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At least 145 records · Page 8

In-situ and wavelength-dependent photocatalytic strain evolution of a single Au nanoparticle on a TiO 2 film

Photocatalysis is a promising technique due to its capacity to efficiently harvest solar energy and its potential to address the global energy crisis. However, the structure–activity relationships of photocatalyst during wavelength-dependent photocatalytic reactions remains largely unexplored because it is difficult to measure under operating conditions. Here we show the photocatalytic strain evolution of a single Au nanoparticle (AuNP) supported on a TiO 2 film by combining three-dimensional (3D) Bragg coherent X-ray diffraction imaging with an external light source. The wavelength-dependent generation of reactive oxygen species (ROS) has significant effects on the structural deformation of the AuNP, leading to its strain evolution. Density functional theory (DFT) calculations are employed to rationalize the induced strain caused by the adsorption of ROS on the AuNP surface. These observations provide insights of how the photocatalytic activity impacts on the structural deformation of AuNP, contributing to the general understanding of the atomic-level catalytic adsorption process.

14 SOLAR ENERGY↗

Strain-associated nanoscale fluctuating lithium transport within single-crystalline LiNi 1/3 Mn 1/3 Co 1/3 O 2 cathode particles

Solid-state lithium diffusion dynamics are critical for the rate capability and longevity of Li-ion batteries. Conventionally, nanoscale lithium diffusion within individual battery particles has been simplified as being primarily driven by concentration gradients, despite the associated processes inducing local lattice expansion, contraction, and strain fields. Using operando scanning transmission soft X-ray microscopy with high spatial resolution and chemical sensitivity to track nanoscale intraparticle lithium transport, and post-cycling Bragg coherent diffraction X-ray imaging to directly reveal three-dimensional intraparticle strain fields, we uncover strain-associated lithium transport dynamics within single-crystalline LiNi 1/3 Mn 1/3 Co 1/3 O 2 (scNMC) particles during cycling. Contrary to the expected thermodynamic solid-solution behavior of scNMC, our observations reveal near-uniform but fluctuating regions of lithium-dense and lithium-dilute areas during cycling. These fluctuations suggest that nanoscale lithium diffusion can proceed counter to concentration gradients. Additionally, we demonstrate that an increased presence of lithium-dilute regions near the surface enhances lithium surface insertion kinetics, emphasizing the importance of controlling surface lithium distribution to improve rate performance. Our study provides insights into nanoscale solid-state ion transport, with potential applications in batteries, solid-state fuel cells, and memristors.

Lee, Danwon [Seoul National Univ. (Korea, Republic↗

Origin of structural degradation in Li-rich layered oxide cathode

Li- and Mn-rich (LMR) cathode materials that utilize both cation and anion redox can yield substantial increases in battery energy density 1,2,3 . However, although voltage decay issues cause continuous energy loss and impede commercialization, the prerequisite driving force for this phenomenon remains a mystery 3,4,5,6 In this work, with in situ nanoscale sensitive coherent X-ray diffraction imaging techniques, we reveal that nanostrain and lattice displacement accumulate continuously during operation of the cell. Evidence shows that this effect is the driving force for both structure degradation and oxygen loss, which trigger the well-known rapid voltage decay in LMR cathodes. By carrying out micro- to macro-length characterizations that span atomic structure, the primary particle, multiparticle and electrode levels, we demonstrate that the heterogeneous nature of LMR cathodes inevitably causes pernicious phase displacement/strain, which cannot be eliminated by conventional doping or coating methods. We therefore propose mesostructural design as a strategy to mitigate lattice displacement and inhomogeneous electrochemical/structural evolutions, thereby achieving stable voltage and capacity profiles. These findings highlight the significance of lattice strain/displacement in causing voltage decay and will inspire a wave of efforts to unlock the potential of the broad-scale commercialization of LMR cathode materials.

25 ENERGY STORAGE↗

Static and dynamic topological defects in the domain textures in the helical antiferromagnet Ni 2 ⁢CoTeO 6

Real-space Bragg coherent x-ray-diffractive imaging unveils the formation of bubble and stripe antiferromagnetic (AFM) phase domains on the surface of Ni 2 ⁢CoTeO 6 single crystal. The stripe domains exhibit dislocation-type topological defects. The defects typically form as defect-antidefect pairs and can be created or annihilated by temperature changes and local heating. Thermal fluctuations of the AFM domain walls are observed near the Néel temperature. Topological defect pairs dynamically form and disappear in the fluctuating state. These observations provide a real-space perspective on the dynamics of the AFM phase transition in a helical antiferromagnet. Finally, the remarkable tunability of AFM domain walls in a helical antiferromagnet underscores their potential for AFM spintronics applications.

36 MATERIALS SCIENCE↗

Evolution of ferroelastic domain walls during phase transitions in barium titanate nanoparticles

In this work, ferroelastic domain walls inside BaTiO 3 (BTO) tetragonal nanocrystals are distinguished by Bragg peak position and studied with Bragg coherent x-ray diffraction imaging (BCDI). Convergence-related features of the BCDI method for strongly phased objects are reported. A ferroelastic domain wall inside a BTO crystal has been tracked and imaged across the tetragonal-cubic phase transition and proves to be reversible. The linear relationship of relative displacement between two twin domains with temperature is measured and shows a different slope for heating and cooling, while the tetragonality reproduces well over temperature changes in both directions. An edge dislocation is also observed and found to annihilate when heating the crystal close to the phase transition temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals

Significance Monitoring the real-space motion of the electrons directly involved in ultrafast molecular dynamics is a challenging goal, hindered by the strong contributions of the remaining inactive electrons. Molecular quantum coherences can provide a direct window into elementary electronic dynamics, but they could not be separately imaged so far. Here, we demonstrate a time- and frequency-resolved X-ray diffraction technique, which can employ existing stochastic X-ray pulses to separately image the coherence contributions. The technique can selectively follow the relevant electrons involved in the ultrafast dynamics and identify the confined molecular regions covered by their motion. It enables readily feasible measurements and can be straightforwardly extended to full three-dimensional imaging via X-ray and electron diffraction.

74 ATOMIC AND MOLECULAR PHYSICS↗

Laboratory demonstration of image reconstruction for coherent optical system of modular imaging collectors (COSMIC)

The first physical demonstration of the principle of image reconstruction using a set of images from a diffraction-blurred elongated aperture is reported. This is an optical validation of previous theoretical and numerical simulations of the COSMIC telescope array (coherent optical system of modular imaging collectors). The present experiment utilizes 17 diffraction blurred exposures of a laboratory light source, as imaged by a lens covered by a narrow-slit aperture; the aperture is rotated 10 degrees between each exposure. The images are recorded in digitized form by a CCD camera, Fourier transformed, numerically filtered, and added; the sum is then filtered and inverse Fourier transformed to form the final image. The image reconstruction process is found to be stable with respect to uncertainties in values of all physical parameters such as effective wavelength, rotation angle, pointing jitter, and aperture shape. Future experiments will explore the effects of low counting rates, autoguiding on the image, various aperture configurations, and separated optics.

Traub, W. A.↗

Perfection of Apoferritin Crystals: An Advanced X-Ray Imaging and Diffraction Study

Ferritin is a well-known iron-storage protein, and is a spherical shell that consists of 24 identical subunits packed in a 432 symmetry. The typically large protein size and its distinction from lysozyme as to chemical and physical characteristics make ferritin an attractive model protein for crystal growth and perfection investigation-as an alternative to the most widely studied lysozyme. In this contribution, the latest results obtained from coherence-based x-ray diffraction imaging and diffraction experiments will be presented on octahedral apoferritin (a demetalized form of ferritin) crystals grown from various growth conditions. Crystal specimens, which have the measured rocking-curve widths varying from a few arcseconds to several tens arcseconds (or more), are comparatively examined by intrinsically highly sensitive mapping of lattice perfection and defects. The richness of the observed defects and growth features offers insight into perfection and growth of protein crystals. Beautiful interference fringe patterns formed in diffraction images and fine oscillation structure of rocking curves observed will be discussed for understanding of physical origins and the underlying impact.

Hu, Z. W.↗

Snapshot multispectral imaging using a diffractive optical network

Abstract Multispectral imaging has been used for numerous applications in e.g., environmental monitoring, aerospace, defense, and biomedicine. Here, we present a diffractive optical network-based multispectral imaging system trained using deep learning to create a virtual spectral filter array at the output image field-of-view. This diffractive multispectral imager performs spatially-coherent imaging over a large spectrum, and at the same time, routes a pre-determined set of spectral channels onto an array of pixels at the output plane, converting a monochrome focal-plane array or image sensor into a multispectral imaging device without any spectral filters or image recovery algorithms. Furthermore, the spectral responsivity of this diffractive multispectral imager is not sensitive to input polarization states. Through numerical simulations, we present different diffractive network designs that achieve snapshot multispectral imaging with 4, 9 and 16 unique spectral bands within the visible spectrum, based on passive spatially-structured diffractive surfaces, with a compact design that axially spans ~72 λ m , where λ m is the mean wavelength of the spectral band of interest. Moreover, we experimentally demonstrate a diffractive multispectral imager based on a 3D-printed diffractive network that creates at its output image plane a spatially repeating virtual spectral filter array with 2 × 2 = 4 unique bands at terahertz spectrum. Due to their compact form factor and computation-free, power-efficient and polarization-insensitive forward operation, diffractive multispectral imagers can be transformative for various imaging and sensing applications and be used at different parts of the electromagnetic spectrum where high-density and wide-area multispectral pixel arrays are not widely available.

36 MATERIALS SCIENCE↗

Quantitative phase measurements of human cell nuclei using X-ray ptychography

The human cell nucleus serves as an important organelle holding the genetic blueprint for life. In this work, X-ray ptychography was applied to assess the masses of human cell nuclei using its unique phase shift information. Measurements were carried out at the I13-1 beamline at the Diamond Light Source that has extremely large transverse coherence properties. Furthermore, the ptychographic diffractive imaging approach allowed imaging of large structures that gave quantitative measurements of the phase shift in 2D projections. In this paper a modified ptychography algorithm that improves the quality of the reconstruction for weak scattering samples is presented. The application of this approach to calculate the mass of several human nuclei is also demonstrated.

59 BASIC BIOLOGICAL SCIENCES↗

Multiscale aperture synthesis imager

Synthetic aperture imaging has enabled breakthrough observations from radar to astronomy. However, optical implementation remains challenging due to stringent wavefield synchronization requirements among multiple receivers. Here we present the multiscale aperture synthesis imager (MASI), which utilizes parallelism to break complex optical challenges into tractable sub-problems. MASI employs a distributed array of coded sensors that operate independently yet coherently to surpass the diffraction limit of single receiver. It combines the propagated wavefields from individual sensors through a computational phase synchronization scheme, eliminating the need for overlapping measurement regions to establish phase coherence. Light diffraction in MASI naturally expands the imaging field, generating phase-contrast visualizations that are substantially larger than sensor dimensions. Without using lenses, MASI resolves sub-micron features at ultralong working distances and reconstructs 3D shapes over centimeter-scale fields. MASI transforms the intractable optical synchronization problem into a computational one, enabling practical deployment of scalable synthetic aperture systems at optical wavelengths.

electrical and electronic engineering↗

Transport of intensity equation: a tutorial

When it comes to “phase measurement” or “quantitative phase imaging”, many people will automatically connect them with “laser” and “interferometry”. Indeed, conventional quantitative phase imaging and phase measurement techniques generally rely on the superposition of two beams with a high degree of coherence: complex interferometric configurations, stringent requirements on the environmental stabilities, and associated laser speckle noise severely limit their applications in optical imaging and microscopy. On a different note, as one of the most well-known phase retrieval approaches, the transport of intensity equation (TIE) provides a new non-interferometric way to access quantitative phase information through intensity only measurement. Despite the insufficiency for interferometry, TIE is applicable under partially coherent illuminations (like the Köhler’s illumination in a conventional microscope), permitting optimum spatial resolution, higher signal-to-noise ratio, and better image quality. In this tutorial, we give an overview of the basic principle, research fields, and representative applications of TIE, focus particularly on optical imaging, metrology, and microscopy. The purpose of this tutorial is twofold. It should serve as a self-contained introduction to TIE for readers with little or no knowledge of TIE. On the other hand, it attempts to give an overview of recent developments in this field. These results highlight a new era in which strict coherence and interferometry are no longer prerequisites for quantitative phase imaging and diffraction tomography, paving the way toward new generation label-free three-dimensional microscopy, with applications in all branches of biomedicine.

42 ENGINEERING↗

Diffraction image formation in optical systems with polarization aberrations. II - Amplitude response matrices for rotationally symmetric systems

In the previous paper in this series (McGuire and Chipman, 1990), a formulation was established for the calculation and analysis of diffraction image quality in polarizing optical systems illuminated with partially polarized, partially coherent light. In the present paper, the effect of second- and fourth-order polarization aberrations on the image plane diffraction patterns are examined. The amplitude response matrix is calculated for optical systems with small numerical apertures. Numerical results are presented for optical systems with circular apertures for three of the aberration types.

Mcguire, James P., Jr.↗

Image processing system to analyze droplet distributions in sprays

An image processing system was developed which automatically analyzes the size distributions in fuel spray video images. Images are generated by using pulsed laser light to freeze droplet motion in the spray sample volume under study. This coherent illumination source produces images which contain droplet diffraction patterns representing the droplets degree of focus. The analysis is performed by extracting feature data describing droplet diffraction patterns in the images. This allows the system to select droplets from image anomalies and measure only those droplets considered in focus. Unique features of the system are the totally automated analysis and droplet feature measurement from the grayscale image. The feature extraction and image restoration algorithms used in the system are described. Preliminary performance data is also given for two experiments. One experiment gives a comparison between a synthesized distribution measured manually and automatically. The second experiment compares a real spray distribution measured using current methods against the automatic system.

Bertollini, Gary P.↗

SpeckleNN: a unified embedding for real-time speckle pattern classification in X-ray single-particle imaging with limited labeled examples

With X-ray free-electron lasers (XFELs), it is possible to determine the three-dimensional structure of noncrystalline nanoscale particles using X-ray single-particle imaging (SPI) techniques at room temperature. Classifying SPI scattering patterns, or `speckles', to extract single-hits that are needed for real-time vetoing and three-dimensional reconstruction poses a challenge for high-data-rate facilities like the European XFEL and LCLS-II-HE. Here, we introduce SpeckleNN, a unified embedding model for real-time speckle pattern classification with limited labeled examples that can scale linearly with dataset size. Trained with twin neural networks, SpeckleNN maps speckle patterns to a unified embedding vector space, where similarity is measured by Euclidean distance. We highlight its few-shot classification capability on new never-seen samples and its robust performance despite having only tens of labels per classification category even in the presence of substantial missing detector areas. Without the need for excessive manual labeling or even a full detector image, our classification method offers a great solution for real-time high-throughput SPI experiments.

47 OTHER INSTRUMENTATION↗

Coherent optical determination of the leaf angle distribution of corn

A coherent optical technique for the diffraction analysis of an image is presented. Developments in radar remote sensing shows a need to understand plant geometry and its relationship to plant moisture, soil moisture, and the radar backscattering coefficient. A corn plant changes its leaf angle distribution, as a function of time, from a uniform distribution to one that is strongly vertical. It is shown that plant and soil moisture may have an effect on plant geometry.

Ulaby, F. T.↗