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The exit-wave power-cepstrum transform for scanning nanobeam electron diffraction: robust strain mapping at subnanometer resolution and subpicometer precision
Scanning nanobeam electron diffraction (NBED) with fast pixelated detectors is a valuable technique for rapid, spatially resolved mapping of lattice structure over a wide range of length scales. However, intensity variations caused by dynamical diffraction and sample mistilts can hinder the measurement of diffracted disk centers as necessary for quantification. Robust data processing techniques are needed to provide accurate and precise measurements for complex samples and non-ideal conditions. Here we present an approach to address these challenges using a transform, called the exit wave power cepstrum (EWPC), inspired by cepstral analysis in audio signal processing. The EWPC transforms NBED patterns into real-space patterns with sharp peaks corresponding to inter-atomic spacings. We describe a simple analytical model for interpretation of these patterns that cleanly decouples lattice information from the intensity variations in NBED patterns caused by tilt and thickness. With tracking the inter-atomic spacing peaks in EWPC patterns, strain mapping is demonstrated for two practical applications: mapping of ferroelectric domains in epitaxially strained PbTiO 3 films and mapping of strain profiles in arbitrarily oriented core-shell Pt-Co nanoparticle fuel-cell catalysts. The EWPC transform enables lattice structure measurement at sub-pm precision and sub-nm resolution that is robust to small sample mistilts and random orientations.
Direct observation of elemental fluctuation and oxygen octahedral distortion-dependent charge distribution in high entropy oxides
The enhanced compositional flexibility to incorporate multiple-principal cations in high entropy oxides (HEOs) offers the opportunity to expand boundaries for accessible compositions and unconventional properties in oxides. Attractive functionalities have been reported in some bulk HEOs, which are attributed to the long-range compositional homogeneity, lattice distortion, and local chemical bonding characteristics in materials. However, the intricate details of local composition fluctuation, metal-oxygen bond distortion and covalency are difficult to visualize experimentally, especially on the atomic scale. Here, we study the atomic structure-chemical bonding-property correlations in a series of perovskite-HEOs utilizing the recently developed four-dimensional scanning transmission electron microscopy techniques which enables to determine the structure, chemical bonding, electric field, and charge density on the atomic scale. The existence of compositional fluctuations along with significant composition-dependent distortion of metal-oxygen bonds is observed. Consequently, distinct variations of metal-oxygen bonding covalency are shown by the real-space charge-density distribution maps with sub-ångström resolution. The observed atomic features not only provide a realistic picture of the local physico-chemistry of chemically complex HEOs but can also be directly correlated to their distinctive magneto-electronic properties.
Correlating 3D Surface Atomic Structure and Catalytic Activities of Pt Nanocrystals
Active sites and catalytic activity of heterogeneous catalysts is determined by their surface atomic structures. However, probing the surface structure at an atomic resolution is difficult, especially for solution ensembles of catalytic nanocrystals, which consist of heterogeneous particles with irregular shapes and surfaces. In this study, we constructed 3D maps of the coordination number (CN) and generalized CN ($\bar{C}\bar{N}$) for individual surface atoms of sub-3 nm Pt nanocrystals. Our results reveal that the synthesized Pt nanocrystals are enclosed by islands of atoms with nonuniform shapes that lead to complex surface structures, including a high ratio of low-coordination surface atoms, reduced domain size of low-index facets, and various types of exposed high-index facets. 3D maps of $\bar{C}\bar{N}$ are directly correlated to catalytic activities assigned to individual surface atoms with distinct local coordination structures, which explains the origin of high catalytic performance of small Pt nanocrystals in important reactions such as oxygen reduction reactions and CO electro-oxidation.
Local Resistance Measurement for Degradation of c-Si Heterojunction with Intrinsic Thin Layer (HIT) Solar Modules
Silicon heterojunction with intrinsic thin layer (or HIT) modules typically degrade at a rate of less than 1% annually in solar fields with dominant degradation in open-circuit voltage and some degradation in series resistance. However, detailed mechanisms can differ from module to module. Here, we study increases in local series resistance that occur over long-term field deployment, indicated by cell areas where the photoluminescence intensity does not degrade but the electroluminescence degrades significantly. To directly measure the local series resistance, we have cored out the local electroluminescence-degraded area, and we measured the sheet resistance by 4-point-probe and local nm-scale resistance using scanning spreading resistance microscopy (SSRM). The results by 4-point-probe show scattered sheet resistance that can be caused, for example, by nonuniform current paths through the transparent conductive oxide layer, the a-Si:H emitter, or the near-junction c-Si inversion layer. In contrast, the SSRM results indicate a relatively uniform and non-degraded resistivity on smaller nanometer spatial scales. SSRM is an atomic force microscopy-based two-terminal resistance mapping technique that measures the local resistance in nm-volume beneath the probe. The consistent resistances measured on the control and degraded samples can exclude the degradation of transparent conductive oxide resistance.
Accelerated screening of functional atomic impurities in halide perovskites using high-throughput computations and machine learning
The pressing need for novel materials that can serve rising demands in solar cell and optoelectronic technologies makes the nexus of halide perovskites, high-throughput computations, and machine learning, very promising. Ever increasing amounts of data on the structure, fundamental properties, and device performance of halide perovskites provide opportunities for learning chemical rules and design principles that make these materials attractive, and applying them across wide chemical spaces. In this work, we show that impurity properties of halide perovskites computed using density functional theory (DFT) can be combined with machine learning (ML) to deliver predictive models and quick identification of optoelectronically active impurity atoms. Our computation lead to the largest reported dataset of the formation energies and charge transition levels of Pb-site impurities in methylammonium lead halide (MAPbX 3 ) perovskites. Descriptors are defined to uniquely represent any impurity atom in any MAPbX 3 compound and mapped to the computed impurity properties using regression techniques such as Gaussian process regression, neural networks, and random forests. We use the best optimized predictive models to make predictions for hundreds of impurities across 9 MAPbX 3 compounds and create lists of dominating impurities, that is, impurities that can shift the equilibrium Fermi level in the perovskite as determined by native point defects. Finally, this accelerated screening powered by computations and machine learning can guide the identification of problematic impurities that may cause undesired recombination of charge carriers, as well as impurities that can be deliberately introduced to tune the perovskite conductivity and resulting photovoltaic absorption.
Characterization of boundary precipitation in a heavy ion irradiated tungsten heavy alloy under the simulated fusion environment
In the concerted effort to identify materials capable of surviving the adverse environment of a fusion reactor interior, tungsten heavy alloys have been put forth as leading candidates. Experimental trials and behavioral studies have yielded positive results for their adoption by taking advantage of the alloy’s unique balance of inherently high fracture toughness and low sputter yields; yet due to their relative novelty in the fusion community, there remains a lack of understanding on the response of these materials to the extended high temperature irradiation environment of the reactor interior. Further, to alleviate this issue and provide the necessary data on the behavior of tungsten heavy alloys to the simulated fusion environment, a 90W-7Ni-3Fe alloy has been subjected to elevated temperature sequential Ni + and He + ion irradiations to mimic the expected displacement damage and gas production expected after five years of service as a plasma facing material component. Atomic-scale structural analyses and nanoscale chemical mapping have identified the formation of two distinct precipitation structures, a surface localized η-carbide and an a-W 2 C type tungsten carbide, both of which appear to originate at the bi-phase interface between W and the ductile phase. This irradiation assisted and induced precipitate formation respectively is anticipated to adversely affect these materials by selective embrittlement at bi-phase interfaces leading to a reduction in the material’s overall fracture toughness during prolonged high temperature irradiation. It is asserted that any potential exposure to C during fusion reactor operational service should be minimized as to prevent the formation of these phases.
On the Operando Structure of Ruthenium Oxides during the Oxygen Evolution Reaction in Acidic Media
In the search for rational design strategies for oxygen evolution reaction (OER) catalysts, linking the catalyst structure to activity and stability is key. However, highly active catalysts such as IrO x and RuO x undergo structural changes under OER conditions, and hence, structure–activity–stability relationships need to take into account the operando structure of the catalyst. Under the highly anodic conditions of the oxygen evolution reaction (OER), electrocatalysts are often converted into an active form. Here, we studied this activation for amorphous and crystalline ruthenium oxide using X-ray absorption spectroscopy (XAS) and electrochemical scanning electron microscopy (EC-SEM). We tracked the evolution of surface oxygen species in ruthenium oxides while in parallel mapping the oxidation state of the Ru atoms to draw a complete picture of the oxidation events that lead to the OER active structure. Our data show that a large fraction of the OH groups in the oxide are deprotonated under OER conditions, leading to a highly oxidized active material. The oxidation is centered not only on the Ru atoms but also on the oxygen lattice. This oxygen lattice activation is particularly strong for amorphous RuO x . We propose that this property is key for the high activity and low stability observed for amorphous ruthenium oxide.
Revealing the Hidden Third Dimension of Point Defects in Two-Dimensional MXenes
Point defects govern many important functional properties of two-dimensional (2D) materials. However, resolving the three-dimensional (3D) arrangement of these defects in multi-layer 2D materials remains a fundamental challenge, hindering rational defect engineering. Here, we overcome this limitation using an artificial intelligence-guided electron microscopy workflow to map the 3D topology and clustering of atomic vacancies in Ti3C2TX MXene. Our approach reconstructs the 3D coordinates of vacancies across hundreds of thousands of lattice sites, generating robust statistical insight into their distribution that can be correlated with specific synthesis pathways. This large-scale data enables us to classify a hierarchy of defect structures-from isolated vacancies to nanopores-revealing their preferred formation and interaction mechanisms, as corroborated by molecular dynamics simulations. This work provides a generalizable framework for understanding and ultimately controlling point defects across large volumes, paving the way for the rational design of defect-engineered functional 2D materials.
Mapping causal patterns in crystalline solids
The evolution of the atomic structures of the combinatorial library of Sm-substituted thin film BiFeO 3 along the phase transition boundary from the ferroelectric rhombohedral phase to the non-ferroelectric orthorhombic phase is explored using scanning transmission electron microscopy. Localized properties, including polarization, lattice parameter, and chemical composition, are parameterized from atomic-scale imaging, and their causal relationships are reconstructed using a linear non-Gaussian acyclic model. This approach is further extended to explore the spatial variability of the causal coupling using the sliding window transform method, which revealed that new causal relationships emerged at both the expected locations, such as domain walls and interfaces, and at additional regions forming clusters in the vicinity of the walls or spatially distributed features. While the exact physical origins of these relationships are unclear, they likely represent nanophase-separated regions in the morphotropic phase boundaries. Overall, we posit that an in-depth understanding of complex disordered materials away from thermodynamic equilibrium necessitates understanding not only the generative processes that can lead to observed microscopic states but also the causal links between multiple interacting subsystems.
Evidence for Ga clusters in β-Ga 2 O 3 from Raman spectroscopy and density functional theory
Monoclinic gallium oxide (β-Ga 2 O 3 ) single crystals have a Raman mode at ∼250 cm −1 that is strongly correlated with free-electron density. Prior work attributed this peak to an electronic excitation of a shallow donor impurity band. However, heavily n-type thin films grown by metalorganic chemical vapor deposition or molecular beam epitaxy do not have the peak. In the present work, an alternate model is proposed: the 250 cm −1 Raman peak arises from Ga clusters, defined as two or more Ga atoms that form Ga–Ga bonds. Raman mapping reveals variations in the frequency that are consistent with a distribution of cluster sizes. The intensity of the peak decreases as the temperature is raised, attributed to melting of the Ga clusters. First-principles calculations indicate that the 250 cm −1 mode is due to Ga–Ga bond-stretching vibrations. As the Fermi energy is raised, the formation of Ga–Ga dimers becomes energetically favorable, explaining the correlation between n-type conductivity and the appearance of the Raman peak.
Multiband superconductivity in strongly hybridized 1 T ' - WTe 2 / NbSe 2 heterostructures
The interplay of topology and superconductivity has become a subject of intense research in condensed-matter physics for the pursuit of topologically nontrivial forms of superconducting pairing. An intrinsically normal-conducting material can inherit superconductivity via electrical contact to a parent superconductor via the proximity effect, usually understood as Andreev reflection at the interface between the distinct electronic structures of two separate conductors. However, at high interface transparency, strong coupling inevitably leads to changes in the band structure, locally, owing to hybridization of electronic states. Here, we investigate such strongly proximity-coupled heterostructures of monolayer $1T$' - $\mathrm{WTe_2}$ grown on NbSe 2 by van der Waals epitaxy. The superconducting local density of states, resolved in scanning tunneling spectroscopy down to 500 mK, reflects a hybrid electronic structure well described by a multiband framework based on the McMillan equations which captures the multiband superconductivity inherent to the NbSe 2 substrate and that is induced by proximity to $\mathrm{WTe_2}$ self-consistently. Our material-specific tight-binding model captures the hybridized heterostructure quantitatively and confirms that strong interlayer hopping gives rise to a semimetallic density of states in the two-dimensional $\mathrm{WTe_2}$ bulk, even for nominally band-insulating crystals. The model further accurately predicts the measured order parameter Δ ≅ 0.6 meV induced in the $\mathrm{WTe_2}$ monolayer bulk, stable beyond a 2 T magnetic field. So we believe that our detailed multiband analysis of the hybrid electronic structure provides a useful tool for sensitive spatial mapping of induced order parameters in proximitized atomically thin topological materials.
Quantum optical memory for entanglement distribution
Optical photons are powerful carriers of quantum information, which can be delivered in free space by satellites or in fibers on the ground over long distances. Entanglement of quantum states over long distances can empower quantum computing, quantum communications, and quantum sensing. Quantum optical memories are devices designed to store quantum information in the form of stationary excitations, such as atomic coherence, and are capable of coherently mapping these excitations to flying qubits. Quantum memories can effectively store and manipulate quantum states, making them indispensable elements in future long-distance quantum networks. Over the past two decades, quantum optical memories with high fidelities, high efficiencies, long storage times, and promising multiplexing capabilities have been developed, especially at the single-photon level. In this review, we introduce the working principles of commonly used quantum memory protocols and summarize the recent advances in quantum memory demonstrations. We also offer a vision for future quantum optical memory devices that may enable entanglement distribution over long distances.
Solar wind latitude variations and multiple scattering from Galileo interplanetary Lyman-alpha observations
The Galileo Ultraviolet Spectrometer Experiment (UVS) obtained a map of the celestial sphere from interplanetary Lyman-alpha (IPLA) on 13, 14 December 1990 during the Earth1 encounter. The Galileo spacecraft was near the downwind interstellar axis during the encounter and the map view directions filled the downwind hemisphere. The ratio between the observation and a single scattering model is attributed to a direct measurement of the multiple scattering correction required to model IPLA in the inner solar system. Analysis of this data set, referred to as an antisun map, shows that the solar wind charge exchange rate with interplanetary gas is 25 percent less over the solar poles than in the ecliptic at solar maximum. A model of the interstellar wind based on the antisun map observation exhibits a number density of atomic hydrogen far from the solar system, inside the heliosphere, of 0.16 +/- 0.05/cu cm.
Atomic oxygen between 80 and 120 km - Evidence for a latitudinal variation in vertical transport near the mesopause
Analysis of the OGO 6 OI green line nightglow photometer experiment has been carried out for eight cases when the alignment of the spacecraft was such that local emission rates could be determined below the altitude of maximum emission and down to about 80 km. The results obtained show that the vertical gradient of the emission rate between 95 and 80 km alternates between regions of very rapid variation and very slow variation spaced on a scale of 5-10 deg of latitude. Maps showing isoemissivity contours and isodensity contours for atomic oxygen concentration in vertical meridional planes are presented. The densities are computed under three assumptions concerning excitation mechanisms. Comparisons of the vertical variations of oxygen density with the results of a time dependent theory suggest the regions of strong downward transport alternate in latitude with regions of weak transport near 90 km. In the first case, conversion of O to O3 at night appears to be overwhelmed by downward transport of O.
The global characteristics of atmosphere emissions in the lower thermosphere and their aeronomic implications
The green line of atomic oxygen and the Herzberg bands of molecular oxygen as observed from the OGO-4 airglow photometer are discussed in terms of their spatial and temporal distributions and their relation to the atomic oxygen content in the lower thermosphere. Daily maps of the distribution of emissions show considerable structure (cells, patches, and bands) with appreciable daily changes. When data are averaged over periods of several days in length, the resulting patterns have occasional tendencies to follow geomagnetic parallels. The Seasonal variations are characterized by maxima in both the Northern and Southern Hemispheres in October, with the Northern Hemisphere having substantially higher emission rates. Formulae are derived relating the vertical column emission rates of the green line and the Herzberg bands to the atomic oxygen peak density. Global averages for the time period for these data (August 1967 to January 1968), when converted to maximum atomic oxygen densities near 95 km, have a range of 2.0 x 10 to the 11th power/cu cm 2.7 x 10 to the 11th power/cu cm.
The global characteristics of atmospheric emissions in the lower thermosphere and their aeronomic implications
The green line (555.7 nm) of atomic oxygen and the Herzberg bands of molecular oxygen (measured between 250 and 280 nm) as observed from the Ogo 4 airglow photometer from August 1967 through January 1968 are discussed in terms of their spatial and temporal distributions and their relation to the atomic oxygen content in the lower thermosphere. Daily maps of the distribution of emissions show considerable structure (cells, patches, and bands) with appreciable changes from day to day. When data are averaged over periods of several days in length, the resulting patterns have only occasional tendencies to follow geomagnetic parallels. The seasonal variation is characterized by maxima in both the Northern and Southern Hemispheres in October, the Northern Hemisphere having substantially higher emission rates. These maxima tend to move toward the poles, leaving very low values of emission at low latitudes in December and January. Noting the similarity of the atomic oxygen profiles in the lower thermosphere to the profile of a Chapman distribution, formulae are derived relating the vertical column emission rates of the green line and the Herzberg bands to the atomic oxygen peak density.
Probing the Kitaev honeycomb model on a neutral-atom quantum computer
Quantum simulations of many-body systems are among the most promising applications of quantum computers. In particular, models based on strongly correlated fermions are central to our understanding of quantum chemistry and materials problems, and can lead to exotic, topological phases of matter. However, owing to the non-local nature of fermions, such models are challenging to simulate with qubit devices. Here we realize a digital quantum simulation architecture for two-dimensional fermionic systems based on reconfigurable atom arrays. We utilize a fermion-to-qubit mapping based on Kitaev’s model on a honeycomb lattice, in which fermionic statistics are encoded using long-range entangled states. We prepare these states efficiently using measurement and feedforward, realize subsequent fermionic evolution through Floquet engineering with tunable entangling gates interspersed with atom rearrangement, and improve results with built-in error detection. Leveraging this fermion description of the Kitaev spin model, we efficiently prepare topological states across its complex phase diagram and verify the non-Abelian spin-liquid phase by evaluating an odd Chern number. We further explore this two-dimensional fermion system by realizing tunable dynamics and directly probing fermion exchange statistics. Finally, we simulate strong interactions and study the dynamics of the Fermi–Hubbard model on a square lattice. These results pave the way for digital quantum simulations of complex fermionic systems for materials science, chemistry and high-energy physics.