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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Nanometer Resolution Structure‐Emission Correlation of Individual Quantum Emitters via Enhanced Cathodoluminescence in Twisted Hexagonal Boron Nitride

Understanding the atomic structure of quantum emitters, often originating from point defects or impuritie, is essential for designing and optimizing materials for quantum technologies such as quantum computing, communication, and sensing. Despite the availability of atomic-resolution scanning transmission electron microscopy and nanoscale cathodoluminescence microscopy, experimentally determining the atomic structure of individual emitters is challenging due to the conflicting needs for thick samples to generate strong cathodoluminescence signals and thin samples for structural analysis. To overcome this challenge, significantly enhanced cathodoluminescence at twisted interfaces is leveraged to achieve sub-nanometer localization precision for the first time in mapping individual quantum emitters in carbon-implanted hexagonal boron nitride. This unprecedent spatial sensitivity, together with correlative electron energy loss spectroscopy quantitative scanning transmission electron microscopy imaging, and first principles density functional theory calculations, enables the identification of the atomic structure of the 440 nm blue emitter in hexagonal boron nitride as a substituted vertical carbon dimer. Building on the atomic structure insights, nanoscale spatially precise creation of blue emitters is demonstrated by electron beam irradiation of carbon-coated hexagonal boron nitride. This advancement in correlating atomic structures with optical properties lays the foundation for a deeper understanding and precise engineering of quantum emitters, significantly advancing the development of cutting-edge quantum information technologies.

2D material↗
DOE OSTI2024

Atomic scale etching of diamond: insights from molecular dynamics simulations

Diamond is a promising material for multiple applications in quantum information processing and sensing as well as applications in microelectronics. However, diamond devices can be limited by surface defects that compromise charge stability and spin coherence, among others. Improved strategies in plasma etching of diamond could play an important role in minimizing or eliminating these defects. In this work, we explore plasma-assisted atomic scale etching of diamond using argon ions (Ar + ), hydrogen ions (H + ) and hydrogen atoms (H). We employ classical molecular dynamics (MD) simulations and test several interatomic potentials based on the Reactive Empirical Bond Order (REBO) form with comparisons to a variety of published experimental results. We performed MD simulations of low-energy hydrogen ($\leqslant$50 eV) and argon ( $\leqslant$200 eV) ion bombardment of diamond surfaces. Ar + bombardment can be used to locally smooth initially rough diamond surfaces via the formation of an amorphous C layer, the thickness of which increases with argon ion energy. Subsequent exposure with hydrogen ions (or fast neutrals) will selectively etch this amorphous C layer, leaving the underlying diamond layer mostly intact if the H energy is maintained below about 10 eV. The simulations suggest that combining Ar + smoothing with selective, near threshold energy H removal of amorphous C can be an effective strategy for diamond surface engineering, leading to more reliable and sensitive diamond color center devices.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Plasmonic Ag nanocomposite phosphate glasses produced via γ-ray irradiation as reduction route

This paper reports on the impact of γ-ray irradiation (10, 100 kGy) on melt-quenched Ag + -doped phosphate glass and the effects of subsequent thermal processing leading to the production of plasmonic Ag nanocomposites. The γ-irradiated glasses were characterized alongside the pristine by differential scanning calorimetry (DSC), Raman spectroscopy, electron paramagnetic resonance (EPR) spectroscopy, optical absorption, and photoluminescence (PL) spectroscopy. DSC characterization showed consistent glass transition temperatures (T g ) before and after γ-irradiation whereas the crystallization temperatures tended to decrease with increasing γ-ray dose. However, a lack of alteration of the glass network structure was supported by Raman spectroscopy. Room temperature EPR spectra clearly showed the formation of phosphorus oxygen hole center (POHC) defects in the undoped host, in addition to another doublet likely associated with a P 3 defect. The presence of paramagnetic silver species encompassing Ag 2+ and 107/109 Ag 0 atoms was also indicated in the silver-activated glass together with POHC defects. Optical absorption spectra were also consistent with the presence of various radiation-induced centers. Further analyzing the glass absorption edge via Tauc plots suggested the formation of electron center (EC) defects in γ-irradiated samples wherein the silver-doped glass exhibited decreasing band gap energies with increasing γ-ray dose. The PL characterization showed the silver-related radio-PL effect was induced exhibiting broad band emission with two maxima around 500 and 625 nm stemming from various molecular Ag$^{x+}_{n}$ clusters. Emission decay analyses revealed that the longer wavelength emission exhibited slower decay. The highest radiation dose of 100 kGy however resulted in weaker emission and faster decay kinetics attributed to energy transfer between the luminescent silver species and POHC defects. Finally subjecting the γ-irradiated Ag-doped glasses to heat treatment near the T g at 490 °C led to the development of the surface plasmon resonance of Ag nanoparticles (NPs) and the vanishing of the Ag$^{x+}_{n}$ clusters luminescence. In conclusion, the presence of the matrix-related EC defects was deemed accountable for the thermally induced reduction and consequent precipitation of Ag NPs making the plasmonic glasses attractive for photonic applications such as nonlinear optics.

36 MATERIALS SCIENCE↗
NASA NTRS2001

Atomically Flat Surfaces Developed for Improved Semiconductor Devices

New wide bandgap semiconductor materials are being developed to meet the diverse high temperature, -power, and -frequency demands of the aerospace industry. Two of the most promising emerging materials are silicon carbide (SiC) for high-temperature and high power applications and gallium nitride (GaN) for high-frequency and optical (blue-light-emitting diodes and lasers) applications. This past year Glenn scientists implemented a NASA-patented crystal growth process for producing arrays of device-size mesas whose tops are atomically flat (i.e., step-free). It is expected that these mesas can be used for fabricating SiC and GaN devices with major improvements in performance and lifetime. The promising new SiC and GaN devices are fabricated in thin-crystal films (known as epi films) that are grown on commercial single-crystal SiC wafers. At this time, no commercial GaN wafers exist. Crystal defects, known as screw defects and micropipes, that are present in the commercial SiC wafers propagate into the epi films and degrade the performance and lifetime of subsequently fabricated devices. The new technology isolates the screw defects in a small percentage of small device-size mesas on the surface of commercial SiC wafers. This enables atomically flat surfaces to be grown on the remaining defect-free mesas. We believe that the atomically flat mesas can also be used to grow GaN epi films with a much lower defect density than in the GaN epi films currently being grown. Much improved devices are expected from these improved low-defect epi films. Surface-sensitive SiC devices such as Schottky diodes and field effect transistors should benefit from atomically flat substrates. Also, we believe that the atomically flat SiC surface will be an ideal surface on which to fabricate nanoscale sensors and devices. The process for achieving atomically flat surfaces is illustrated. The surface steps present on the "as-received" commercial SiC wafer is also illustrated. because of the small tilt angle between the crystal "basal" plane and the polished wafer surface. These steps are used in normal SiC epi film growth in a process known as stepflow growth to produce material for device fabrication. In the new process, the first step is to etch an array of mesas on the SiC wafer top surface. Then, epi film growth is carried out in the step flow fashion until all steps have grown themselves out of existence on each defect-free mesa. If the size of the mesas is sufficiently small (about 0.1 by 0.1 mm), then only a small percentage of the mesas will contain an undesired screw defect. Mesas with screw defects supply steps during the growth process, allowing a rough surface with unwanted hillocks to form on the mesa. The improvement in SiC epi surface morphology achievable with the new technology is shown. An atomic force microscope image of a typical SiC commercial epilayer surface is also shown. A similar image of an SiC atomically flat epi surface grown in a Glenn laboratory is given. With the current screw defect density of commercial wafers (about 5000 defects/cm2), the yield of atomically free 0.1 by 0.l mm mesas is expected to be about 90 percent. This is large enough for many types of electronic and optical devices. The implementation of this new technology was recently published in Applied Physics Letters. This work was initially carried out in-house under a Director's Discretionary Fund project and is currently being further developed under the Information Technology Base Program.

Powell, J. Anthony↗
DOE OSTI2025

Single-Atom-Resolved Vibrational Spectroscopy of a Dislocation

Dislocations in III-nitride semiconductors impede heat transport, leading to localized overheating, which severely limits the performance and reliability of optoelectronic and power devices. Current research on phonon–dislocation interactions primarily addresses bulk materials, focusing on the average effects at specific dislocation densities. However, phonon resistance from dislocation scattering arises from both short-range core interactions and long-range strain field interactions, which remain largely unexplored. Here, in this study, electron energy-loss spectroscopy is used to investigate a GaN dislocation. Vibrational modes localized on specific core atoms are revealed, reflecting short-range interactions. Additionally, phonon energy shifts driven by strain fields surrounding the dislocation are observed, reflecting long-range interactions. Ab initio calculations support these findings and draw out additional details. This work establishes a paradigm for probing defect-induced phonon scattering at the single-atom level, revealing how dislocations affect phonon behavior through atomic reconstruction and strain engineering, thus offering insights for designing improved material functionalities.

III-nitride semiconductors↗
NASA NTRS1991

Ground and space based optical analysis of materials degradation in low-Earth-orbit

There is strong interest in being able to accurately and sensitively monitor materials degradation in both ground-based and space-based environments. Two optical techniques for sensitive degradation monitoring are reviewed: spectroscopic ellipsometry and photothermal spectroscopy. These techniques complement each other in that ellipsometry is sensitive to atomically thin surface and subsurface changes, and photothermal spectroscopy is sensitive to local defects, pin-holes, subsurface defects, and delamination. Progress in applying these spectroscopies (both ex situ and in situ) to atomic oxygen degradation of space materials is reviewed.

Woollam, John A.↗
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↗
DOE OSTI2026

Interfacial Void Formation and Self-Healing in Oxide Scales on Al-containing High-Entropy Alloy

The exceptional high-temperature oxidation resistance of Al-containing high-entropy alloys (HEAs) is often attributed to the formation of a protective α-Al 2 O 3 scale. However, the dynamic, atomic-scale mechanisms governing the stability of this scale—including interfacial void formation and the often-postulated but rarely visualized “self-healing” capacity—remain poorly understood. Herein, we reveal the complex evolution of the triple-layer oxide scale on an Al 10 CoCrFeNi HEA through combined electron microscopy and diffraction study. We show that interfacial voids are an inherent consequence of the scaling process, originating from two distinct mechanisms: the Kirkendall effect at the interface between the γ-Al 2 O 3 /α-Al 2 O 3 and alloy driven by cationic diffusion imbalance and volumetric contraction due to phase transformations at the spinel/Cr 2 O 3 interface. Crucially, we provide microstructural evidence consistent with an intrinsic self-healing response. This process is driven by coupled inward diffusion of oxygen and outward diffusion of metal cations, leading to the in-situ formation of transient θ-Al 2 O 3 and spinel phases that partially fill and seal the voids. Here, these results provide atomic-scale insights into the phase evolution, defect formation, and self-repair of oxide scales in HEAs—highlighting pathways to enhance their oxidation resistance in extreme environments.

High-entropy alloy↗
NASA NTRS2002

Ceramic Inclusions In Powder Metallurgy Disk Alloys: Characterization and Modeling

Powder metallurgy alloys are increasingly used in gas turbine engines, especially as the material chosen for turbine disks. Although powder metallurgy materials have many advantages over conventionally cast and wrought alloys (higher strength, higher temperature capability, etc.), they suffer from the rare occurrence of ceramic defects (inclusions) that arise from the powder atomization process. These inclusions can have potentially large detrimental effect on the durability of individual components. An inclusion in a high stress location can act as a site for premature crack initiation and thereby considerably reduce the fatigue life. Because these inclusions are exceedingly rare, they usually don't reveal themselves in the process of characterizing the material for a particular application (the cumulative volume of the test bars in a fatigue life characterization is typically on the order of a single actual component). Ceramic inclusions have, however, been found to be the root cause of a number of catastrophic engine failures. To investigate the effect of these inclusions in detail, we have undertaken a study where a known population of ceramic particles, whose composition and morphology are designed to mimic the 'natural' inclusions, are added to the precursor powder. Surface connected inclusions have been found to have a particularly large detrimental effect on fatigue life, therefore the volume of ceramic 'seeds' added is calculated to ensure that a minimum number will occur on the surface of the fatigue test bars. Because the ceramic inclusions are irregularly shaped and have a tendency to break up in the process of extrusion and forging, a method of calculating the probability of occurrence and expected intercepted surface and embedded cross-sectional areas were needed. We have developed a Monte Carlo simulation to determine the distributions of these parameters and have verified the simulated results with observations of ceramic inclusions found in macro slices from extrusions and forgings. The ultimate goal of this study will be to use probabilistic methods to determine the reliability detriment that can be attributed to these ceramic inclusions.

Bonacuse, Pete↗
NASA NTRS1979

Structure and electrical activity of planar defects in EFG ribbons

Optical, electron beam induced current (EBIC), and transmission electron microscopy were used to study the structure and electrical activity of planar defects in EFG silicon. What appears to be twin boundaries by both optical microscopy plus etching, and by EBIC are in reality systems of microtwins, some of which are only a few atomic lattice planes thick. The electrical activity of planar defects appears to be correlated with emission of dislocations especially at termination points. Impurity effects may also play a role. Twin boundaries per se appear not to be electrically active.

Ast, D. G.↗
DOE OSTI2026

Active site design enables industrial scale H 2 O 2 electrosynthesis with metal-free catalysts

The electrosynthesis of hydrogen peroxide (H 2 O 2 ) via a two-electron oxygen reduction reaction enables decentralized H 2 O 2 production. While metal-free carbon catalysts are sustainable and low-cost, their performance is hindered by poorly defined active sites and uncontrolled defect states. Here, we resolve these challenges through active site design and catalyst screening using fluorine (F) and nitrogen (N) codoped carbons as model materials. Statistical analysis combined with density functional theoretical calculations reveals that F-induced structural modification and defect passivation optimize OOH* binding, with F-doping and adjacent F atoms predominantly lowering abs ΔG(OOH*). Experimental results confirm that semi-ionic C–F bonds passivate defects in nitrogen-doped carbon, enhancing catalytic activity and durability. The resulting (N, F)-codoped carbon achieves nearly 100% H 2 O 2 selectivity at 0.5–0.65 V versus the reversible hydrogen electrode and maintains > 95% across 0.01–0.65 V versus the reversible hydrogen electrode. In an electrolyzer, (N, F)-codoped carbon exhibits an H 2 O 2 yield rate of 74.35 mol g cat. −1 h -1 and sustains 300 mA cm -2 for 105 hours with ~95% faradaic efficiency. Coupling the two-electron oxygen reduction reaction with methanol oxidation further reduces cell voltage and enhances productivity. This work provides a means to design efficient catalysts for industrial H 2 O 2 electrosynthesis.

H2O2 electrosynthesis↗
DOE OSTI2024

Ion velocity effect governs damage annealing process in defective KTaO 3

Effects of electronic to nuclear energy losses (S e /S n ) ratio on damage evolution in defective KTaO 3 have been investigated by irradiating pre-damaged single crystal KTaO 3 with intermediate energy O ions (6 MeV, 8 MeV and 12 MeV) at 300 K. By exploring these processes in pre-damaged KTaO 3 containing a fractional disorder level of 0.35, the results demonstrate the occurrence of a precursory stage of damage production before the onset of damage annealing process in defective KTaO 3 that decreases with O ion energy. The observed ionization-induced annealing process by ion channeling analysis has been further mirrored by high resolution transmission electron microscopy analysis. In addition, the reduction of disorder level is accompanied by the broadening of the disorder profiles to greater depth with increasing ion fluence, and enhanced migration is observed with decreasing O ion energy. Since S e (~3.0 keV nm –1 ) is nearly constant for all 3 ion energies across the pre-damaged depth, the difference in behavior is due to the so-called 'velocity effect': the lower ion velocity below the Bragg peak yields a confined spread of the electron cascade and hence an increased energy deposition density. Here, the inelastic thermal spike calculation has further confirmed the existence of a velocity effect, not previously reported in KTaO 3 or very scarcely reported in other materials for which the existence of ionization-induced annealing has been reported. In other words, understanding of ionization-induced annealing has been advanced by pointing out that ion velocity effect governs the healing of pre-existing defects, which may have significant implication for the creation of new functionalities in KTaO 3 through atomic-level control of microstructural modifications, but may not be limited to KTaO 3 .

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Probing Basal and Prismatic Planes of Graphitic Materials for Metal Single Atom and Subnanometer Cluster Stabilization

Abstract Supported metal single atom catalysis is a dynamic research area in catalysis science combining the advantages of homogeneous and heterogeneous catalysis. Understanding the interactions between metal single atoms and the support constitutes a challenge facing the development of such catalysts, since these interactions are essential in optimizing the catalytic performance. For conventional carbon supports, two types of surfaces can contribute to single atom stabilization: the basal planes and the prismatic surface; both of which can be decorated by defects and surface oxygen groups. To date, most studies on carbon‐supported single atom catalysts focused on nitrogen‐doped carbons, which, unlike classic carbon materials, have a fairly well‐defined chemical environment. Herein we report the synthesis, characterization and modeling of rhodium single atom catalysts supported on carbon materials presenting distinct concentrations of surface oxygen groups and basal/prismatic surface area. The influence of these parameters on the speciation of the Rh species, their coordination and ultimately on their catalytic performance in hydrogenation and hydroformylation reactions is analyzed. The results obtained show that catalysis itself is an interesting tool for the fine characterization of these materials, for which the detection of small quantities of metal clusters remains a challenge, even when combining several cutting‐edge analytical methods.

Vidal, Mathieu↗
DOE OSTI2025

Origin of reduced efficiency in GaN-based micro-LEDs studied by scanning near-field optical microscopy

The quantum efficiency of micro-light emitting diodes (micro-LEDs) is lower than that of large area LEDs. This efficiency reduction is typically attributed to the nonradiative Shockley–Read–Hall recombination at the surface defects and current leakage through the sidewall region without a clear distinction between these effects. In this work, we attempt to find out which of these phenomena is most critical for the reduced efficiency of micro-LEDs. This has been done by mapping electroluminescence (EL) and photoluminescence (PL) and measuring PL dynamics in blue GaN micro-LEDs fabricated by dry etching. It has been found that in the as-etched device, the EL intensity is much lower than in devices with KOH etching and atomic layer deposition of SiO 2 . This effect is especially pronounced close to the sidewalls. On the other hand, PL decay times are similar in as-etched and passivated devices, both in their center and at the sidewalls. This allows concluding that the main mechanism of the reduced efficiency of micro-LEDs fabricated by dry etching is the current leakage in the sidewall region and not the nonradiative recombination. The KOH etching has been found to be the most efficient means to eliminate the current leakage.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Characterizing Defects Inside Hexagonal Boron Nitride Using Random Telegraph Signals in van der Waals 2D Transistors

Single-crystal hexagonal boron nitride (hBN) is used extensively in many two-dimensional electronic and quantum devices, where defects significantly impact performance. Therefore, characterizing and engineering hBN defects are crucial for advancing these technologies. Here, we examine the capture and emission dynamics of defects in hBN by utilizing low-frequency noise (LFN) spectroscopy in hBN-encapsulated and graphene-contacted MoS 2 field-effect transistors (FETs). The low disorder of this heterostructure allows the detection of random telegraph signals (RTS) in large device dimensions of 100 μm 2 at cryogenic temperatures. Analysis of gate bias- and temperature-dependent LFN data indicate that RTS originates from a single trap species within hBN. By performing multi-space density functional theory (MS-DFT) calculations on a gated defective hBN/MoS 2 heterostructure model, we assign substitutional carbon atoms in boron sites as the atomistic origin of RTS. This study demonstrates the utility of LFN spectroscopy combined with MS-DFT analysis on a low-disorder all-vdW FET as a powerful means for characterizing the atomistic defects in single-crystal hBN.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

GPU-Accelerated Solution of the Bethe–Salpeter Equation for Large and Heterogeneous Systems

We present a massively parallel GPU-accelerated implementation of the Bethe–Salpeter equation (BSE) for the calculation of the vertical excitation energies (VEEs) and optical absorption spectra of condensed and molecular systems, starting from single-particle eigenvalues and eigenvectors obtained with density functional theory. The algorithms adopted here circumvent the slowly converging sums over empty and occupied states and the inversion of large dielectric matrices through a density matrix perturbation theory approach and a low-rank decomposition of the screened Coulomb interaction, respectively. Further computational savings are achieved by exploiting the nearsightedness of the density matrix of semiconductors and insulators to reduce the number of screened Coulomb integrals. We scale our calculations to thousands of GPUs with a hierarchical loop and data distribution strategy. The efficacy of our method is demonstrated by computing the VEEs of several spin defects in wide-band-gap materials, showing that supercells with up to 1000 atoms are necessary to obtain converged results. We discuss the validity of the common approximation that solves the BSE with truncated sums over empty and occupied states. In conclusion, we then apply our GW-BSE implementation to a diamond lattice with 1727 atoms to study the symmetry breaking of triplet states caused by the interaction of a point defect with an extended line defect.

Absorption spectra↗
DOE OSTI2025

Scalable Bottom-Up Synthesis of Nanoporous Hexagonal Boron Nitride ( h -BN) for Large-Area Atomically Thin Ceramic Membranes

Nanopores embedded within monolayer hexagonal boron nitride (h-BN) offer possibilities of creating atomically thin ceramic membranes with unique combinations of high permeance (atomic thinness), high selectivity (via molecular sieving), increased thermal stability, and superior chemical resistance. However, fabricating size-selective nanopores in monolayer h-BN via scalable top-down processes remains nontrivial due to its chemical inertness, and characterizing nanopore size distribution over a large area remains extremely challenging. Here, we demonstrate a facile and scalable approach of exploiting the chemical vapor deposition (CVD) process temperature to enable direct incorporation of subnanometer/nanoscale pores into the monolayer h-BN lattice, in combination with manufacturing compatible polymer casting to fabricate centimeter-scale nanoporous atomically thin ceramic membranes. We leverage diffusive transport of analytes including size-selective Ficoll sieving to characterize subnanometer-scale and nanoscale defects that manifest as pores in centimeter-scale h-BN membranes, overcoming previous limitations in large-area characterization of nanoscale defects in h-BN. Our approach opens a new frontier to advance atomically thin membranes to 2D ceramic materials, such as h-BN via facile and direct formation of nanopores, for size-selective separations.

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

Graphene-driven correlated electronic states in one dimensional defects within WS2

Tomonaga-Luttinger liquid (TLL) behavior in one-dimensional systems has been predicted and shown to occur at semiconductor-to-metal transitions within two-dimensional materials. Reports of one-dimensional defects hosting a Fermi liquid or a TLL have suggested a dependence on the underlying substrate, however, unveiling the physical details of electronic contributions from the substrate require cross-correlative investigation. Here, we study TLL formation within defectively engineered WS2 atop graphene, where band structure and the atomic environment is visualized with nano angle-resolved photoelectron spectroscopy, scanning tunneling microscopy and spectroscopy, and non-contact atomic force microscopy. Correlations between the local density of states and electronic band dispersion elucidated the electron transfer from graphene into a TLL hosted by one-dimensional metal (1DM) defects. It appears that the vertical heterostructure with graphene and the induced charge transfer from graphene into the 1DM is critical for the formation of a TLL.

Rossi, Antonio↗