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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Aqueous Synthesis of Concave Rh Nanotetrahedra with Defect-Rich Surfaces: Insights into Growth-, Defect-, and Plasmon-Enhanced Catalytic Energy Conversion

The control of morphology in the synthesis of Rh nanocrystals can be used to precisely tailor the electronic surface structure; this in turn directly influences their performance in catalysis applications. Many works have brought attention to the development of Rh nanostructures with low-index surfaces, but limited effort has been devoted to the study of high-index and surface defect-enriched nanocrystals as they are not favored by thermodynamics because of the involvement of high-energy surfaces and increased surface-to-volume ratios. Here, we demonstrate an aqueous synthesis of concave Rh nanotetrahedra (CTDs) serving as efficient catalysts for energy conversion reactions. CTDs are surface defect-rich structures that form through a slow growth rate and follow the four-step model of metallic nanoparticle growth. Via the tuning of the surfactant concentration, the morphology of Rh CTDs evolved into highly excavated nanotetrahedra (HETDs) and twinned nanoparticles (TWs). Unlike the CTD surfaces with abundant adatoms and vacancies, HETDs and TWs have more regular surfaces with layered terraces. Each nanocrystal type was evaluated for methanol electrooxidation and hydrogen evolution from hydrolysis of ammonia borane, and the CTDs significantly showed the best catalytic performance because of defect enrichment, which benefits the surface reactivity of adsorbates. In addition, both CTDs and HETDs have strong absorption near the visible light region (382 and 396 nm), for which they show plasmon-enhanced performance in photocatalytic hydrogen evolution under visible light illumination. CTDs are more photoactive than HETDs, likely because of more pronounced localized surface plasmon resonance hot spots. Lastly, this facile aqueous synthesis of large-surface-area, defect-rich Rh nanotetrahedra is exciting for the fields of nanosynthesis and catalysis.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ion irradiation and modification: The role of coupled electronic and nuclear energy dissipation and subsequent nonequilibrium processes in materials

Understanding material responses to energy deposition from energetic charged particles is important for defect engineering, ion-beam processing, ion-beam analysis and modification, geologic aging, space exploration, and nuclear applications. As an incident ion penetrates a solid, its energy is transferred to electrons and to atomic nuclei of the solid. Much of this electronic energy deposition is subsequently transferred to the atomic structure via electron–phonon (e–ph) coupling, leading to local inelastic thermal spikes in which energy dissipation is influenced by the local environment. In addition, intense ionization can lead to high densities of localized electronic excitations in wide-bandgap materials and ceramics that can affect defect dynamics and atomic mobility. Specifically, energy exchange between electrons and atomic nuclei, along with localized electronic excitations, can lead to substantial competitive (ionization-induced annealing), additive (both electronic and nuclear energy depositions contributing to damage production), and synergistic (more damage than the sums of separate damage processes) effects. Although nonmonotonic effects of the e–ph coupling strength and athermal processes are demonstrated for pre-existing defects and residual damage during ion–solid interactions, there is limited understanding of when such electronic effects must be considered in atomic-scale models of damage production and evolution in a broad variety of materials. Complex ceramics and chemically disordered solid solution alloys with different constituent elements allow a systematic evaluation of defect dynamics and irradiation performance with increasing complexity. Current knowledge regarding tuning of bonding characteristics and chemical disorder to control atomic-level dynamics is reviewed. Although a lack of fundamental understanding obstructs the advancement of reliable predictions for ion beam material modification, it highlights challenges and opens research opportunities. Insights into the complex electronic and atomic correlations with extreme energy deposition will strengthen our ability to design materials and predict ion-irradiation-induced damage in a radiation environment, and they may pave the way to better control fundamental processes and design new material functionalities for advanced technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Metal-insulator transition in V 2 O 3 with intrinsic defects

Vanadium sesquioxide (V 2 O 3 ) is a Mott insulator exhibiting a temperature-dependent metal-insulator transition (MIT) at 165 K accompanied by both a magnetic and structural transition. Although it is expected to be a metal under conventional band theory, electron interactions at low temperature cause it to behave like an insulator, making it difficult to accurately model its electronic properties with standard ab initio methods. As such, accurate theoretical assessments of the MIT with point defects requires special attention to the type of functionals used. In this study, we conclude that the PBE + U functional provides the best compromise between accuracy and efficiency in calculating the properties related to the MIT between low-temperature and high-temperature V 2 O 3 . We use this functional to explore the various influences that intrinsic point defects will have on the MIT in V 2 O 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Metal-Insulation REBCO Pancake Coil With Solder Surface Shunt: Testing and Modeling

Rare-earth barium copper oxide (REBCO) high-temperature superconducting (HTS) magnets can generate very high magnetic fields with superior engineering current density and robust mechanical integrity. The no-insulation (NI) winding technique, including its metal-insulation (MI) variant, enables “self-protection” against localized overheating through inter-turn current sharing, improving defect tolerance and allowing temporary current overloads. In REBCO pancake coils, the current-sharing path is predominantly confined to the edges of the REBCO tapes due to insulating buffer layers. Applying a surface shunt using solder can effectively enhance current sharing in NI/MI coils via the REBCO tape edges. Here, in this paper, we present both experimental and numerical research on the current distribution in surface-shunt metal-insulation (SSMI) REBCO pancake coils. We tested a stainless steel co-wound MI REBCO double-pancake coil, before and after applying a soldered surface shunt, in a saturated liquid nitrogen bath. The SSMI coil was modeled using the H-formulation and rotated anisotropic resistivity to study its dynamic behavior, including inter-turn current sharing and intra-turn screening currents. Benchmarked by experimental data, the numerical model is able to study the defect tolerance of the SSMI coil during energization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Role of morphology in defect formation and photo-induced carrier instabilities in amorphous indium oxide

Ab initio molecular dynamics liquid-quench simulations and hybrid density functional calculations are performed to model the effects of room-temperature atomic fluctuations and photo-illumination on the structural and electronic properties of amorphous sub-stoichiometric In 2 O 2.96 . A large configurational ensemble is employed to reliably predict the distribution of localized defects as well as their response to the thermal and light activation. The results reveal that the illumination effects on the carrier concentration are greater in amorphous configurations with shorter In–O bond length and reduced polyhedral sharing as compared to the structures with a more uniform morphology. Further, the obtained correlation between the photo-induced carrier density and the reduction in the number of fully coordinated In-atoms implies that metal oxides with a significant fraction of crystalline/amorphous interfaces would show a more pronounced response to illumination. Photo-excitation also produces In–O 2 –In defects that have not been previously found in sub-stoichiometric amorphous oxides; these defects are responsible for carrier instabilities due to overdoping.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Strain release by 3D atomic misfit in fivefold twinned icosahedral nanoparticles with amorphization and dislocations

Multiple twinning to form fivefold twinned nanoparticles in crystal growth is common and has attracted broad attention ranging from crystallography research to physical chemistry and materials science. Lattice-misfit strain and defects in multiple twinned nanoparticles (MTP) are key to understand and tailor their electronic properties. However, the structural defects and related strain distributions in MTPs are poorly understood in three dimensions (3D). Here, we show the 3D atomic misfit and strain relief mechanism in fivefold twinned icosahedral nanoparticles with amorphization and dislocations by using atomic resolution electron tomography. We discover a two-sided heterogeneity in variety of structural characteristics. A nearly ideal crystallographic fivefold face is always found opposite to a less ordered face, forming Janus-like icosahedral nanoparticles with two distinct hemispheres. The disordered amorphous domains release a large amount of strain. Molecular dynamics simulations further reveal the Janus-like icosahedral nanoparticles are prevalent in the MTPs formed in liquid-solid phase transition. This work provides insights on the atomistic models for the modelling of formation mechanisms of fivefold twinned structures and computational simulations of lattice distortions and defects. We anticipate it will inspire future studies on fundamental problems such as twin boundary migration and kinetics of structures in 3D at atomic level.

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

Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution

Here, the development of many optical quantum technologies depends on the availability of solid-state single quantum emitters with near-perfect optical coherence. However, a standing issue that limits systematic improvement is the significant sample heterogeneity and lack of mechanistic understanding of microscopic energy flow at the single emitter level and ultrafast timescales. Here we develop solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. We apply this technique to single quantum emitters in two-dimensional hexagonal boron nitride, which suffers from significant heterogeneity and low quantum efficiency. From millisecond to nanosecond timescales, the translation diffusion, metastable-state-related bunching shoulders, rotational dynamics, and antibunching features are disentangled by their distinct photon-correlation timescales, which collectively quantify the normalized two-photon emission quantum yield. Leveraging its femtosecond resolution, spectral selectivity and ultralow noise (two orders of magnitude improvement over solid-state methods), we visualize electron-phonon coupling in the time domain at the single defect level, and discover the acceleration of polaronic formation driven by multi-electron excitation. Corroborated with results from a theoretical polaron model, we show how this translates to sample-averaged photon fidelity characterization of cascaded emission efficiency and optical decoherence time. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Quantitative Observation of Threshold Defect Behavior in Memristive Devices with Operando X-ray Microscopy

Memristive devices are an emerging technology that enables both rich interdisciplinary science and novel device functionalities, such as nonvolatile memories and nanoionics-based synaptic electronics. Recent work has shown that the reproducibility and variability of the devices depend sensitively on the defect structures created during electroforming as well as their continued evolution under dynamic electric fields. However, a fundamental principle guiding the material design of defect structures is still lacking due to the difficulty in understanding dynamic defect behavior under different resistance states. Here, we unravel the existence of threshold behavior by studying model, single-crystal devices: resistive switching requires that the pristine oxygen vacancy concentration reside near a critical value. Theoretical calculations show that the threshold oxygen vacancy concentration lies at the boundary for both electronic and atomic phase transitions. Through operando , multimodal X-ray imaging, we show that field tuning of the local oxygen vacancy concentration below or above the threshold value is responsible for switching between different electrical states. Lastly, these results provide a general strategy for designing functional defect structures around threshold concentrations to create dynamic, field-controlled phases for memristive devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures

Carrier recombination is a crucial process governing the optical properties of a semiconductor. Although various theoretical approaches have been utilized to describe carrier behaviors, a quantitative understanding of the impact of defects and interfaces in low dimensional semiconductor systems is still elusive. Here, we develop a model system consisting of chemically tunable, highly luminescent halide perovskite nanocrystals to illustrate the role of carrier diffusion and material dimensionality on the carrier recombination kinetics and luminescence efficiency. Our advanced synthetic methods provide a well-controlled colloidal system consisting of nanocrystals with different aspect ratios, halide compositions, and surface conditions. Using this system, we reveal the scaling laws of photoluminescence quantum yield and radiative lifetime with respect to the aspect ratio of nanocrystals. The scaling laws derived herein are not only a phenomenological observation but proved a powerful tool disentangling the carrier dynamics of microscopic systems in a quantitative and interpretable manner. The investigation of our model system and theoretical formulation bring to light the dimensionality, as a hidden constraint on carrier dynamics, and identify the diffusion length as an important parameter that distinguishes nanoscale and macroscale carrier behaviors. Furthermore, the conceptual distinction in carrier dynamics in different dimensionality regimes informs new design rules for optical devices where complex microstructures are involved.

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

Boltzmann machine modeling of layered MoS 2 synthesis on a quantum annealer

Two-dimensional layered materials are usually synthesized by chemical vapor deposition (CVD). Here we use the Restricted Boltzmann Machine (RBM) and its enhancement called Limited Boltzmann Machine (LBM) on a quantum computer to model the chemical vapor deposition (CVD) growth data for a MoS 2 monolayer. The CVD data for Boltzmann machines are generated by reactive molecular dynamics (RMD) simulations. The Boltzmann machines give insight into the semiconducting (2H) and metallic (1T) phases and defects generated during the CVD growth of MoS 2 . We compare the performances of the two types of Boltzmann machine models, i.e. RBM versus augmented topologies with limited intra-layer coupling between the hidden units (LBM). We show that limited topologies have a performance advantage over restricted topologies. We examine connectivity within our topological variants, explore hardware qubit mapping schemes, and discuss what performance differences may imply about locality within the data without prior knowledge.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Effect of environmental screening and strain on optoelectronic properties of two-dimensional quantum defects

Point defects in hexagonal boron nitride (hBN) are promising candidates as single-photon emitters (SPEs) in nanophotonics and quantum information applications. The precise control of SPEs requires in-depth understanding of their optoelectronic properties. However, how the surrounding environment of host materials, including the number of layers, substrates, and strain, influences SPEs has not been fully understood. Here, in this work, we study the dielectric screening effect due to the number of layers and substrates, and the strain effect on the optical properties of carbon dimer and nitrogen vacancy defects in hBN from first-principles many-body perturbation theory. We report that environmental screening causes a lowering of the quasiparticle gap and exciton binding energy, leading to nearly constant optical excitation energy and exciton radiative lifetime. We explain the results with an analytical model starting from the Bethe–Salpeter equation Hamiltonian with Wannier basis. We also show that optical properties of quantum defects are largely tunable by strain with highly anisotropic response, in good agreement with experimental measurements. Our work clarifies the effect of environmental screening and strain on optoelectronic properties of quantum defects in two-dimensional insulators, facilitating future applications of SPEs and spin qubits in low-dimensional systems.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Ab Initio Investigation of Charge Trapping Across the Crystalline- Si -Amorphous- Si O 2 Interface

Accurate microscopic description of the charge-trapping process from semiconductor to defects in the dielectric-oxide layer is of paramount importance for understanding many microelectronic devices such as complementary metal-oxide-semiconductor (CMOS) transistors, as well as electrochemical reactions. Unfortunately, most current microscopic descriptions of such processes are based on empirical models with parameters fitted to experimental device performance results or simplified approximations like the Wentzel-Kramers-Brillouin (WKB) method. Some critical questions are still unanswered, including: What controls the charge-hopping rate, the coupling strength between the defect level to semiconductor level, or the energy difference? How does the hopping rate decay with defect-semiconductor distance? What is the fluctuation of the defect level, especially in amorphous dielectrics? Many of these questions can be answered by ab initio calculations. However, to date, there are few ab initio studies for this problem mainly due to technical challenges from atomic-structure construction to large-system calculations. Here, using the latest advances in calculation methods and codes, we study the carrier-trapping problem using density-functional theory (DFT) based on the Heyd-Scuseria-Ernzerhof (HSE) exchange correlation functional. The valence bond random-switching method is used to construct the crystalline-Si-amorphous-SiO2 (c-Si/a-SiO2) interfacial atomic structure, and the HSE yields a band offset that agrees well with experiments. The hopping rate is calculated with the Marcus theory, and the hopping-rate dependences on the gate potential and defect distances are revealed, as well as the range of fluctuation results from amorphous structural variation. We also analyze the result with the simple WKB model and find a major difference in the description of the coupling constant decay with the defect-semiconductor distance. Our results provide the ab initio simulation insights for this important carrier-trapping process for device operation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Prediction of Subsidence of Buildings as a Result of Earthquakes by Gaussian Process Regression

Subsidence of a foundation caused by liquefaction of sandy soil is a critical step in the creation of a building. Seven measured indicators of soil liquefaction in the course of an earthquake were selected as key impacting indicators that predict subsidence of a building. These indicators are the earthquake intensity EI, length–height ratio L/H, average contact pressure p, width-depth ratio, relative density D{sub R}, thickness of the non-liquefied layer, and the depth of the gravel layer. Furthermore, as a probabilistic machine learning kernel and powerful tool for solving highly nonlinear problems, Gaussian process regression (GPR model) can meet execution time requirements and assure a high level of precision of subsidence prediction due to the intrinsic defects of theoretical analysis and numerical calculation. A total of 41 groups of typical cases were first selected as a training sample and 20 groups of typical cases were defined as a test sample, where these cases possess input test value and were obtained at the yield of the prediction accuracy from the GPR model. Next, the PLS method, MLR method and LSSVM method were selected to verify the validity and reliability of the GPR model. Finally, the simulation result shows that the GPR model can improve the prediction precision for the case of the above problems and is of great value for practical applications.

58 GEOSCIENCES↗
DOE OSTI2021

Observation of Single-Electron Transport and Charging on Individual Point Defects in Atomically Thin WSe 2

Defects significantly impact the properties of 2D semiconductors, providing in-gap quantum states that can serve as a natural platform for single-electron operations, localization sites for excitons to serve as single-photon sources, and potentially quantum spin memories. To date, however, a microscopic observation of such a single-electron transport (SET) behavior has been rarely reported on single defects of 2D semiconductors. In this study, we report a SET and charge-state transition on individual point-defect states buried in the bilayer WSe 2 using scanning tunneling microscopy. SET characteristics of their states is evidenced by both the Coulomb staircase and the saturation behavior of the transport current, consistent with the SET model. Furthermore, we demonstrate that, through the local field of a scanning tunneling microscope tip, it is possible to successively charge the defects by single electrons, suggested by both the ring structures and charging peaks in dI/dV measurements. Our results provide new insights into the quantum nature of these defect-bound states, as well as the possibility of using their single-electron behavior and response for applications in quantum information and local-field sensing.

2D semiconductor↗
DOE OSTI2022

Predicting defects in laser powder bed fusion using in-situ thermal imaging data and machine learning

Variation in the local thermal history during the Laser Powder Bed Fusion (LPBF) process in Additive Manufacturing (AM) can cause micropore defects, which add to the uncertainty of the mechanical properties (e.g., fatigue life, tensile strength) of the built materials. In-situ sensing has been proposed for monitoring the AM process to minimize defects, but successful minimization requires establishing a quantitative relationship between the sensing data and the porosity, which is particularly challenging with a large number of variables (e.g., laser speed, power, scan path, powder property). Physics-based modeling can simulate such an in-situ sensing-porosity relationship, but it is computationally costly. In this work, we develop Machine Learning (ML) models that can use in-situ thermographic data to predict the micropore of LPBF stainless steel materials. This work considers two identified key features from the thermal histories: the time above the apparent melting threshold ($\tau$) and the maximum radiance ( T max ). These features are computed, stored for each voxel in the built material, and then used as inputs. The binary state of each voxel, either defective or normal, is the output. Different ML models are trained and tested for the binary classification task. In addition to using the thermal features of each voxel to predict its own state, the thermal features of neighboring voxels are also included as inputs. This is shown to improve the prediction accuracy, which is consistent with thermal transport physics around each voxel contributing to its final state. Among the models trained, the F1 scores on test sets reach above 0.96 for Random Forests. Feature importance analysis based on the ML models shows that T max is more important to the voxel state than $\tau$ . The analysis also finds that the thermal history of the voxels above the present voxel is more influential than those beneath it. Our study significantly extends the capability of using in-situ thermographic data to predict porosity in LPBF materials. Finally, since ML models are fast, they may play integral roles in the optimization and control of such AM technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Defect annihilation in heavy ion irradiated polycrystalline gold

In this study, we explore the interaction of electron wind force (EWF) with defects originating from ion irradiation in-situ inside a transmission electron microscope. Nanocrystalline gold specimens were self-ion irradiated to a dose of 5 × 10 15 ions/cm 2 (45 displacement per atom) to generate a high density of displacement damage. We also developed a molecular dynamics simulation model to understand the associated atomic scale mechanisms. Both experiments and simulations show that the EWF can impart significant defect mobility even at low temperatures, resulting in the migration and elimination of defects in a few minutes. Overall, we propose that the EWF interacts with defects to create highly glissile Shockley partial dislocations, which makes the fast and low temperature defect annihilation possible.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Ultrafast Electron Trapping and Defect-Mediated Recombination in NiO Probed by Femtosecond Extreme Ultraviolet Reflection–Absorption Spectroscopy

Understanding the chemical nature of defect sites as well as the mechanism of defect-mediated recombination is critical for the rational design of energy conversion materials with improved efficiency. Using femtosecond extreme ultraviolet (XUV) spectroscopy in conjunction with X-ray photoelectron spectroscopy (XPS), we present results on the ultrafast electron dynamics in NiO prepared with varying concentrations of defect states. We find that oxygen vacancy defects do not serve as the primary recombination center, but rather the recombination rate scales linearly with the density of Ni metal defects. This suggests that grain boundaries between Ni metal and NiO are responsible for fast carrier recombination in partially reduced NiO. Here, our kinetic model shows that the photoexcited electrons self-trap via small polaron formation on the subpicosecond time scale. Additionally, we estimate an absolute measurement of small polaron formation rates, direct versus defect-mediated recombination rates, and the small polaron diffusion coefficient in NiO. This study provides important parameters for engineering NiO based materials for solar energy harvesting applications.

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

Modeling shock-induced void collapse in single-crystal Ta systems at the mesoscales

Understanding the role of microstructural heterogeneities on the shock wave propagation and defect evolution behavior is essential to predicting the dynamic response of metals. Heterogeneities, such as voids, provide challenges to understanding the wave propagation behavior as the shock-void interaction can collapse the void and result in large plastic strains and significant heating (hot spot formation) in the metal. Accurate modeling of this phenomenon requires predicting the void collapse mechanisms and the related heat generation and dissipation mechanisms (hotspot formation) that determine the microstructure evolution. While molecular dynamics (MD) simulations can model the void collapse behavior, the time/length scale capabilities pose a challenge to connect with continuum models or the experimental scales. Here, this study presents the capability of the newly developed quasi-coarse-grained dynamics (QCGD) method that extends the MD simulations to larger system sizes and longer times to model this phenomenon. This study uses QCGD simulations to investigate the mechanisms of shock wave interactions with pre-existing voids in single-crystal Ta microstructures for variations in shock pressures, void size, and loading orientations. For a given orientation, the plasticity contributions and rates of void collapse are observed to vary with shock pressures and void size. The larger void sizes and higher pressures result in increased temperatures (hot spots) and faster void collapse rates and unravel the variations in the plasticity contributions. In addition, QCGD simulations investigate the post-collapse microstructure evolution as a release wave travels through the hot spot region. The simulations reveal that the reduction in temperatures due to heat dissipation initiates the dynamic recrystallization behavior in the hotspot regions.

36 MATERIALS SCIENCE↗