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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Growth of Crystallographically Aligned PbSe Films of Controlled Thickness on Amorphous Substrates

Lead selenide (PbSe) has extensively been investigated due to its thermoelectric and photoconductive properties. More recently, predictions of emergent properties have focused synthetic efforts on preparing ultra-smooth layers of crystallographically aligned PbSe layers with a thickness equal to an integer number of monolayers. While rough films are typically formed through Volmer-Weber growth on heated substrates, we report the data presented herein indicates that a crystallographically aligned, ultrathin layer with a defined number of PbSe layers forms on mostly amorphous Mo-Se and V-Se coated Si substrates during nominally room temperature deposition. Since the films are uniform in thickness, the number of PbSe bilayers formed depends on the amount of Pb (or Se) deposited. If the amount of Pb deposited is close to that required for an integral number of unit cells and there is sufficient Se, Laue oscillations are present in the as-deposited samples. The Laue oscillations reflect the quality and uniformity of the crystalline PbSe domains. This study demonstrates that the substrate does not need to be crystalline to form uniform, crystallographically aligned, integer monolayer thick PbSe films. These results suggest that tuning the strength of interactions be-tween substrate and growing film is necessary to form smooth, crystallographically aligned layers. The substrate does not need to be crystalline for these interactions to be strong enough to enable growth of crystallographically aligned films.

36 MATERIALS SCIENCE↗
NASA NTRS2004

In situ Pulsed Laser Deposition of C-Axis Oriented MgB2 Films and Their Characterization

The recent discovery of an intermetallic superconductor MgB2 has renewed interest in the area of superconductivity not only because of fundamental understanding of superconductivity but also due to its potential applicability in devices such as thermal detectors. Considerable amount of research has been devoted to obtain MgB2 films by an all in situ growth technique. We have grown MgB2 thin films by an all in situ pulsed laser deposition process from pure B and Mg targets. Ultrathin layers of B and Mg were deposited in a multilayer configuration. Hundreds of such Mg-B bilayers with a capping Mg layer on the top were deposited on sapphire substrate. These depositions were done in high vacuum (approx. 10(exp -7) Torr) and at room temperature. After deposition, such a configuration was annealed at high temperature for a short time in a forming gas (4% H2 in Ar). The best films, obtained by this procedure, showed superconducting transition temperature approx. 30 K. These films have been characterized by x-ray diffraction, Rutherford Backscattering Spectrometry, AC susceptibility-, resistivity- (with and without magnetic field) and 1/f noise-measurements. The physical properties of these films will be presented and discussed.

Shinde, Sanjay↗
DOE OSTI2022

Application of ultrathin TiO 2 layers in solar energy conversion devices

Abstract A vital pursuit in solar energy research is to achieve high efficiency and long‐term stability in energy conversion devices. Coating or sandwiching an ultrathin layer of TiO 2 onto active solar components has been demonstrated to be a remarkably effective and facile strategy to improve their stability. The TiO 2 film acts as a protection layer and enhances solar energy conversion efficiency by passivating surface recombination sites or facilitating electron transport. To date, numerous efforts have been devoted to applying ultrathin TiO 2 layers in various kinds of solar energy conversion devices. In this study, we review deposition techniques, characterization methods of the resulting ultrathin TiO 2 layer, as well as its applications in dye‐sensitized solar cells, organic–inorganic hybrid solar cells, and photoelectrochemical cells.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ultrathin conformal OCVD PEDOT coatings on porous electrodes and applications thereof

The present disclosure relates to electrodes comprising a polymer film and a substrate, wherein the polymer film has a thickness of about 5 nm to about 600 nm. The present disclosure also relates to electrochemical cells and batteries comprising the electrodes disclosed herein. The present disclosure also relates to methods of making the electrodes disclosed herein.

Gleason, Karen K.↗
DOE OSTI2025

Superconductivity in an ultrathin multilayer nickelate

We report the appearance of superconductivity in single-unit-cell Nd 6 Ni 5 O 12 , exhibiting a transition temperature similar to that of thicker films. In situ synchrotron x-ray scattering performed during growth of the parent phase, Nd 6 Ni 5 O 16 , shows that the necessary layer-by-layer deposition sequence does not follow the sequence of the formula unit but an alternate order due to the relative stability of the perovskite unit cell. We exploit this insight to grow ultrathin Nd 6 Ni 5 O 16 heterostructures and conduct in situ studies of topotactic reduction, finding that formation of the square-planar phase occurs rapidly and is highly sensitive to reduction temperature, with small deviations from the optimum condition leading to inhomogeneity and the loss of superconductivity. The fluorite layer within the unit cell facilitates reduction by initially stabilizing the square-planar phase in the upper half of the unit cell. Our findings provide insight into growth of the Ruddlesden-Popper nickelates, highlighting the need for in situ studies of the metastable phases key to superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

A Study on the Synthesis and Proton Transport Behavior of Multilayered ZSM-5 Zeolite Nanosheet Membranes Laminated on Polymer Substrates

Single crystalline ZSM-5 ZNs with thicknesses around 6 nm were obtained by secondary growth of silicalite nanoparticles using diquaternary bis-1,5(tripropyl ammonium) pentamethylene diiodide (dC5) as a structure-directing agent (SDA). The dC5 could be effectively removed from the ZN pores by either high-temperature calcination or UV irradiation in air at room temperature but not by the piranha solution treatment. Ultrathin ZN-laminated membranes (ZNLMs) were fabricated by sandwiching a UV-activated multilayered ZN film between two recast Nafion® layers (ZNLM-Nafion) and by filtration coating from a suspension of thermally activated ZNs on a nonionic porous PVDF (ZNLM-PVDF). The ZNLMs on both supports demonstrated the ability of highly proton-selective ion conduction with low resistances in aqueous electrolyte solutions. The ZNLM-PVDF with PVDF binder was structurally stable, and it achieved a comparably low ASR but much higher proton selectivity compared with a Nafion membrane of same overall thickness. However, detachment between the ZNLM and Nafion layers occurred when the ZNLM-Nafion operated in aqueous electrolyte solutions. Results of this study show the potential for developing ZNLMs as efficient proton-conducting membranes without using expensive ionic polymer matrices. However, the development of polymer-supported ZNLMs is hindered by the current inefficiency in preparing well-dispersed suspensions of open-pore ZNs. Future development of efficient methods for synthesizing open-pore ZNs in dispersed states is key to realizing high-performance ZNLMs on polymers.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Dimensional Control of Octahedral Tilt in SrRuO 3 via Infinite-Layered Oxides

Manipulation of octahedral distortion at atomic scale is an effective means to tune the ground states of functional oxides. Previous work demonstrates that strain and film thickness are variable parameters to modify the octahedral parameters. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetism in SrRuO 3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO 2 (SCO) layers. The infinite-layered CuO 2 exhibits a structural transformation from “planar-type” to “chain-type” with reduced film thickness. Two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and orbital hybridization strength, leading to a significant change in the magnetoresistance and anomalous Hall resistivity. Furthermore, these findings could launch investigations into adaptive control of functionalities in quantum oxide heterostructures using oxygen coordination.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Scalable Polymeric Few-Nanometer Organosilica Membranes with Hydrothermal Stability for Selective Hydrogen Separation

Nanoporous silica membranes exhibit excellent H 2 /CO 2 separation properties for sustainable H 2 production and CO 2 capture but are prepared via complicated thermal processes above 400 °C, which prevent their scalable production at a low cost. Here, we demonstrate the rapid fabrication (within 2 min) of ultrathin silica-like membranes (~3 nm) via an oxygen plasma treatment of polydimethylsiloxane-based thin-film composite membranes at 20 °C. The resulting organosilica membranes unexpectedly exhibit H2 permeance of 280-930 GPU (1 GPU = 3.347 x 10 -10 mol m -2 s -1 Pa -1 ) and H2/CO2 selectivity of 93-32 at 200 °C, far surpassing state-of-the-art membranes and Robeson’s upper bound for H 2 /CO 2 separation. When challenged with a 3 d simulated syngas test containing water vapor at 200 °C and a 340 d stability test, the membrane shows durable separation performance and excellent hydrothermal stability. The robust H 2 /CO 2 separation properties coupled with excellent scalability demonstrate the great potential of these organosilica membranes for economic H 2 production with minimal carbon emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Enhanced Switching Reliability of Hf 0.5 Zr 0.5 O 2 Ferroelectric Films Induced by Interface Engineering

Ferroelectric materials have been widely researched for applications in memory and energy storage. Among these materials and benefiting from their excellent chemical compatibility with complementary metal–oxide–semiconductor (CMOS) devices, hafnia-based ferroelectric thin films hold great promise for highly scaled semiconductor memories, including nonvolatile ferroelectric capacitors and transistors. However, variation in the switched polarization of this material during field cycling and a limited understanding of the responsible mechanisms have impeded their implementation in technology. Here, we show that ferroelectric Hf 0.5 Zr 0.5 O 2 (HZO) capacitors that are nearly free of polarization “wake-up”─a gradual increase in switched polarization as a function of the number of switching cycles─can be achieved by introducing ultrathin HfO 2 buffer layers at the HZO/electrodes interface. High-resolution transmission electron microscopy (HRTEM) reveals crystallite sizes substantially greater than the film thickness for the buffer layer capacitors, indicating that the presence of the buffer layers influences the crystallization of the film (e.g., a lower ratio of nucleation rate to growth rate) during postdeposition annealing. This evidently promotes the formation of a polar orthorhombic (O) phase in the as-fabricated buffer layer samples. Synchrotron X-ray diffraction (XRD) reveals the conversion of the nonpolar tetragonal (T) phase to the polar orthorhombic (O) phase during electric field cycling in the control (no buffer) devices, consistent with the polarization wake-up observed for these capacitors. The extent of T–O transformation in the nonbuffer samples is directly dependent on the duration over which the field is applied. Here these results provide insight into the role of the HZO/electrodes interface in the performance of hafnia-based ferroelectrics and the mechanisms driving the polarization wake-up effect.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Interlayer Exciton Polarons in Mesoscopic V 2 O 5 for Broadband Optoelectronic Synapses

Persistent photoconductivity and optoelectronic synaptic behavior are demonstrated in solution-processed mesoscopic α-phase vanadium pentoxide (V 2 O 5 ) thin films. First-principles simulations coupled with the two-site Holstein polaron hopping model show that vacancies at the terminal oxygen position lead to long recombination times because photoexcited electrons and holes reside on different layers separated by the van der Waals gap, forming a weakly coupled interlayer exciton polaron. Mid-gap polaronic states also significantly broaden the photoresponse of the films to span across visible and infrared wavelengths. By controlling the amplitude/intensity, duration, and/or number of optical pulses, tunable optoelectronic memory functions, such as short-term and long-term plasticity, are experimentally established in V 2 O 5 -based optoelectronic synapses. Furthermore, device fabrication was extended to mechanically flexible ultrathin glass substrates. Flexible optoelectronic synapses maintained high performance after 150 bending cycles.

Phan, Thanh Luan [National Renewable Energy Labora↗
DOE OSTI2023

Ultrathin quasi-2D amorphous carbon dielectric prepared from solution precursor for nanoelectronics

Abstract Materials keeping thickness in atomic scale but extending primarily in lateral dimensions offer properties attractive for many emerging applications. However, compared to crystalline counterparts, synthesis of atomically thin films in the highly disordered amorphous form, which avoids nonuniformity and defects associated with grain boundaries, is challenging due to their metastable nature. Here we present a scalable and solution-based strategy to prepare large-area, freestanding quasi-2D amorphous carbon nanomembranes with predominant sp 2 bonding and thickness down to 1–2 atomic layers, from coal-derived carbon dots as precursors. These atomically thin amorphous carbon films are mechanically strong with modulus of 400 ± 100 GPa and demonstrate robust dielectric properties with high dielectric strength above 20 MV cm −1 and low leakage current density below 10 −4 A cm −2 through a scaled thickness of three-atomic layers. They can be implemented as solution-deposited ultrathin gate dielectrics in transistors or ion-transport media in memristors, enabling exceptional device performance and spatiotemporal uniformity.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

On the Topotactic Phase Transition Achieving Superconducting Infinite‐Layer Nickelates

Abstract Topotactic reduction is critical to a wealth of phase transitions of current interest, including synthesis of the superconducting nickelate Nd 0.8 Sr 0.2 NiO 2 , reduced from the initial Nd 0.8 Sr 0.2 NiO 3 /SrTiO 3 heterostructure. Due to the highly sensitive and often damaging nature of the topotactic reduction, however, only a handful of research groups have been able to reproduce the superconductivity results. A series of in situ synchrotron‐based investigations reveal that this is due to the necessary formation of an initial, ultrathin layer at the Nd 0.8 Sr 0.2 NiO 3 surface that helps to mediate the introduction of hydrogen into the film such that apical oxygens are first removed from the Nd 0.8 Sr 0.2 NiO 3 / SrTiO 3 (001) interface and delivered into the reducing environment. This allows the square‐planar / perovskite interface to stabilize and propagate from the bottom to the top of the film without the formation of interphase defects. Importantly, neither geometric rotations in the square planar structure nor significant incorporation of hydrogen within the films is detected, obviating its need for superconductivity. These findings unveil the structural basis underlying the transformation pathway and provide important guidance on achieving the superconducting phase in reduced nickelate systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

MOCVD Growth and Characterization of ZnSnN 2

Since the first few reports of its synthesis in 2011 and 20121-3, interest in ZnSnN 2 for diverse applications, including photovoltaics1,3,4, visible light photocatalysis5, and optoelectronics, has been growing. Novel nitride-based LED device designs promise high gains in efficiency at emission wavelengths into the green, amber and even red.6-8 Their realization requires the precise insertion of an ultrathin layer of ZnGeN 2 or ZnSnN 2 into the active region of an InGaAs-GaAs LED structure. While thin films of ZnSnN 2 have been synthesized by RF sputtering1,9 and by MBE 2,10,11, and thin films of ZnGeN 2 , ZnSiN 2 and their alloys by MOCVD, the synthesis of ZnSnN 2 thin films by MOCVD has not yet been reported. It is a challenging goal, given the narrow temperature window between efficient activation of ammonia and the thermal decomposition of ZnSnN 2 at near-atmospheric pressures. We report here the results of studies of ZnSnN 2 films grown on r- and c-plane sapphire substrates, GaN templates on sapphire, and In 0.15 Ga 0.85 N templates on GaN-on-sapphire, at temperatures from 500 °C to 560 °C, using tetramethyltin (TMSn), diethylzinc (DEZn), germane and ammonia. Chamber pressures were varied between 200 and 500 torr. In addition, the ratios of the cation precursors and the total cation-to-anion precursor ratios were varied. Single crystal growth, as evidenced by 2θ-ω x-ray diffraction scans, was achieved on all of these substrates. Wurtzitic (0002) ZnSnN 2 diffraction were observed at 2θ ~ 32.90 for the samples grown on c-sapphire, GaN (0001) and InGaN (0001) templates, and wurtzitic (11-20) peak at 2θ ~ 54.80 for the films grown on r-sapphire. Higher pressures and higher temperatures promoted better crystallinity and more continuous films, as revealed by scanning electron microscopy (SEM) images and 2θ-ω x-ray diffraction peak widths and intensities. Crystal quality was observed to be highly dependent on growth temperature. For example, in one series a 10 °C change in growth temperature resulting in a factor of 15 increase in diffraction peak intensity. SEM images show that films grown on the GaN templates had better uniformity in nucleation than those grown on sapphire. The presence of satellite peaks around the Bragg peak in the XRD 2θ-ω scan for a film grown on a GaN template, and the absence of satellite peaks for the films grown simultaneously on c- and r-sapphire, also indicate superior quality for the film grown on GaN. HAADF-STEM images of films grown on these templates showed smooth interfaces at the film-substrate boundary and show growth rates as high as 167 nm/h, considerably higher than reported previously for MBE growth.9,10 Electron diffraction patterns show single crystallinity. Rocking curves show FWHM as low as 0.100. RMS surfaces roughnesses, measured by atomic force microscopy, are of the order of 3 nm for 1µm x 1µm areas. Current work is focusing on optimizing growth on InGaN templates. These templates are promising for their relatively lower lattice mismatch with ZnSnN 2 . Their use is a next step toward producing LED device structures.

Jayatunga, Benthara Hewage Dinushi↗
DOE OSTI2020

Uncovering the Effects of Metal Contacts on Monolayer MoS 2

Metal contacts are a key limiter to the electronic performance of two-dimensional (2D) semiconductor devices. In this work, we present a comprehensive study of contact interfaces between seven metals (Y, Sc, Ag, Al, Ti, Au, Ni, with work functions from 3.1 to 5.2 eV) and monolayer MoS 2 grown by chemical vapor deposition. We evaporate thin metal films onto MoS 2 and study the interfaces by Raman spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, transmission electron microscopy, and electrical characterization. We uncover that (1) ultrathin oxidized Al dopes MoS 2 n-type (>2 × 1012 cm –2 ) without degrading its mobility, (2) Ag, Au, and Ni deposition causes varying levels of damage to MoS 2 (e.g. broadening Raman E' peak from <3 to >6 cm –1 ), and (3) Ti, Sc, and Y react with MoS 2 . Reactive metals must be avoided in contacts to monolayer MoS 2 , but control studies reveal the reaction is mostly limited to the top layer of multilayer films. Finally, we find that (4) thin metals do not significantly strain MoS 2 , as confirmed by X-ray diffraction. These are important findings for metal contacts to MoS 2 and broadly applicable to many other 2D semiconductors.

2D materials↗
DOE OSTI2026

Interference-Limited Absorption in Dense Molecular Nanolayers Near Reflecting Surfaces

We investigate linear resonant absorption by a dense ensemble of molecules confined to a sub-wavelength layer in two geometries: (i) a free-standing film in a homogeneous space and (ii) the same film placed at a controlled distance from a reflecting surface. In both cases, increasing the effective light–matter coupling (via molecular density/oscillator strength) produces a nonmonotonic response: absorption rises to an optimum and then decreases as the film becomes increasingly radiatively bright and reflective. Finite-difference time-domain simulations and analytical transfer-matrix calculations agree quantitatively and yield compact ridge conditions for the optimum. We interpret the trends using a scattering/port picture: the isolated film is a symmetric two-port system (reflection and transmission), which bounds single-sided resonant absorption to ≤50% in the ultrathin limit (reflecting transition saturation), whereas adding a mirror suppresses transmission and converts the structure into an effectively one-port absorber. In the mirror-backed geometry, interference can cancel reflection, and unity absorption is obtained at critical coupling, when radiative leakage is balanced by intrinsic molecular loss. These results clarify fundamental limits and design rules for collective absorption in dense molecular layers near dielectric or metallic boundaries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

A magnetic sensor using a 2D van der Waals ferromagnetic material

Two-dimensional (2D) van der Waals ferromagnetic materials are emerging as promising candidates for applications in ultra-compact spintronic nanodevices, nanosensors, and information storage. Our recent discovery of the strong room temperature ferromagnetism in single layers of VSe2 grown on graphite or MoS2 substrate has opened new opportunities to explore these ultrathin magnets for such applications. In this paper, we present a new type of magnetic sensor that utilizes the single layer VSe2 film as a highly sensitive magnetic core. The sensor relies in changes in resonance frequency of the LC circuit composed of a soft ferromagnetic microwire coil that contains the ferromagnetic VSe2 film subject to applied DC magnetic fields. We define sensitivity as the slope of the characteristic curve of our sensor, df0/dH, where f0 is the resonance frequency and H is the external magnetic field. The sensitivity of the sensor reaches a large value of 16×106Hz/Oe, making it a potential candidate for a wide range of magnetic sensing applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Thin film block copolymer self-assembly for nanophotonics

The nanophotonic engineering of light–matter interactions has profoundly changed research behind the design and fabrication of optical materials and devices. Metasurfaces—arrays of subwavelength nanostructures that interact resonantly with electromagnetic radiation—have emerged as an integral nanophotonic platform for a new generation of ultrathin lenses, displays, polarizers and other devices. Their success hinges on advances in lithography and nanofabrication in recent decades. While existing nanolithography techniques are suitable for basic research and prototyping, issues of cost, throughput, scalability, and substrate compatibility may preclude their use for many metasurface applications. Patterning via spontaneous self-assembly of block copolymer thin films offers an enticing alternative for nanophotonic manufacturing that is rapid, inexpensive, and applicable to large areas and diverse substrates. This review discusses the advantages and disadvantages of block copolymer-based nanopatterning and highlights recent progress in their use for broadband antireflection, surface enhanced Raman spectroscopy, and other nanophotonic applications. Here recent advances in diversification of self-assembled block copolymer nanopatterns and improved processes for enhanced scalability of self-assembled nanopatterning using block copolymers are also discussed, with a spotlight on directions for future research that would enable a wider array of nanophotonic applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Fully Inkjet‐Printed, 2D Materials‐Based Field‐Effect Transistor for Water Sensing

Abstract Despite significant progress in solution‐processing of 2D materials, it remains challenging to reliably print high‐performance semiconducting channels that can be efficiently modulated in a field‐effect transistor (FET). Herein, electrochemically exfoliated MoS 2 nanosheets are inkjet‐printed into ultrathin semiconducting channels, resulting in high on/off current ratios up to 10 3 . The reported printing strategy is reliable and general for thin film channel fabrication even in the presence of the ubiquitous coffee‐ring effect. Statistical modeling analysis on the printed pattern profiles suggests that a spaced parallel printing approach can overcome the coffee‐ring effect during inkjet printing, resulting in uniform 2D flake percolation networks. The uniformity of the printed features allows the MoS 2 channel to be hundreds of micrometers long, which easily accommodates the typical inkjet printing resolution of tens of micrometers, thereby enabling fully printed FETs. As a proof of concept, FET water sensors are demonstrated using printed MoS 2 as the FET channel, and printed graphene as the electrodes and the sensing area. After functionalization of the sensing area, the printed water sensor shows a selective response to Pb 2+ in water down to 2 ppb. This work paves the way for additive nanomanufacturing of FET‐based sensors and related devices using 2D nanomaterials.

36 MATERIALS SCIENCE↗