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DOE OSTI2026

Analytical model for balling defects in laser melting using rivulet theory and solidification

In laser welding and additive manufacturing communities, the balling (humping) defect is primarily attributed to the Plateau–Rayleigh fluid instability (PRI) with a few authors suggesting fluid jetting and volume conservation as alternative mechanisms. As analytical descriptions of these mechanisms are unavailable, combining them into a single formalism is unfeasible. We present a new model of PRI with higher accuracy, accounting for competition with solidification, to compare the expected behavior with known experimental trends when fluid jetting is neglected. We adapt a rivulet instability model from fluid physics to account for the stabilizing effects of the substrate, which the traditional cylindrical-jet geometry does not account for and estimate the instability growth rate. Our model yields a continuous transition from non-balling to balling hitherto lacking in current literature and predicts instability growth at higher wavelengths with strong sensitivity to the solidification front curvature. While the fluid surface is most unstable for shallow melt pools, the absolute magnitude of balling relevant to printing defects scales with melt pool depth and has a maximum for a given melt pool geometry. Synchrotron-based x-ray radiography of thin samples indicates that PRI growth rates and solidification can be comparable in magnitude and thus compete, as we find in this work. We predict that deviations between model predictions and our experimental results demonstrate the importance of fluid flows and heat transport in the balling process. Our experiments further demonstrate at least one mechanism by which the melt pool length and the balling wavelength are not equivalent, as commonly claimed.

Taylor, Z. [Stanford Univ., CA (United States); SL↗

DOE OSTI2024

Scanning probe spectroscopy of sulfur vacancies and MoS 2 monolayers in side-contacted van der Waals heterostructures

We investigate the interplay between vertical tunneling and lateral transport phenomena in electrically contacted van der Waals heterostructures made from monolayer MoS 2 , hBN, and graphene. We compare data taken by low-temperature scanning tunneling spectroscopy to results from room-temperature conductive atomic force spectroscopy on monolayer MoS 2 with sulfur vacancies and with varying hBN layers. We show that for thick hBN barrier layers, where tunneling currents into the conductive substrate are suppressed, a side-contact still enables addressing the defect states in the scanning tunneling microscopy via the lateral current flow. Few-layer hBN realizes an intermediate regime in which the competition between vertical tunneling and lateral transport needs to be considered. The latter is relevant for device structures with both a thin tunneling barrier and a side-contact to the semiconducting layers.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Modularization of Ceramic Hollow Fiber Membrane Technology for Air Separation

This proposed project is aimed at studying high performance and economically competitive ceramic membrane technology for air separation and high-purity oxygen production using hollow fiber ceramic membrane stack and module technology. The design of the single permeate membrane is a hollow fiber substrate-supported thin tri-layer structure. Radially well-aligned micro-channels are embedded in the thick substrate and open at the inner surface of the substrate, enabling facile air/gas diffusion. The tri-layer structure of thin dense membrane layer (~ 10 µm) sandwiched by porous surface layer on either side is then built on the substrate using advanced fabrication process. The tri-layer structure design allows different materials to be used in different layers, where the materials of surface layers have high surface exchange coefficients while the material of dense layer has high bulk diffusivity. Such a synergetic combination leads to high permeation performance. The focus of the proposed project will be on membrane stack/module development using the developed single hollow fiber membranes, including: 1) fabrication and characterization of novel single hollow fiber membranes; 2) membrane stack design and assembly using fabricated single membranes; 3) stack modeling and analysis to guide membrane stack designs; 4) permeation performance testing and characterization of membrane stacks. The hollow fiber feature and simple sealing requirement enable very compact design of membrane stacks, which have excellent flexibility for further modularizations at different scales. The operations of such membrane stack and module may employ the exhaust heat from other components of Integrated Gasification Combined Cycle and oxy-combustion systems. Therefore, modularization of such an air separation membrane technology can be incorporated into the DOE’s REMS (radically engineered modular systems)-gasification skid and support the oxidant feed of an oxygen-blown REMS gasifier scaled to different ranges.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2020

Formation of wide-blocky calcite veins by extreme growth competition

Liassic limestones on the coast of Somerset in the UK contain dense arrays of calcite microveins with a common, but poorly understood microstructure, characterized by laterally wide crystals that form bridges across the vein. We investigated the mechanisms of formation and evolution of these ‘wide-blocky’ vein microstructures using a combination of high-resolution analytical methods, including virtual petrography, optical cathodoluminescence and scanning electron microscopy techniques (e.g. energy-dispersive X-ray spectrometry, back-scattered electron imaging, cathodoluminescence and electron back-scattered diffraction), laboratory experiments and multiphase field modelling. Our results indicate that the studied veins formed in open, fluid-filled fractures, each in a single opening and sealing episode. As shown by the optical and electron back-scattered diffraction images, the vein crystals grew epitaxially on grains of the wall rock and we hypothesize that their growth rates differed depending on whether the crystals were on a wall rock grain substrate that fractured intergranularly (slow growth rates) or transgranularly (rapid growth rates). Our multiphase field models support this hypothesis, showing that wide, blocky crystals only form where there are significant differences in the growth rate and are dependent on the type of seed grain. These results provide strong evidence for extreme growth competition, a process that we propose controls vein-filling in many micritic carbonate reservoirs, as well as demonstrate that the characteristics of the fracture wall can affect the filling processes in syntaxial veins. Supplementary material: The description and images of the studied thin sections are available at https://doi.org/10.6084/m9.figshare.c.5172371 . High-resolution optical microscopy mosaics (under plane-polarized- and crossed polarized light) of the thin section collection in PetroScan file format are available on request from the authors.

Geology↗

DOE OSTI2021

Noncollinear magnetic configurations and substrate-mediated interactions in Mn trimers on the GaN (000$\bar{1}$) surface

Collinear and noncollinear calculations based on density functional theory are carried out to elucidate the magnetic ordering of Mn trimers on a GaN ($000\bar{1}$) substrate. These trimers had previously been observed in $3a \times 3a$ surface reconstructions through Mn deposition onto the N-polar face of wurtzite GaN($000\bar{1}$). In this work, we start off by studying the effect of spin orbit coupling for the case of monomers and dimers of Mn atoms on top of a GaN surface. Based on an effective spin Hamiltonian, we estimate the magnetic anisotropy energy (MAE) for those cases and found that it is four orders of magnitude weaker than the exchange magnetic coupling between Mn adatoms. In the Mn trimer case, the magnetic ground state has the Mn spins in-plane with the GaN surface in which the relative spin orientation within each trimer is noncollinear due to the competition between the two antiferromagnetic interactions that affect each Mn spin in the trimer, which leads to the found energy minimum with 120 degree angles between the spins. By exploring the nature and fundamental mechanisms for the magnetic interaction among the Mn trimers, we find that the surface states of the substrate play a key role, involving a Ruderman-Kittel-Kasuya-Yosida (RKKY)-type interaction. We report on an electron-mediated long-distance exchange coupling between localized magnetic moments on a GaN($000\bar{1}$) surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Role of Axial Ligation in Gating the Reactivity of Dimethylplatinum(III) Diimine Radical Cations

Electrochemical methods are coupled with chemical oxidant-based analytical strategies to evaluate the oxidative reactivity of the platinum(II) diimine complex (bpy)Pt II (CH 3 ) 2 (bpy = 2,2'-bipyridine) in coordinating and non-coordinating media. Through this mechanistic analysis, we show that the one-electron oxidation of (bpy)Pt II (CH 3 ) 2 generates a highly reactive, 15-electron Pt III radical cation and identify three reaction pathways that can follow this oxidation: radical–substrate dimerization, radical-radical dimerization, and oxidative disproportionation. Axial ligation of the initially generated [(bpy)Pt III (CH 3 ) 2 ] •+ species is a critical driver of this reactivity, gating the available mechanistic pathways and tuning the competition between radical–radical dimerization and oxidative disproportionation.

14 SOLAR ENERGY↗

DOE OSTI2025

Microbes display broad diversity in cobamide preferences

ABSTRACT Cobamides, the vitamin B 12 (cobalamin) family of cofactors, are used by most organisms but produced by only a fraction of prokaryotes, and are thus considered key shared nutrients among microbes. Cobamides are structurally diverse, with multiple different cobamides found in most microbial communities. The ability to use different cobamides has been tested for several bacteria and microalgae, and nearly all show preferences for certain cobamides. This approach is limited by the commercial unavailability of cobamides other than cobalamin. Here, we have extracted and purified seven commercially unavailable cobamides to characterize bacterial cobamide preferences based on growth in specific cobamide-dependent conditions. The tested bacteria include engineered strains of Escherichia coli , Sinorhizobium meliloti , and Bacillus subtilis expressing native or heterologous cobamide-dependent enzymes, cultured under conditions that functionally isolate specific cobamide-dependent processes such as methionine synthesis. Comparison of these results to those of previous studies of diverse bacteria and microalgae revealed that a broad diversity of cobamide preferences exists not only across different organisms but also between different cobamide-dependent metabolic pathways within the same organism. The microbes differed in the cobamides that support growth most efficiently, cobamides that do not support growth, and the minimum cobamide concentrations required for growth. The latter differ by up to four orders of magnitude across organisms from different environments and by up to 20-fold between cobamide-dependent enzymes within the same organism. Given that cobamides are shared, required for use of specific growth substrates, and essential for central metabolism in certain organisms, cobamide preferences likely impact community structure and function. IMPORTANCE Nearly all bacteria are found in microbial communities with tens to thousands of other species. Molecular interactions such as metabolic cooperation and competition are key factors underlying community assembly and structure. Cobamides, the vitamin B 12 family of enzyme cofactors, are one such class of nutrients, produced by only a minority of prokaryotes but required by most microbes. A unique aspect of cobamides is their broad diversity, with nearly 20 structural forms identified in nature. Importantly, this structural diversity impacts growth as most bacteria that have been tested show preferences for specific cobamide forms. We measured cobamide-dependent growth in several model bacteria and compared the results to those of previous analyses of cobamide preference. We found that cobamide preferences vary widely across bacteria, showing the importance of characterizing these aspects of cobamide biology to understand the impact of cobamides on microbial communities.

Mok, Kenny C. (ORCID:0000000252276987)↗

DOE OSTI2026

Temperature effects on cobalt hydroxide–cobalt carbonate competitive growth on carbonate surfaces

Cobalt (Co), a critical metal essential for various environmental and industrial processes, undergoes speciation and immobilization in natural systems, primarily interacting with existing mineral surfaces. Understanding the underlying mechanisms of Co immobilization on abundant carbonate surfaces under different environmental conditions is critical for predicting Co mobility, availability, and recovery. In this study, we investigated the temperature-dependent competition between CoCO 3 and Co(OH) 2 formation on calcite (CaCO 3 ) and magnesite (MgCO 3 ) surfaces. Using X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDS), we analyzed carbonate substrates exposed to CoCl 2 solutions at varying concentrations (0–500 μM) and temperatures (22, 50, and 80 °C). Magnesite surfaces promoted CoCO 3 formation due to its low lattice mismatch with sphaerocobaltite (CoCO 3 ). However, this slow-growing CoCO 3 component was progressively outcompeted by Co(OH) 2 formation as the temperature and/or initial Co concentration increased. On calcite surfaces, the poor lattice mismatch between calcite and sphaerocobaltite led to Co(OH) 2 outcompeting CoCO 3 formation at all three temperatures. These findings provide critical insights into the roles of substrate composition, solution chemistry, and temperature in controlling Co speciation and mobility. They carry important implications for environmental transport, geochemical cycling, and industrial recovery of cobalt in carbonate-rich systems.

Calcite↗

NASA NTRS1995

Site-Competition Epitaxy for N-Type and P-Type Dopant Control in CVD Sic Epilayers

The use of site-competition epitaxy, which is based on intentional variation of the Si/C ratio during epitaxy, has now been reproduced in numerous national and international laboratories. However, previous reports have only considered dopant incorporation control for epitaxy on the Si-face 6H-SiC(OOO1) substrates. Presented in this paper is the extension of this technique for control of phosphorous incorporation and also a comparison of controlled doping on C-face 6H-SiC(OOO1) versus Si-face 6H-SiC(OOO1) substrates for aluminum, boron, nitrogen, and phosphorous.

Larkin, D. J.↗

NASA NTRS2018

Developing a Novel Platform for Characterizing Thermoelectric Materials for Uncooled Detectors for Land Imaging Applications

Thermal land imaging (imaging at ~8-14 micron optical wavelength) is an essential tool for understanding and managing terrestrial freshwater resources. Current thermal imaging instruments employ low temperature detectors, which require cryocoolers. Consequently, cost-saving reductions in size, weight, and power can be achieved by employing uncooled detectors. One uncooled detector concept, which NASA is pursuing, is a thermopile detector with sub-micron thick doped-Si thermoelectric materials. In order to characterize the thermoelectric properties of the doped silicon, we designed and optimized a novel apparatus. This simple apparatus measures the Seebeck coefficient with thermally isolated stages and LABVIEW automation. We optimized thermal stability using PID tuning and optimized the thermal contact between the thin film samples and stages using electrically conductive springs. Utilizing our apparatus, we measured the Seebeck coefficient of 0.45 micron thick phosphorus-doped single crystal Si samples bonded to alumina substrates. Using these Seebeck coefficient measurements and four-wire electrical resistivity measurements, we determined the relationship between the thermoelectric figure of merit and dopant concentration. These characterization results for doped-Si will guide our thermopile detector design to provide an optimal and competitive detector alternative for future thermal imaging instruments.

Reid, Riley A.↗

NASA NTRS1982

Preparation, characterization, physical testing and performance of fluorocarbon membranes and separators

The direct fluorination method of converting carefully selected hydrocarbon substrates to fluorinated membranes was successfully applied to produce promising, novel membranes for electrochemical devices. A family of polymer blends was identified which permits wide latitude in the concentration of both crosslinks and carboxyl groups in hydrocarbon membranes. These membranes were successfully fluorinated and are potentially competitive with commercial membranes in performance, and potentially much cheaper in price.

Lagow, R. J.↗

DOE OSTI2021

Structure-property relationships and mobility optimization in sputtered La-doped BaSn O 3 films: Toward 100cm 2 V -1 s -1

he wide band gap semiconducting perovskite BaSnO 3 is of high current interest due to outstanding room temperature mobility at high electron density, fueled by potential applications in oxide, transparent, and power electronics. Due in part to a lack of lattice-matched substrates, BaSnO 3 thin films suffer from high defect densities, however, limiting electron mobility. Additionally, the vast majority of BaSnO 3 thin film research has focused on pulsed laser deposition or molecular beam epitaxy. In this work, we present an exhaustive optimization of the mobility of Ba 0.98 La 0.02 SnO 3 films grown by a scalable, high-throughput method: high-pressure-oxygen sputter deposition. Considering target synthesis conditions, substrate selection, buffer layer structure, deposition temperature, deposition rate, thickness, and postdeposition annealing conditions, and by combining high-resolution x-ray diffraction, reciprocal space mapping, rocking curve analysis, scanning transmission electron microscopy, atomic force microscopy, and temperature-dependent electronic transport measurements, detailed understanding of synthesis-structure-property relationships is attained. Optimized room temperature mobility of 96 cm 2 V –1 s –1 is achieved in vacuum-annealed GdScO 3 (110)/BaSnO 3 (120 nm)/Ba 0.98 La 0.02 SnO 3 (200 nm) heterostructures, as well as 92 cm 2 V –1 s –1 on unbuffered substrates and 87 2 V –1 s –1 without postdeposition annealing. These results, including important trends in defect densities and a surprising dependence of mobility on lattice mismatch, substantially expand the understanding of the interplay between deposition conditions, microstructure, and transport in doped BaSnO 3 films, establishing competitive mobilities in films fabricated via a scalable, high-throughput, industry-standard technique.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Atomic‐Scale Surface Imaging of Bulk Epitaxial CsPbBr 3 Perovskite Single Crystals on Mica Using Light Assisted Scanning Tunneling Microscopy at Low‐Temperature (80 K)

Epitaxial single-crystalline CsPbBr 3 perovskite films on mica, prepared ex situ, are explored using a low-temperature scanning tunneling microscope (STM) by probing the unoccupied electronic states of their surface in ultra-high vacuum (UHV) at 80 K. Light-assisted STM measurements under a broadband illumination with visible light were employed to enhance and stabilize surface conductivity. STM imaging across the surface of macroscopic bulk CsPbBr 3 films reveals large flat terraces characterized by a specific type of surface reconstruction, consisting of parallel rows of U-shaped atomic nanostructures. These structures are spaced by 12 Å and exhibit an internal feature size of 5.1 Å. Density functional theory (DFT) calculations reproduce the experimental observations and reveal a competition between different orthorhombic CsPbBr 3 (110) surface reconstructions: a Cs-rich structure, identified as the most energetically stable, and three alternative Pb–Br-rich reconstructions, which are slightly higher in energy yet remain consistent with the STM data. Additional analyses that explicitly account for the mica substrate exclude the cubic CsPbBr 3 phase and other orthorhombic surface orientations, while showing that variations in the mica surface termination do not alter the preferred CsPbBr 3 (110) reconstruction. In conclusion, this combined approach thereby confirms our assignment and resolves previous STM interpretations of CsPbBr 3 .

36 MATERIALS SCIENCE↗

DOE OSTI2024

Diaminopurine in Nonenzymatic RNA Template Copying

In the RNA World before the emergence of an RNA polymerase, nonenzymatic template copying would have been essential for the transmission of genetic information. However, the products of chemical copying with the canonical nucleotides (A, U, C, and G) are heavily biased toward the incorporation of G and C, which form a more stable base pair than A and U. We therefore asked whether replacing adenine (A) with diaminopurine (D) might lead to more efficient and less biased nonenzymatic template copying by making a stronger version of the A:U pair. As expected, primer extension substrates containing D bound to U in the template more tightly than substrates containing A. However, primer extension with D exhibited elevated reaction rates on a C template, leading to concerns about fidelity. Our crystallographic studies revealed the nature of the D:C mismatch by showing that D can form a wobble-type base pair with C. We then asked whether competition with G would decrease the mismatched primer extension. We performed nonenzymatic primer extension with all four activated nucleotides on randomized RNA templates containing all four letters and used deep sequencing to analyze the products. We found that the DUCG genetic system exhibited a more even product distribution and a lower mismatch frequency than the canonical AUCG system. Furthermore, primer extension is greatly reduced following all mismatches, including the D:C mismatch. Our study suggests that D deserves further attention for its possible role in the RNA World and as a potentially useful component of artificial nonenzymatic RNA replication systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Manipulation of Magnetic Skyrmion in a 2D van der Waals Heterostructure via Both Electric and Magnetic Fields

As a promising candidate for the much-desired low power consumption spintronic devices, 2D magnetic van der Waals material also provides a versatile platform for the design and control of topological spin textures. In this work on WTe 2 /CrCl 3 bilayer van der Waals heterostructures, a complete Néel-type skyrmion–bimeron–ferromagnet phase transition is demonstrated, accompanied by the evolution of the topological number. This cyclic transition, mediated by a perpendicular magnetic field, is largely driven by the competition between the out-of-plane magnetocrystalline anisotropy and magnetic dipole–dipole interaction. In the presence of a driving current, the Néel-type skyrmion gains a higher velocity yet larger skyrmion Hall angle, in comparison to the bimeron. By incorporating a ferroelectric CuInP 2 S 6 monolayer as a substrate, writing and erasing of skyrmions may be regulated using a ferroelectric polarization. Here this work sheds light on a novel approach to the design and control of magnetic skyrmions on 2D van der Waals materials.

multiferroic↗

DOE OSTI2025

How transparent is graphene? A surface science perspective on remote epitaxy

Remote epitaxy is the synthesis of a single crystalline film on a graphene-covered substrate, where the film adopts epitaxial registry to the substrate as if the graphene is transparent. Despite many exciting applications for flexible electronics, strain engineering, and heterogeneous integration, an understanding of the fundamental synthesis mechanisms remains elusive. Here we offer a perspective on the synthesis mechanisms, focusing on the foundational assumption of graphene transparency. We identify challenges for quantifying the strength of the remote substrate potential that permeates through graphene, and propose Fourier and beating analysis as a bias-free method for decomposing the lattice potential contributions from the substrate, from graphene, and from surface reconstructions, each at different frequencies. We highlight the importance of graphene-induced reconstructions on epitaxial templating, drawing comparison to moiré epitaxy. We highlight the role of the remote potential in tuning surface diffusion and adatom kinetics on graphene, which are crucial for navigating the competition between remote epitaxy and defect-seeded mechanisms like pinhole epitaxy. In light of this weak remote potential, we re-evaluate the current state-of-the-art experimental evidence, highlighting why it remains challenging to experimentally validate a ‘remote’ epitaxy mechanism that cannot be explained by alternatives, such as pinhole-seeded epitaxy or serial van der Waals epitaxy. We end with one experimental example that, to out knowledge, cannot be explained by competing mechanisms: a different long-range epitaxial relationship for GdPtSb films grown on graphene/sapphire, compared to direct epitaxy on sapphire. We suggest for future experiments that directly measure the remote potential and impact of tuneable growth kinetics.

epitaxy↗

DOE OSTI2023

Microbial sensitivity to temperature and sulfate deposition modulates greenhouse gas emissions from peat soils

Abstract Peatlands are among the largest natural sources of atmospheric methane (CH 4 ) worldwide. Microbial processes play a key role in regulating CH 4 emissions from peatland ecosystems, yet the complex interplay between soil substrates and microbial communities in controlling CH 4 emissions as a function of global change remains unclear. Herein, we performed an integrated analysis of multi‐omics data sets to provide a comprehensive understanding of the molecular processes driving changes in greenhouse gas (GHG) emissions in peatland ecosystems with increasing temperature and sulfate deposition in a laboratory incubation study. We sought to first investigate how increasing temperatures (4, 21, and 35°C) impact soil microbiome–metabolome interactions; then explore the competition between methanogens and sulfate‐reducing bacteria (SRBs) with increasing sulfate concentrations at the optimum temperature for methanogenesis. Our results revealed that peat soil organic matter degradation, mediated by biotic and potentially abiotic processes, is the main driver of the increase in CO 2 production with temperature. In contrast, the decrease in CH 4 production at 35°C was linked to the absence of syntrophic communities and the potential inhibitory effect of phenols on methanogens. Elevated temperatures further induced the microbial communities to develop high growth yield and stress tolerator trait‐based strategies leading to a shift in their composition and function. On the other hand, SRBs were able to outcompete methanogens in the presence of non‐limiting sulfate concentrations at 21°C, thereby reducing CH 4 emissions. At higher sulfate concentrations, however, the prevalence of communities capable of producing sufficient low‐molecular‐weight carbon substrates for the coexistence of SRBs and methanogens was translated into elevated CH 4 emissions. The use of omics in this study enhanced our understanding of the structure and interactions among microbes with the abiotic components of the system that can be useful for mitigating GHG emissions from peatland ecosystems in the face of global change.

AminiTabrizi, Roya↗

NASA NTRS1983

Electrochemical Studies of Redox Systems for Energy Storage

Particular attention was paid to the Cr(II)/Cr(III) redox couple in aqueous solutions in the presence of Cl(-) ions. The aim of this research has been to unravel the electrode kinetics of this redox couple and the effect of Cl(1) and electrode substrate. Gold and silver were studied as electrodes and the results show distinctive differences; this is probably due to the role Cl(-) ion may play as a mediator in the reaction and the difference in state of electrical charge on these two metals (difference in the potential of zero charge, pzc). The competition of hydrogen evolution with CrCl3 reduction on these surfaces was studied by means of the rotating ring disk electrode (RRDE). The ring downstream measures the flux of chromous ions from the disk and therefore separation of both Cr(III) and H2 generation can be achieved by analyzing ring and disk currents. The conditions for the quantitative detection of Cr(2+) at the ring electrode were established. Underpotential deposition of Pb on Ag and its effect on the electrokinetics of Cr(II)/Cr(III) reaction was studied.

Wu, C. D.↗