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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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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Phonon-Assisted Intervalley Scattering Determines Ultrafast Exciton Dynamics in MoSe 2 Bilayers

While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster timescale in MoSe 2 bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the K valley to other lower-energy Γ and Λ valleys in the bilayer. Our combined experimental and theoretical studies unequivocally establish different microscopic mechanisms that determine exciton quantum dynamics in TMDC monolayers and bilayers. Understanding exciton quantum dynamics provides critical guidance to the manipulation of spin-valley degrees of freedom in TMDC bilayers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

A Metal-on-Metal Growth Approach to Metal–Metal Oxide Core–Shell Nanostructures with Plasmonic Properties

Hybrid core–shell nanoparticles integrate the material properties from individual components; however, the synthesis of core–shell nanoparticles with dissimilar materials remains challenging. Herein, we applied a metal-on-metal thin film growth approach to control the conformal deposition of non-precious metal shells on the Cu-based metal cores to form core–shell structures of metal–metal oxide hybrids (M–M'O x , where M = AuCu 3 or Cu, M' = Fe, Mn, and Ni). The deposition kinetics were controlled by a temperature-regulated thermal decomposition of zerovalent transition metal complexes. It is predicted that the conformal deposition can be promoted by keeping the initial deposition temperature close to the thermal decomposition temperature of the zerovalent precursors. The mechanisms of strain reduction and interdiffusion facilitate conformal deposition over island growth in the synthesis with slow reaction kinetics. This study provides insightful guidance to metal-on-metal growth in solution at the nanoscale and thus the seed-mediated approach to hybrid core–shell structures. The optical properties of these metal–metal oxide hybrids were investigated experimentally and interpreted by theoretical simulations. Despite damping effects, the plasmonic properties of these Cu-based core-metal oxide shell structures may have the potential to enable plasmon-enhanced applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Universal chemomechanical design rules for solid-ion conductors to prevent dendrite formation in lithium metal batteries

Dendrite formation during electrodeposition while charging lithium metal batteries compromises their safety. Although high-shear-modulus ( G s ) solid-ion conductors (SICs) have been prioritized to resolve the pressure-driven instabilities that lead to dendrite propagation and cell shorting, it is unclear whether these or alternatives are needed to guide uniform lithium electrodeposition, which is intrinsically density-driven. Here, we show that SICs can be designed within a universal chemomechanical paradigm to access either pressure-driven dendrite-blocking or density-driven dendrite-suppressing properties, but not both. This dichotomy reflects the competing influence of the SIC’s mechanical properties and the partial molar volume of Li + $(V_{\mathrm{Li}^+})$ relative to those of the lithium anode ( G Li and V Li ) on plating outcomes. Within this paradigm, we explore SICs in a previously unrecognized dendrite-suppressing regime that are concomitantly ‘soft’, as is typical of polymer electrolytes, but feature an atypically low $(V_{\mathrm{Li}^+})$ that is more reminiscent of ‘hard’ ceramics. Li plating (1 mA cm -2 ; T = 20 °C) mediated by these SICs is uniform, as revealed using synchrotron hard X-ray microtomography. As a result, cell cycle life is extended, even when assembled with thin Li anodes (~30 µm) and either high-voltage NMC-622 cathodes (1.44 mAh cm -2 ) or high-capacity sulfur cathodes (3.02 mAh cm -2 ).

25 ENERGY STORAGE↗
DOE OSTI2021

Thin-film synthesis of superconductor-on-insulator A15 vanadium silicide

Abstract We present a new method for thin-film synthesis of the superconducting A15 phase of vanadium silicide with critical temperature higher than 13 K. Interdiffusion between a metallic vanadium film and the underlying silicon device layer in a silicon-on-insulator substrate, at temperatures between 650 and 750 °C, favors formation of the vanadium-rich A15 phase by limiting the supply of available silicon for the reaction. Energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction verify the stoichiometry and structure of the synthesized thin films. We measure superconducting critical currents of more than 10 6 amperes per square centimeter at low temperature in micron-scale bars fabricated from the material, and an upper critical magnetic field of 20 T, from which we deduce a superconducting coherence length of 4 nm, consistent with previously reported bulk values. The relatively high critical temperature of A15 vanadium silicide is an appealing property for use in silicon-compatible quantum devices and circuits.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Activating Layered Metal Oxide Nanomaterials via Structural Engineering as Biodegradable Nanoagents for Photothermal Cancer Therapy

Layered metal oxides including MoO 3 and WO 3 have been widely explored for biological applications owing to their excellent biocompatibility, low toxicity, and easy preparation. However, they normally exhibit weak or negligible near-infrared (NIR) absorption and thus are inefficient for photo-induced biomedical applications. Herein, the structural engineering of layered MoO 3 and WO 3 nanostructures is first reported to activate their NIR-II absorption for efficient photothermal cancer therapy in the NIR-II window. White-colored micrometre-long MoO 3 nanobelts are transformed into blue-colored short, thin, defective, interlayer gap-expanded MoO 3–x nanobelts with a strong NIR-II absorption via the simple lithium treatment. The blue MoO 3–x nanobelts exhibit a large extinction coefficient of 18.2 L g –1 cm –1 and high photothermal conversion efficiency of 46.9% at 1064 nm. After surface modification, the MoO 3–x nanobelts can be used as a robust nanoagent for photoacoustic imaging-guided photothermal therapy to achieve efficient cancer cell ablation and tumor eradication under irradiation by a 1064 nm laser. Importantly, the biodegradable MoO 3–x nanobelts can be rapidly degraded and excreted from body. We report the study highlights that the structural engineering of layered metal oxides is a powerful strategy to tune their properties and thus boost their performances in given applications.

36 MATERIALS SCIENCE↗
NASA NTRS1988

Hybrid solar cells based on dc magnetron sputtered films of n-ITO on APMOVPE grown p-InP

Hybrid indium-tin-oxide (ITO)/InP solar cells are discussed. The cells are constructed by dc magnetron sputter deposition of ITO onto high-quality InP films grown by atmospheric pressure metal-organic vapor-phase epitaxy (APMOVPE). A record efficiency of 18.9 percent, measured under standard Solar Energy Research Institute reporting conditions, has been obtained. The p-InP surface is shown to be type converted, principally by the ITO, but with the extent of conversion being modified by the nature of the sputtering gas. The deposition process, in itself, is not responsible for the type conversion. Dark currents have been suppressed by more than three orders of magnitude by the addition of hydrogen to the sputtering gas during deposition of a thin (5 nm) interface layer. Without this layer, and using only the more usual argon/oxygen mixture, the devices had poorer efficiencies and were unstable. A discussion of associated quantum efficiencies and capacitance/voltage measurements is also presented from which it is concluded that further improvements in efficiency will result from better control over the type-conversion process.

Coutts, T. J.↗
DOE OSTI2024

Boosting Thermoelectric Performance in Nanocrystalline Ternary Skutterudite Thin Films through Metallic CoTe 2 Integration

Metal–semiconductor nanocomposites have emerged as a viable strategy for concurrently tailoring both thermal and electronic transport properties of established thermoelectric materials, ultimately achieving synergistic performance. In this investigation, a series of nanocomposite thin films were synthesized, embedding metallic cobalt telluride (CoTe 2 ) nanophase within the nanocrystalline ternary skutterudite (Co(Ge 1.22 Sb 0.22 )Te 1.58 or CGST) matrix. Our approach harnessed composition fluctuation-induced phase separation and in situ growth during thermal annealing to seamlessly integrate the metallic phase. The distinctive band structures of both materials have developed an ohmic-type contact characteristic at the interface, which raised carrier density considerably yet negligibly affected the mobility counterpart, leading to a substantial improvement in electrical conductivity. The intricate balance in transport properties is further influenced by the metallic CoTe 2 phase’s role in diminishing lattice thermal conductivity. The presence of the metallic phase instigates enhanced phonon scattering at the interface boundaries. Consequently, a 2-fold enhancement in the thermoelectric figure of merit (zT ~ 1.30) is attained with CGST-7 wt. % CoTe 2 nanocomposite film at 655 K compared to that of pristine CGST.

36 MATERIALS SCIENCE↗
NASA NTRS2003

Development of Highly-Conductive Polyelectrolytes for Lithium Batteries

Future NASA and Air Force missions require reliable and safe sources of energy with high specific energy and energy density that can provide thousands of charge-discharge cycles at more than 40% depth- of-discharge and that can operate at low temperatures. All solid-state batteries have substantial advantages with respect to stability, energy density, storage fife and cyclability. Among all solid-state batteries, those with flexible polymer electrolytes offer substantial advantages in cell dimensionality and commensurability, low temperature operation and thin film design. The above considerations suggest that lithium-polymer electrolyte systems are promising for high energy density batteries and should be the systems of choice for NASA and US Air Force applications. Polyelectrolytes (single ion conductors) are among most promising avenues for achieving a major breakthrough 'in the applicability of polymer- based electrolyte systems. Their major advantages include unit transference number for the cation, reduced cell polarization, minimal salt precipitation, and favorable electrolyte stability at interfaces. Our research is focused on synthesis, modeling and cell testing of single ion carriers, polyelectrolytes. During the first year of this project we attempted the synthesis of two polyelectrolytes. The synthesis of the first one, the poly(ethyleneoxide methoxy acrylateco-lithium 1,1,2-trifluorobutanesulfonate acrylate, was attempted few times and it was unsuccessful. We followed the synthetic route described by Cowie and Spence. The yield was extremely low and the final product could not be separated from the impurities. The synthesis of this polyelectrolyte is not described in this report. The second polyelectrolyte, comb polysiloxane polyelectrolyte containing oligoether and perfluoroether sidechains, was synthesized in sufficient quantity to study the range of properties such as thermal stability, Li- ion- conductivity and stability toward lithium metal. Also, the batteries containing this polyelectrolyte were assembled and tested. The results are detailed below. The synthesis of another polyelectrolyte similar to polysiloxane polyelectrolyte has been started, however, the synthesis was not completed due to termination of the project.

Shriver, D. F.↗
DOE OSTI2023

Large-area epitaxial growth of InAs nanowires and thin films on hexagonal boron nitride by metal organic chemical vapor deposition

Large-area epitaxial growth of III–V nanowires and thin films on van der Waals substrates is key to developing flexible optoelectronic devices. In our study, large-area InAs nanowires and planar structures are grown on hexagonal boron nitride templates using metal organic chemical vapor deposition method without any catalyst or pre-treatments. The effect of basic growth parameters on nanowire yield and thin film morphology is investigated. Under optimised growth conditions, a high nanowire density of 2.1 x 10 9 cm -2 is achieved. A novel growth strategy to achieve uniform InAs thin film on h-BN/SiO 2 /Si substrate is introduced. The approach involves controlling the growth process to suppress the nucleation and growth of InAs nanowires, while promoting the radial growth of nano-islands formed on the h-BN surface. A uniform polycrystalline InAs thin film is thus obtained over a large area with a dominant zinc-blende phase. The film exhibits near-band-edge emission at room temperature and a relatively high Hall mobility of 399 cm -2 /(Vs). This work suggests a promising path for the direct growth of large-area, low-temperature III–V thin films on van der Waals substrates.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Tuning Exciton Emission via Ferroelectric Polarization at a Heterogeneous Interface between a Monolayer Transition Metal Dichalcogenide and a Perovskite Oxide Membrane

Here we demonstrate the integration of a thin BaTiO 3 (BTO) membrane with monolayer MoSe 2 in a dual gate device that enables in-situ manipulation of the BTO ferroelectric polarization with a voltage pulse. While two-dimensional (2D) transition metal dichalcogenides (TMDs) offer remarkable adaptability, their hybrid integration with other families of functional materials beyond the realm of 2D materials has been challenging. Released functional oxide membranes offer a solution for 2D/3D integration via stacking. 2D TMD excitons can serve as a local probe of the ferroelectric polarization in BTO at a heterogeneous interface. Using photoluminescence (PL) of MoSe 2 excitons to optically readout the doping level, we find that the relative population of charge carriers in MoSe 2 depends sensitively on the ferroelectric polarization. This finding points to a promising avenue for future-generations versatile sensing devices with high sensitivity, fast read-out, and diverse applicability for advanced signal processing.

42 ENGINEERING↗
DOE OSTI2023

Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO 3 thin films

Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO 3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO 3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO 6 octahedral rotations throughout LaCoO 3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO 3 films while suggesting potential applications toward low-power spintronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ion irradiation induced phase transformation in gold nanocrystalline films

Gold is a noble metal typically stable as a solid in a face-centered cubic (FCC) structure under ambient conditions; however, under particular circumstances aberrant allotropes have been synthesized. In this work, we document the phase transformation of 25 nm thick nanocrystalline (NC) free-standing gold thin-film via in situ ion irradiation studied using atomic-resolution transmission electron microscopy (TEM). Utilizing precession electron diffraction (PED) techniques, crystallographic orientation and the radiation-induced relative strains were measured and furthermore used to determine that a combination of surface and radiation-induced strains lead to an FCC to hexagonal close packed (HCP) crystallographic phase transformation upon a 10 dpa radiation dose of Au 4+ ions. Contrary to previous studies, HCP phase in nanostructures of gold was stabilized and did not transform back to FCC due to a combination of size effects and defects imparted by damage cascades.

36 MATERIALS SCIENCE↗
NASA NTRS2005

Nanostructure Engineered Chemical Sensors for Hazardous Gas and Vapor Detection

A nanosensor technology has been developed using nanostructures, such as single walled carbon nanotubes (SWNTs) and metal oxides nanowires or nanobelts, on a pair of interdigitated electrodes (IDE) processed with a silicon based microfabrication and micromachining technique. The IDE fingers were fabricated using thin film metallization techniques. Both in-situ growth of nanostructure materials and casting of the nanostructure dispersions were used to make chemical sensing devices. These sensors have been exposed to hazardous gases and vapors, such as acetone, benzene, chlorine, and ammonia in the concentration range of ppm to ppb at room temperature. The electronic molecular sensing in our sensor platform can be understood by electron modulation between the nanostructure engineered device and gas molecules. As a result of the electron modulation, the conductance of nanodevice will change. Due to the large surface area, low surface energy barrier and high thermal and mechanical stability, nanostructured chemical sensors potentially can offer higher sensitivity, lower power consumption and better robustness than the state-of-the-art systems, which make them more attractive for defense and space applications. Combined with MEMS technology, light weight and compact size sensors can be made in wafer scale with low cost.

Li, Jing↗
DOE OSTI2020

Phonon Transport Controlled by Ferromagnetic Resonance

The resonant coupling of phonons and magnons is important for the interconversion of phononic and spin degrees of freedom. We study the phonon transmission in LiNbO 3 manipulated by the dynamic magnetization in a Ni thin film. It is observed that the phonons can be absorbed strongly through resonant magnon-phonon coupling, which is realized by our modifying the magnon-phonon coupling within the Ni itself as well as our optimizing the interfacial coupling between Ni and LiNbO 3 . The line shapes of phonon transmission are further investigated considering the magnon-phonon interconversion in the elastically driven ferromagnetic resonance process. The results promote unique routes for phonon manipulation and detection in the presence of magnetization dynamics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Hybridized Exciton-Photon-Phonon States in a Transition Metal Dichalcogenide van der Waals Heterostructure Microcavity

Excitons in atomically thin transition-metal dichalcogenides (TMDs) have been established as an attractive platform to explore polaritonic physics, owing to their enormous binding energies and giant oscillator strength. Basic spectral features of exciton polaritons in TMD microcavities, thus far, were conventionally explained via two-coupled-oscillator models. This ignores, however, the impact of phonons on the polariton energy structure. Here we establish and quantify the threefold coupling between excitons, cavity photons, and phonons. For this purpose, we employ energy-momentum-resolved photoluminescence and spatially resolved coherent two-dimensional spectroscopy to investigate the spectral properties of a high-quality-factor microcavity with an embedded WSe 2 van der Waals heterostructure at room temperature. Our approach reveals a rich multibranch structure which thus far has not been captured in previous experiments. Simulation of the data reveals hybridized exciton-photon-phonon states, providing new physical insight into the exciton polariton system based on layered TMDs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Solvent-Free Coating of Organic Semiconductor Membranes with Centimetric Crystalline Domains

Organic semiconductors (OSCs) have shown great promise in a variety of applications. Although solution processing of OSCs has resulted in high-quality films, exquisite control of structural development to minimize defect formation during large-scale fabrication remains formidable. Compounding this challenge is the use of halogenated organic solvents, which poses significant health and environmental hazards. However, the solvent-free techniques introduced thus far impose additional limitations on solidification kinetics; the resulting OSC thin films are often more defective than those processed from solution. Here, a solvent-free technique is reported to prepare OSC membranes with centimetric crystalline domains. Leveraging the tendency for liquid crystalline materials to preferentially orient, OSCs are “prealigned” by depositing them from the melt over a metal frame to form a freely suspended membrane. Additionally, crystallization from this prealigned phase affords membranes with unprecedented structural order across macroscopic distances. Field-effect transistors comprising membranes of dioctyl[1]-benzothieno[3,2-b][1]benzothiophene (C8BTBT) and didodecyl[1]-benzothieno[3,2-b][1]benzothiophene (C12BTBT) having centimeter-sized domains as active layers exhibit a hole mobility of ≈8.6 cm2 V -1 s -1 , superseding the mobility of any transistors whose active layers are deposited from melt. This technique is scalable to yield membranes with large crystalline domains over wafer dimensions, making it amenable for broad applications in large-area organic electronics.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Observation of single-defect memristor in an MoS2 atomic sheet

Non-volatile resistive switching, also known as memristor effect, where an electric field switches the resistance states of a two-terminal device, has emerged as an important concept in the development of high-density information storage, computing and reconfigurable systems. The past decade has witnessed substantial advances in non-volatile resistive switching materials such as metal oxides and solid electrolytes. It was long believed that leakage currents would prevent the observation of this phenomenon for nanometre-thin insulating layers. However, the recent discovery of non-volatile resistive switching in two-dimensional monolayers of transition metal dichalcogenide and hexagonal boron nitride sandwich structures (also known as atomristors) has refuted this belief and added a new materials dimension owing to the benefits of size scaling. Here we elucidate the origin of the switching mechanism in atomic sheets using monolayer MoS 2 as a model system. Atomistic imaging and spectroscopy reveal that metal substitution into a sulfur vacancy results in a non-volatile change in the resistance, which is corroborated by computational studies of defect structures and electronic states. These findings provide an atomistic understanding of non-volatile switching and open a new direction in precision defect engineering, down to a single defect, towards achieving the smallest memristor for applications in ultra-dense memory, neuromorphic computing and radio-frequency communication systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Dislocation-induced stop-and-go kinetics of interfacial transformations

Most engineering materials are based on multiphase microstructures produced either through the control of phase equilibria or by the fabrication of different materials as in thin-film processing. In both processes, the microstructure relaxes towards equilibrium by mismatch dislocations (or geometric misfit dislocations) across the heterophase interfaces (1-5) . Despite their ubiquitous presence, directly probing the dynamic action of mismatch dislocations has been unachievable owing to their buried nature. In this work, using the interfacial transformation of copper oxide to copper as an example, we demonstrate the role of mismatch dislocations in modulating oxide-to-metal interfacial transformations in an intermittent manner, by which the lateral flow of interfacial ledges is pinned at the core of mismatch dislocations until the dislocation climbs to the new oxide/metal interface location. Together with atomistic calculations, we identify that the pinning effect is associated with the non-local transport of metal atoms to fill vacancies at the dislocation core. These results provide mechanistic insight into solid-solid interfacial transformations and have substantial implications for utilizing structural defects at buried interfaces to modulate mass transport and transformation kinetics.

25 ENERGY STORAGE↗