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Results for “Coherent Diffractive Imaging”

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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Inversion of dynamical Bragg intensities to complex structure factors by iterated projections. For Ultramic. 2020. ("Pico" Festschrift, May 2021)

We discuss a method for recovering complex structure factors from many simultaneously excited Bragg beam intensities is described. The method is applied to simulated transmission electron diffraction data over a wide range of crystal thickness and beam energies. The method is based on iterated projections between structure and scattering matrices, which are related by a matrix unitary transformation, exponential, which we invert. The algorithm removes multiple-scattering perturbations from diffraction data and might be extended to other fields, including X-ray and neutron diffraction and cryo-electron microscopy. Because coherent multiple scattering involves interference between Bragg beams, the method also solves the phase problem. Unlike dynamical inversion from electron microscope images or ptychography data, the method, which starts with Bragg beam intensities, provides complex structure factors unaffected by focusing errors or resolution limitations imposed by lenses. We provide inversions from simulated data with 441 simultaneously excited Bragg beams over a range of thickness and beam energy. We discuss the retrieval of chirality information from enantiomorphs, the efficient incorporation of symmetry information using the irreducible representation of the group of structure matrices, and the effect of HOLZ lines to provide three-dimensional information.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Reuniting crystallography with real space: Ab initio structure elucidation with 4D-STEM

Structure elucidation via single-crystal methods has historically lacked experimental access to real-space information, instead relying exclusively on diffraction-space measurements of Bragg reflections. Here we exploit the dual-space imaging power of 4D scanning transmission electron microscopy to meaningfully integrate real-space information into the crystallographic workflow. We show that virtual apertures assembled by segmentation of high-angle annular dark-field images enable i) pixel-by-pixel separation of coherent Bragg signal from clusters of closely spaced nanocrystals and ii) selective extraction of integrated intensities from thinner subregions of individual specimens, facilitating retroactive tuning of multiple scattering artifacts. This strategy empowers us to simply pick and choose whichever nanoscale regions of interest generate the highest-quality diffraction patterns, allowing us to solve several independent structures of the metal-organic framework UiO-66 from specimens whose agglomerated morphology proved intractable for conventional microcrystal electron diffraction. Our method is compatible with both rotational and serial approaches to data processing, ultimately divulging the first scanning nanobeam electron diffraction structures determined by direct methods at subangstrom resolution.

Saha, Ambarneil↗
DOE OSTI2020

Three dimensions, two microscopes, one code: Automatic differentiation for x-ray nanotomography beyond the depth of focus limit

Conventional tomographic reconstruction algorithms assume that one has obtained pure projection images, involving no within-specimen diffraction effects nor multiple scattering. Advances in x-ray nanotomography are leading toward the violation of these assumptions, by combining the high penetration power of x-rays, which enables thick specimens to be imaged, with improved spatial resolution that decreases the depth of focus of the imaging system. We describe a reconstruction method where multiple scattering and diffraction effects in thick samples are modeled by multislice propagation and the 3D object function is retrieved through iterative optimization. We show that the same proposed method works for both full-field microscopy and for coherent scanning techniques like ptychography. Our implementation uses the optimization toolbox and the automatic differentiation capability of the open-source deep learning package TensorFlow, demonstrating a straightforward way to solve optimization problems in computational imaging with flexibility and portability.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Correlative image learning of chemo-mechanics in phase-transforming solids

We report constitutive laws underlie most physical processes in nature. However, learning such equations in heterogeneous solids (for example, due to phase separation) is challenging. One such relationship is between composition and eigenstrain, which governs the chemo-mechanical expansion in solids. Here we developed a generalizable, physically constrained image-learning framework to algorithmically learn the chemo-mechanical constitutive law at the nanoscale from correlative four-dimensional scanning transmission electron microscopy and X-ray spectro-ptychography images. We demonstrated this approach on Li X FePO 4 , a technologically relevant battery positive electrode material. We uncovered the functional form of the composition–eigenstrain relation in this two-phase binary solid across the entire composition range (0 ≤ X ≤ 1), including inside the thermodynamically unstable miscibility gap. The learned relation directly validates Vegard’s law of linear response at the nanoscale. Our physics-constrained data-driven approach directly visualizes the residual strain field (by removing the compositional and coherency strain), which is otherwise impossible to quantify. Heterogeneities in the residual strain arise from misfit dislocations and were independently verified by X-ray diffraction line profile analysis. Our work provides the means to simultaneously quantify chemical expansion, coherency strain and dislocations in battery electrodes, which has implications on rate capabilities and lifetime. Broadly, this work also highlights the potential of integrating correlative microscopy and image learning for extracting material properties and physics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Diffractive Imaging of Conical Intersections Amplified by Resonant Infrared Fields

The fate of virtually all photochemical reactions is determined by conical intersections. These are energetically degenerate regions of molecular potential energy surfaces that strongly couple electronic states, thereby enabling fast relaxation channels. Their direct spectroscopic detection relies on weak features that are often buried beneath stronger, less interesting contributions. For azobenzene photoisomerization, a textbook photochemical reaction, we demonstrate how a resonant infrared field can be employed during the conical intersection passage to significantly enhance its coherence signatures in time-resolved Xray diffraction while leaving the product yield intact. Furthermore, this transition-state amplification holds promise to bring signals of conical intersections above the detection threshold.

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

Complex-valued universal linear transformations and image encryption using spatially incoherent diffractive networks

As an optical processor, a diffractive deep neural network (D2NN) utilizes engineered diffractive surfaces designed through machine learning to perform all-optical information processing, completing its tasks at the speed of light propagation through thin optical layers. With sufficient degrees of freedom, D2NNs can perform arbitrary complex-valued linear transformations using spatially coherent light. Similarly, D2NNs can also perform arbitrary linear intensity transformations with spatially incoherent illumination; however, under spatially incoherent light, these transformations are nonnegative, acting on diffraction-limited optical intensity patterns at the input field of view. Here, we expand the use of spatially incoherent D2NNs to complex-valued information processing for executing arbitrary complex-valued linear transformations using spatially incoherent light. Through simulations, we show that as the number of optimized diffractive features increases beyond a threshold dictated by the multiplication of the input and output space-bandwidth products, a spatially incoherent diffractive visual processor can approximate any complex-valued linear transformation and be used for all-optical image encryption using incoherent illumination. The findings are important for the all-optical processing of information under natural light using various forms of diffractive surface-based optical processors.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ultrafast Imaging of Molecules with Electron Diffraction

Photoexcited molecules convert light into chemical and mechanical energy through changes in electronic and nuclear structure that take place on femtosecond timescales. Gas phase ultrafast electron diffraction (GUED) is an ideal tool to probe the nuclear geometry evolution of the molecules and complements spectroscopic methods that are mostly sensitive to the electronic state. GUED is a passive probing tool that does not alter the molecular properties during the probing process and is sensitive to the spatial distribution of charge in the molecule, including both electrons and nuclei. Improvements in temporal resolution have enabled GUED to capture coherent nuclear motions in molecules in the excited and ground electronic states with femtosecond and subangstrom resolution. Here we present the basic theory of GUED and explain what information is encoded in the diffraction signal, review how GUED has been used to observe coherent structural dynamics in recent experiments, and discuss the advantages and limitations of the method.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Projective imaging of high-energy nuclei via coherent exclusive vector meson production in electron-nucleus collisions

One of the major goals of modern nuclear experiments is to study the distributions of gluons inside nuclei at high energy. A key measurement is the coherent exclusive vector meson (VM) production in diffractive electron-nucleus collisions, where the gluon spatial distribution inside the nucleus can be obtained through a Fourier transform of the squared nuclear momentum transfer (|t|) distribution. This research aims to overcome the two main obstacles of the |t| measurement: limited precision in measuring |t| arising from the momentum resolution of the outgoing electron and the overwhelming incoherent background. We demonstrate that by measuring the projected |t| distribution along the direction perpendicular to the electron scattering plane, the effect of the outgoing electron’s momentum resolution can be effectively mitigated, and the diffractive pattern is largely restored. Furthermore, we propose to measure the angular distribution of the VM’s decay daughters to statistically remove the incoherent background.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Imaging Nanoscale Energy Transport and Conversion with Ultrafast Electron Microscopy (Final Technical Report)

Light-matter interactions are ubiquitous in nature and reside at the heart of innumerable technologies. The cascade of processes that occur when a material absorbs a photon of light are exceedingly complex and are interwoven in both space and time, rendering precise determination of the atomic-scale and ultrafast mechanisms immensely challenging. The advent of methods for generating short pulses of light several decades ago led to major advances in understanding the initial moments of light absorption and the resultant effects, though directly interrogating the response of the atoms within the material continued to prove challenging. More recently, methods for generating ultrashort pulses of X-rays and fast electrons have opened the way to probing photoinduced structural dynamics of a wide range of matter in multiple phases. An especially promising laboratory-scale method is ultrafast electron microscopy (UEM), wherein the modalities of conventional transmission electron microscopes (imaging, diffraction, spectroscopy) are extended into the femtosecond temporal regime. Here, the ultrafast imaging and diffraction modalities of UEM were used to study the transient structural aspects of photoexcitation of semiconducting materials (e.g., spatially-resolved electron-phonon coupling, excitation and emission of acoustic phonons, and discrete nanoscale scattering processes). The project had three main objectives: (1) determination of the excitation mechanisms of dense, hypersonic charge-carrier waves and the spatially mediated means by which they couple to the lattice via coherent phonon emission, especially with UEM imaging, wherein effects of nanoscale structural and morphological features on the coupling and relaxation dynamics are expected to dictate nucleation sites and preferred wave vectors, (2) elucidation of photoinduced acoustic-phonon seeding, emergence, propagation, and decay over nanoscale crystal regions and especially with respect to local strain fields and atomic-scale disruptions in lattice order, and (3) interwoven with the first two were efforts aimed at realizing combined angstrom-femtosecond spatiotemporal imaging with UEM. The outcomes and impacts of this project were the generation of new knowledge with respect to fundamental light-matter interactions and, especially, the spatially-mediated excitation and evolution of the structural response of materials following coherent photoexcitation. Importantly, the spatial and temporal resolutions of the UEM imaging modalities used are well-suited for such studies and enable spatially-resolved mechanisms to be determined as a function of atomic order, structural features, and morphology. In addition, ultrafast crystallographic measurements were used to correlate real- and reciprocal-space dynamics in order to determine atomic-scale preferential wave vectors and ultrafast scattering mechanisms, especially as dictated by specimen boundary conditions. The obtained results, as detailed in peer-reviewed publications and presentations, illustrate the importance of ultrafast, angstrom-scale real-space imaging for developing a comprehensive understanding of energy transport and conversion in materials.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Airy light-sheet Raman imaging

Light-sheet fluorescence microscopy has greatly improved the speed and overall photostability of optically sectioning cellular and multi-cellular specimens. Similar gains have also been conferred by light-sheet Raman imaging; these schemes, however, rely on diffraction limited Gaussian beams that hinder the uniformity and size of the imaging field-of-view, and, as such, the resulting throughput rates. Here, we demonstrate that a digitally scanned Airy beam increases the Raman imaging throughput rates by more than an order of magnitude than conventional diffraction-limited beams. Overall, this, spectrometer-less, approach enabled 3D imaging of microparticles with high contrast and 1 µm axial resolution at 300 msec integration times per plane and orders of magnitude lower irradiation density than coherent Raman imaging schemes. We detail the apparatus and its performance, as well as its compatibility with fluorescence light-sheet and quantitative-phase imaging towards rapid and low phototoxicity multimodal imaging.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Opportunities for imaging light nuclei with a second interaction region at the Electron-Ion Collider

The upcoming Electron-Ion Collider (EIC) will address several outstanding puzzles in modern nuclear physics. Key questions—such as the partonic structure of nucleons and nuclei and the origin of their mass and spin—can be explored through high-energy electron-proton and electron-nucleus collisions. Here, to maximize its scientific reach, the EIC community has advocated for the addition of a second interaction region equipped with a detector complementary to the EIC general purpose collider detector, ePIC. The preconceptual design of this interaction region aims to provide a different configuration from the first interaction region, which enhances forward acceptance at very small scattering angles (𝜃 ∼0 mrad). This machine configuration would significantly benefit exclusive, tagging, and diffractive physics programs, complementing those of the ePIC experiment. In particular, accessing coherent diffractive processes on light nuclei by tagging of the full, intact nucleus is essential for mapping their spatial parton distributions. In this work, we present an exploratory study of the detection capabilities for light nuclei at a second EIC interaction region, with a detailed discussion of the accessible kinematic phase space and its implications for imaging.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1991

All-optical photochromic spatial light modulators based on photoinduced electron transfer in rigid matrices

A single material (not a multi-element structure) spatial light modulator may be written to, as well as read out from, using light. The device has tailorable rise and hold times dependent on the composition and concentration of the molecular species used as the active components. The spatial resolution of this device is limited only by light diffraction as in volume holograms. The device may function as a two-dimensional mask (transmission or reflection) or as a three-dimensional volume holographic medium. This device, based on optically-induced electron transfer, is able to perform incoherent to coherent image conversion or wavelength conversion over a wide spectral range (ultraviolet, visible, or near-infrared regions).

Beratan, David N.↗
DOE OSTI2021

Conical Intersection Passages of Molecules Probed by X-ray Diffraction and Stimulated Raman Spectroscopy

Conical intersections (CoIns) play an important role in ultrafast relaxation channels. Their monitoring remains a formidable experimental challenge. We theoretically compare the probing of the S 2 → S 1 CoIn passage in 4-thiouracil by monitoring its vibronic coherences, using off-resonant X-ray-stimulated Raman spectroscopy (TRUECARS) and time resolved X-ray diffraction (TRXD). The quantum nuclear wavepacket (WP) dynamics provides an accurate picture of the photoinduced dynamics. Upon photoexcitation, the WP oscillates among the Franck–Condon point, the S2 minimum, and the CoIn with a 70 fs period. A vibronic coherence first emerges at 20 fs and can be observed until the S 2 state is fully depopulated. The distribution of the vibronic frequencies involved in the coherence is recorded by the TRUECARS spectrogram. Here, the TRXD signal provides spatial images of electron densities associated with the CoIn. In combination, the two signals provide a complementary picture of the nonadiabatic passage, which helps in the study of the underlying photophysics in thiobases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1990

Diffraction image formation in optical systems with polarization aberrations. I - Formulation and example

This paper is the first in a series that will examine image formation in optical systems with polarization aberrations. The present paper derives the point-spread function (PSF) and the optical transfer function for optical systems with polarization aberration and explores how image formation depends on the coherence and polarization state of the source. It is shown that the scalar PSF of Fourier optics can be generalized in the presence of polarization aberration to a 4 x 4 point-spread matrix (PSM) in Mueller matrix notation. A similar 4 x 4 optical transfer matrix (OTM) is shown to be an appropriate generalization of the optical transfer function. The PSM and the OTM are associated with the optical system and are independent of the incident polarization state but dependent on the coherence of the illumination. Since an optical system with polarization aberrations will have a different PSF and optical transfer function for different incident polarization states, the PSM and the OTM act as filters with regard to the incident polarization state. Example calculations are performed for a circularly retarding lens.

Mcguire, James P., Jr.↗
DOE OSTI2023

Invited article: X-ray phase contrast imaging in inertial confinement fusion and high energy density research

X-ray phase contrast imaging (XPCI) provides enhanced image contrast beyond absorption-based x-ray imaging alone due to refraction and diffraction from gradients in the object material density. It is sensitive to small variations in density, such as internal voids, cracks, grains, defects, and material flow, as well as to stronger density variations such as from a shock wave. Beyond its initial use in biology and materials science, XPCI is now routinely used in inertial confinement fusion (ICF) and high energy density (HED) research, first to characterize ICF capsules and targets, and later applied in dynamic experiments, where coherent x-ray sources, ultrafast x-ray pulses, and high temporal and spatial resolution are required. In this Review article, XPCI image formation theory is presented, its diverse use in ICF and HED research is discussed, the unique requirements for ultrafast XPCI imaging are given, as well as current challenges and issues in its use.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Phase retrieval and reconstruction of coherent synthesis by genetic algorithm

Abstract In the context of diffractive optics, phase retrieval is a heavily investigated process of recreating an entire complex electric field from partial amplitude-only information through iterative algorithms. However, existing methods can fall into local minima during reconstructions or struggle to recover unusual and novel electric field distributions. We present a numerical method based on a global-optimization genetic algorithm that reconstructs non-trivial electric field distributions from single diffracted intensity distributions. Diffraction and propagation of the optical fields over arbitrary distances is modeled through implementation of the angular spectrum technique. Additionally, a coherently-locked laser array system is used as an experimental case-study demonstrating 0.09 π phase reconstruction accuracy of initial laser parameters from single intensity images.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS2006

MegaMIR: The Megapixel Mid-Infrared Instrument for the Large Binocular Telescope Interferometer

The Megapixel Mid-infrared Instrument (MegaMIR) is a proposed Fizeau-mode camera for the Large Binocular Telescope operating at wavelengths between 5 and 28 micrometers. The camera will be used in conjunction with the Large Binocular Telescope Interferometer (LBTI), a cryogenic optical system that combines the beams from twin 8.4-m telescopes in a phase coherent manner. Unlike other interferometric systems, the co-mounted telescopes on the LBT satisfy the sine condition, providing diffraction-limited resolution over the 40" field of view of the camera. With a 22.8-m baseline, MegaMIR will yield 0.1" angular resolution, making it the highest resolution wide field imager in the thermal infrared for at least the next decade. MegaMIR will utilize a newly developed 1024 x 1024 pixel Si:As detector array that has been optimized for use at high backgrounds. This new detector is a derivative of the Wide-field Infrared Survey Explorer (WISE) low-background detector. The combination of high angular resolution and wide field imaging will be a unique scientific capability for astronomy. Key benefits will be realized in planetary science, galactic, and extra-galactic astronomy. High angular resolution is essential to disentangle highly complex sources, particularly in star formation regions and external galaxies, and MegaMIR provides this performance over a full field of view. Because of the great impact being made by space observatories like the Spitzer Space Telescope, the number of available targets for study has greatly increased in recent years, and MegaMIR will allow efficient follow up science.

ultraluminous galaxies↗