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At least 883 records · Page 49
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Understanding the Reactions Between Fe and Se Binary Diffusion Couples

Spurred by recent discoveries of high-temperature superconductivity in Fe-Se based materials, the magnetic, electronic, and catalytic properties of iron-chalcogenides have drawn significant attention. Furthermore, much remains to be understood about the sequence of phase formation in these systems. In this work, we shed light on this issue by preparing a series of binary Fe-Se ultrathin diffusion couples via designed thin film precursors and investigating their structural evolution as a function of composition and annealing temperature. Two previously unreported Fe-Se phases crystallized during the deposition process on a nominally room-temperature Si substrate in the 27-33% and 37-47% Fe (atomic percent) composition regimes. Both phases completely decompose after annealing to 200°C in a nitrogen glovebox. At higher temperatures, the sequence of phase formation is governed by Se loss in the annealing process, consistent with what would be expected from the phase diagram. Films rich in Fe (53-59% Fe) crystalized during deposition as β-FeSe (P4/nmm) with preferred c-axis orientation to the amorphous SiO 2 substrate surface, providing a means to non-epitaxial self-assembly of crystallographically aligned, iron-rich β-FeSe for future research. Our findings suggest the crystallization of binary Fe-Se compounds at room temperature via near diffusionless transformations should be a significant consideration in future attempts to prepare metastable ternary and higher order compounds containing Fe and Se.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Enantioselective Se lattices for stable chiroptoelectronic processing media

Chiroptoelectronic devices are crucial for applications in quantum computing, spin optical communications, and magnetic recording. However, the limited efficiency and low stability of conventional circularly polarized light (CPL)-sensing materials have restricted their broader use. Here, we introduce atomic chiral Se nanorod (NRs) films as broadband CPL detectors, leveraging the intrinsic chirality and stability of Se nanocrystals. We also perform incident circular polarization (ICP)-Raman optical activity (ROA) to explore the chiroptical activity of the large-area films. The Se NRs thin films detected CPL across a broad range from ultraviolet (UV) to short-wavelength infrared (SWIR), with a responsivity dissymmetry factor of up to 0.4, maintaining high stability under ambient conditions for longer than 13 months. CPL-sensitive Se NRs with intrinsic chirality have potential applications in chiral photonic synapses, chiral spin devices, and CPL-sensitive photocatalysts. ICP-ROA mapping also advances the analysis of 2D chiral materials.

Nanophotonics and plasmonics↗
DOE OSTI2020

A high-energy and long-cycling lithium–sulfur pouch cell via a macroporous catalytic cathode with double-end binding sites

Lithium-sulfur batteries are attractive alternatives to lithium-ion batteries because of their high theoretical specific energy and natural abundance of sulfur. However, the practical specific energy and cycle life of Li-S pouch cells are significantly limited by the use of thin sulfur electrodes/flooded electrolytes and polysulfides shuttle/Li metal degradation, respectively. In this work we propose a cathode design concept to achieve good Li-S pouch cell performances. The cathode is composed of uniformly embedded ZnS nanoparticles and Co-N-C single-atom catalyst to form double-end biding sites inside a highly oriented macroporous host, which can effectively immobilize and catalytically convert polysulfides intermediates during cycling, thus eliminating the shuttle effect and lithium metal corrosion. The ordered macropores enhance ionic transport under high sulfur loading by forming sufficient catalyst/conductive support/electrolyte triple-phase boundaries. This prevents the formation of inactive sulfur (dead sulfur). Our cathode structure shows improved performances in a pouch cell configuration under high sulfur loading and lean electrolyte operation. An Ah-level pouch cell with only 100% lithium excess can deliver a cell specific energy of > 300 Wh kg –1 with a Coulombic efficiency >95% for 80 cycles.

25 ENERGY STORAGE↗
DOE OSTI2020

Facile and quantitative estimation of strain in nanobubbles with arbitrary symmetry in 2D semiconductors verified using hyperspectral nano-optical imaging

When layers of van der Waals materials are deposited via exfoliation or viscoelastic stamping, nanobubbles are sometimes created from aggregated trapped fluids. Though they can be considered a nuisance, nanobubbles have attracted scientific interest in their own right owing to their ability to generate large in-plane strain gradients that lead to rich optoelectronic phenomena, especially in the semiconducting transition metal dichalcogenides. Determination of the strain within the nanobubbles, which is crucial to understanding these effects, can be approximated using elasticity theory. However, the Föppl–von Kármán equations that describe strain in a distorted thin plate are highly nonlinear and often necessitate assuming circular symmetry to achieve an analytical solution. Here, we present an easily implemented numerical method to solve for strain tensors of nanobubbles with arbitrary symmetry in 2D crystals. The method only requires topographic information from atomic force microscopy and the Poisson ratio of the 2D material. We verify that this method reproduces the strain for circularly symmetric nanobubbles that have known analytical solutions. Finally, we use the method to reproduce the Grüneisen parameter of the E' mode for 1L-WS2 nanobubbles on template-stripped Au by comparing the derived strain with measured Raman shifts from tip-enhanced Raman spectroscopy, demonstrating the utility of our method for estimating localized strain in 2D crystals.

2D materials↗
DOE OSTI2020

Mixed-flow design for microfluidic printing of two-component polymer semiconductor systems

The rational creation of two-component conjugated polymer systems with high levels of phase purity in each component is challenging but crucial for realizing printed soft-matter electronics. Here, we report a mixed-flow microfluidic printing (MFMP) approach for two-component π -polymer systems that significantly elevates phase purity in bulk-heterojunction solar cells and thin-film transistors. MFMP integrates laminar and extensional flows using a specially microstructured shear blade, designed with fluid flow simulation tools to tune the flow patterns and induce shear, stretch, and pushout effects. This optimizes polymer conformation and semiconducting blend order as assessed by atomic force microscopy (AFM), transmission electron microscopy (TEM), grazing incidence wide-angle X-ray scattering (GIWAXS), resonant soft X-ray scattering (R-SoXS), photovoltaic response, and field effect mobility. For printed all-polymer (poly[(5,6-difluoro-2-octyl-2H-benzotriazole-4,7-diyl)-2,5-thiophenediyl[4,8-bis[5-(2-hexyldecyl)-2-thienyl]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl]-2,5-thiophenediyl]) [J51]:(poly{[N,N′-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)}) [N2200]) solar cells, this approach enhances short-circuit currents and fill factors, with power conversion efficiency increasing from 5.20% for conventional blade coating to 7.80% for MFMP. Moreover, the performance of mixed polymer ambipolar [poly(3-hexylthiophene-2,5-diyl) (P3HT):N2200] and semiconducting:insulating polymer unipolar (N2200:polystyrene) transistors is similarly enhanced, underscoring versatility for two-component π -polymer systems. Mixed-flow designs offer modalities for achieving high-performance organic optoelectronics via innovative printing methodologies.

42 ENGINEERING↗
DOE OSTI2020

Local electrical degradations of solid-state electrolyte by nm-scale operando imaging of ionic and electronic transports

We report on degradation mechanisms of solid-state electrolyte (SSE) based on insights from nm-scale ionic conduction and electronic leakage for solid-state batteries. The significantly different local degradations revealed by nm-scale ionic and electronic transport imaging demonstrate the need for this nm-scale investigation. State-of-the-art lithium-ion conductive glass ceramic (Li 2 O–Al 2 O 3 –SiO 2 –P 2 O5–TiO2-GeO2) SSE shows at least two types of degradations spatially separated within the SSE, namely: (1) ionic conduction blocking and slight electronic leaking and (2) highly electronic shunting. Degradation was significantly suppressed by application of a Li-containing polyacrylonitrile thin coating on both sides of the ceramic SSE. With this coating, the ionic conduction was not reduced by the extensive cycling; instead, it improved slightly, although accompanied by a slight increase in electronic leaking. Our nm-scale transport imaging was achieved using an atomic force microscopy (AFM)-based half-cell setup and a logarithmic-scale amplifier with current sensitivity down to the fA (10-15 A) range. This half-cell setup consisting of an AFM-probe/SSE/Li structure can distinguish the ionic from the electronic current by flipping the bias-voltage polarity. This nm-scale operando imaging opens up novel characterization of ionic and electronic transport in the field of solid-state batteries.

42 ENGINEERING↗
DOE OSTI2021

Impact of n -Butylammonium Bromide on the Chemical and Electronic Structure of Double-Cation Perovskite Thin Films

2D/3D perovskite heterostructures have emerged as a promising material composition to reduce nonradiative recombination in perovskite-based LEDs and solar cells. Such heterostructures can be created by a surface treatment with large organic cations, for example, n-butylammonium bromide (BABr). To understand the impact of the BABr surface treatment on the double-cation (Cs 0.17 FA 0.83 Pb(I 0.6 Br 0.4 ) 3 ) (FA = formamidinium) perovskite thin film and further optimize the corresponding structures, an in-depth understanding of the chemical and electronic properties of the involved surfaces, interfaces, and bulk is required. We study the impact of the BABr treatment with a combination of surface-sensitive X-ray photoelectron spectroscopy and bulk-sensitive resonant inelastic soft X-ray scattering (RIXS). A quantitative analysis of the BABr-treated perovskite thin film shows a modified chemical perovskite surface environment of carbon, nitrogen, bromine, iodine, and lead, indicating that the treatment leads to a perovskite surface with a modified composition and bonding structure. With K-edge RIXS, the local environment at the nitrogen and carbon atoms is probed, allowing us to identify the presence of BABr in the perovskite bulk albeit with a modified bonding environment. This, in turn, identifies a "hidden parameter" for the optimization of the BABr treatment and overall performance of 2D/3D perovskite solar cell absorbers.

2D/3D perovskite heterostructure↗
DOE OSTI2022

Effect of Near-Interface Compensation of CdSeTe Absorber Layers on Solar Cell Performance

Arsenic has been shown to be an effective p-type dopant of CdTe. However, challenges remain in the fabrication of high efficiency CdTe solar cells using As. As-doped CdTe is prone to self-compensation and observed accumulation of dopant atoms in CdTe near the interface with MgZnO (MZO) suggests that this could be occurring. In this study, we use SCAPS 1-D modeling software to investigate the effect of near-interface compensation. We consider three cases: shallow donors, deep recombination centers, and a thin layer of excess positive charge accumulation. All of these cases are shown to have significant effects on the current-voltage characteristics, while the thin charge layer also affects capacitance-voltage measurements.

arsenic↗
DOE OSTI2023

Initial Delayed Critical Configuration of SHEBA I and Subcritical Measurements by Californium Source-Driven Noise Analysis

In September 1980, the initial delayed critical configuration of the Solution High-Energy Burst Assembly (SHEBA I) was assembled, and the US Department of Energy’s Oak Ridge National Laboratory (ORNL) staff performed near critical and subcritical measurements using the californium source-driven noise analysis (CSDNA) method at the Los Alamos National Laboratory (LANL) Critical Experiments Facility. An unreflected 56 cm outside diameter stainless-steel cylindrical tank was partially filled with uranyl fluoride solution (235U enrichment was 4.95 wt %) until delayed criticality was achieved. Then, measurements were performed for various fuel solution heights from delayed critical to 60% of the height required for delayed criticality. The stainless-steel tank had an inside diameter of 54.6 cm and a height of 105 cm and was partially (20–36.5 cm) filled with an aqueous solution of uranyl fluoride (with a density of 2.162 g/cm 3 ). The density of the uranium in solution was 1.042 g/cm 3 , and the solution had a H/U atomic ratio of 20.43. The tank had a 6.35 mm wall thickness and an axial reentrant tube with an inside diameter of 6.02 cm and wall thickness of 0.165 cm. The tank was essentially unreflected on the top and sides because it was in a thin metal shed. The reactivity of the near–delayed critical configuration was −10.4 cents, which corresponds to a k eff value of 0.99922. In addition to the CSDNA measurements, the prompt neutron decay constants were determined from break frequency noise analysis (BNFA) measurements. The subcritical neutron multiplication factors from CSDNA and BFNA compared extremely well. These data can be used as the basis of International Nuclear Criticality Safety Evaluation benchmark for the near-critical configuration, and the k eff values at various subcritical configurations can be used as subcritical benchmarks. Furthermore, the measured prompt neutron decay constants can be used as reactor physics benchmarks. This report documents the experimental information for the measurements performed so that, at a later date, researchers could perform the required uncertainty and calculational analyses and documentation to use these data for an International Criticality Safety Benchmark Evaluation Program (ICSBEP) or Nuclear Energy Agency benchmarks. The measured prompt neutron decay constants can be used as the basis of a benchmark for the International Reactor Physics Evaluation Program (IRPhEP). The data from these measurements are available from the ORNL Records Management Services Department, and the logbook is available from ICSBEP at Idaho National Laboratory.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Novel white light-emitting CdSe:Mn 2+ synthesized by photo-assisted chemical bath deposition

Nowadays, white light-emitting materials have attracted extensive research due to their potential applications in lighting devices and displaying images. Several semiconductor nanoparticles have been explored to achieve efficient white light emission. In this work, we report on novel white light-emitting CdSe:Mn 2+ thin films synthesized by photo-assisted chemical bath deposition. The effect of varying the Mn 2+ ion concentrations on the thin film structure, morphology, and optical properties was investigated. X-ray powder diffraction results indicated that all the films annealed at 250 degrees C possessed a cubic structure, with crystallite sizes in the range of 1-130 nm. Scanning electron microscopy demonstrated spherical nanoparticles with no significant changes with varying Mn 2+ doping concentrations. Energy dispersive X-ray spectroscopy confirmed the presence of the anticipated elements. The atomic force microscope revealed that the surface roughness has decreased with an increase in Mn 2+ ion concentrations but decreased for 0.7 %Mn 2+ . The UV-Vis absorption spectra showed absorption edges around 600-650 nm. Photoluminescence emission spectra excited at 3.8 eV (325 nm) showed emission bands at around 1.75 eV (709 nm), and 1.88 eV (659 nm), which were attributed to the band-to-band emission, and 4 T 1 ( 4 G)-> 6 A 1 ( 6 S) transitions of Mn 2+ ions, respectively, while emission bands at 2.35 eV (528 nm), and prominent at 3.17 eV (391 nm) were due to the glass substrate. The temperature-dependent luminescence showed a decrease in relative emission intensity with the increase in the operating temperature. The chromaticity colour coordinates showed white light-emitting thin films. These present findings open a new door to developing white light using CdSe thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Preparation of ultrathin sputtered gold films on palladium as efficient oxygen reduction electro-catalysts

Herein, we present the preparation of ultrathin gold (Au) films on different M (M = Pd, Pt, Rh, Ir, and Ru) electrodes (Au/M) using magnetron sputtering deposition for oxygen reduction reaction (ORR). The ORR electro-catalytic activities of prepared Au/M catalysts increase as follows: Au/Ru < Au/Ir < Au/Rh < Au/Pt < Au/Pd. Accordingly, the oxygen reduction catalytic behaviors of the Au-modified palladium (Au/Pd) thin films with various Au thicknesses (0.16, 0.24, 0.5, and 1 nm) are investigated in acidic environments. It is found that Au modifications can promote oxygen reduction performances due to the development of more catalytic active sites on the Pd catalyst through the existence of Au atoms. Noticeably, Au/Pd samples exhibit a connection in oxygen reduction ability as a function of Au thickness, with the ultrathin 0.16 nm Au/Pd being the most active ORR catalyst. Significantly, the 0.16 nm Au/Pd material demonstrates superior stability after 1000 potential cycles compared with the 0.16 nm Pt/Pd owing to the influence of Au coating and structurally stable surfaces. Therefore, surface modification with the deposition of Au films on Pd represents a favorable technique to boost both the ORR capability and stability of the electro-catalysts.

Magnetron sputtering↗
DOE OSTI2022

The mechanism behind the high radiation tolerance of Fe-Cr alloys

With the great demand for high radiation tolerant materials for advanced nuclear energy technologies, Fe-Cr alloys are at the forefront with long standing validated performance. Yet, the real mechanism behind their high radiation resistance is in question and understanding the effect of varying Cr percentage is a grand challenge limiting further improvements. Here we applied depth resolved atomic scale probe of defects to uncover the real mechanism on how Cr improves radiation resistance and explain the controversial impact of increasing Cr percentage. By combining depth-resolved positron annihilation lifetime spectroscopy and Doppler broadening spectroscopy we investigated the effect of Cr alloying on the formation and evolution of atomic size clusters induced by ion irradiation in Fe. We also used atom probe tomography to investigate the possible presence of Cr clusters or a’ phase with high Cr composition. The study reveals that the well-known resistance to radiation in Fe-Cr alloys arises from the stabilization of vacancy clusters around Cr atoms which act as sinks for radiation-induced defects. Thus, Cr atoms do not provide a direct sink for interstitials; rather defect complexes for that consist of Cr atoms and vacancies in turn act as sinks for irradiation-induced vacancies and interstitials. Most importantly, we find that lower amounts of Cr create smaller, uniformly distributed defect clusters that act as efficient sinks for radiation damage, but larger quantities of Cr form a defect structure that is less homogenous in size and spatial distribution, resulting in less efficient damage recombination. No evidence of phase a’ was found before or after irradiation, which indicates that it does not contribute to the observed radiation tolerance.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effect of substrate temperature on the growth of Nb$_3$Sn film on Nb by multilayer sputtering

Nb3Sn films were fabricated by multilayer sequential sputtering on Nb substrates at substrate temperatures ranging from room temperature to 250 °C. The film material properties were characterized by X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, atomic force microscopy, and transmission electron microscopy. The films’ superconducting properties were studied by four-point probe resistivity measurements from room temperature to below the superconducting critical temperature Tc. The highest Tc was17.76 K, when the multilayers were deposited at room temperature. A superconducting Nb3Sn thin film with a smoother surface morphology but a lower Tc of 17.58 K was obtained on the film deposited at a substrate temperature of 250 °C.

Sayeed, Md. Nizam↗
DOE OSTI2021

Atomic-scale visualization of topological spin textures in the chiral magnet MnGe

Peeking into magnetic textures Topological spin textures hold promise as robust carriers of information and have been observed in bulk materials with a specific crystal structure. One of these materials, manganese germanide (MnGe), exhibits unusual textures in bulk form. Repicky et al . used spin-polarized scanning tunneling microscopy to study surface magnetism in thin films of MnGe. Achieving high spatial resolution, the researchers observed stripe-like features consistent with a helical state. In regions where the film was slightly curved due to strain, the intersection of domain walls led to characteristic closed patterns that could be manipulated with current/voltage pulses. —JS

Science & Technology - Other Topics↗
DOE OSTI2021

Origin of the enhanced Nb3Sn performance by combined Hf and Ta doping

Abstract In recent years there has been an increasing effort in improving the performance of Nb 3 Sn for high-field applications, in particular for the fabrication of conductors suitable for the realization of the Future Circular Collider (FCC) at CERN. This challenging task has led to the investigation of new routes to advance the high-field pinning properties, the irreversibility and the upper critical fields ( H Irr and H c2 , respectively). The effect of hafnium addition to the standard Nb-4Ta alloy has been recently demonstrated to be particularly promising and, in this paper, we investigate the origins of the observed improvements of the superconducting properties. Electron microscopy, Extended X-ray Absorption Fine Structure Spectroscopy (EXAFS) and Atom Probe Tomography (APT) characterization clearly show that, in presence of oxygen, both fine Nb 3 Sn grains and HfO 2 nanoparticles form. Although EXAFS is unable to detect significant amounts of Hf in the A15 structure, APT does indeed reveal some residual intragrain metallic Hf. To investigate the layer properties in more detail, we created a microbridge from a thin lamella extracted by Focused Ion Beam (FIB) and measured the transport properties of Ta-Hf-doped Nb 3 Sn. H c2 (0) is enhanced to 30.8 T by the introduction of Hf, ~ 1 T higher than those of only Ta-doped Nb 3 Sn, and, even more importantly the position of the pinning force maximum exceeds 6 T, against the typical ~ 4.5–4.7 T of the only Ta-doped material. These results show that the improvements generated by Hf addition can significantly enhance the high-field performance, bringing Nb 3 Sn closer to the requirements necessary for FCC realization.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ultralow effective Gilbert damping and induced orbital moment in strain-engineered FeGe films with Curie temperature exceeding room temperature

We report the magnetic and magnetodynamic properties of strained epitaxial FeGe thin films on Ge(111) substrates, and confirm the generation of orbital moment in tensile-strained FeGe not seen in bulk or unstrained films. In-plane tensile strain resulted in an increase of the magnetic transition temperature to 350 K, likely the result of decreased Fe–Fe bond lengths that increase spin–orbit coupling strength. X-ray magnetic circular dichroism (XMCD) shows orbital-to-spin magnetic moment ratios of 0.18 and 0.14 for films of 18 nm and 72 nm thickness, respectively, indicative of partially quenched atomic orbitals. Finally, a very low effective Gilbert damping parameter, α eff = 0.003 ± 0.001 at room temperature was observed, suggesting that strained FeGe could be useful for spintronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Improved Self-Assembly of P3HT with Pyrene-Functionalized Methacrylates

A block copolymer with discotic liquid crystalline behavior was synthesized using Grignard metathesis polymerization (GRIM) and initiators for continuous activator regeneration atom transfer radical polymerization (ICAR-ATRP). A novel discotic liquid crystalline mesogen, 6-(pyren-1-yloxy)hexyl methacrylate (PyMA), comprises a block that is attached to regioregular poly(3- hexylthiophene) (rr-P 3 HT) generated by GRIM and subjected to end-group modification. Due to the continuous regeneration of Cu + in the reaction mixture in ICAR-ATRP compared to conventional methods, the synthesis was successfully performed with less catalyst. The purity and yield of the final product are increased by eliminating rigorous post-synthesis purification. Stacked pyrene units have contributed to the enhanced long-range π-π interactions and aligning of the P 3 HT block as observed in thin-film X-ray diffraction (XRD). Furthermore, field-effect mobilities in the order of 10 -2 cm 2 V -1 s -1 in bottom-gate, top-contact organic field-effect transistors (OFETs) suggest an enhancement in charge transport due to the discotic electron-rich pyrene units that help mitigate the insulating effect of the methacrylate backbone. The formation of uniform microdomains of P 3 HT-bpoly(PyMA) observed with tapping mode atomic force microscopy (TMAFM) on the channel regions of OFETs indicates the unique packing of the block copolymer in comparison to pristine P 3 HT. Thermotropic properties of the novel discotic mesogen in the presence and absence of P3HT were observed with both the poly(3-hexylthiophene)-b-poly(6-(pyren-1-yloxy)hexyl methacrylate) (P3HT-b-poly(PyMA)) block copolymer and poly(6-(pyren-1-yloxy)hexyl methacrylate) (poly(PyMA)) homopolymer using polarized optical microscopy (POM) and differential scanning calorimetry (DSC).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Intergranular corrosion of Ni-30Cr in high-temperature hydrogenated water after removing surface passivating film

Abstract High-resolution transmission electron microscopy and atom probe tomography are used to characterize the initial passivation and subsequent intergranular corrosion of degraded grain boundaries in a model Ni-30Cr alloy exposed to 360 °C hydrogenated water. Upon initial exposure for 1000 h, the alloy surface directly above the grain boundary forms a thin passivating film of Cr 2 O 3 , protecting the underlying grain boundary from intergranular corrosion. However, the metal grain boundary experiences severe Cr depletion and grain boundary migration during this initial exposure. To understand how Cr depletion affects further corrosion, the local protective film was sputtered away using a glancing angle focused ion beam. Upon further exposure, the surface fails to repassivate, and intergranular corrosion is observed through the Cr-depleted region. Through this combination of high-resolution microscopy and localized passive film removal, we show that, although high-Cr alloys are resistant to intergranular attack and stress corrosion cracking, degradation-induced changes in the underlying metal at grain boundaries make the material more susceptible once the initial passive film is breached.

(S)TEM↗