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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

Cloning the Dirac cones of bilayer graphene to the zone center by selenium adsorption

Dirac cones can foster extraordinary electronic effects, as exemplified by the case of graphene layers. Angle-resolved photoemission reveals that adsorption of selenium (Se) vapor on bilayer graphene creates a symmetric hybrid clone of the Dirac cones at the zone center. A detailed analysis aided by first-principles calculations shows that the adsorbed layer consists of an ordered array of Se 8 molecules. The uncovered cloning mechanism illustrates a method to generate electronic features of scientific and technological interests by gentle surface modification via van der Waals adsorption.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nitrogen-doped graphene nanomaterials for electrochemical catalysis/reactions: A review on chemical structures and stability

The electronic structure of the carbon-based nanomaterials can be modulated by doping heteroatoms into them. When nitrogen is doped into the graphene structure with different bonding configurations, it changes the material's electronic properties in a variety of ways. Because of the tuned electronic properties, nitrogen-doped graphene (N-G) is applicable in electrochemical systems as catalyst. Despite having tremendous prospects, a holistic view of the structural and functional properties of N-G is still unclear. Moreover, to our knowledge, significant findings on the properties of N-G are not well documented yet, which creates an obstacle to the further improvement of this nanomaterial. Keeping our focus on the catalytic activities, in this paper, we presented an in-detailed review of the overall chemical structure and functional properties of N-G nanomaterials. Starting from the structural properties of major precursor materials for N-G synthesis, we reviewed the physical features and its dependence on the synthesis parameters. Also, a detailed study has been conducted on the key nitrogen functional groups' structural properties, favorable formation environment, influence on the electronic structure of N-G, and role in the catalytic activity. Finally, current progress on the stability of N-G nanocatalysts is reported with an insight into the degradation mechanism.

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

Near-Threshold Photoemission from Graphene-Coated Cu(110)

In this article, the brightness of electron beams emitted from photocathode sources plays a critical role in determining the performance of x-ray free-electron lasers and ultrafast electron-diffraction applications. In order to achieve the maximum brightness, the electrons need to be emitted from a photocathode with the lowest-possible mean transverse energy (MTE). Recent investigations have shown that capping a Cu(110) photocathode with a monolayer of graphene can protect the quantum efficiency (QE) from long-term exposure to varying vacuum conditions. However, there have been no studies that investigate the effects that a monolayer of graphene has on the MTE. Here, we report on measurements of a graphene-coated Cu(110) single crystal near the photoemission threshold for room and liquid-nitrogen temperatures. At room temperature, a minimum MTE of 25 meV is measured at 295 nm. At liquid-nitrogen temperatures, a minimum MTE of 9 meV is measured at the photoemission threshold of 290 nm.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Production of warm ions in electron beam generated E × B plasma

Several recent experiments have demonstrated low-damage processing of 2D materials, such as graphene and single crystal diamond, using electron beam (e-beam) generated plasmas with applied crossed electric and magnetic (E × B) fields. Here, the low damage of these sensitive materials is commonly attributed to the low energy of ions incident to the substrate surface and the ion confinement in E x B fields. In this work, measurements of atom and ion velocity distribution functions in an e-beam E × B plasma at sub-mTorr argon pressures using a laser-induced fluorescence diagnostic revealed the presence of a warm population of ions with temperatures of ~ 1 eV that are sufficient to destroy the ion confinement in E × B fields and drive the ion flux by cross field diffusion in the direction opposite to the applied electric field, toward the plasma-bounded walls or substrate. Thus, it is this nearly ambipolar diffusion process that is responsible for the flux of charged particles impinging on the wall/substrate surface.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Observation of Electrically Tunable van Hove Singularities in Twisted Bilayer Graphene from NanoARPES

The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue toward engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. Direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines the effect of electrical doping on the electronic band structure of twisted bilayer graphene using a back-gated device architecture for angle-resolved photoemission measurements with a nano-focused light spot. A twist angle of 12.2° is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. Finally, the doping dependence of these features is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.

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

Enzymatic Laser-Induced Graphene Biosensor for Electrochemical Sensing of the Herbicide Glyphosate

Glyphosate is a globally applied herbicide yet it has been relatively undetectable in-field samples outside of gold-standard techniques. Its presumed nontoxicity toward humans has been contested by the International Agency for Research on Cancer, while it has been detected in farmers’ urine, surface waters and crop residues. Rapid, on-site detection of glyphosate is hindered by lack of field-deployable and easy-to-use sensors that circumvent sample transportation to limited laboratories that possess the equipment needed for detection. Herein, the flavoenzyme, glycine oxidase, immobilized on platinum-decorated laser-induced graphene (LIG) is used for selective detection of glyphosate as it is a substrate for GlyOx. The LIG platform provides a scaffold for enzyme attachment while maintaining the electronic and surface properties of graphene. The sensor exhibits a linear range of 10–260 µm, detection limit of 3.03 µm, and sensitivity of 0.991 nA µm -1 . The sensor shows minimal interference from the commonly used herbicides and insecticides: atrazine, 2,4-dichlorophenoxyacetic acid, dicamba, parathion-methyl, paraoxon-methyl, malathion, chlorpyrifos, thiamethoxam, clothianidin, and imidacloprid. Sensor function is further tested in complex river water and crop residue fluids, which validate this platform as a scalable, direct-write, and selective method of glyphosate detection for herbicide mapping and food analysis.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Local spectroscopy of a gate-switchable moiré quantum anomalous Hall insulator

Abstract In recent years, correlated insulating states, unconventional superconductivity, and topologically non-trivial phases have all been observed in several moiré heterostructures. However, understanding of the physical mechanisms behind these phenomena is hampered by the lack of local electronic structure data. Here, we use scanning tunnelling microscopy and spectroscopy to demonstrate how the interplay between correlation, topology, and local atomic structure determines the behaviour of electron-doped twisted monolayer–bilayer graphene. Through gate- and magnetic field-dependent measurements, we observe local spectroscopic signatures indicating a quantum anomalous Hall insulating state with a total Chern number of ±2 at a doping level of three electrons per moiré unit cell. We show that the sign of the Chern number and associated magnetism can be electrostatically switched only over a limited range of twist angle and sample hetero-strain values. This results from a competition between the orbital magnetization of filled bulk bands and chiral edge states, which is sensitive to strain-induced distortions in the moiré superlattice.

36 MATERIALS SCIENCE↗
DOE OSTI2022

The role of temperature on defect diffusion and nanoscale patterning in graphene

Graphene is of great scientific interest due to a variety of unique properties such as ballistic transport, spin selectivity, the quantum hall effect, and other quantum properties. Nanopatterning and atomic scale modifications of graphene are expected to enable further control over its intrinsic properties, providing ways to tune the electronic properties through geometric and strain effects, introduce edge states and other local or extended topological defects, and sculpt circuit paths. The focused beam of a scanning transmission electron microscope (STEM) can be used to remove atoms, enabling milling, doping, and deposition. Utilization of a STEM as an atomic scale fabrication platform is increasing; however, a detailed understanding of beam-induced processes and the subsequent cascade of aftereffects is lacking. Here, we examine the electron beam effects on atomically clean graphene at a variety of temperatures ranging from 400 to 1000 °C. We find that temperature plays a significant role in the milling rate and moderates competing processes of carbon adatom coalescence, graphene healing, and the diffusion (and recombination) of defects. The results of this work can be applied to a wider range of 2D materials and introduce better understanding of defect evolution in graphite and other bulk layered materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

An epitaxial graphene platform for zero-energy edge state nanoelectronics

Graphene’s original promise to succeed silicon faltered due to pervasive edge disorder in lithographically patterned deposited graphene and the lack of a new electronics paradigm. Here we demonstrate that the annealed edges in conventionally patterned graphene epitaxially grown on a silicon carbide substrate (epigraphene) are stabilized by the substrate and support a protected edge state. The edge state has a mean free path that is greater than 50 microns, 5000 times greater than the bulk states and involves a theoretically unexpected Majorana-like zero-energy non-degenerate quasiparticle that does not produce a Hall voltage. In seamless integrated structures, the edge state forms a zero-energy one-dimensional ballistic network with essentially dissipationless nodes at ribbon–ribbon junctions. Seamless device structures offer a variety of switching possibilities including quantum coherent devices at low temperatures. This makes epigraphene a technologically viable graphene nanoelectronics platform that has the potential to succeed silicon nanoelectronics.

42 ENGINEERING↗
DOE OSTI2026

4-Electron Oxygen Reduction Reaction (ORR) with Iron Phthalocyanine (FePc) Functionalized Nanowire Templated-3D Fuzzy Graphene (NT-3DFG)

Iron phthalocyanine (FePc) is a promising alternative to platinum-based catalysts for sustainable energy devices; however, the plane-symmetry of Fe-N 4 sites, random aggregation, and poor conductivity of FePc present major barriers for their application as oxygen reduction reaction (ORR) electrocatalysts. Here, we report the synergistic effects of FePc electrocatalysts supported by a nanowire-templated three-dimensional fuzzy graphene (FePc@NT-3DFG) substrate. The in situ functionalized oxygen groups (iFOGs) at the edge of NT-3DFG localize Fe active sites in FePc under alkaline ORR conditions. With a uniform FePc distribution through many single layers of graphene, the NT-3DFG substrates improve O 2 adsorption and catalytic activity while stabilizing the electrochemical activity during reactions. The FePc@NT-3DFG catalyst exhibits fast ORR kinetics with an extremely low Tafel slope of 28.3 ± 2.7 mV dec −1 , a higher half-wave potential of 0.911 ± 0.004 V (vs RHE), and notable long-term stability at 0.5 V (vs RHE) of 96.0 ± 0.4% retention after 30 h. Surface chemistry spectra validate electronic configuration modification of Fe at the iFOGs. Density functional theory calculations indicate that the extra layers of graphene improve oxygen adsorption. Moreover, additional exploration of other transition metal phthalocyanines supports the effects of iFOGs through the transition toward 4e − ORR. This work offers an expanded strategy for active site modification through edge-based graphene substrates for 4e − ORR.

X-ray absorption spectroscopy↗
DOE OSTI2025

Spectroscopy of the fractal Hofstadter energy spectrum

Hofstadter’s butterfly, the predicted energy spectrum for non-interacting electrons confined to a two-dimensional lattice in a magnetic field, is one of the most remarkable fractal structures in nature. At rational ratios of magnetic flux quanta per lattice unit cell, this spectrum shows self-similar distributions of energy levels that reflect its recursive construction. For most materials, Hofstadter’s butterfly is predicted under experimental conditions that are unachievable using laboratory-scale magnetic fields. More recently, electrical transport studies have provided evidence for Hofstadter’s butterfly in materials engineered to have artificially large lattice constants, such as those with moiré superlattices. Yet, so far, direct spectroscopy of the fractal energy spectrum predicted by Hofstadter nearly 50 years ago has remained out of reach. Here, in this work, we use high-resolution scanning tunnelling microscopy/spectroscopy (STM/STS) to investigate the flat electronic bands in twisted bilayer graphene (TBG) near the predicted second magic angle, an ideal setting for spectroscopic studies of Hofstadter’s spectrum. Our study shows the fractionalization of flat moiré bands into discrete Hofstadter subbands and discerns experimental signatures of self-similarity of this spectrum. Moreover, our measurements uncover a spectrum that evolves dynamically with electron density, showing phenomena beyond that of Hofstadter’s original model owing to the combined effects of strong correlations, Coulomb interactions and the quantum degeneracy of electrons in TBG.

electronic properties and materials↗
DOE OSTI2023

Production of graphene-derivatives using organic molecules for supercapacitors and beyond

Graphene is rapidly expanding for applications ranging from nanoelectronics to space exploration. A material with such enormous potential requires a variety of synthesis methods. Here, we report a library of relatively sustainable redox-active organic molecules for the reduction of graphene oxide (GO) namely N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD), 7,7,8,8-tetracyanoquinodimethane (TCNQ), ferrocene (Ferro), and decamethylferrocene (DFerro). Among them, the reduction of GO using TMPD starts even with simple hand-shaking for just a few minutes. By controlling the sonication time under ambient conditions, one can control the electronic properties of the reduced graphene oxide (rGO). The resulting free-standing films delivered a capacitance of 185 F/g when tested them as supercapacitor electrodes. We also demonstrated that TMPD can exfoliate graphite into few-layer graphene sheets with simple sonication. Here, we further show that under mild heating, these molecules can serve as dopants during the reduction process to produce nitrogen-doped graphene. Our results may guide researchers to explore sustainable organic molecules for the large-scale production of graphene-based materials for diverse applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Effects of lithium intercalation in twisted bilayer graphene

In this work, we investigate the effects of lithium intercalation in twisted bilayers of graphene, using first-principles electronic structure calculations. To model this system we employ commensurate supercells that correspond to twist angles of 7.34° and 2.45°. From the energetics of lithium absorption we demonstrate that for low Li concentration the intercalants cluster in the AA regions with double the density of a uniform distribution. The charge donated by the Li atoms to the graphene layers results in modifications to the band structure that can be qualitatively captured using a continuum model with modified interlayer couplings in a region of parameter space that has yet to be explored either experimentally or theoretically. Thus, the combination of intercalation and twisted layers simultaneously provides the means for spatial control over material properties and an additional knob with which to tune moiré physics in twisted bilayers of graphene, with potential applications ranging from energy storage and conversion to quantum information.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Carbon-Based Quantum Information Science with Symmetry Protected Topological States (Final Report, DOE-BES award DE-SC0023105)

This research program established the scientific foundation for the rational, bottom-up design, synthesis, isolation, and investigation of symmetry-protected topological (SPT) electron spin qubits embedded in graphene nanoribbons (GNRs). The work focused on integrating atomically precise low-dimensional carbon nanostructures with emerging quantum logic architectures, providing a pathway toward scalable quantum materials for next-generation computing and sensing technologies. A central component of the program was the elucidation of fundamental relationships between real-space molecular architecture, local spin density distributions, electronic band dispersion, and energy level alignment in atomically precise GNR systems. These correlations define key operational parameters of SPT qubits and were systematically investigated to establish quantitative benchmarks against established molecular and solid-state spin qubit platforms. Attention was given to properties critical for quantum device performance, e.g. decoherence times, spectral sharpness of energy transitions, and tunable exchange interactions between spin states. The research demonstrated that these parameters can be engineered with atomic precision through scalable bottom-up synthetic strategies. Theory-guided design played a central role in identifying candidate structures hosting topologically protected spin states. Experimental validation was performed using both ensemble measurements and single-molecule characterization. In addition to advances in quantum materials synthesis, the program developed and applied spin-sensitive scanning probe microscopy techniques capable of directly probing quantum states and dynamic processes with atomic-scale spatial resolution. These capabilities enabled direct observation and characterization of quantum structures at the single-atom level. While the research activities were primarily hypothesis-driven fundamental investigations, the program adopted a comprehensive materials-by-design framework aimed at translating scientific discoveries into technological concepts compatible with scalable and intelligent manufacturing approaches.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Andreev Reflection and Klein Tunneling in High-Temperature Superconductor-Graphene Junctions

Scattering processes in quantum materials emerge as resonances in electronic transport, including confined modes, Andreev states, and Yu-Shiba-Rusinov states. However, in most instances, these resonances are driven by a single scattering mechanism. Here, in this paper, we show the appearance of resonances due to the combination of two simultaneous scattering mechanisms, one from superconductivity and the other from graphene p-n junctions. These resonances stem from Andreev reflection and Klein tunneling that occur at two different interfaces of a hole-doped region of graphene formed at the boundary with superconducting graphene due to proximity effects from Bi 2 Sr 2 Ca 1 Cu 2 O 8+δ . The resonances persist with gating from p + -p and p-n configurations. The suppression of the oscillation amplitude above the bias energy which is comparable to the induced superconducting gap indicates the contribution from Andreev reflection. Our experimental measurements are supported by quantum transport calculations in such interfaces, leading to analogous resonances. Our results put forward a hybrid scattering mechanism in graphene–high-temperature superconductor heterojunctions of potential impact for graphene-based Josephson junctions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

High Layer Uniformity of Two-Dimensional Materials Demonstrated Surprisingly from Broad Features in Surface Electron Diffraction

Paradoxically, a very broad diffraction background, named the bell-shaped-component (BSC), has been established as a feature of graphene growth. Recent diffraction studies as a function of electron energy have shown that the BSC is not related to scattering interference. Here, additional experiments are carried out as a function of temperature over the range in which single-layer graphene (SLG) grows. Quantitative fitting of the profiles shows that the BSC follows the increase of the Gr(10) spot, proving directly that the BSC indicates high-quality graphene. Additional metal deposition experiments provide more information about the BSC. The BSC is insensitive to metal deposition, and it increases with metal intercalation, because a more uniform interface forms between graphene and SiC. These experiments support the conclusion that the BSC originates from electron confinement within SLG, and surprisingly, it is an excellent measure of graphene uniformity.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Atomistic-Scale Simulations on Graphene Bending Near a Copper Surface

Molecular insights into graphene-catalyst surface interactions can provide useful information for the efficient design of copper current collectors with graphitic anode interfaces. As graphene bending can affect the local electron density, it should reflect its local reactivity as well. Using ReaxFF reactive molecular simulations, we have investigated the possible bending of graphene in vacuum and near copper surfaces. We describe the energy cost for graphene bending and the binding energy with hydrogen and copper with two different ReaxFF parameter sets, demonstrating the relevance of using the more recently developed ReaxFF parameter sets for graphene properties. Moreover, the draping angle at copper step edges obtained from our atomistic simulations is in good agreement with the draping angle determined from experimental measurements, thus validating the ReaxFF results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗