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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 55 records · Page 3

Multimodal Nanoscale Tomographic Imaging for Battery Electrodes

Accurate representations of the 3D structure within a lithium-ion battery are key to understanding performance limitations. However, obtaining exact reconstructions of electrodes, where the active particles, the carbon black and polymeric binder domain, and the pore space are visualized is challenging. In this work, it is shown that multimodal imaging can be used to overcome this challenge. High-resolution ptychographic X-ray computed tomography are combined with lower resolution but higher contrast transmission X-ray tomographic microscopy to obtain 3D reconstructions of pristine and cycled graphite-silicon composite electrodes. This cross-correlation enables quantitative analysis of the surface of active particles, including the heterogeneity of carbon-black and binder domain and solid-electrolyte interphase coverage. Capturing the active particles as well as the carbon black-binder domain allows using these segmented structures for electrochemical simulations to highlight the influence of the particle embedding on local state of charge heterogeneities.

25 ENERGY STORAGE↗

Field-Dependent Magnetic Domain Behavior in van der Waals Fe 3 GeTe 2

Two-dimensional magnetic van der Waals (vdW) materials can show a variety of topological nontrivial spin textures, such as Bloch- or Néel-type stripe, skyrmion, or bubble domains under certain external stimuli. It is critical to understand the magnetic domain behavior in vdW materials in order to control their size and density in response to external stimuli, such as electric and magnetic fields. In this study, we examine the magnetic field dependence of topologically non-trivial magnetization spin textures in vdW Fe 3 GeTe 2 . Néel-type stripe domains and skyrmions are formed depending on the magnetic field-cooling protocol used during in situ Lorentz transmission electron microscopy (LTEM) experiments. Use of quantitative reconstruction of magnetic induction maps and micromagnetic simulations allow for the understanding of the LTEM results of Néel-type stripe domains as well as skyrmions. In addition, the deformation of skyrmion contrast is observed as a result of the introduction of an in-plane magnetic field. We demonstrate the stability of the stripe domains and skyrmions in response to an externally applied magnetic field due to an energy barrier for domain wall annihilation. Our results establish an understanding of the energy landscape that governs the behavior of the topologically non-trivial spin textures in vdW materials which can be harnessed for spintronic applications.

36 MATERIALS SCIENCE↗

Bidentate Ligand-Induced Oriented Transformation of CsPbBr 3 Perovskite Nanocrystals into Nanowires for X-ray Photodetectors

We report shape and dimensionality control by ligands is an efficient way to fabricate high-quality perovskite nanocrystals (NCs) with optoelectronic properties. Herein, to realize oriented transformations between different morphologies of CsPbBr 3 nanocrystals, we conceived of the use of defects and bidentate ligands to synergistically drive the reorientation of CsPbBr3nanocrystals into CsPbBr 3 nanowires (NWs). By employing aminocaproic acid as the bidentate ligand, CsPbBr 3 NWs were reconstructed from the CsPbBr 3 NCs (~7 nm) with 20-60 nm in width and several micrometers in length, as well as a 527 nm photoluminescence (PL) peak, 59% PL quantum yield, and 98.5 ns PL lifetime. The bidentate ligand-directed anisotropic shape evolution and growth of perovskite NWs from NCs was elucidated by transmission electronmicroscopy and PL studies. The photodetectors fabricated with the reconstructed CsPbBr 3 NWs displayed a photocurrent enhancement (2.75 × 10 -11 A) compared with that of the devices based on solution-synthesized NWs (2.28 × 10 -11 A). The device also showed a short response time, indicating its more sensitive photoelectric response. This process provides a viable approach to engineering diverse morphologies of perovskite nanocrystals for optoelectronic applications.

36 MATERIALS SCIENCE↗

The interplay between surface facet and reconstruction on isopropanol conversion over SrTiO 3 nanocrystals

Strontium titanate (SrTiO 3 ) is an extensively investigated perovskite for various applications due to its optical, electrical and chemical properties. To gain an in-depth understanding of the active sites involved in heterogeneous catalysis over the broadly used SrTiO 3 (STO), we studied a model reaction, isopropanol conversion, on three differently shape-controlled nanocrystals: cube, truncated cube and dodecahedra. SEM, XRD and XPS confirmed the morphology, phase and composition of STO shapes. Low energy ion scattering (LEIS) revealed the occurrence of surface reconstruction over STO shapes during O 2 pretreatment at different temperatures. Based on the catalytic activities, scanning transmission electron microscopy images and density functional theory calculations, the step sites on STO derived from surface reconstruction were proposed to be the active sites for isopropanol conversion. This was further confirmed by steady state isotopic kinetic analysis (SSITKA) which demonstrated similar intrinsic turnover frequencies (TOFs) for the differently reconstructed STO shapes. It is concluded that the crystal facets impose an indirect effect on the catalysis of STO via controlling the degrees of surface reconstruction: the less stable STO (1 1 0) facet (dodecahedra) leads to more step sites after reconstruction and hence higher overall reaction rate than the more stable (1 0 0) facet (cube). This work highlights the important interplay between the crystal facet and surface reconstruction in controlling the nature and density of active sties and thus catalysis over complex oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Are suspensory ligaments important for middle ear reconstruction?

As the resolution of 3D printing techniques improves, the possibility of individualized, 3-ossicle constructions adds a new dimension to middle ear prostheses. In order to optimize these designs, it is essential to understand how the ossicles and ligaments work together to transmit sound, and thus how ligaments should be replicated in a middle ear reconstruction. The middle ear ligaments are thought to play a significant role in maintaining the position of the ossicles and constraining axis of rotation. Paradoxically, investigations of the role of ligaments to date have shown very little impact on middle ear sound transmission. We explored the role of the two attachments in the gerbil middle ear analogous to human ligaments, the posterior incudal ligament and the anterior mallear process, severing both attachments and measuring change in hearing sensitivity. The impact of severing the attachments on the position of the ossicular chain was visualized using synchrotron microtomography imaging of the middle ear. In contrast to previous studies, a threshold change on the order of 20 dB across a wide range of frequencies was found when both ligaments were severed. Concomitantly, a shift in position of the ossicles was observed from the x-ray imaging and 3D renderings of the ossicular chain. These findings contrast with previous studies, demonstrating that these ligaments play a significant role in the transmission of sound through the middle ear. It appears that both mallear and incudal ligaments must be severed in order to impair sound transmission. The results of this study have significance for middle ear reconstructive surgery and the design of 3D-printed three-ossicle biocompatible prostheses.

3D printing↗

Semi-Automated, Object-Based Tomography of Dislocation Structures

The characterization of the three-dimensional arrangement of dislocations is important for many analyses in materials science. Dislocation tomography in transmission electron microscopy is conventionally accomplished through intensity-based reconstruction algorithms. Although such methods work successfully, a disadvantage is that they require many images to be collected over a large tilt range. Here, we present an alternative, semi-automated object-based approach that reduces the data collection requirements by drawing on the prior knowledge that dislocations are line objects. Our approach consists of three steps: (1) initial extraction of dislocation line objects from the individual frames, (2) alignment and matching of these objects across the frames in the tilt series, and (3) tomographic reconstruction to determine the full three-dimensional configuration of the dislocations. Drawing on innovations in graph theory, we employ a node-line segment representation for the dislocation lines and a novel arc-length mapping scheme to relate the dislocations to each other across the images in the tilt series. We demonstrate the method for a dataset collected from a dislocation network imaged by diffraction-contrast scanning transmission electron microscopy. Based on these results and a detailed uncertainty analysis for the algorithm, we discuss opportunities for optimizing data collection and further automating the method.

47 OTHER INSTRUMENTATION↗

Ultrafast optical modulation of vibrational strong coupling in ReCl(CO) 3 (2,2-bipyridine)

Polaritons – hybrid light-matter states formed from the strong coupling of a bright molecular transition with a confined photonic mode – may offer new opportunities for optical control of molecular behavior. Vibrational strong coupling (VSC) has been reported to impact ground-state chemical reactivity, but its influence on electronic excited-state dynamics remains unexplored. Here, we take a first step towards excited-state VSC by demonstrating optical modulation of the ReCl(CO) 3 (bpy), (bpy = 2,2-bipyridine) complex under VSC using femtosecond ultraviolet (UV)-pump/infrared (IR)-probe spectroscopy. We establish ground-state VSC of ReCl(CO) 3 (bpy) in a microfluidic Fabry-Pérot cavity equipped with indium tin oxide (ITO)-coated mirrors. ITO is effectively dichroic as it is reflective in the IR and transmissive in the UV-visible and therefore minimizes optical interference. Excitation with UV pump light drives ReCl(CO) 3 (bpy) into a manifold of electronic excited states that subsequently undergo non-radiative relaxation dynamics. We probe the transient response of the strongly-coupled system in the mid-IR, observing both Rabi contraction and cavity-filtered excited-state absorption signatures. We reconstruct the intrinsic response of intracavity molecules from the transient cavity transmission spectra to enable quantitative comparison with extracavity control experiments. We report no changes in the excited-state dynamics of ReCl(CO) 3 (bpy) under ground-state VSC. However, we do observe significant amplification of transient vibrational signals due to classical cavity-enhanced optical effects. This effort lays the groundwork to pursue direct excited-state VSC aimed at modulating photochemical reactivity.

cavity-enhanced spectroscopy↗

Machine learning enables reconstruction of past fire regimes from charcoal-derived fire intensity and fuel composition

Background Fire is a foundational ecological process that shapes ecosystem structure, diversity, and resilience. Quantifying paleofire regime attributes such as frequency, severity, and intensity is essential for understanding the historical range of variability in fire behavior and its ecological effects. While frequency and severity are often reconstructed in paleofire studies, quantitative reconstructions of fire intensity remain limited. Recent work has shown that maximum pyrolysis temperature—a proxy for fire intensity—and plant species type can be inferred from charcoal using transmission Fourier-transform infrared (FTIR) spectroscopy. However, the sample preparation for transmission FTIR is destructive and time-consuming, limiting application and reuse of materials for other analyses. We evaluated reflectance FTIR spectroscopy as a non-destructive alternative for reconstructing combustion temperature and plant species from laboratory-generated charcoal. We also examined the influence of contrasting airflow environments (ambient air versus nitrogen-rich) on pyrolysis temperature and plant species reconstruction prediction accuracies and compared predictive performance between a novel, neural network–based deep learning model with the traditional modern analogue technique (MAT) using k-nearest neighbor functions. As proof of concept, we apply our enhanced methodology to ancient charcoal to demonstrate applicability at improving long-term fire regime reconstructions and the ability to link paleofire records with contemporary fire ecology. Results Our analysis shows that transmission and reflectance FTIR spectra yield comparable spectral profiles. However, sample preparation for reflectance FTIR is minimal and non-destructive, unlike transmission FTIR which is destructive. We demonstrate that oxygen environments improved reconstruction accuracy relative to nitrogen-rich conditions. Finally, our deep learning neural network (DL) achieved testing accuracies of 98.7% for temperature and 96.2% for species identification, outperforming MAT’s k-NN approach (89.8% and 65.9%, respectively). A Shapley importance analysis identified 5 key spectral regions that greatly influenced the model’s temperature or species categorization. When applied to ancient charcoal, our results show historic fires from the most recent past primarily burned at low intensities (400–500 °C), reflective of natural fire regimes in ponderosa pine forests. Our results corroborate charcoal morphology data that suggests all ancient charcoal originated from burned woody plant types. Conclusions By combining reflectance FTIR spectroscopy with a deep learning approach, we provide the first accuracies high enough to confidently identify both species and temperature from laboratory-produced charcoal, improving quantitative reconstructions of fire intensity and fuel composition from paleofire records. This opens a wide range of research into the link between fire and larger drivers (i.e., climate or human) and greater ecological understanding of fire regimes beyond that of burn scars or recent observations. These methodological improvements have direct relevance for fire management by improving interpretation of historical fire behavior, informing fuel–fire relationships, and providing a scalable analytical framework applicable to both long-term ecological studies and contemporary fire science.

54 ENVIRONMENTAL SCIENCES↗

Rotational and dilational reconstruction in transition metal dichalcogenide moiré bilayers

Abstract Lattice reconstruction and corresponding strain accumulation plays a key role in defining the electronic structure of two-dimensional moiré superlattices, including those of transition metal dichalcogenides (TMDs). Imaging of TMD moirés has so far provided a qualitative understanding of this relaxation process in terms of interlayer stacking energy, while models of the underlying deformation mechanisms have relied on simulations. Here, we use interferometric four-dimensional scanning transmission electron microscopy to quantitatively map the mechanical deformations through which reconstruction occurs in small-angle twisted bilayer MoS 2 and WSe 2 /MoS 2 heterobilayers. We provide direct evidence that local rotations govern relaxation for twisted homobilayers, while local dilations are prominent in heterobilayers possessing a sufficiently large lattice mismatch. Encapsulation of the moiré layers in hBN further localizes and enhances these in-plane reconstruction pathways by suppressing out-of-plane corrugation. We also find that extrinsic uniaxial heterostrain, which introduces a lattice constant difference in twisted homobilayers, leads to accumulation and redistribution of reconstruction strain, demonstrating another route to modify the moiré potential.

74 ATOMIC AND MOLECULAR PHYSICS↗

Oscillatory redox behavior in oxides: Cyclic surface reconstruction and reactivity modulation via the Mars–van Krevelen mechanism

The breaking of translational symmetry at oxide surfaces gives rise to coordinatively unsaturated cations/anions and surface restructuring—key factors that govern surface reactivity. Using direct in situ environmental transmission electron microscopy (TEM) observations along with atomistic modeling, we report oscillatory redox behavior in CuO under H 2 , where cyclic surface reconstruction and reactivity modulation occur via the Mars–van Krevelen (MvK) mechanism. We observe self-switching between oxygen-rich and oxygen-deficient surface reconstructions, alternately activating and deactivating the surface for H 2 O formation. During periods of chemical inactivity, the oxygen-deficient surface undergoes slow reoxidation via lattice oxygen diffusing from subsurface and bulk reservoirs, restoring the active oxygen-rich surface termination. The inherent disparity in chemical activity among undercoordinated surface ions, along with sluggish subsurface-to-surface oxygen replenishment, drives this oscillatory redox cycle, modulating H2-induced loss of lattice oxygen at the surface and its delayed replenishment from the subsurface. This creates spatiotemporally separated redox steps at the oxide surface. The phenomena and atomistic insights presented here have significant implications for manipulating the surface reactivity of oxides by tuning the separation of these redox steps.

36 MATERIALS SCIENCE↗

Machine‐Learning‐Driven Exploration of Surface Reconstructions of Reduced Rutile TiO 2

Titanium dioxide (TiO 2 ) is widely used as a catalyst support due to its stability, tunable electronic properties, and surface oxygen vacancies, which are crucial for catalytic processes such as the reverse water-gas shift (RWGS) reaction. Reduced TiO 2 surfaces undergo complex surface reconstructions that endow unique properties but are computationally challenging to describe. In this study, we utilize machine-learning interatomic potentials (MLIPs) integrated with an active-learning workflow to efficiently explore reduced rutile TiO 2 surfaces. This approach enabled the prediction of a phase diagram as a function of oxygen chemical potential, revealing a variety of reconstructed phases, including a previously unreported subsurface shear plane structure. We further investigate the electronic properties of these surfaces and validate our results by comparing experimental and theoretical high-resolution transmission electron microscopy (HRTEM). Our findings provide new insights into how extreme surface reductions influence the structural and electronic properties of TiO 2 , with potential implications for catalyst design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cu–Ni Oxidation Mechanism Unveiled: A Machine Learning-Accelerated First-Principles and in Situ TEM Study

Here, the development of accurate methods for determining how alloy surfaces spontaneously restructure under reactive and corrosive environments is a key, long-standing, grand challenge in materials science. Using machine learning-accelerated density functional theory and rare-event methods, in conjunction with in situ environmental transmission electron microscopy (ETEM), we examine the interplay between surface reconstructions and preferential segregation tendencies of CuNi(100) surfaces under oxidation conditions. Our modeling approach predicts that oxygen-induced Ni segregation in CuNi alloys favors Cu(100)-O c(2 × 2) reconstruction and destabilizes the Cu(100)-O (2√2 × √2)R45° missing row reconstruction (MRR). In situ ETEM experiments validate these predictions and show Ni segregation followed by NiO nucleation and growth in regions without MRR, with secondary nucleation and growth of Cu 2 O in MRR regions. Our approach based on combining disparate computational components and in situ ETEM provides a holistic description of the oxidation mechanism in CuNi, which applies to other alloy systems.

36 MATERIALS SCIENCE↗

Visualizing defects and pore connectivity within metal–organic frameworks by X-ray transmission tomography

Metal–Organic Frameworks (MOFs) have the potential to change the landscape of molecular separations in chemical processes owing to their ability of selectively binding molecules. Their molecular sorting properties generally rely on the micro- and meso-pore structure, as well as on the presence of coordinatively unsaturated sites that interact with the different chemical species present in the feed. In this work, we show a first-of-its-kind tomographic imaging of the crystal morphology of a metal– organic framework by means of transmission X-ray microscopy (TXM), including a detailed data reconstruction and processing approach. Corroboration with Focused Ion Beam-Scanning Electron Microscopy (FIB-SEM) images shows the potential of this strategy for further (non-destructively) assessing the inner architecture of MOF crystals. By doing this, we have unraveled the presence of large voids in the internal structure of a MIL-47(V) crystal, which are typically thought of as rather homogeneous lattices. This challenges the established opinion that hydrothermal syntheses yield relatively defect-free material and sheds further light on the internal morphology of crystals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Multiple monoenergetic gamma radiography (MMGR) with a compact superconducting cyclotron

Smuggling of special nuclear materials and nuclear devices through borders and ports of entry constitutes a major risk to global security. Technologies are needed to reliably screen the flow of commerce for the presence of high-Z materials such as uranium and plutonium. Here, we present an experimental proof-of-concept of a technique that uses inelastic (p,p') nuclear reactions to generate monoenergetic photons, which provide means to measure the areal density and the effective-Z (Z eff ) of an object with an accuracy surpassing that achieved by current methods. We use an ION-12 SC superconducting 12 MeV proton cyclotron to produce 4.4, 6.1, 6.9, and 7.1 MeV photons from a variety of nuclear reactions. Using these photons in a transmission mode, we show that we are able to accurately reconstruct the areal densities and Zeff of a test object. This methodology could enable mobile applications to screen commercial cargoes with high material specificity, providing a means of distinguishing common cargo materials from high-Z materials that include uranium and plutonium.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Hyperspectral imaging of exciton confinement within a moiré unit cell with a subnanometer electron probe

Electronic and optical excitations in two-dimensional systems are distinctly sensitive to the presence of a moiré superlattice. Here we used cryogenic transmission electron microscopy and spectroscopy to simultaneously image the structural reconstruction and associated localization of the lowest-energy intralayer exciton in a rotationally aligned WS 2 -WSe 2 moiré superlattice. In conjunction with optical spectroscopy and ab initio calculations, we determined that the exciton center-of-mass wave function is confined to a radius of approximately 2 nanometers around the highest-energy stacking site in the moiré unit cell. Our results provide direct evidence that atomic reconstructions lead to the strongly confining moiré potentials and that engineering strain at the nanoscale will enable new types of excitonic lattices.

36 MATERIALS SCIENCE↗

Towards libraries of different ultrasmall amorphous silica cage topologies

Cage topology controlled at the nanometer length scale is expected to enable original functionalities, e.g., in catalysis and therapeutics. Cages are fundamental structural motifs of clathrates and their topological duals, Frank-Kasper phases, and are constituents of mesoporous silica frameworks. However, with one exception, they have not been synthesized as discrete particles. By varying reactant ratios of surfactant, oil, and silane, we report the discovery of 5(12)6(2) and 5(12)6(8) amorphous silica polyhedra, each coexisting with the previously identified 5(12) cage, using combined cryo-transmission electron microscopy (cryo-TEM) and single-particle reconstruction (SPR). Notably, the 5(12)6(8) polyhedron represents a topology not previously observed in mesoporous silica frameworks. Control over structural features is demonstrated, and insights into cage formation mechanisms are provided. Structural outcomes are summarized in a ternary morphology diagram alongside prior results, bridging serendipitous discovery and intentional design of silica cages displaying a level of control over silica polymerization rivaling nature.

Jang, Dong June [Department of Materials Science a↗

On-chip spectrometers using stratified waveguide filters

We present an ultra-compact single-shot spectrometer on silicon platform for sparse spectrum reconstruction. It consists of 32 stratified waveguide filters (SWFs) with diverse transmission spectra for sampling the unknown spectrum of the input signal and a specially designed ultra-compact structure for splitting the incident signal into those 32 filters with low power imbalance. Each SWF has a footprint less than 1 µm × 30,µm, while the 1 × 32 splitter and 32 filters in total occupy an area of about 35 µm × 260 µm, which to the best of our knowledge, is the smallest footprint spectrometer realized on silicon photonic platform. Experimental characteristics of the fabricated spectrometer demonstrate a broad operating bandwidth of 180 nm centered at 1550 nm and narrowband peaks with 0.45 nm Full-Width-Half-Maximum (FWHM) can be clearly resolved. This concept can also be implemented using other material platforms for operation in optical spectral bands of interest for various applications.

42 ENGINEERING↗

An algebraic convolution formulation for multiple-scattering correction in small-angle neutron scattering

Multiple scattering in small-angle neutron scattering (SANS) redistributes spectral weight and distorts structural interpretation, particularly for thick or strongly scattering samples. We develop a finite-dimensional spectral desmearing framework that corrects multiple scattering without resorting to integral transforms or model-dependent extrapolation. The primary intensity is expanded in an orthonormal basis adapted to the isotropic transverse-momentum measure, under which convolution reduces to a recursive tensor contraction, allowing the Poisson-weighted multiple-scattering series to be evaluated directly in a finite-dimensional basis representation. This formulation yields a stable forward–inverse mapping between apparent and primary spectra. Numerical tests demonstrate convergence under repeated convolution and accurate recovery of the single-scattering intensity. Application to SANS measurements collected at multiple neutron facilities, including the Spallation Neutron Source, the High Flux Isotope Reactor, and the Institut Laue-Langevin, shows the quantitative reconstruction of the underlying primary spectrum across a wide range of transmission conditions, including strongly attenuating samples. Here, the method provides a stable, model-agnostic framework for multiple-scattering correction in SANS and enables consistent structural interpretation across instruments and scattering regimes.

Tung, Chi-Huan [Oak Ridge National Laboratory (ORN↗