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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Self-Assembled BaTiO 3 –Au x Ag 1– x Low-Loss Hybrid Plasmonic Metamaterials with an Ordered “Nano-Domino-like” Microstructure

Metallic plasmonic hybrid nanostructures have attracted enormous research interest due to the combined physical properties coming from different material components and the broad range of applications in nanophotonic and electronic devices. However, the high loss and narrow range of property tunability of the metallic hybrid materials have limited their practical applications. In this study, a metallic alloy-based self-assembled plasmonic hybrid nanostructure, i.e., a BaTiO 3 –Au x Ag 1– x (BTO) vertically aligned nanocomposite, has been integrated by a templated growth method for low-loss plasmonic systems. Comprehensive microstructural characterizations including high-resolution scanning transmission electron microscopy (HRSTEM), energy-dispersive X-ray spectroscopy (EDS), and three-dimensional (3D) electron tomography demonstrate the formation of an ordered “nano-domino-like” morphology with Au 0.4 Ag 0.6 nanopillars as cylindrical cores and BTO as square shells. By comparing with the BTO–Au hybrid thin film, the BTO–Au 0.4 Ag 0.6 alloyed film exhibits much broader plasmon resonance, hyperbolic dispersion, low-loss, and thermally robust features in the UV–vis–NIR wavelength region. This study provides a feasible platform for a complex alloyed plasmonic hybrid material design with low-loss and highly tunable optical properties toward all-optical integrated devices.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Self-Assembled, Nanostructured, Tunable Metamaterials via Spinodal Decomposition

Self-assembly via nanoscale phase separation offers an elegant route to fabricate nanocomposites with physical properties unattainable in single-component systems. One important class of nanocomposites are optical metamaterials which exhibit exotic properties and lead to opportunities for agile control of light propagation. Such metamaterials are typically fabricated via expensive and hard-to-scale top-down processes requiring precise integration of dissimilar materials. In turn, there is a need for alternative, more efficient routes to fabricate large-scale metamaterials for practical applications with deep-subwave length resolution. Here, we demonstrate a bottom-up approach to fabricate scalable nanostructured metamaterials via spinodal decomposition. To demonstrate the potential of such an approach, we leverage the innate spinodal decomposition of the VO 2 -TiO 2 system, the metal-to-insulator transition in VO 2 , and thin-film epitaxy, to produce self-organized nanostructures with coherent interfaces and a structural unit cell down to 15 nm (tunable between horizontally and vertically aligned lamellae) wherein the iso-frequency surface is temperature-tunable from elliptic to hyperbolic dispersion producing metamaterial behavior. These results provide an efficient route for the fabrication of nanostructured metamaterials and other nanocomposites for desired functionalities.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Micro glow plasma for localized nanostructural modification of carbon nanotube forest

This paper reports the localized selective treatment of vertically aligned carbon nanotubes, or CNT forests, for radial size modification of the nanotubes through a micro-scale glow plasma established on the material. An atmospheric-pressure DC glow plasma is shown to be stably sustained on the surface of the CNT forest in argon using micromachined tungsten electrodes with diameters down to 100 μm. Experiments reveal thinning or thickening of the nanotubes under the micro glow depending on the process conditions including discharge current and process time. These thinning and thickening effects in the treated nanotubes are measured to be up to ∼30% and ∼300% in their diameter, respectively, under the tested conditions. The elemental and Raman analyses suggest that the treated region of the CNT forest is pure carbon and maintains a degree of crystallinity. The local plasma treatment process investigated may allow modification of material characteristics in different domains for targeted regions or patterns, potentially aiding custom design of micro-electro-mechanical systems and other emerging devices enabled by the CNT forest.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

ZnO-Au x Cu 1-x Alloy and ZnO-Au x Al 1-x Alloy Vertically Aligned Nanocomposites for Low-Loss Plasmonic Metamaterials

Hyperbolic metamaterials are a class of materials exhibiting anisotropic dielectric function owing to the morphology of the nanostructures. In these structures, one direction behaves as a metal, and the orthogonal direction behaves as a dielectric material. Applications include subdiffraction imaging and hyperlenses. However, key limiting factors include energy losses of noble metals and challenging fabrication methods. In this work, self-assembled plasmonic metamaterials consisting of anisotropic nanoalloy pillars embedded into the ZnO matrix are developed using a seed-layer approach. Alloys of Au x Al 1-x or Au x Cu 1-x are explored due to their lower losses and higher stability. Optical and microstructural properties were explored. The ZnO-Au x Cu 1-x system demonstrated excellent epitaxial quality and optical properties compared with the ZnO-Au x Al 1-x system. Both nanocomposite systems demonstrate plasmonic resonance, hyperbolic dispersion, low losses, and epsilon-near-zero permittivity, making them promising candidates towards direct photonic integration.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Self-Assembled Ordered Three-Phase Au-BaTiO 3 -ZnO Vertically Aligned Nanocomposites Achieved by a Templating Method

Complex multiphase nanocomposite designs present enormous opportunities for developing next-generation integrated photonic and electronic devices. Here, a unique three-phase nanostructure combining a ferroelectric BaTiO 3 , a wide-bandgap semiconductor of ZnO, and a plasmonic metal of Au toward multifunctionalities is demonstrated. By a novel two-step templated growth, a highly ordered Au–BaTiO 3 –ZnO nanocomposite in a unique “nanoman”-like form, i.e., self-assembled ZnO nanopillars and Au nanopillars in a BaTiO 3 matrix, is realized, and is very different from the random three-phase ones with randomly arranged Au nanoparticles and ZnO nanopillars in the BaTiO 3 matrix. The ordered three-phase “nanoman”-like structure provides unique functionalities such as obvious hyperbolic dispersion in the visible and near-infrared regime enabled by the highly anisotropic nanostructures compared to other random structures. Such a self-assembled and ordered three-phase nanocomposite is obtained through a combination of vapor–liquid–solid (VLS) and two-phase epitaxy growth mechanisms. In this study, we open up new possibilities in the design, growth, and application of multiphase structures and provides a new approach to engineer the ordering of complex nanocomposite systems with unprecedented control over electron–light–matter interactions at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Optimization of the CVD parameters for ZnO nanorods growth: Its photoluminescence and field emission properties

Highlights: • Home-made CVD reactor fabricated and successfully used for growing ZnO nanorods. • Growth of nanostructures depends on several CVD process parameters. • CVD parameters, flow rate of carrier gas, substrate temperature, Au catalyst droplet size, growth time duration, etc. optimized. • The mechanism of crystal growth understood by studying FESEM/TEM/XRD. • Photoluminescence and Field emission studies done for defects and applications. - Abstract: Vertically aligned single crystalline ZnO nanorods arrays were grown on a silicon substrate in a CVD reactor using Au as a catalyst. The CVD parameters such as substrate temperature, catalyst layer thickness/morphology and reaction time play a crucial role in the synthesis of nanostructures by the vapor-liquid-solid process. By optimizing these various CVD parameters, highly controlled guided growth of ZnO nanorods was achieved. The structural and morphological properties of resultant ZnO nanorods were studied by means of X-ray diffraction, high-resolution transmission electron microscopy, selected area electron diffraction and field emission scanning electron microscopy. The photoluminescence spectroscopy was also done to investigate the defects in grown ZnO nanorods. The field emission results of nanorods array indicated that the properties of the field emission follow Fowler–Nordheim law. The nanorods (grown for 20 min) are vertically aligned on the substrate surface without entanglements and with good crystal quality as well which is very important for several applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

Strain Enhanced Functionality in a Bottom-Up Approach Enabled 3D Super-Nanocomposites

The ability to control nanoparticle size, concentration, and distribution in epitaxial nanocomposite films has been a formidable challenge in the synthesis of nanostructured composite materials. In this paper, a novel 3D super-nanocomposite (3D-sNC) architecture is successfully demonstrated by integrating superlattice and vertically aligned nanocomposite structures. In the 3D-sNC architecture, the feature size and distribution of the nanocylinders such as the height/lateral dimension and the vertical/lateral spacing of nanocylinders can be precisely controlled. The microstructure parameters such as nanocylinder height and spacing modulated interfacial area control the lattice strain, which further tunes the magnetotransport property. These results demonstrate that 3D-sNC is a simple and yet effective architecture to achieve controlled functionalities via the precise control of nanocylinder size, spacing, concentration, and distribution. Lastly, such a 3D-sNC structure can be used to design advanced nanostructures with desired physical properties for a variety of material systems.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Hybrid plasmonic Au–TiN vertically aligned nanocomposites: a nanoscale platform towards tunable optical sensing

Tunable plasmonic structure at the nanometer scale presents enormous opportunities for various photonic devices. In this work, we present a hybrid plasmonic thin film platform: i.e., a vertically aligned Au nanopillar array grown inside a TiN matrix with controllable Au pillar density. Compared to single phase plasmonic materials, the presented tunable hybrid nanostructures attain optical flexibility including gradual tuning and anisotropic behavior of the complex dielectric function, resonant peak shifting and change of surface plasmon resonances (SPRs) in the UV-visible range, all confirmed by numerical simulations. Lastly, the tailorable hybrid platform also demonstrates enhanced surface plasmon Raman response for Fourier-transform infrared spectroscopy (FTIR) and photoluminescence (PL) measurements, and presents great potentials as designable hybrid platforms for tunable optical-based chemical sensing applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2004

The Role of Plasma in Plasma Enhanced Chemical Vapour Deposition of Nanostructure Growth

Chemical vapour deposition (CVD) has become the preferred process for high yield growth of carbon nanotubes and nanofibres because of its ability to pattern growth through lithographic positioning of transition metal catalysts on substrates. Many potential applications of nanotubes such as field emitters [1] require not only patterned growth but also vertical alignment. Some degree of ali,ment in thermal CVD processes can be obtained when carbon nanotubes are grown closely together as a result of van der Waals interactions. The ali,onment however is marginal, and the van der Waals prerequisite makes growth of freestanding nanofibres with thermal CVD unrealizable. The application of electric fields as a means of ali,onment has been shown to overcome this limitation [2-5], and highly aligned nanostructures can be grown if electric fields on the order of 0.5 V/microns are employed. Plasma enhanced CVD in various configurations including dc, rf, microwave, inductive and electron cyclotron resonance has been pursued as a means of enabling alignment in the CVD process. However, the sheath fields for the non-dc sources are in general not sufficient for a high degree of ali,pment and an additional dc bias is usually applied to the growth substrate. This begs the question as to the actual role of the plasma. It is clear that the plasma itself is not required for aligned growth as references [3] and [4] employed fields through small applied voltages (3-20 V) across very small electrode spacings (10-100 microns) and thus avoided striking a discharge.

Hash, David B.↗
DOE OSTI2023

Electrochemically Grown Ultrathin Platinum Nanosheet Electrodes with Ultralow Loadings for Energy-Saving and Industrial-Level Hydrogen Evolution

Nanostructured catalyst-integrated electrodes with remarkably reduced catalyst loadings, high catalyst utilization and facile fabrication are urgently needed to enable cost-effective, green hydrogen production via proton exchange membrane electrolyzer cells (PEMECs). Herein, benefitting from a thin seeding layer, bottom-up grown ultrathin Pt nanosheets (Pt-NSs) were first deposited on thin Ti substrates for PEMECs via a fast, template- and surfactant-free electrochemical growth process at room temperature, showing highly uniform Pt surface coverage with ultralow loadings and vertically well-aligned nanosheet morphologies. Combined with an anode-only Nafion 117 catalyst-coated membrane (CCM), the Pt-NS electrode with an ultralow loading of 0.015 mg Pt cm -2 demonstrates superior cell performance to the commercial CCM (3.0 mg Pt cm -2 ), achieving 99.5% catalyst savings and more than 237-fold higher catalyst utilization. The remarkable performance with high catalyst utilization is mainly due to the vertically well-aligned ultrathin nanosheets with good surface coverage exposing abundant active sites for the electrochemical reaction. Overall, this study not only paves a new way for optimizing the catalyst uniformity and surface coverage with ultralow loadings but also provides new insights into nanostructured electrode design and facile fabrication for highly efficient and low-cost PEMECs and other energy storage/conversion devices.

42 ENGINEERING↗
DOE OSTI2020

Resolving Triblock Terpolymer Morphologies by Vapor-Phase Infiltration

The spontaneous formation of well-organized three-dimensional (3D) nanostructures from self-assembled block copolymers (BCPs) holds promise for nanofabrication and lithography. The addition of a third block to BCPs provides access to a plethora of 3D geometries, but it remains difficult to resolve the geometry of such “three-color” structures when there is low contrast between the polymeric components at length scales of a few nm. Here, we apply vapor-phase infiltration synthesis to a silicon-containing triblock terpolymer, poly(1,1- dimethyl silacyclobutane-b-styrene-b-lactide) (PDMSB-b-PS-b-PLA or DSL) to distinguish the 3D microdomain morphologies of the two organic blocks, PLA and PS. Selective infiltration of ZnO within the PLA microdomains reveals morphologies consisting of three-color lamellae or lamellae combined with vertically aligned core-shell cylinders, depending on the volume fractions of each block. The infiltration produces ZnO nanoparticles throughout the 260 nm thickness of the DSL film, generating 3D nanocomposites containing ZnO and SiO x . These results provide a strategy for synthesizing multicomponent 3D nanostructures as well as visualizing the phase behavior of multi-block copolymers.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Titanium Disulfide Coated Carbon Nanotube Hybrid Electrodes Enable High Energy Density Symmetric Pseudocapacitors

While electrochemical supercapacitors often show high power density and long operation lifetimes, they are plagued by limited energy density. Pseudocapacitive materials, in contrast, operate by fast surface redox reactions and are shown to enhance energy storage of supercapacitors. Furthermore, several reported systems exhibit high capacitance but restricted electrochemical voltage windows, usually no more than 1 V in aqueous electrolytes. Here, it is demonstrated that vertically aligned carbon nanotubes (VACNTs) with uniformly coated, pseudocapacitive titanium disulfide (TiS 2 ) composite electrodes can extend the stable working range to over 3 V to achieve a high capacitance of 195 F g -1 in an Li-rich electrolyte. A symmetric cell demonstrates an energy density of 60.9 Wh kg -1 —the highest among symmetric pseudocapacitors using metal oxides, conducting polymers, 2D transition metal carbides (MXene), and other transition metal dichalcogenides. Nanostructures prepared by an atomic layer deposition/sulfurization process facilitate ion transportation and surface reactions to result in a high power density of 1250 W kg -1 with stable operation over 10 000 cycles. In conclusion, a flexible solid-state supercapacitor prepared by transferring the TiS 2 –VACNT composite film onto Kapton tape is demonstrated to power a 2.2 V light emitting diode (LED) for 1 min.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Large-Scale Plasmonic Hybrid Framework with Built-In Nanohole Array as Multifunctional Optical Sensing Platforms

Light coupling with patterned subwavelength hole arrays induces enhanced transmission supported by the strong surface plasmon mode. In this work, a nanostructured plasmonic framework with vertically built-in nanohole arrays at deep-subwavelength scale (6 nm) is demonstrated using a two-step fabrication method. The nanohole arrays are formed first by the growth of a high-quality two-phase (i.e., Au–TiN) vertically aligned nanocomposite template, followed by selective wet-etching of the metal (Au). Such a plasmonic nanohole film owns high epitaxial quality with large surface coverage and the structure can be tailored as either fully etched or half-way etched nanoholes via careful control of the etching process. The chemically inert and plasmonic TiN plays a role in maintaining sharp hole boundary and preventing lattice distortion. Optical properties such as enhanced transmittance and anisotropic dielectric function in the visible regime are demonstrated. Numerical simulation suggests an extended surface plasmon mode and strong field enhancement at the hole edges. Furthermore, two demonstrations, including the enhanced and modulated photoluminescence by surface coupling with 2D perovskite nanoplates and the refractive index sensing by infiltrating immersion liquids, suggest the great potential of such plasmonic nanohole array for reusable surface plasmon-enhanced sensing applications.

42 ENGINEERING↗
DOE OSTI2017

Morphological and spectroscopic studies on the vertically aligned zinc oxide nanorods grown on low and high temperature deposited seed layer

Vertically aligned zinc oxide nanorods were grown on low and high temperature deposited aluminium doped zinc oxide seed layer by hydrothermal method and annealed to improve crystallinity. The morphology of the seed layer and the grown nanorods were studied by field emission scanning electron microscopy characterization technique. The properties of the zinc oxide nanorods were analyzed using laser spectroscopic studies. Resonant Raman spectroscopy reveals the unique increase in the A{sub 1}(LO) mode of vibration with increase in count. The luminescence property of the nanorods was studied with photoluminescence spectrometer. The vertically aligned zinc oxide nanorods show, the very high band edge emission in the ultraviolet region of the electromagnetic spectrum.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nitride-Oxide-Metal Heterostructure with Self-Assembled Core–Shell Nanopillar Arrays: Effect of Ordering on Magneto-Optical Properties

Magneto-optical (MO) coupling incorporates photon-induced change of magnetic polarization that can be adopted in ultrafast switching, optical isolators, mode convertors, and optical data storage components for advanced optical integrated circuits. However, integrating plasmonic, magnetic, and dielectric properties in one single material system poses challenges since one natural material can hardly possess all these functionalities. Here, co-deposition of a three-phase heterostructure composed of a durable conductive nitride matrix with embedded core–shell vertically aligned nanopillars, is demonstrated. Additionally, the unique coupling between ferromagnetic NiO core and atomically sharp plasmonic Au shell enables strong MO activity out-of-plane at room temperature. Further, a template growth process is applied, which significantly enhances the ordering of the nanopillar array. The ordered nanostructure offers two schemes of spin polarization which result in stronger antisymmetry of Kerr rotation. The presented complex hybrid metamaterial platform with strong magnetic and optical anisotropies is promising for tunable and modulated all-optical-based nanodevices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Vertically Aligned Single-Crystalline CoFe 2 O 4 Nanobrush Architectures with High Magnetization and Tailored Magnetic Anisotropy

Micrometer-tall vertically aligned single-crystalline CoFe 2 O 4 nanobrush architectures with extraordinarily large aspect ratio have been achieved by the precise control of a kinetic and thermodynamic non-equilibrium pulsed laser epitaxy process. Direct observations by scanning transmission electron microscopy reveal that the nanobrush crystal is mostly defect-free by nature, and epitaxially connected to the substrate through a continuous 2D interface layer. In contrast, periodic dislocations and lattice defects such as anti-phase boundaries and twin boundaries are frequently observed in the 2D interface layer, suggesting that interface misfit strain relaxation under a non-equilibrium growth condition plays a critical role in the self-assembly of such artificial architectures. Further, magnetic property measurements have found that the nanobrushes exhibit a saturation magnetization value of 6.16 μB/f.u., which is much higher than the bulk value. The discovery not only enables insights into an effective route for fabricating unconventional high-quality nanostructures, but also demonstrates a novel magnetic architecture with potential applications in nanomagnetic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Size-controlled synthesis of anatase nanobrush structures with higher crystal density

Highlights: • Application of AAO as template for TiO{sub 2} nanowires synthesis. • Non-hydrolytic sol-gel method as an implementation of TiO{sub 2} into AAO template. • Vertical anchorage of TiO2 nanowires to the polymer support. • Photocatalytic oxidation of methyl orange correlate with geometric surface area of TiO{sub 2}. - Abstract: Titanium dioxide was synthesized in multistep process applying of AAO (Anode Aluminum Oxide) as a template. The TiO{sub 2} nanowires were obtained by deposition of titanium precursors inside the pores of AAO membranes (non-hydrolytic sol-gel technique), calcined at 875 K with subsequent removal of alumina matrix by leaching it with phosphoric acid. During the AAO synthesis, it was proved that the electrical work can serve as the unified factor influencing the amount of formed AAO. The diameters of obtained titania nanowires were consequence of used AAO membranes. The higher density of titania elementary cell was observed for all synthesized nanostructures. It was confirmed by XRD and SAED measurements. The TiO{sub 2} nanowires attached vertically to polymer disc (50 mm diameter) were used in photocatalytic decomposition of methyl orange. All nanomaterials showed ten times higher photocatalytic activity than P-25. High photoactivity of obtained material is related to external area of vertically aligned titania nanowires.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Core-shell metallic alloy nanopillars-in-dielectric hybrid metamaterials with magneto-plasmonic coupling

Combining plasmonic and magnetic properties, namely magneto-plasmonic coupling, inspires great research interest and the search for magneto-plasmonic nanostructure becomes considerably critical. In this work, we designed a nanopillar-in-matrix structure with core–shell alloyed nanopillars for both BaTiO 3 (BTO)-Au 0.5 Co 0.5 (AuCo) and BTO-Au 0.25 Cu 0.25 Co 0.25 Ni 0.25 (AuCuCoNi) hybrid systems, i.e., ferromagnetic alloy cores (e.g., Co or CoNi) with plasmonic shells (e.g., Au or Au/Cu). These core–shell alloy nanopillars are uniformly embedded into a dielectric BTO matrix to form a vertically aligned nanocomposite (VAN) structure. Both hybrid systems present excellent epitaxial quality and interesting multi-functionality, e.g., high magnetic anisotropy, magneto-optical coupling response, tailorable plasmonic resonance wavelength, tunable hyperbolic properties and strong optical anisotropy. These alloyed nanopillars-in-matrix designs provide enormous potential for complex hybrid material designs with multi-functionality and demonstrate strong interface enabled magneto-plasmonic coupling along with plasmonic and magnetic performance.

36 MATERIALS SCIENCE↗