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At least 1,567 records · Page 87
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Atom-at-a-Time Radioactive Molecule Identification: Looking toward Studies of Superheavy Elements

The chemical behavior of superheavy elements (SHEs, Z > 103) remains poorly understood. Their chemical properties are expected to deviate from established trends, challenging the predictive power of the periodic table. To investigate these elements experimentally, they must first be synthesized through nuclear reactions and then quickly subjected to chemical studies before they decay. Given the low production rates of these reactions and the need for measurements on an atom-at-a-time basis, innovative techniques are needed. Here, to address these challenges, a novel gas-phase chemistry method has been developed at Lawrence Berkeley National Laboratory, utilizing the Berkeley Gas-filled Separator and FIONA. This technique enables the production, identification, and study of molecular species formed by SHEs. As a proof of concept, we present measurements on the formation and identification of 151,152 HoO + molecules, demonstrating the capability to study the production of radioactive molecules under controlled conditions and directly identify them via their mass-to-charge ratio. These measurements validate the effectiveness of this technique for low-statistics SHE studies, highlighting the potential of this approach to ignite the next generation of experimental SHE chemistry research, offering a path to re-evaluate SHE placement on the periodic table.

Chemistry↗
DOE OSTI2019

Atom Probe Tomography for understanding microstructural and chemical changes in nuclear materials

Atom Probe Tomography (APT) is routinely employed to determine 3D microstructure and chemistry changes in structural materials used in reactor to understand irradiation effect. These findings help to correlate changes to mechanical and physical properties of nuclear materials which are subjected to extreme reactor conditions. With safety and economics of a reactor in mind, it is essential to be able to predict the changes in the fuel composition and microstructure as a function of burnup. Also, there is current need to develop advanced fuels with improved properties and performance which requires the experimental data on changes in microstructure, physical and chemical properties after irradiation for feedback process. A novel approach is presented to determine the local burnup in irradiated fuels using isotopic quantification obtained by Atom Probe Tomography (APT). Considering the volume of sample used (<100?µm3) for APT experiments using the lift-out process in a scanning electron microscope equipped with a Focused Ion Beam (FIB), the presented method determines the local burnup from a nuclear fuel, where a minimal amount of waste is produced. In this work, three samples were analyzed with different burnup conditions to quantify the isotopes of 235U, 236U, and 238U for burnup calculation in the irradiated metallic U–7Mo dispersion fuel. The calculated values were found in excellent agreement with MCNP calculations. With regard to structural materials, one of the primary factors limiting the utilization of fuel rods of Zr alloys is hydrogen pick up during oxidation. Past experimental studies have shown that the hydrogen pickup in Zirconium alloys is influenced by the alloy composition as well by irradiation temperature and neutron dose. Oftentimes, it is not feasible to carry out comprehensive studies on understanding the microstructural evolution in neutron irradiated materials since in reactor irradiation programs are extremely costly, lengthy and logistically complicated. The use of ion irradiation as a substitute has grown in recent years for several reasons including less radioactivity, faster irradiations and lower costs. In the framework of the MUZIC 3 project, samples of Zircaloy-4 have been proton and Zr2+ irradiated at the Michigan Ion Beam Lab (MIBL) facility with aim to create a microstructure that is similar to that observed after in-reactor service. The temperature of the environment is adjusted to compensate for the higher dose rate, as has been done previously. As a first step in this project the irradiated microstructures have been characterized using Transmission Electron Microscopy and Atom Probe Tomography to elucidate the microstructural changes, including precipitate amorphization and dissolution and the formation of dislocation loops. This presentation plans to highlight initial finding of this project.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Unraveling the individual influences of supports and ionic liquid coatings on the catalytic properties of supported iridium complexes and iridium clusters

In this work, supported iridium complexes were synthesized by the reaction of Ir(CO) 2 (acac) (acac = acetylacetonato) with SiO 2 , γ-Al 2 O 3 , and MgO. Extended X-ray absorption fine structure (EXAFS) and infrared (IR) spectra demonstrate that the iridium was present as atomically dispersed species anchored to each support. The samples were treated in flowing H 2 at 673 K to form supported iridium clusters. EXAFS spectra and high-angle annular dark-field scanning transmission electron microscopy images demonstrate that the average diameter of the iridium clusters on each support was approximately 1.2 nm. Furthermore, the catalysts before and after cluster formation were coated with each of a family of 1,3-dialkylimidazolium ionic liquids (ILs) having varying electron-donor tendencies probed by their υ(C2H) frequencies determined by IR spectroscopy. The coated and uncoated samples were tested as catalysts for partial hydrogenation of 1,3-butadiene in a flow reactor at 333 K, with turnover frequencies determined from differential conversions. The individual influences of the IL coatings and supports on the catalyst performance were found to depend strongly on whether the iridium was site-isolated complexes or present in clusters. The IL coatings as ligands exerted dominant effects on the clusters as catalysts, whereas the supports exerted dominant effects on the isolated iridium atoms. The results indicate how to tune the effects of metal nuclearity, IL coatings, and supports on the electronic environments and catalytic properties of the metals.

1,3-Butadiene hydrogenation↗
DOE OSTI2021

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

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

36 MATERIALS SCIENCE↗
NASA NTRS2002

Durability of Solar Selective Coatings in a Simulated Space Environment

Solar selective coatings are being considered for heat engine and thermal switching applications on minisatellites. Such coatings must have the combined properties of high solar absorptance and low infrared emittance. High solar absorptance is needed to collect solar energy as efficiently as possible while low infrared emittance is needed to minimize radiant energy loss at operating temperature. These properties are achieved in sputter deposited thin films through the use of molecular mixtures of metal and dielectric. Solar selective coatings having a solar absorptance to infrared emittance ratio of 9 have been successfully deposited using a mixture of nickel and aluminum oxide. The space environment, however, presents some challenges for the use of materials on the exterior of spacecraft, including durability to atomic oxygen and vacuum ultraviolet radiation. To address these concerns, several candidate solar selective coatings were exposed to atomic oxygen in a plasma asher and to ultraviolet radiation in a vacuum facility equipped with calibrated deuterium lamps. The optical properties of the coatings were monitored as a function of time to evaluate their performance over long term exposure to the simulated space environment. Several coatings were found to be durable to both the atomic oxygen and the vacuum ultraviolet environments.

Jaworske, Donald A.↗
DOE OSTI2025

Programmable simulations of molecules and materials with reconfigurable quantum processors

Simulations of quantum chemistry and quantum materials are believed to be among the most important applications of quantum information processors. However, realizing practical quantum advantage for such problems is challenging because of the prohibitive computational cost of programming typical problems into quantum hardware. Here we introduce a simulation framework for strongly correlated quantum systems represented by model spin Hamiltonians that uses reconfigurable qubit architectures to simulate real-time dynamics in a programmable way. Our approach also introduces an algorithm for extracting chemically relevant spectral properties via classical co-processing of quantum measurement results. We develop a digital–analogue simulation toolbox for efficient Hamiltonian time evolution using digital Floquet engineering and hardware-optimized multi-qubit operations to accurately realize complex spin–spin interactions. As an example, we propose an implementation based on Rydberg atom arrays. In addition, we show how detailed spectral information can be extracted from the dynamics through snapshot measurements and single-ancilla control, enabling the evaluation of excitation energies and finite-temperature susceptibilities from a single dataset. To illustrate the approach, we show how to use the method to compute key properties of a polynuclear transition-metal catalyst and two-dimensional magnetic materials.

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↗
NASA NTRS1999

Mars Environmental Compatibility Assessment (MECA): Identifying the Hazards of the Martian Soil

Sometime in the next decade NASA will decide whether to send a human expedition to explore the planet Mars. The Mars Environmental Compatibility Assessment (MECA) has been selected by NASA to evaluate the Martian environment for soil and dust hazards to human exploration. The integrated MECA payload contains three elements: a wet-chemistry laboratory, a microscopy station, and enhancements to a lander robot-arm system incorporating arrays of material patches and an electrometer to identify triboelectric charging during soil excavation. The wet-chemistry laboratory will evaluate samples of Martian soil in water to determine the total dissolved solids, redox potential, pH, and quantify the concentration of many soluble ions using ion-selective electrodes. These electrodes can detect potentially dangerous heavy-metal ions, emitted pathogenic gases, and the soil's corrosive potential. MECA's microscopy station combines optical and atomic-force microscopy with a robot-arm camera to provide imaging over nine orders of magnitude, from meters to nanometers. Soil particle properties including size, shape, color, hardness, adhesive potential (electrostatic and magnetic), will be determined on the microscope stage using an ar-ray of sample receptacles and collection substrates, and an abrasion tool,. The simple, rugged atomic-force microscope will image in the submicron size range and has the capability of performing a particle-by-particle analysis of the dust and soil. Although selected by NASA's Human Exploration and Development of Space Enterprise, the MECA instrument suite also has the capability to address basic geology, paleoclimate, and exobiology issues. To understand both contemporaneous and ancient processes on Mars, the mineralogical, petrological, and reactivity of Martian surface materials should be constrained: the NMCA experiment will shed light on these quantities through its combination of chemistry and microscopy. On Earth, the earliest forms of life are preserved as microfossils. The atomic-force microscope will have the required resolution to image down to the scale of terrestrial microfossils and beyond.

Meloy, T. P.↗
DOE OSTI2022

Optical and magneto-optical properties of ferromagnetic monolayer CrBr 3 : A first-principles G W and G W plus Bethe-Salpeter equation study

The discovery of atomically thin two-dimensional (2D) magnetic semiconductors has triggered enormous research interest recently. In this paper, we use first-principles many-body perturbation theory to study a prototypical 2D ferromagnetic semiconductor, monolayer chromium tribromide (CrBr 3 ). With broken time-reversal symmetry, spin-orbit coupling, and excitonic effects included through the full-spinor GW and GW plus Bethe-Salpeter equation (GW-BSE) methods, we compute the frequency-dependent layer polarizability tensor and dielectric function tensor that govern the optical and magneto-optical (MO) properties. In addition, we provide a detailed theoretical formalism for simulating magnetic circular dichroism, MO Kerr effect, and Faraday effect, demonstrating the approach with monolayer CrBr 3 . Due to reduced dielectric screening in 2D and the localized nature of the Cr d orbitals, we find strong self-energy effects on the quasiparticle band structure of monolayer CrBr 3 that give a 3.8 eV indirect bandgap. Also, excitonic effects dominate the low-energy optical and MO responses in monolayer CrBr 3 where a large exciton binding energy of 2.3 eV is found for the lowest bright exciton state with excitation energy at 1.5 eV. We further find that the MO signals demonstrate strong dependence on the excitation frequency and substrate refractive index. Furthermore, our theoretical framework for modeling optical and MO effects could serve as a powerful theoretical tool for future study of optoelectronic and spintronics devices consisting of van der Waals 2D magnets.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Modeling Liquid Water by Climbing up Jacob’s Ladder in Density Functional Theory Facilitated by Using Deep Neural Network Potentials

Within the framework of Kohn–Sham density functional theory (DFT), the ability to provide good predictions of water properties by employing a strongly constrained and appropriately normed (SCAN) functional has been extensively demonstrated in recent years. Here, we further advance the modeling of water by building a more accurate model on the fourth rung of Jacob’s ladder with the hybrid functional, SCAN0. In particular, we carry out both classical and Feynman path-integral molecular dynamics calculations of water with the SCAN0 functional and the isobaric–isothermal ensemble. To generate the equilibrated structure of water, a deep neural network potential is trained from the atomic potential energy surface based on ab initio data obtained from SCAN0 DFT calculations. For the electronic properties of water, a separate deep neural network potential is trained by using the Deep Wannier method based on the maximally localized Wannier functions of the equilibrated trajectory at the SCAN0 level. The structural, dynamic, and electric properties of water were analyzed. The hydrogen-bond structures, density, infrared spectra, diffusion coefficients, and dielectric constants of water, in the electronic ground state, are computed by using a large simulation box and long simulation time. For the properties involving electronic excitations, we apply the GW approximation within many-body perturbation theory to calculate the quasiparticle density of states and bandgap of water. Compared to the SCAN functional, mixing exact exchange mitigates the self-interaction error in the meta-generalized-gradient approximation and further softens liquid water toward the experimental direction. For most of the water properties, the SCAN0 functional shows a systematic improvement over the SCAN functional. However, some important discrepancies remain. The H-bond network predicted by the SCAN0 functional is still slightly overstructured compared to the experimental results.

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

Formation and optical properties of indium nanoparticle arrays for deep-UV plasmonics

We utilize a combined computational-experimental approach to examine the influence of indium nanoparticle (NP) array distributions on deep-ultraviolet (UV) plasmon resonances. For photon energies < 5.7 eV, analysis of ellipsometric spectra reveals an increase in silicon reflectance induced by indium NP arrays on silicon. For various energies in the range 5.7–7.0 eV, a decrease in reflectance is induced by the NP arrays. Similar trends in reflectance are predicted from finite-difference time-domain (FDTD) simulations using NP size distributions extracted from atomic-force micrographs as input. In addition, in the energy range of 7.4–9.2 eV, the FDTD simulations reveal reflectance minima, characteristic of localized surface plasmon resonances. Here, electron energy-loss spectroscopy collected from individual indium NPs reveals the presence of LSPR at ≈ 8 eV, further supporting the promise of indium NP arrays on silicon for deep-UV plasmonics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Stabilization of Dinuclear Rhodium and Iridium Clusters on Layered Titanate and Niobate Supports

Atomically dispersed organometallic clusters can provide well-defined nuclearity of active sites for both fundamental studies as well as new regimes of activity and selectivity in chemical transformations. More recently, dinuclear clusters adsorbed onto solid surfaces have shown novel catalytic properties resulting from the synergistic effect of two metal centers to anchor different reactant species. Difficulty in synthesizing, stabilizing, and characterizing isolated atoms and clusters without agglomeration challenges allocating catalytic performance to atomic structure. Here, we explore the stability of dinuclear rhodium and iridium clusters adsorbed onto layered titanate and niobate supports using molecular precursors. Both systems maintain their nuclearity when Statistical analysis of HAADF-STEM images revealed that rhodium and iridium dimers had mean cluster-to-cluster distances very similar to what is expected from a random distribution of atoms over a large area, indicating that they are dispersed without aggregation. The stability of dinuclear rhodium clusters supported on titanate nanosheets was also investigated by X-ray absorption fine structure (EXAFS), DRIFTS, and first-principles calculations. Both X-ray absorption spectroscopy and HAADF-STEM simulations, guided by density functional theory (DFT)-optimized structure models, suggested that rhodium dimers adsorb onto the nanosheets in an end-on binding mode that is stable up to 100 degrees C under reducing conditions. Finally, this study highlights that crystalline nanosheets derived from layered metal oxides can be used as model supports to selectively stabilize dinuclear clusters, which could have implications for heterogeneous catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1984

Electronic structure and properties of magnetic defects in Co(1+x)Al(1-x) and Fe(1+x)Al(1-x) alloys

CoAl and FeAl compounds are developed along two directions. Magnetic susceptibility and specific heat at low temperature on (NiCo)Al and (CoFe)Al ternary alloys are in good agreement with band calculations. Results on magnetization and specific heat under field at low temperature on nonstoichiometric compounds show clearly the importance of the nearest neighbor effects. In the case of CoAl, the isolated cobalt atoms substituting aluminum are characterized by a Kondo behavior, and, for FeAl, the isolated extra iron atoms are magnetic and polarize the matrix. Moreover, for the two compounds, clusters of higher order play a considerable part in the magnetic properties for CoAl, these clusters also seem to be characterized by a Kondo behavior, for FeAl, these clusters whose moment is higher than in the case of isolated atoms, could be constituted of excess parts of iron atoms.

Abbe, D.↗
DOE OSTI2024

Local atomic and magnetic structure of multiferroic (Sr,Ba)⁢(Mn,Ti)⁢O 3

Here, we present a detailed study of the local atomic and magnetic structure of the type-I multiferroic perovskite system (Sr,Ba)(Mn,Ti)O 3 using x-ray and neutron pair distribution function (PDF) analysis, polarized neutron scattering, and muon spin relaxation (μSR) techniques. The atomic PDF analysis reveals widespread nanoscale tetragonal distortions of the crystal structure even in the paraelectric phase with average cubic symmetry, corresponding to incipient ferroelectricity in the local structure. Magnetic PDF analysis, polarized neutron scattering, and μSR likewise confirm the presence of short-range antiferromagnetic correlations in the paramagnetic state, which grow in magnitude as the temperature approaches the magnetic transition. We show that these short-range magnetic correlations coincide with a reduction of the tetragonal (i.e., ferroelectric) distortion in the average structure, suggesting that short-range magnetism can play an important role in magnetoelectric and/or magnetostructural phenomena even without genuine long-range magnetic order. The reduction of the tetragonal distortion scales linearly with the local magnetic order parameter, pointing to spontaneous linear magnetoelectric coupling in this system. These findings provide greater insight into the multiferroic properties of (Sr,Ba)(Mn,Ti)O 3 and demonstrate the importance of investigating the local atomic and magnetic structure to gain a deeper understanding of the intertwined degrees of freedom in multiferroics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Fission gas diffusion and release for Cr 2 O 3 -doped UO 2 : From the atomic to the engineering scale

Here, the anticipated benefits of large grains in Cr 2 O 3 -doped UO 2 pellets include improved mechanical and fission gas retention properties. To support the assessment of fission gas release (FGR) from doped pellets, the impact of doping on fission gas diffusivity for in-reactor conditions must be understood. In this work, we tackle this issue by informing the fission gas model within the BISON fuel performance code using material models developed at the atomic scale. The investigation of intra-granular fission gas diffusivity in Cr 2 O 3 -doped UO 2 is carried out by adapting a cluster dynamics model that, accounting for UO 2 thermochemistry, is capable of describing Xe diffusion under irradiation in undoped UO 2 as the starting point. Using a thermodynamic analysis, it is shown that in stoichiometric UO 2 with additions of Cr 2 O 3 the oxygen potential is defined by the Cr-Cr 2 O 3 two-phase equilibrium. Using the cluster dynamics model, the predicted Xe diffusivity in doped UO 2 was significantly increased in both the intrinsic and irradiation-enhanced regimes compared to undoped UO 2 as a result of higher concentrations of uranium and oxygen vacancies, respectively. This is a consequence of the more oxidizing conditions at high temperature, and more reducing conditions at low temperature, as a result of doping. Arrhenius functions have been fitted to the cluster dynamics results to enable implementation of the new diffusivities in the BISON fission gas behavior model. BISON simulations were carried out, showing the competing effects of the enlarged grains and the new fission gas diffusivity model, which act to suppress and enhance fission gas release, respectively. The new physics-informed model was validated against in-reactor experimental measurements under normal operation. Additionally, benchmarking was carried out for power ramp conditions. The predicted fission gas release agreed well with the experimental data, showing noticeable improvements over the standard UO 2 model.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Single-ion magnetism in the extended solid-state: insights from X-ray absorption and emission spectroscopy

Large single-ion magnetic anisotropy is observed in lithium nitride doped with iron. The iron sites are two-coordinate, putting iron doped lithium nitride amongst a growing number of two coordinate transition metal single-ion magnets (SIMs). Uniquely, the relaxation times to magnetisation reversal are over two orders of magnitude longer in iron doped lithium nitride than other 3d-metal SIMs, and comparable with high-performance lanthanide-based SIMs. To understand the origin of these enhanced magnetic properties a detailed characterisation of electronic structure is presented. Access to dopant electronic structure calls for atomic specific techniques, hence a combination of detailed single-crystal X-ray absorption and emission spectroscopies are applied. Together K-edge, L 2,3 -edge and Kβ X-ray spectroscopies probe local geometry and electronic structure, identifying iron doped lithium nitride to be a prototype, solid-state SIM, clean of stoichiometric vacancies where Fe lattice sites are geometrically equivalent. Extended X-ray absorption fine structure and angular dependent single-crystal X-ray absorption near edge spectroscopy measurements determine Fe I dopant ions to be linearly coordinated, occupying a D 6h symmetry pocket. The dopant engages in strong 3dπ-bonding, resulting in an exceptionally short Fe–N bond length (1.873(7) Å) and rigorous linearity. It is proposed that this structure protects dopant sites from Renner–Teller vibronic coupling and pseudo Jahn–Teller distortions, enhancing magnetic properties with respect to molecular-based linear complexes. The Fe ligand field is quantified by L 2,3 -edge XAS from which the energy reduction of 3d z 2 due to strong 4s mixing is deduced. Quantification of magnetic anisotropy barriers in low concentration dopant sites is inhibited by many established methods, including far-infrared and neutron scattering. We deduce variable temperature L 3 -edge XAS can be applied to quantify the J = 7/2 magnetic anisotropy barrier, 34.80 meV (~280 cm –1 ), that corresponds with Orbach relaxation via the first excited, M J = ±5/2 doublet. The results demonstrate that dopant sites within solid-state host lattices could offer a viable alternative to rare-earth bulk magnets and high-performance SIMs, where the host matrix can be tailored to impose high symmetry and control lattice induced relaxation effects.

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

Atomically resolved edges and defects in lead halide perovskites

Although edges and defects constitute only a small fraction of crystalline materials, they exert an outsized impact on a material′s properties. Organic–inorganic halide perovskites are promising next-generation semiconductor materials with superior cost effectiveness and interesting optoelectronic properties. However, clear images of their edges have remained challenging to obtain owing to their extreme sensitivity. Using truly high-speed ultralow-dose four-dimensional scanning transmission electron microscopy with dose fractionation, we perform ptychography at, to our knowledge, the lowest-dose atomic resolution to date, revealing not only the detailed atomic structure of the edges of a halide perovskite but also their structural dynamics. Here, a majority methylammonium (MA) and iodine (I) edge termination is observed in methylammonium lead iodide (MAPbI 3 ), and the damage rate of its edges and internal defects is found to depend on the concentration and type of vacancies present, with a preponderance of I vacancies in particular correlating with higher rates of damage.

4D-STEM↗
DOE OSTI2022

Spin-orbit–driven ferromagnetism at half moiré filling in magic-angle twisted bilayer graphene

Strong electron correlation and spin-orbit coupling (SOC) can have a profound influence on the electronic properties of materials. We examined their combined influence on a two-dimensional electronic system at the atomic interface between magic-angle twisted bilayer graphene and a tungsten diselenide crystal. We found that strong electron correlation within the moiré flatband stabilizes correlated insulating states at both quarter and half filling, and that SOC transforms these Mott-like insulators into ferromagnets, as evidenced by a robust anomalous Hall effect with hysteretic switching behavior. The coupling between spin and valley degrees of freedom could be demonstrated through control of the magnetic order with an in-plane magnetic field or a perpendicular electric field. Our findings establish an experimental knob to engineer topological properties of moiré bands in twisted bilayer graphene and related systems.

36 MATERIALS SCIENCE↗