still generally lacking. Here we use a unique combination of depth-sensitive nanoscale characterization techniques to uncover a tunable passivation strategy and mechanism found in perovskite PV devices that were the first to reach the >25% PCE milestone. Namely, treatment with hexylammonium bromide leads to the simultaneous formation of an iodide-rich 2D layer along with a Br halide gradient that extends from defective surfaces and grain boundaries into the bulk three-dimensional (3D) layer. This interface can be optimized to extend the charge carrier lifetime to record values >30 μs and to reduce interfacial recombination velocities to values as low as <7 cm s −1 .
Role of the electronically-active amorphous state in low-temperature processed In2O3 thin-film transistors
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High-performance magnesium metal batteries via switching the passivation film into a solid electrolyte interphase
Mg 2+ electroplating has been an obstacle for Mg metal batteries due to the passivating nature of Mg metal. Here, a unique current collector based on an amorphous MgO-wrapped Zn-skeleton enabled Mg 2+ electroplating for a high-voltage Mg metal battery.
Amorphous-to-crystalline transition of thin-film TiO2 precursor films to brookite, anatase, and rutile polymorphs
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Thermal Conductivity of β-Phase Ga 2 O 3 and (Al x Ga 1– x ) 2 O 3 Heteroepitaxial Thin Films
Heteroepitaxy of β-phase gallium oxide (β-Ga 2 O 3 ) thin films on foreign substrates shows promise for the development of next-generation deep ultraviolet solar blind photodetectors and power electronic devices. In this work, the influences of the film thickness and crystallinity on the thermal conductivity of ($\bar{2}01$)-oriented β-Ga 2 O 3 heteroepitaxial thin films were investigated. Unintentionally doped β-Ga 2 O 3 thin films were grown on c-plane sapphire substrates with off-axis angles of 0° and 6° toward $\langle$$11\bar{2}0$$\rangle$ via metal–organic vapor phase epitaxy (MOVPE) and low-pressure chemical vapor deposition. The surface morphology and crystal quality of the β-Ga 2 O 3 thin films were characterized using scanning electron microscopy, X-ray diffraction, and Raman spectroscopy. The thermal conductivities of the β-Ga 2 O 3 films were measured via time-domain thermoreflectance. The interface quality was studied using scanning transmission electron microscopy. The measured thermal conductivities of the submicron-thick β-Ga 2 O 3 thin films were relatively low as compared to the intrinsic bulk value. The measured thin film thermal conductivities were compared with the Debye–Callaway model incorporating phononic parameters derived from first-principles calculations. The comparison suggests that the reduction in the thin film thermal conductivity can be partially attributed to the enhanced phonon-boundary scattering when the film thickness decreases. They were found to be a strong function of not only the layer thickness but also the film quality, resulting from growth on substrates with different offcut angles. Growth of β-Ga 2 O 3 films on 6° offcut sapphire substrates was found to result in higher crystallinity and thermal conductivity than films grown on on-axis c-plane sapphire. However, the β-Ga 2 O 3 films grown on 6° offcut sapphire exhibit a lower thermal boundary conductance at the β-Ga 2 O 3 /sapphire heterointerface. In addition, the thermal conductivity of MOVPE-grown ($\bar{2}01$)-oriented β-(Al x Ga 1–x ) 2 O 3 thin films with Al compositions ranging from 2% to 43% was characterized. Because of phonon-alloy disorder scattering, the β-(Al x Ga 1–x ) 2 O 3 films exhibit lower thermal conductivities (2.8–4.7 W/m∙K) than the β-Ga 2 O 3 thin films. The dominance of the alloy disorder scattering in β-(Al x Ga 1–x ) 2 O 3 is further evidenced by the weak temperature dependence of the thermal conductivity. This work provides fundamental insight into the physical interactions that govern phonon transport within heteroepitaxially grown β-phase Ga 2 O 3 and (Al x Ga 1–x ) 2 O 3 thin films and lays the groundwork for the thermal modeling and design of β-Ga 2 O 3 electronic and optoelectronic devices.
Continuous polymer films deposited on top of porous substrates using plasma-enhanced atomic layer deposition and molecular layer deposition
Molecular layer deposition (MLD) is able to produce ultrathin polymer films with control over thickness, cross-linking, and chemical composition. With these capabilities, MLD should be useful in the fabrication of novel polymer membranes on porous supports. However, confining a continuous MLD film to the surface of porous substrates is difficult because of MLD film growth in the pores. The deposition in the pores lowers the conductance of the porous support. This paper presents a method to deposit continuous polymer films on top of porous substrates. In this method, Al2O3 plasma-enhanced atomic layer deposition (PE-ALD) using trimethylaluminum and oxygen plasma as the reactants was first used to cap the pores of the substrate. Subsequently, a polyamide MLD film was deposited on the Al2O3 PE-ALD capping layer using m-phenylenediamine and trimesoyl chloride as the reactants. The Al2O3 pore caps were then removed from the porous substrate by etching from the backside using a timed exposure to a dilute sodium hydroxide solution. This method was demonstrated using anodic aluminum oxide (AAO) and polyethersulfone (PES) porous substrates. Al2O3 PE-ALD film growth was limited to the top of the porous substrate, resulting in rapid surface recombination or high sticking coefficients for the reactive plasma species within the pores. Gas permeance measurements confirmed the pore capping of the AAO substrates. The reopening of the pores by dissolving the Al2O3 pore caps with a sodium hydroxide solution was monitored using gas permeance versus etch time. The removal of the Al2O3 pore caps from the PES substrates could also dissolve the Al2O3 layer underneath the MLD film. The loss of this Al2O3 layer led to the detachment of the MLD film from the PES substrate. However, the MLD film could be anchored to the PES support at fractures located in the Al2O3 film prior to the MLD. The Al2O3 film fracture allowed the MLD film to anchor firmly to the PES substrate by MLD in the pores of the PES porous substrate. The distance between the anchor points was a function of fracture density. This distance could be controlled by applying a tensile stress to the Al2O3 PE-ALD film to fracture the film through sample bending. This method produced firmly anchored polymer MLD films on top of the PES porous substrates.
Metalorganic chemical vapor deposition of ZnGeN 2 films on GaN: effects of cation stoichiometry on surface morphology and crystallinity
Novel optoelectronic device designs based on the heterostructures of III-N and II-IV-N 2 are promising to advance device performance significantly. For example, by utilizing InGaN-ZnGeN 2 quantum well (QW) structures instead of pure InGaN, the band structure engineering in the QW active region can lead to improved electron-hole wavefunction overlap, and thus enhance the radiative efficiency for photon generation. These novel heterostructures have great potential to address the current challenge of low quantum efficiency in InGaN QW based light emitting diodes emitting in green and beyond. The materials development of ZnGeN 2 is still at an early stage as compared to the much matured GaN material system. In an ideal octet rule preserving ordered structure of ZnGeN 2 , every N atom is coordinated by exactly two Zn and two Ge atoms. However, local violation of octet rule can be caused by non-ideal coordination of N by the cations. The disordered structure is thermodynamically less favorable but can still be achieved, for example, in kinetics-limited growth regime. The ordered ZnGeN 2 has a bandgap very close to that of GaN (~3.4 eV) and a lattice mismatch of <0.1% with GaN. Interestingly, the valence band of ZnGeN 2 has been predicted to be ~1 eV above that of GaN, which has inspired novel designs for high efficiency light emitters. In this work, we investigated the metalorganic chemical vapor deposition (MOCVD) of ZnGeN 2 films on GaN/c-sapphire templates. Diethylzinc (DEZn), germane (GeH4) and ammonia were used as the precursors for Zn, Ge and N, respectively. A systematic study was conducted to investigate the cation stoichiometry as a function of growth temperature (TG), total reactor pressure (P) and DEZn/GeH 4 molar flow rate ratio (RII/IV). Under the investigated growth window, the Zn/(Zn+Ge) composition in the films, determined from energy dispersive X-ray spectroscopy, decreased monotonically with increase in TG but increased with increase in P and RII/IV. Atom probe tomography data did not indicate the presence of any secondary phases such as Zn 3 N 2 or Ge 3 N 4 . The surface morphology and crystallinity of the grown films had strong correlation with the Zn/(Zn+Ge) composition. The scanning electron microscopy images showed that the near-stoichiometric films have planar surfaces whereas Zn-rich films had crystallites on their surface and the Zn-poor films had faceted surface. Scanning transmission electron microscopy (STEM) imaging revealed that the Zn-rich and Zn-poor films have columnar and filament-like morphology, respectively, whereas the near-stoichiometric films have continuous film-like cross-sectional morphology. TEM nano-diffraction patterns as well as X-ray diffraction 2θ-ω scan profiles indicate that the near stoichiometric films are single crystalline. Nano-diffraction pattern of the stoichiometric films resembled that of a disordered ZnGeN 2 structure. Room temperature Raman spectra of near-stoichiometric films showed only the phonon density of states like features of a cation disordered ZnGeN 2 . Cathodoluminescence and photoluminescence spectra measured at different temperatures had similar features with peak emission wavelength at ~ 2 eV. In conclusion, the stoichiometry of ZnGeN 2 films can be widely tuned by tuning the MOCVD growth parameters. The surface morphology and the crystallinity of the films were found to have strong correlation with the Zn/(Zn+Ge) composition. The stoichiometric ZnGeN 2 films grown on GaN were demonstrated with uniform surface morphology and high crystalline quality. The results from this work will provide pathway to implement ZnGeN 2 in device structures.
Analysis and Design for Sustainable Circularity of Barrier Films Used in Sheet Molding Composites Production
Sheet molding composites (SMC) are thermoset based molding compounds with a global market size of USD 2.1 billion in 2020. SMC is usually processed with multilayer barrier/carrier films to prevent emissions from volatile organic compounds (VOC). The plastic barriers are separated from SMC after the curing process and discarded. To illustrate the high consumption volume of SMC barrier/carrier films, Kohler Co., a company which uses SMC in their bath and showering product lines, alone generates over 1M lb/year of SMC barrier/carrier film waste. Therefore, high amount of SMC barrier/carrier film plastic waste creates a great opportunity for reusing, recycling, or valorization at its end of life. This can be achieved through transition from a linear to a circular supply chain design. However, this transition will not be feasible without overcoming the technical and economic barriers. This project aims to tackle this by making the film circular. Different end of life alternatives will be evaluated experimentally. The reusability of the film will be studied through applying different mechanical and solvent cleaning techniques. The operability concerns regarding the utilization of the cleaned film for long run operations will be addressed by thermally stitching the film. Pelletizing of the cleaned film will also be investigated as a viable technique for recycling or downcycling of the film as molded products. In addition to technical barriers, designing a sustainable circular supply chain for SMC carrier film products requires uncovering the collaboration opportunities between suppliers and users at different stages of the value chain to expand its use to other products. These opportunities will be investigated by finding companies willing to buy or treat the plastic film waste. Finally, the economic viability and environmental impacts of these circular design alternatives will be evaluated through techno-economic assessment (TEA) and life cycle analysis (LCA). Techno-economic and life cycle inventory data for various pathways will also be made available as one of the main outcomes of this project. Preliminary LCA results indicate that the current SMC film supply chain (base case) emits 5.81 tonne CO2 eq. and consumes 104 GJ energy per tonne of SMC film. It is estimated that alternative circular pathways result in 14-20% less CO2 emissions and 34-44% reduction in embodied energy. This project will develop a tool to analyze the circularity and sustainability of hundreds of combinations of alternatives in different life cycle stages. Users of this tool will be able to choose the best combination among these alternatives with respect to the selected economic, environmental and circularity objectives.