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Broadband Performance of TPF's High-contrast Imaging Testbed: Modeling and Simulations
The broadband performance of the high-contrast imaging testbed (HCIT) at JPL is investigated through optical modeling and simulations. The analytical tool is an optical simulation algorithm developed by combining the HCIT's optical model with a speckle-nulling algorithm that operates directly on coronagraphic images, an algorithm identical to the one currently being used on the HCIT to actively suppress scattered light via a deformable mirror. It is capable of performing full three-dimensional end-to-end near-field diffraction analysis on the HCIT's optical system. By conducting speckle-nulling optimization, we clarify the HCIT's capability and limitations in terms of its broadband contrast performance under various realistic conditions. Considered cases include non-ideal occulting masks, such as a mask with optical density and wavelength dependent parasitic phase-delay errors (i.e., a not band-limited occulting mask) and the one with an optical-density profile corresponding to a measured, non-standard profile, as well as the independently measured phase errors of all optics. Most of the information gathered on the HCIT's optical components through measurement and characterization over the last several years at JPL has been used in this analysis to make the predictions as accurate as possible. The best contrast values predicted so far by our simulations obtainable on the HCIT illuminated with a broadband light having a bandwidth of 80nm and centered at 800nm wavelength are Cm=1.1x10-8 (mean) and C4=4.9x10-8 (at 4(lamda)/D), respectively. In this paper we report our preliminary findings about the broadband light performance of the HCIT.
High-Temperature Neutron Diffraction Study of Vanadium and Vanadium–Niobium Null-Matrix Alloy for Spectrum Normalization
This study systematically evaluates a vanadium–niobium (V 94.1 Nb 5.9 ) null-matrix alloy as a reference material for neutron spectrum normalization and compares its performance with that of pure vanadium under identical experimental conditions. Neutron diffraction experiments are conducted on the VULCAN Engineering Materials Diffractometer at the Spallation Neutron Source, Oak Ridge National Laboratory, over a temperature range from room temperature to 1200 °C under vacuum. Pure vanadium exhibited distinct Bragg peaks across all temperatures, with its diffraction behavior influenced by both sample orientation and temperature. As the temperature increased, the diffraction peaks shifted to larger d-spacings and decreased in intensity, while spectral deviation near d ≈ 2.8 Å exceeded 10% at 1200 °C. In contrast, the V–Nb alloy produced a nearly featureless spectrum over the full d-spacing range, confirming near-complete cancellation of coherent scattering over the wide temperature range. Its spectra were insensitive to sample orientation, temperature, and microstructural evolution, with spectral deviation around d ≈ 2.8 Å exceeded 5% at 1200 °C. In conclusion, these results demonstrate that the V–Nb null-matrix alloy provides a thermally stable, efficient, and reliable normalization standard for time-of-flight diffractometers or other instrument where it is needed, enabling reduced data acquisition time and improved data quality in high-temperature neutron diffraction experiments.
Scattering of a Tightly Focused Beam by an Optically Trapped Particle
Near-forward scattering of an optically trapped 5 m radius polystyrene latex sphere by the trapping beam was examined both theoretically and experimentally. Since the trapping beam is tightly focused, the beam fields superpose and interfere with the scattered fields in the forward hemisphere. The observed light intensity consists of a series of concentric bright and dark fringes centered about the forward scattering direction. Both the number of fringes and their contrast depend on the position of the trapping beam focal waist with respect to the sphere. The fringes are caused by diffraction due to the truncation of the tail of the trapping beam as the beam is transmitted through the sphere.
Quantitative agreement between dynamical rocking curves in ultrafast electron diffraction for x-ray lasers
Electron diffraction through a thin patterned silicon membrane can be used to create complex spatial modulations in electron distributions. By precisely varying parameters such as crystallographic orientation and wafer thickness, the intensity of reflections in the diffraction plane can be controlled and by placing an aperture to block all but one spot, we can form an image with different parts of the patterned membrane, as is done for bright-field imaging in microscopy. The patterned electron beams can then be used to control phase and amplitude of subsequent x-ray emission, enabling novel coherent x-ray methods. Furthermore, the electrons themselves can also be used for femtosecond time resolved diffraction and microscopy. As a first step toward patterned beams, we demonstrate experimentally and through simulation the ability to accurately predict and control diffraction spot intensities. We simulate MeV transmission electron diffraction patterns using the multislice method for various crystallographic orientations of a single crystal Si(001) membrane near beam normal. The resulting intensity maps of the Bragg reflections are compared to experimental results obtained at the Accelerator Structure Test Area Ultrafast Electron Diffraction (ASTA UED) facility at SLAC. Furthermore, the fraction of inelastic and elastic scattering of the initial charge is estimated along with the absorption of the membrane to determine the contrast that would be seen in a patterned version of the Si(001) membrane.
Maximum-Likelihood Parameter Estimation for High-Contrast Wavefront Sensing & Control
Stellar coronagraphs use closed-loop focal-plane wavefront sensing and control algorithms to create high-contrast dark zones suitable for imaging exoplanets and exozodiacal dust clouds around nearby stars. At present, the deepest contrast has been achieved using model-based algorithms, which use the predicted focal-plane influence of the coronagraph's deformable mirrors to drive diffracted starlight toward zero over time in an optimal control framework. However, model-based algorithms are susceptible to model mismatch, wherein a departure of the coronagraph's true optical characteristics from the model predictions causes reduced control loop performance. Here, we report on a technique for maximum-likelihood estimation of the wavefront control Jacobian matrix and noise statistics of the coronagraph focal-plane electric field from data acquired in situ during closed-loop wavefront control operations. By empirically tuning the Jacobian and noise properties in a statistically rigorous fashion, the maximum-likelihood approach mitigates model mismatch and recovers near-optimal control loop performance.
Quadratic magnetoresistance across the insulator–metal transition in V4O7 thin films
We present a comparative magnetotransport study of V4O7 thin films grown simultaneously on single-crystal Al2O3 (r-cut) and amorphous SiO2 substrates, to examine substrate-induced effects on electronic transport across the insulator–metal transition (IMT). Temperature-dependent resistivity reveals a broad electronic ordering regime below the IMT, with both films exhibiting similar transition temperatures but differing by nearly an order of magnitude in absolute resistivity. Despite this strong substrate dependence of the resistivity scale, the magnetoresistance remains predominantly quadratic in magnetic field over wide temperature intervals for both substrates. Analysis of the quadratic magnetoresistance defines an effective mobility scale that evolves systematically across the IMT and exhibits a similar temperature dependence for the two films. Structural characterization, including atomic-resolution scanning transmission electron microscopy of the V4O7/Al2O3 interface and azimuthal X-ray diffraction measurements, reveals a sharp interface and well-defined in-plane crystallographic registry for the r-cut film, in contrast to the rotationally averaged in-plane structure expected for films grown on amorphous SiO2. These results indicate that while substrate-controlled structural registry modifies the resistivity scale, the quadratic magnetotransport response across the IMT remains largely robust, providing a consistent diagnostic of electronic transport in V4O7 thin films.
Terrestrial Planet Finder Coronagraph Optical Modeling
The Terrestrial Planet Finder Coronagraph will rely heavily on modeling and analysis throughout its mission lifecycle. Optical modeling is especially important, since the tolerances on the optics as well as scattered light suppression are critical for the mission's success. The high contrast imaging necessary to observe a planet orbiting a distant star requires new and innovative technologies to be developed and tested, and detailed optical modeling provides predictions for evaluating design decisions. It also provides a means to develop and test algorithms designed to actively suppress scattered light via deformable mirrors and other techniques. The optical models are used in conjunction with structural and thermal models to create fully integrated optical/structural/thermal models that are used to evaluate dynamic effects of disturbances on the overall performance of the coronagraph. The optical models we have developed have been verified on the High Contrast Imaging Testbed. Results of the optical modeling verification and the methods used to perform full three-dimensional near-field diffraction analysis are presented.
Zircon (U-Th)/He Impact Crater Thermochronometry and the Effects of Shock Microstructures on Helium Diffusion Kinetics
Absolute age determination of impact cratering events remains difficult and often controversial; a challenge that has resulted in < 50% of known impact craters regarded as accurately and precisely dated. Besides conventional 40Ar/39Ar and U-Pb methods, zircon (U-Th)/He (ZHe) dating of impactites has been applied to large- to medium-sized impact structures. ZHe dates can be fully reset in minutes at 1000°C, which is commonly reached in central sections of the melt sheet, whereas resetting of ZHe at <300°C, which might be encountered near the crater margins or persist in post-impact hydrothermal systems, may take >103-6 years. There is a critical need to quantify the effects of shock-induced microstructures and impact metamorphism on helium diffusion kinetics in well-characterized, variably shocked zircon to further establish the reliability of (U-Th)/He for dating impacts. For this purpose, we investigated suevite and impact melt samples from two impact structures, the Chicxulub multi-ring basin and the Ries complex crater, which enables us to compare zircon helium diffusion kinetics from impact structures with differing sizes, ages, and hydrothermal system longevities. Shock microstructures were characterized by backscattered-electron (BSE) imaging prior to diffusion step-heating fractional release experiments using light-bulb furnace with prograde and retrograde incremental 10°C steps from 250°C to 600°C. Afterward, we characterize the diffusion domain sizes and their interconnectivity within the shocked zircon grains using electron backscatter diffraction (EBSD). We find that zircon with few shock microstructures exhibit no significant deviation from helium diffusion kinetics of undamaged zircon. In contrast, zircon grains with planar deformation features (PDFs) and granular textures classified by BSE and EBSD are characterized by a dramatic decrease in helium retentivity, similar to radiation damaged grains, due to a reduction in the effective domain size and the introduction of interconnected fast diffusion pathways created by shock microstructures. A subset of grains were dated by ZHe after the external morphology of the grains was determined by BSE imaging. The euhedral grains yielded a weighted mean age within the uncertainty of the accepted impact ages, whereas the grains with PDFs or granular textures exhibited younger ages. Thus, these diffusion experiments and ZHe dates suggest that the dramatic decrease in domain size likely renders shocked grains more susceptible to impact-induced hydrothermal resetting and subsequent overprinting. Hence, characterization of shock microstructures is critical for determining accurate impact ages using ZHe methods especially when applied to previously unconstrained craters. The thermochronometer also offers the opportunity to determine the magnitude and duration of post-impact hydrothermal circulation.
The FastrSHWFS Project Development Motivation, Analysis, & Test Results
The recent 2020 Decadal Survey of Astronomy and Astrophysics listed habitable exoplanet imaging with future extreme adaptive optics (AO) on 30m-class telescopes as a key priority in the coming decade. However, there is a current 100x contrast gap between the best systems today and what is needed to enable this goal. Astronomical AO is a required approach to enable ground-based diffraction-limited imaging of exoplanets on future extremely large telescopes. Time lag between the end of an exposure and the application of deformable mirror commands is a major contributor to the error budget in many AO systems, and detector read time is often a large component of this lag. We present two designs for a modified Shack Hartmann wavefront sensor (SHWFS), named Focal plane Actualized Shifted Technique Realized for a SHWFS (fastrSHWFS), to reduce the time lag component. This design steers the spot pattern at the focal plane into a rectangular or linear array with a custom aspect ratio, reducing readout time. The mask with focus yields aberrated results while the mask with tip/tilt only yields some defined spots. This essay outlines the current SHWFS concept, our fastrSHWFS theoretical solution to addressing time lag, reflection and quality analysis of printed mask designs, and results from testing both masks on the High Contrast Testbed at Lawrence Livermore National Lab. This work follows the test of a previous fastrSHWFS design.
Atomic Structure, Dynamics, Changes in Chemical Bonding and Semiconductor-Metal Transition in Sb 2 Se 3 : A Remarkable Material for Quantum Networks and Energy Applications
Antimony sesquiselenide has become an outstanding functional material for photovoltaics, energy storage and transformation, memory and photonic applications. Sb 2 Se 3 is one of the most successful emerging solar light absorbers and has also been identified as a highly promising ultralow-loss phase-change material (PCM) for next-generation coherent nanophotonic processors, photonic tensor cores, quantum and neuromorphic networks. Unlike benchmark telluride PCMs, Sb 2 Se 3 features a quasi-one-dimensional (1D) crystalline structure consisting of (Sb 4 Se 6 ) ∞ ribbons, lacks the typical PCM chemical bonding, and undergoes an extended semiconductor-metal transition above the melting point. Consequently, the origin of high optical contrast between crystalline (SET) and amorphous (RESET) logic states remains elusive and presents a significant challenge. Using high-energy X-ray diffraction and Raman spectroscopy over a wide temperature range, supported by first-principles simulations and complemented by thermal, optical and electrical measurements, as well as by 121 Sb-Mossbauer spectroscopy, the quasi-1D network of orthorhombic antimony sesquiselenide was found to undergo significant evolution in amorphous and supercooled Sb 2 Se 3 , leading to lower coordination, shorter interatomic distances and a higher p-electron density on antimony, indicating changes in chemical bonding. The observed novel Sb 2 Se 3 nanocrystalline polymorph, characterized by trigonal antimony coordination and more isolated Sb-Se ribbons, could help reduce multiple trapping defect states in the bandgap, which are typical of orthorhombic Sb 2 Se 3 , thereby enhancing the power-conversion efficiency of photovoltaic devices. Semimetallic and metallic liquid Sb 2 Se 3 exhibit a gradual transformation into a denser 2D and/or 3D network with higher antimony coordination. Localized electron states in the pseudogap are becoming extended, leading to an increase in electronic conductivity σ following the relationship σ ∝ N(E F ) 2 . Liquid Sb 2 Se 3 also appears to be strongly fragile, with a nonmonotonic change in viscosity and higher atomic mobility in the metallic liquid. Furthermore, these results explain extraordinary functionalities of Sb 2 Se 3 for photonic and energy applications.
Competing antiferromagnetic-ferromagnetic states in a d 7 Kitaev honeycomb magnet
The Kitaev model is a rare example of an analytically solvable and physically instantiable Hamiltonian yielding a topological quantum spin liquid ground state. Here we report signatures of Kitaev spin liquid physics in the honeycomb magnet Li 3 Co 2 SbO 6 , built of high-spin d 7 (Co 2+ ) ions, in contrast to the more typical low-spin d 5 electron configurations in the presence of large spin-orbit coupling. Neutron powder diffraction measurements, heat capacity, and magnetization studies support the development of a long-range antiferromagnetic order space group of C C 2/m, below T N = 11K at μ 0 H = 0T. The magnetic entropy recovered between T = 2 and 50 K is estimated to be 0.6Rln2, in good agreement with the value expected for systems close to a Kitaev quantum spin liquid state. The temperature-dependent magnetic order parameter demonstrates a β value of 0.19(3), consistent with XY anisotropy and in-plane ordering, with Ising-like interactions between layers. Further, we observe a spin-flop-driven crossover to ferromagnetic order with space group of C2/m under an applied magnetic field of μ 0 H ≈ 0.7T at T = 2K. Magnetic structure analysis demonstrates these magnetic states are competing at finite applied magnetic fields even below the spin-flop transition. Both the d 7 compass model, a quantitative comparison of the specific heat of Li 3 Co 2 SbO 6 , and related honeycomb cobaltates to the anisotropic Kitaev model further support proximity to a Kitaev spin liquid state. Furthermore, this material demonstrates the rich playground of high-spin d 7 systems for spin liquid candidates and complements known d 5 Ir- and Ru-based materials.
Unconventional crystal-field splitting in noncentrosymmetric BaTiO 3 thin films
Understanding the crystal-field splitting and orbital polarization in noncentrosymmetric systems such as ferroelectric materials is fundamentally important. In this work, taking BaTiO 3 as a representative material, we investigate titanium crystal-field splitting and orbital polarization in noncentrosymmetric TiO 6 octahedra with resonant x-ray linear dichroism at the Ti L 2,3 edge. The high-quality BaTiO 3 thin films were deposited on DyScO 3 (110) single crystal substrates in a layer-by-layer way by pulsed laser deposition. The reflection high-energy electron diffraction and element specific x-ray absorption spectroscopy were performed to characterize the structural and electronic properties of the films. In sharp contrast to conventional crystal-field splitting and orbital configuration (d xz /d yz < d xy < d 3z 2 -r 2 < d x 2 -y 2 or d xy < d xz /d yz < d x 2 -y 2 < d 3z 2 -r 2 ) expected from compressive or tensile epitaxial strain, respectively, it is revealed that d xz , d yz , and d xy orbitals are nearly degenerate, whereas d 3z 2 -r 2 and d x 2 -y 2 orbitals are split with an energy gap ~100 meV in the epitaxial BaTiO 3 films. We find that the unexpected degenerate orbitals d xz /d yz /d xy result from the competition between the orbital splitting induced by epitaxial strain and that induced by polar distortions of BaTiO 3 films. Our results provide a route to manipulate orbital degree of freedom by switching electric polarization in ferroelectric materials.
Design of Experiment for the Measurement of Aerosol Droplet Size Distribution of Temperature-Controlled Thermally Atomized Printed Electronic Inks
In-Space Manufacturing (ISM) centers around NASA’s growing need and ability to produce space technologies on demand in space. As the future of long term presence in space and deep space exploration approach, fundamental questions of our dependence on earth resupply to Low Earth Orbit (LEO) remain unanswered. ISM is leading various effort to evaluate the feasibility of producing essential spares and redundant parts on demand to enable a sustainable space-based supply chain model for part resupply. Among the parts and systems being considered, Avionics form the neural network of modern day aircraft and space vehicles providing a wealth of information ranging from Guidance, Navigation, and Control (GN&C) systems to on board Environmental Control and Life Support (ECLS) systems. Recent advances in the use of Aerosol Jet Technology to print Avionics components ranging from electrical traces on a circuit board to complex transistors and sensors raise the possibility of using such technology to reproduce or recreate electronic parts on demand with the help of custom electronics 3D printers. The challenge herein lies within the ability of such printers to generate and deposit an aerosol of electronic material utilizing processes independent of or enhanced by gravity to ensure controllably identical or improved behavior of the aerosol in an International Space Station (ISS) laboratory and on the ground. The behavior as well as the hazards and properties associated with such aerosols in a microgravity environment must be understood well in order to merit a feasible approach to utilizing them for manufacturing in space. In this report, we outline the experimental setup of a modified conventional vaping device to be used as the ideal gravity independent thermal atomization mechanism to generate aerosol. Our objective is to identify the ideal mass, density, and volume of our aerosolized droplets of ink to conclude that there exist a threshold of aerosolized ink droplet sizes that are indeed independent of the effects of gravity and remain stable after atomization. We use a Malvern Spraytec® Spray Particle Size Analyzer to perform real-time laser diffraction measurement of our ink droplets during atomization. The droplet size between conductive ink, dielectric ink and vegetable glycerin have been measured and contrasted. Furthermore, the mechanism of thermal atomization versus traditional pneumatic and ultrasonic atomization for operation in microgravity have been explored.
Visualizing the Internal Nanocrystallinity of Calcite Due to Nonclassical Crystallization by 3D Coherent X–Ray Diffraction Imaging
The internal crystallinity of calcite is investigated for samples synthesized using two approaches: precipitation from solution and the ammonium carbonate diffusion method. Scanning electron microscopy (SEM) analyses reveal that the calcite products precipitated using both approaches have a well–defined rhombohedron shape, consistent with the euhedral crystal habit of the mineral. The internal structure of these calcite crystals is characterized using Bragg coherent diffraction imaging (BCDI) to determine the 3D electron density and the atomic displacement field. BCDI reconstructions for crystals synthesized using the ammonium carbonate diffusion approach have the expected euhedral shape, with internal strain fields and few internal defects. In contrast, the crystals synthesized by precipitation from solution have very complex external shapes and defective internal structures, presenting null electron density regions and pronounced displacement field distributions. These heterogeneities are interpreted as multiple crystalline domains, created by a nonclassical crystallization mechanism, where smaller nanoparticles coalescence into the final euhedral particles. The combined use of SEM, X–ray diffraction (XRD), and BCDI allows for structurally differentiating calcite crystals grown with different approaches, opening new opportunities to understand how grain boundaries and internal defects alter calcite reactivity.
Robust atom optics for Bragg atom interferometry
Multi-photon Bragg diffraction is a powerful method for fast, coherent momentum transfer of atom waves. However, laser noise, Doppler detunings, and cloud expansion limit its efficiency in large momentum transfer (LMT) pulse sequences. We present simulation studies of robust Bragg pulses developed through numerical quantum optimal control. Optimized pulse performance under noise and cloud inhomogeneities is analyzed and compared to analogous Gaussian and adiabatic rapid passage pulses in simulated LMT Mach–Zehnder interferometry sequences. The optimized pulses maintain robust population transfer and phase response over a broader range of noise, resulting in superior contrast in LMT sequences with thermal atom clouds and intensity inhomogeneities. Large optimized LMT sequences use lower pulse area than Gaussian pulses, making them less susceptible to spontaneous emission loss. The optimized sequences maintain over five times better contrast with tens of momentum separation and offer more improvement with greater LMT. Such pulses could allow operation of Bragg atom interferometers with unprecedented sensitivity, improved contrast, and hotter atom sources.
Resolution-enhanced X-ray fluorescence microscopy via deep residual networks
Abstract Multimodal hard X-ray scanning probe microscopy has been extensively used to study functional materials providing multiple contrast mechanisms. For instance, combining ptychography with X-ray fluorescence (XRF) microscopy reveals structural and chemical properties simultaneously. While ptychography can achieve diffraction-limited spatial resolution, the resolution of XRF is limited by the X-ray probe size. Here, we develop a machine learning (ML) model to overcome this problem by decoupling the impact of the X-ray probe from the XRF signal. The enhanced spatial resolution was observed for both simulated and experimental XRF data, showing superior performance over the state-of-the-art scanning XRF method with different nano-sized X-ray probes. Enhanced spatial resolutions were also observed for the accompanying XRF tomography reconstructions. Using this probe profile deconvolution with the proposed ML solution to enhance the spatial resolution of XRF microscopy will be broadly applicable across both functional materials and biological imaging with XRF and other related application areas.
Pressure‐Induced Structural and Optoelectronic Modulations in 2D Dion‐Jacobson Hybrid Lead Iodide Perovskites With a Rigid Spacer
2D hybrid organic-inorganic perovskites (HOIPs) are known for their superior chemical and thermal stability over 3D variants, positioning them as promising materials for advanced optoelectronic applications. Applying external high pressure is an effective strategy to modify their structures and tune their optoelectronic properties. This study examines the high-pressure behavior of a Dion-Jacobson type 2D HOIP, DPDAPbI 4 , which incorporates the rigid organic spacer N,N-dimethylphenylene-p-diammonium (DPDA). Utilizing photoluminescence, UV–visible absorption, vibrational spectroscopy, and in situ synchrotron powder X-ray diffraction, an isostructural phase transition is identified near 1.5 GPa, marked by a notable shift in photoluminescence intensity linked to free exciton emission. Synchrotron X-ray diffraction reveals significant anisotropic compression along the c-axis, while structural analysis indicates the rare phenomenon of reduced lead-iodide octahedral distortion below 2 GPa, contrasting with the increased octahedral distortion reported in most previous studies on lead-based 2D HOIPs. Density functional theory calculations elucidate the structural origins and mechanisms driving the pressure-induced phase transition and optoelectronic tuning. These findings underscore the critical interplay between rigid organic spacers and inorganic octahedra in modulating high-pressure optoelectronic properties, offering valuable insights for designing future 2D HOIPs with tailored functionalities.