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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Majorana modes with side features in magnet-superconductor hybrid systems

Magnet-superconductor hybrid (MSH) systems represent promising platforms to host Majorana zero modes (MZMs), the elemental building blocks for fault-tolerant quantum computers. Theoretical description of such MSH structures is mostly based on simplified models, not accounting for the complexity of real materials. Here, based on density functional theory, we derive a superconducting 80-band model to study an MSH system consisting of a magnetic manganese chain on the s wave superconductor niobium. For a wide range of values of the superconducting order parameter, the system is a topological superconductor, with MZMs exhibiting non-universal spatial patterns and a drastic accumulation of spectral weight on both sides along the magnetic chain. These side feature states can be explained by an effective model which is guided by the ab initio results. Performing scanning tunneling spectroscopy experiments on the same system, we observe a spatial structure in the low-energy local density of states that is consistent with the theoretical findings. Our results open a first-principle approach to the discovery of topological superconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2022

A near-field study of VO2/(100)TiO2 film and its crack-induced strain relief

Temperature-induced metal–insulator transition (MIT) in vanadium dioxide (VO2) has been under intense research interest for decades both theoretically and experimentally. Due to the complex nature of electron correlations, the underlying physics behind the MIT in VO2 has yet to be fully grasped. In this work, we utilize the fine resolution of the scattering-type scanning near-field optical microscope to investigate the MIT in an epitaxial VO2 thin film on the (100)R TiO2 substrate with mid-infrared light. Bidirectional tweed-like metal–insulator phase coexistence patterns are observed and understood under the Landau free energy paradigm. More interestingly, delayed metallic nucleation is observed near the surface cracks due to local strain relief. This research proposes ideas in investigating the temperature–pressure phase diagram and tuning the interplay between local strain and MIT in oxide thin films.

Chen, Xinzhong (ORCID:0000000261033848)↗
DOE OSTI2022

Investigation of Scanning Droplet Cell Technology for Electrochemical Deposition of Custom Three-Dimensional Alloys

The goal of this project was to assess the feasibility of a new method of electroplating, which we have termed “electroprinting”, for fabricating millimeter to centimeter metal parts with full density, and eventually, with bespoke 3D internal density patterns. Alloys, gradients and varying density is beyond the scope of this work, and efforts were focused on developing the technology to be capable of printing solid parts, beyond the lines and columns previously reported in the literature. Enabling this technology would expand the design space possible for the WPD program, allowing for smooth and complex density gradients in parts rather than discrete density steps between multilayers. We successfully designed and built an electroprinting apparatus, capable of printing copper in customizable 1-D patterns, which can be printed in stacked layers to form 3D parts. We successfully characterized the flat printed patterns, however, have encountered difficulty in characterizing multilayer prints. We have partially addressed the feasibility question, by developing the method for electroprinting 3D parts, however, some questions about the internal porosity and density of these parts still remain.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Structure of V-defects in long wavelength GaN-based light emitting diodes

The V-defect is a naturally occurring inverted hexagonal pyramid structure that has been studied in GaN and InGaN growth since the 1990s. Strategic use of V-defects in pre-quantum well superlattices or equivalent preparation layers has enabled record breaking efficiencies for green, yellow, and red InGaN light emitting diodes (LEDs) utilizing lateral injection of holes through the semi-polar sidewalls of the V-defects. In this article, we use advanced characterization techniques such as scattering contrast transmission electron microscopy, high angle annular dark field scanning transmission electron microscopy, x-ray fluorescence maps, and atom probe tomography to study the active region compositions, V-defect formation, and V-defect structure in green and red LEDs grown on (0001) patterned sapphire and (111) Si substrates. We identify two distinct types of V-defects. The “large” V-defects are those that form in the pre-well superlattice and promote hole injection, usually nucleating on mixed (Burgers vector b = ±a±c⁠) character threading dislocations. In addition, “small” V-defects often form in the multi-quantum well region and are believed to be deleterious to high-efficiency LEDs by providing non-radiative pathways. The small V-defects are often associated with basal plane stacking faults or stacking fault boxes. Furthermore, we show through scattering contrast transmission electron microscopy that during V-defect filling, the threading dislocation, which runs up the center of the V-defect, will “bend” onto one of the six {10$\overline{1}$1} semi-polar planes. In conclusion, this result is essential to understanding non-radiative recombination in V-defect engineered LEDs.

42 ENGINEERING↗
DOE OSTI2020

Direct Visualization of Current-Stimulated Oxygen Migration in YBa 2 Cu 3 O 7–δ Thin Films

The past years have witnessed major advancements in all-electrical doping control on cuprates. In the vast majority of cases, the tuning of charge carrier density has been achieved via electric field effect by means of either a ferroelectric polarization or using a dielectric or electrolyte gating. Unfortunately, these approaches are constrained to rather thin superconducting layers and require large electric fields in order to ensure sizable carrier modulations. In this work, we focus on the investigation of oxygen doping in an extended region through current-stimulated oxygen migration in YBa 2 Cu 3 O 7–δ superconducting bridges. The underlying methodology is rather simple and avoids sophisticated nanofabrication process steps and complex electronics. Here, a patterned multiterminal transport bridge configuration allows us to electrically assess the directional counterflow of oxygen atoms and vacancies. Importantly, the emerging propagating front of current-dependent doping δ is probed in situ by optical microscopy and scanning electron microscopy. The resulting imaging techniques, together with photoinduced conductivity and Raman scattering investigations, reveal an inhomogeneous oxygen vacancy distribution with a controllable propagation speed permitting us to estimate the oxygen diffusivity. These findings provide direct evidence that the microscopic mechanism at play in electrical doping of cuprates involves diffusion of oxygen atoms with the applied current. The resulting fine control of the oxygen content would permit a systematic study of complex phase diagrams and the design of electrically addressable devices.

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

Ionic Liquid-Mediated Scanning Probe Electro-Oxidative Lithography as a Novel Tool for Engineering Functional Oxide Micro- and Nano-Architectures

Functional oxides have extensively been investigated as a promising class of materials in a broad range of innovative applications. Harnessing the novel properties of functional oxides in micro- to nano-scale applications hinges on establishing advanced fabrication and manufacturing techniques able to synthesize these materials in an accurate and reliable manner. Oxidative scanning probe lithography (o-SPL), an atomic force microscopy (AFM) technique based on anodic oxidation at the water meniscus formed at the tip/substrate contact, not only combines the advantages of both “top-down” and “bottom-up” fabrication approaches, but also offers the possibility of fabricating oxide nanomaterials with high patterning accuracy. While the use of self-assembled monolayers (SAMs) broadened the application of o-SPL, significant challenges have emerged owing to the relatively limited number of SAM/solid surface combinations that can be employed for o-SPL, which constrains the ability to control the chemistry and structure of oxides formed by o-SPL. Here, in this work, a new o-SPL technique that utilizes room-temperature ionic liquids (RTILs) as the functionalizing material to mediate the electrochemistry at AFM tip/substrate contacts is reported. The results show that the new IL-mediated o-SPL (IL-o-SPL) approach allows sub-100 nm oxide features to be patterned on a model solid surface, namely steel, with an initiation voltage as low as -2 V. Moreover, this approach enables high tunability of both the chemical state and morphology of the patterned iron oxide structures. Owing to the high chemical compatibility of ILs, which derives from the possibility of synthesizing ILs able to adsorb on a wide variety of solid surfaces, IL-o-SPL can be extended to other material surfaces and provide the opportunity to accurately tailor the chemistry, morphology, and electronic properties within nanoscale domains, thus opening new pathways to the development of novel micro- and nano-architectures for advanced integrated devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Seeing structural evolution of organic molecular nano-crystallites using 4D scanning confocal electron diffraction (4D-SCED)

Abstract Direct observation of organic molecular nanocrystals and their evolution using electron microscopy is extremely challenging, due to their radiation sensitivity and complex structure. Here, we introduce 4D-scanning confocal electron diffraction (4D-SCED), which enables direct in situ observation of bulk heterojunction (BHJ) thin films. 4D-SCED combines confocal electron optic setup with a pixelated detector to record focused spot-like diffraction patterns with high angular resolution, using an order of magnitude lower dose than previous methods. We apply it to study an active layer in organic solar cells, namely DRCN5T:PC 71 BM BHJ thin films. Structural details of DRCN5T nano-crystallites oriented both in- and out-of-plane are imaged at ~5 nm resolution and dose budget of ~5 e − /Å 2 . We use in situ annealing to observe the growth of the donor crystals, evolution of the crystal orientation, and progressive enrichment of PC 71 BM at interfaces. This highly dose-efficient method opens more possibilities for studying beam sensitive soft materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

End-to-End Automated Segmentation Framework for Four-Dimensional Scanning Transmission Electron Microscopy Data

Four-dimensional scanning transmission electron microscopy (4D-STEM) is powerful for rapidly characterizing arrays of nanoparticles produced via high-throughput synthesis. However, such 4D-STEM datasets typically contain thousands of nanoparticles, each characterized by thousands of diffraction patterns spatially distributed across the nanoparticle, necessitating efficient and comprehensive analysis. We propose an end-to-end segmentation framework to automatically segment each nanoparticle into regions with distinct composition/orientation of crystal grains, using only the 4D-STEM data. Bragg disk information is extracted in a physics-informed manner from the diffraction patterns at each spatial location and combined with the real space coordinates to form feature vectors. These feature vectors are then used as inputs to a Gaussian mixture model (GMM) to segment the nanoparticle into distinct regions. We also develop two visualization tools based on the GMM outputs to infer the interface transition and the degree of superposition. Our framework comprehensively integrates machine learning tools and physics knowledge, and provides a basis for substantially compressing enormous 4D-STEM datasets, e.g., by replacing the full 4D-STEM dataset for each nanoparticle with only a single set of Bragg disk features for each distinct crystal grain identified in the nanoparticle. In this article, we demonstrate the power of our framework by presenting results for real, complex datasets.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

The Tianlai dish pathfinder array: design, operation, and performance of a prototype transit radio interferometer

ABSTRACT The Tianlai Dish Pathfinder Array is a radio interferometer designed to test techniques for 21 cm intensity mapping in the post-reionization universe as a means for measuring large-scale cosmic structure. It performs drift scans of the sky at constant declination. We describe the design, calibration, noise level, and stability of this instrument based on the analysis of about 5% of 6200 h of on-sky observations through 2019 October. Beam pattern determinations using drones and the transit of bright sources are in good agreement, and compatible with electromagnetic simulations. Combining all the baselines, we make maps around bright sources and show that the array behaves as expected. A few hundred hours of observations at different declinations have been used to study the array geometry and pointing imperfections, as well as the instrument noise behaviour. We show that the system temperature is below 80 K for most feed antennas and that noise fluctuations decrease as expected with integration time, at least up to a few hundred seconds. Analysis of long integrations, from 10 nights of observations of the North Celestial Pole (NCP), yielded visibilities with amplitudes of 20–30 mK, consistent with the expected signal from the NCP radio sky with ${\lt}10\,$ mK precision for 1 MHz × 1 min binning. Hi-pass filtering the spectra to remove smooth spectrum signal yields a residual consistent with zero signal at the $0.5\,$ mK level.

(cosmology:) large-scale structure of the Universe↗
DOE OSTI2022

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

The Structure-Properties Relationship of Alternative Bismaleimide Variants for Candidacy for Additive Manufacturing

Modernizing the manufacturing of high-performance polymer foams such as amino-poly(oxadiazole) bismaleimide (APO-BMI), a bismaleimide resin with superior thermal and compressive strength that incorporates additive manufacturing (AM) techniques, is crucial for its applications, but the parameters for AM can be challenging based on the physical properties of the associated monomer. For our applications, selective laser sintering (SLS) is typically used. SLS is a 3D printing technique that allows for complex shapes and geometries without structural supports while also providing high resolution material. However, printing thermosets like APO-BMI with SLS is challenging due to the complex melting and curing considerations required when selecting parameters. Additionally, the temperature difference between melting and curing of APO-BMI is over a hundred º C, which makes selecting a sintering window especially difficult. This work explores structural modifications of APO-BMI that may be more amenable for selective laser sintering. The effects of how different structural changes such as substitution pattern, heteroatom identity in the bridge, and bridge length affect the thermal properties of the material were also compared. All APO variants were found to have a smaller temperature window between the melting and curing peaks based on differential scanning calorimetry (DSC) which is advantageous for SLS. Small structural changes significantly altered the melting and curing properties of APO. Additionally, DSC revealed significant polymorphisms in APO-BMI and other APO variants which could be attributed to differences in thermal history and would need to be considered when adapting for SLS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Visualizing discrete Fermi surfaces and possible nodal-line to Weyl state evolution in ZrSiTe

Topological nodal line semimetals (TNLSMs) represent a quantum state of topological matter. When the crystal/time-reversal symmetry is broken, a nodal line state is expected to evolve into a Dirac semimetal, a Weyl semimetal, or other topological phases according to theoretical studies. Here, we report scanning tunneling microscopy (STM) based quasiparticle interference (QPI) measurements performed on the surface of TNLSM ZrSiTe single crystal. A discrete Fermi surface with multiple electron/hole pockets and the impurity-induced inter-/intra- pockets scatterings are directly visualized from QPI patterns. Moreover, the degenerated Dirac points at X point evolve into the pairs of Weyl nodes when Fe atoms are deposited, suggesting a possible phase transition from the nodal line to the Weyl state. The calculated band structures and the Weyl points by applying Zeeman splitting energies along x-direction, further confirm the existence of Weyl points in the Fe-doped ZrSiTe induced by the broken of time-reversal symmetry.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Light–ferroelectric interaction in two-dimensional lead iodide perovskites

The unique physical properties of two-dimensional (2D) metal halide perovskites (MHPs) such as nonlinear optics, anisotropic charge transport, and ferroelectricity have made these materials promising candidates for multifunctional applications. Recently, fluorine derivatives such as 4,4-difluoropiperidinium lead iodide perovskite or (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 have shown strong ferroelectricity as compared to other 2D MHPs. Although it was previously addressed that the ferroelectricity in MHPs can be affected by illumination, the underlying physical mechanisms of light–ferroelectricity interaction in 2D MHPs are still lacking. Here, we explore the electromechanical responses in 4,4-(DFPD) 2 PbI 4 thin films using advanced scanning probe microscopy techniques revealing ferroelectric domain structures. In this work, hysteretic ferroelectric loops measured by contact-Kelvin probe force microscopy are dependent on domain structures under dark conditions, while ferroelectricity weakens under illumination. The X-ray diffraction patterns exhibit significant changes in preferential orientation of individual lattice planes under illumination. Particularly, the reduced intensity of the (1 1 1) lattice plane under illumination leads to transitioning from a ferroelectric to a paraelectric phase. The instability of positive ions, especially molecular organic cations, is observed under illumination by time-of-flight secondary ion mass spectrometry. The combination of crystallographic orientation and chemical changes under illumination clearly contributes to the origin of light–ferroelectricity interaction in 2D (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 .

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

Validation of finite element analysis strategy to investigate acoustic levitation in a two-axis acoustic levitator

A two-axis acoustic levitator can be used to generate a standing pressure wave capable of levitating solid and liquid particles at appropriate input conditions. This work proposes a simulation framework to investigate the two-axis levitation particle stability using a commercial, computational fluid dynamics software based on the harmonic solution to the acoustic wave equation. The simulation produced predictions of the standing wave that include a strong "+" shaped pattern of nodes and anti-nodes that are aligned with the levitator axes. To verify the simulation, a levitator was built and used to generate the standing wave. The field was probed with a microphone and a motorized-scanning system. After scaling the simulated pressure to the measured pressure, the magnitudes of the sound pressure level at corresponding high-pressure locations were different by no more than 5%. This is the first time a measurement of a two-axis levitator standing pressure wave has been presented and shown to verify simulations. Furthermore, as an additional verification, the authors consulted high speed camera measurements of a reference-levitator transducer, which was found to have a maximum peak-to-peak displacement of 50 +/- 5 mu m. The reference-levitator is known to levitate water at 160 dB. The system for this work was simulated to match the operation of the reference-levitator so that it produced sound pressure levels of 160 dB. This pressure was achieved when the transducer maximum peak-to-peak displacement was 50.8 mu m. The agreement between the two levitators' displacements provides good justification that the modeling approach presented here produces reliable results.

2 axis levitator↗
DOE OSTI2021

Measurement of electronic structure and surface reconstruction in the superionic Cu 2-x Te

Recently, layered copper chalcogenides Cu 2 X family (X=S, Se, Te) has attracted tremendous research interests due to their high thermoelectric performance, which is partly due to the superionic behavior of mobile Cu ions, making these compounds "phonon liquids."Here, we systematically investigate the electronic structure and its temperature evolution of the less studied single crystal Cu 2-x Te by the combination of angle resolved photoemission spectroscopy (ARPES) and scanning tunneling microscope/spectroscopy (STM/STS) experiments. While the band structure of the Cu 2-x Te shows agreement with the calculations, we clearly observe a 2×2 surface reconstruction from both our low temperature ARPES and STM/STS experiments which survives up to room temperature. Interestingly, our low temperature STM experiments further reveal multiple types of reconstruction patterns, which suggests the origin of the surface reconstruction being the distributed deficiency of liquidlike Cu ions. Our findings reveal the electronic structure and impurity level of Cu 2 Te, which provides knowledge about its thermoelectric properties from the electronic degree of freedom.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Imaging and Segmenting Grains and Subgrains Using Backscattered Electron Techniques

We present two new methods of processing data from backscattered electron signals in a scanning electron microscope to image grains and subgrains. The first combines data from multiple backscattered electron images acquired at different specimen geometries to (1) better reveal grain boundaries in recrystallized microstructures and (2) distinguish between recrystallized and unrecrystallized regions in partially recrystallized microstructures. The second utilizes spherical harmonic transform indexing of electron backscatter diffraction patterns to produce high angular resolution orientation data that enable the characterization of subgrains. Subgrains are produced during high-temperature plastic deformation and have boundary misorientation angles ranging from a few degrees down to a few hundredths of a degree. Here, we also present an algorithm to automatically segment grains from combined backscattered electron image data or grains and subgrains from high angular resolution electron backscatter diffraction data. Together, these new techniques enable rapid measurements of individual grains and subgrains from large populations.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Visualizing Overall Water Splitting on Single Microcrystals of Phosphorus-Doped BiVO 4 by Photo-SECM

Particulate bismuth vanadate (BiVO4) has attracted considerable interest as a promising photo(electro)catalyst for visible-light-driven water oxidation, however, overall water splitting (OWS) has been difficult to attain because its conduction band is too positive for efficient hydrogen evolution. Using photo-scanning electrochemical microscopy (photo-SECM) with a chemically modified nanotip, we visualized for the first time the OWS at a single truncated bipyramidal microcrystal of phosphorus-doped BiVO 4 . The tip simultaneously served as a light guide to illuminate the photocatalyst and as an electrochemical nanoprobe to observe and quantitatively measure local oxygen and hydrogen fluxes. The obtained current patterns for both O 2 and H 2 agree well with the accumulation of photogenerated holes and electrons on {010} basal and {110} lateral facets, respectively. Furthermore, the developed experimental approach is an important step towards nanoelectrochemical mapping of the activity of photocatalyst particles at the sub-facet level.

bismuth vanadate↗
DOE OSTI2025

Local p‐ and n‐Type Doping of an Oxide Semiconductor via Electric‐Field‐Driven Defect Migration

Layered oxides exhibit high ionic mobility and chemical flexibility, attracting interest as cathode materials for lithium-ion batteries and the pairing of hydrogen production and carbon capture. Recently, layered oxides emerged as highly tunable semiconductors. For example, by introducing anti-Frenkel defects, the electronic hopping conductance in hexagonal manganites is increased locally by orders of magnitude. Here, local acceptor and donor doping in Er(Mn,Ti)O3 is demonstrated, facilitated by the controlled splitting of anti-Frenkel defects under applied d.c. voltage. By combining density functional theory calculations, scanning probe microscopy, atom probe tomography, and scanning transmission electron microscopy, it is shown that the oxygen defects can readily be moved through the layered crystal structure, leading to nano-sized interstitial-rich (p-type) and vacancy-rich (n-type) regions. The resulting pattern is comparable to dipolar npn-junctions and stable on the timescale of days. These findings reveal the possibility of temporarily functionalizing oxide semiconductors at the nanoscale, giving additional opportunities for the field of oxide electronics and the development of transient electronics in general.

He, Jiali↗