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DOE OSTI2021

Nanoscale hydration in layered manganese oxides

Birnessite is a layered MnO2 mineral with a nanoscale interlayer region that accommodates layers of intercalated water. Variable distributions of Mn sites with oxidation states of II, III and IV are responsible for the high catalytic reactivity of birnessite in nature and as a valuable candidate for energy storage solutions. We here report water loading capabilities and the vibrational spectral signatures of two forms of birnessite of strongly contrasting particle size. Using X-ray diffraction we find that potassium-birnessite accommodates no more than one monolayer (1W) of water in its interlayer region. Molecular simulations show that this is an energetically favorable hydration state where interlayer potassium-water and direct water-birnessite interactions are greater than at other hydration levels. Simulations also suggest a stable 2W state but that is not achieved experimentally by contact with water vapor. Finally, this work provides a means to predict the distribution of adsorbed and interlayer water molecules using a recently developed composite model.

Cheng, Wei↗

DOE OSTI2021

Bridging the gap of storage ring light sources and linac-driven free-electron lasers

High-gain free-electron lasers (FELs) are driven by short, high-charge density electron beams as only produced at dedicated single pass or recirculating linear accelerators. We describe new conceptual, technical, and modeling solutions to produce subpicosecond, up to ~100 μJ-energy extreme ultra-violet and soft x-ray FEL pulses at high- and tunable repetition rates, from diffraction-limited storage ring light source. In contrast to previously proposed schemes, we show that lasing can be simultaneous to the standard multibunch radiation emission from short insertion devices, and that it can be obtained with limited impact on the storage ring infrastructure. By virtue of the high-average power but moderate pulse energy, the storage ring-driven high-gain FEL would open the door to unprecedented accuracy in time-resolved spectroscopic analysis of matter in the linear response regime, in addition to inelastic scattering experiments.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Quantum annealing-aided design of an ultrathin-metamaterial optical diode

Abstract Thin-film optical diodes are important elements for miniaturizing photonic systems. However, the design of optical diodes relies on empirical and heuristic approaches. This poses a significant challenge for identifying optimal structural models of optical diodes at given wavelengths. Here, we leverage a quantum annealing-enhanced active learning scheme to automatically identify optimal designs of 130 nm-thick optical diodes. An optical diode is a stratified volume diffractive film discretized into rectangular pixels, where each pixel is assigned to either a metal or dielectric. The proposed scheme identifies the optimal material states of each pixel, maximizing the quality of optical isolation at given wavelengths. Consequently, we successfully identify optimal structures at three specific wavelengths (600, 800, and 1000 nm). In the best-case scenario, when the forward transmissivity is 85%, the backward transmissivity is 0.1%. Electromagnetic field profiles reveal that the designed diode strongly supports surface plasmons coupled across counterintuitive metal–dielectric pixel arrays. Thereby, it yields the transmission of first-order diffracted light with a high amplitude. In contrast, backward transmission has decoupled surface plasmons that redirect Poynting vectors back to the incident medium, resulting in near attenuation of its transmission. In addition, we experimentally verify the optical isolation function of the optical diode.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Multiscale Modeling of Vinyl-Addition Polynorbornenes: The Effect of Stereochemistry

Vinyl-addition polynorbornenes are candidates for designing high-performance polymers due to unique characteristics, which include a high glass transition temperature associated with a rigid backbone. Recent studies have established that the processability and properties of these polymers can be fine-tuned by using targeted substitutions. However, synthesis with different catalysts results in materials with distinct properties, potentially due to the presence of various stereoisomers that are difficult to quantify experimentally. Herein, we develop all-atom models of polynorbornene oligomers based on classical force fields and density functional theory. To establish the relationship between chemical architecture, chain conformations, and melt structure, we perform detailed molecular dynamics simulations with the fine-tuned atomistic force field and propose simpler coarse-grained descriptions to address the high molecular weight limit. All-atom simulations of oligomers suggest high glass transition temperatures in the range of 550–600 K. In the melt state (800 K), meso chains form highly rigid extended coils (C∞≈11) with amorphous structural characteristics similar to the X-ray diffraction data observed in the literature. In contrast, simulations with racemo chains predict highly helical tubular chain conformations that could promote assembly into crystalline structures.

Polymer Science↗

NASA NTRS1983

Epitaxial growth of Hg/1-x/Cd/x/Te by chemical vapor transport

The chemical vapor transport technique was applied for the first time to the growth of Hg(1-x)Cd(x)Te epitaxial layers on CdTe substrates using a preannealed source material of Hg(0.8)Cd(0.2)Te. The experiment took place in a pretreated ampoule loaded with source material, HgI2 transport agent, and substrate and sealed under a residual pressure of about 10 to the -5th torr. The temperature of the source region was 590 C and that of the deposition zone 535 C with a nearly sigmoidal shaped profile between the end temperatures. The change in appearance of the substrate surface during the experiment is described, and the structures of the surface of the Hg(1-x)Cd(x)Te layer and of the layer itself as revealed by Nomarski contrast illumination and Laue X-ray diffraction, respectively, are discussed.

Wiedemeier, H.↗

NASA NTRS2014

Simulation of a Method to Directly Image Exoplanets Around Multiple Stars Systems

Direct imaging of extra-solar planets has now become a reality, especially with the deployment and commissioning of the first generation of specialized ground-based instruments such as the GPI, SPHERE, P1640 and SCExAO. These systems will allow detection of planets 107 times fainter than their host star. For space-based missions, such as EXCEDE, EXO-C, EXO-S, WFIRST/AFTA, different teams have shown in laboratories contrasts reaching 10(exp −10) within a few diffraction limits from the star using a combination of a coronagraph to suppress light coming from the host star and a wavefront control system. These demonstrations use a deformable mirror (DM) to remove residual starlight (speckles) created by the imperfections of telescope. However, all these current and future systems focus on detecting faint planets around a single host star or unresolved binaries/multiples, while several targets or planet candidates are located around nearby binary stars such as our neighbor star Alpha Centauri. Until now, it has been thought that removing the light of a companion star is impossible with current technology, excluding binary star systems from target lists of direct imaging missions. Direct imaging around binaries/multiple systems at a level of contrast allowing Earth-like planet detection is challenging because the region of interest, where a dark zone is essential, is contaminated by the light coming from the hosts star companion. We propose a method to simultaneously correct aberrations and diffraction of light coming from the target star as well as its companion star in order to reveal planets orbiting the target star. This method works even if the companion star is outside the control region of the DM (beyond its half-Nyquist frequency), by taking advantage of aliasing effects.

Multiple Stars↗

DOE OSTI2023

Speckle contrast of interfering fluorescence X-rays

With the development of X-ray free-electron lasers (XFELs), producing pulses of femtosecond durations comparable with the coherence times of X-ray fluorescence, it has become possible to observe intensity–intensity correlations due to the interference of emission from independent atoms. This has been used to compare durations of X-ray pulses and to measure the size of a focused X-ray beam, for example. Here it is shown that it is also possible to observe the interference of fluorescence photons through the measurement of the speckle contrast of angle-resolved fluorescence patterns. Speckle contrast is often used as a measure of the degree of coherence of the incident beam or the fluctuations of the illuminated sample as determined from X-ray diffraction patterns formed by elastic scattering, rather than from fluorescence patterns as addressed here. Commonly used approaches to estimate speckle contrast were found to suffer when applied to XFEL-generated fluorescence patterns due to low photon counts and a significant variation of the excitation pulse energy from shot to shot. A new method to reliably estimate speckle contrast under such conditions, using a weighting scheme, is introduced. The method is demonstrated by comparing the speckle contrast of fluorescence observed with pulses of 3 fs to 15 fs duration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRSDate not supplied

Multi-Star Wavefront Control: Update on Technology Development for Roman Space Telescope and Habitable Worlds Observatory

A majority of Sun-like stars have at least one stellar companion that can introduce additional noise into the field of view of any high-contrast imaging instrument, limiting the achievable contrast. These include high-quality target stars such as the A and B components of Alpha Centauri, our nearest stellar neighbor. Enabling direct imaging of binary stars has the potential to increase the scientific yield for coronagraphic instruments planned on NASA's future space missions and concepts, including the Roman Space Telescope and the Astro2020 IR/O/UV flagship. Multi-Star Wavefront Control (MSWC) is a wavefront-control technique that simultaneously removes the (mutually incoherent) stellar leakage from both stellar components, enabling direct imaging of planets in many binary star systems. MSWC is an algorithmic technique and can be used with existing wavefront control systems on coronagraphic instruments (as well as starshades if a deformable mirror is available in the optical path) including planned observations on the upcoming PICTURE-D balloon flight. We report on the latest experimental and numerical results obtained with MSWC as part of the technology development effort to demonstrate compatibility with existing high-contrast imaging platforms for this technique. We first report on functional tests carried out at Subaru's SCExAO instrument operating in-air and showing the sub-Nyquist mode at 4.1e-6 contrast in monochromatic light. The Super-Nyquist regime of MSWC was recently tested in vacuum at JPL's High Contrast Imaging Testbed (HCIT) on the Decadal Survey Testbed (DST) reaching 8.6e-9 contrast in a 10% band. We also report on results for the current stage of vacuum testing at HCIT's Occulting Mask Coronagraph (OMC) testbed using a mask similar to the contributed MSWC mask on the Roman Space Telescope's coronagraph instrument which has demonstrated suppression at the 9.8e-9 contrast at Super-Nyquist separations around the 3rd diffraction order and is planned to use a novel binary source simulator.

high-contrast imaging↗

DOE OSTI2026

Thin Film Synthesis of SrZn2P2 with SrI2 Post-Annealing for Enhanced Crystallinity and Optoelectronic Quality

Ternary Zintl phosphides are promising light-absorbing semiconductors for thin-film optoelectronic applications, but strategies for controlling their microstructure and optoelectronic quality remain underexplored. Here, we report the synthesis of phase-pure SrZn2P2 thin films using radio-frequency co-sputtering in a PH3 + Ar atmosphere and investigate the impact of post-growth processing on their structural and optical properties. Grazing-incidence X-ray scattering and Raman spectroscopy confirm the formation of crystalline SrZn2P2 films over a finite compositional window. Optical measurements reveal clear absorption near the direct-band-gap energy (~1.8 eV) and near-band-edge photoluminescence. Further, we have studied the effects of chemically compatible halide-assisted annealing. It is found that SrI2 treatments lead to pronounced grain growth and reduced diffraction peak broadening while preserving phase purity, in contrast to rapid thermal or forming-gas annealing. Notably, annealing with SrI2 at 450 degrees C significantly enhances both the intensity and spatial uniformity of the photoluminescence, thus connecting the observed microstructural consolidation with improved radiative recombination. Our study demonstrates that halide-assisted annealing provides an effective pathway for microstructural control in SrZn2P2 thin films and highlights a generalizable processing strategy for advancing Zintl phosphide semiconductors toward optoelectronic applications.

14 SOLAR ENERGY↗

NASA NTRS2021

Results From The Laboratory Demonstration Of A PIAACMC Coronagraph With A Segmented Aperture

The phase-induced amplitude apodization complex mask coronagraph (PIAACMC) provides high throughput and small inner working angle with little loss in image quality. Coronagraph compatibility with segmented apertures is essential for the success of habitable planet characterization with future large aperture space telescopes, such as the Large UV/Optical/Infrared (LUVOIR) and HabEx telescope mission concepts. The PIAACMC is compatible with such segmented telescope apertures with little loss of performance. We report the contrast and other performance results of a PIAACMC coronagraph with a LUVOIR-like pupil mask assembled and tested in a vacuum chamber at the JPL high contrast imaging testbed (HCIT). The goals of the demonstration were to achieve 1e-9 mean contrast over a semi-annular field of view from 2 λ/D to 8 λ/D, first with monochromatic light at 650nm, and then over a 10% spectral bandwidth. In addition, the measurement of jitter and its effect on PIAACMC performance will be discussed. As the success of electric field conjugation (EFC) to achieve best contrast on the testbed is dependent upon a diffraction model of the coronagraph, we will also discuss variations of the testbed and its diffraction model with the PIAACMC design, including suspected sources of knowledge error in the EFC diffraction model.

Wilson, Daniel↗

NASA NTRS2012

Beyond Kepler: Direct Imaging of Earth-like Planets

Is there another Earth out there? Is there life on it? People have been asking these questions for over two thousand years, and we finally stand on the verge of answering them. The Kepler space telescope is NASA's first mission designed to study Earthlike exoplanets (exo-Earths), and it will soon tell us how often exo-Earths occur in the habitable zones of their stars. The next natural step after Kepler is spectroscopic characterization of exo-Earths, which would tell us whether they possess an atmosphere, oxygen, liquid water, as well as other biomarkers. In order to do this, directly imaging an exo-Earth may be necessary (at least for Sun-like stars). Directly imaging an exo-Earth is challenging and likely requires a flagship-size optical space telescope with an unprecedented imaging system capable of achieving contrasts of 1(exp 10) very close to the diffraction limit. Several coronagraphs and external occulters have been proposed to meet this challenge and are in development. After first overviewing the history and current state of the field, my talk will focus on the work proceeding at the Ames Coronagraph Experiment (ACE) at the NASA Ames Research Center, where we are developing the Phase Induced Amplitude Apodization (PIAA) coronagraph in a collaboration with JPL. PIAA is a powerful technique with demonstrated aggressive performance that defines the state of the art at small inner working angles. At ACE, we have achieved contrasts of 2(exp -8) with an inner working angle of 2 lambda/D and 1(exp -6) at 1.4 lambda/D. On the path to exo-Earth imaging, we are also pursuing a smaller telescope concept called EXCEDE (EXoplanetary Circumstellar Environments and Disk Explorer), which was recently selected for technology development (Category III) by NASA's Explorer program. EXCEDE will do fundamental science on debris disks as well as serve as a technological and scientific pathfinder for an exo-Earth imaging mission.

Belikov, Ruslan↗

NASA NTRS2018

Technology and Opportunities of Photon Sieve CubeSat with Deployable Optical Membrane

A photon sieve (PS) is a revolutionary optical instrument that provides high resolution imaging at a fraction of the weight of typical telescopes, with an areal density of 0.3 kg/m2 compared to 25 kg/m2 for the James Webb Space Telescope. The photon sieve is a variation of a Fresnel Zone Plate consisting of many small holes arranged in a series of concentric rings. The sieve works by diffracting light of a certain wavelength to a specified focal point for imaging, so that only a specific wavelength can be imaged. Moreover, the better image contrast and higher signal-to-noise ratios come from suppressing higher diffracted orders by apodizing the number of pinholes in the outer rings. Finally, a photon sieve requires less supports and can withstand more deformation without a reduction in the imaging qualities. Due to these properties, various groups have created PS CubeSats for Earth and Sun imaging at a low cost and weight specifically using deployable technology. A team at the Air Force Research Laboratory created a design and prototype of a mechanism that deploys a 20 cm diameter photon sieve. The United States Air Force Laboratory used a similar design to create a CubeSat-based deployable photon sieve. The team at NASA Langley Research Center has researched photon sieves for conducting an Earth-observing experiment using LIDAR (Light Detection and Ranging) with a higher signal-to-noise ratio benefit from the PS. This paper provides a state of the art overview on existing PS CubeSat technology with deployable structures and applications. Especially, the paper introduces PS for LIDAR applications and discusses the CubeSat-based PS challenge being worked at the NASA Langley Research Center.

Hyun Jung Kim↗

NASA NTRS2011

Micro-Fresnel Zone Plate Optical Devices Using Densely Accumulated Ray Points

An embodiment generally relates to an optical device suitable for use with an optical medium for the storage and retrieval of data. The optical device includes an illumination means for providing a beam of optical radiation of wavelength .lamda. and an optical path that the beam of optical radiation follows. The optical device also includes a diffractive optical element defined by a plurality of annular sections. The plurality of annular sections having a first material alternately disposed with a plurality of annular sections comprising a second material. The diffractive optical element generates a plurality of focal points and densely accumulated ray points with phase contrast phenomena and the optical medium is positioned at a selected focal point or ray point of the diffractive optical element.

Choi, Sang H.↗

DOE OSTI2026

Itinerant Magnetism in Hydride-Synthesized CaCo 12 B 6

A new compound in the underexplored Ca–Co–B phase space has been discovered, validating high-throughput computations from the Open Quantum Materials Database, which predicted thermodynamic stability for CaCo 12 B 6 in the SrNi 12 B 6 structure type. The synthetic effects of different boron precursors and the advantages of using CaH 2 instead of Ca metal were demonstrated by the short synthesis duration and high purity of CaCo 12 B 6 , in contrast with traditional synthesis routes. Powder X-ray diffraction (PXRD) confirmed that CaCo 12 B 6 shares the SrNi 12 B 6 structure ( R $\bar{3}$m (#166), a = 9.469(4) Å, c = 7.468(2) Å, Z = 3) and is water- and air-stable. High-temperature in situ PXRD indicates that CaCo 12 B 6 is stable below 1050 K under vacuum in a silica capillary. CaCo 12 B 6 decomposes between 693 and 773 K during spark-plasma sintering. Density functional theory calculations indicate that CaCo 12 B 6 is metallic with a ferromagnetic ground state. X-ray absorption near-edge spectroscopy and Bader charge analysis indicate that Co atoms in CaCo 12 B 6 lack ionic character. Magnetometry reveals room-temperature paramagnetism with μ eff = 1.7(1)μ B per Co atom and a Weiss constant of +190(10)K. Ferromagnetic ordering occurs below 172(1)K, resulting in a saturation moment of 0.46 μ B per Co atom. Our findings demonstrate that the hydride route is a viable strategy for discovery of new ternary alkaline-earth-transition metal borides analogous to rare-earth-containing counterparts.

diffraction↗

DOE OSTI2021

Absolute contrast estimation for soft X-ray photon fluctuation spectroscopy using a variational droplet model

Abstract X-ray photon fluctuation spectroscopy using a two-pulse mode at the Linac Coherent Light Source has great potential for the study of quantum fluctuations in materials as it allows for exploration of low-energy physics. However, the complexity of the data analysis and interpretation still prevent recovering real-time results during an experiment, and can even complicate post-analysis processes. This is particularly true for high-spatial resolution applications using CCDs with small pixels, which can decrease the photon mapping accuracy resulting from the large electron cloud generation at the detector. Droplet algorithms endeavor to restore accurate photon maps, but the results can be altered by their hyper-parameters. We present numerical modeling tools through extensive simulations that mimic previous x-ray photon fluctuation spectroscopy experiments. By modification of a fast droplet algorithm, our results demonstrate how to optimize the precise parameters that lift the intrinsic counting degeneracy impeding accuracy in extracting the speckle contrast. These results allow for an absolute determination of the summed contrast from multi-pulse x-ray speckle diffraction, the modus operandi by which the correlation time for spontaneous fluctuations can be measured.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1970

Multipass holographic interferometer improves image resolution

Multipass holographic interferometer forms a hologram of high diffraction efficiency, and hence provides a bright and high contrast interferogram. It is used to study any effect which changes the index of refraction and to study surface deformations of a flat reflecting surface.

Brooks, R. E.↗

NASA NTRS2016

The Habitable Exoplanet (HabEx) imaging mission concept: preliminary science drivers and technical requirements

HabEx is one of 4 possible NASA flagship mission concepts studied for a possible launch in the 2030s. It will be optimized for direct imaging and spectroscopy of habitable exoplanets, and will also enable a wide range of general astrophysics observations. HabEx shall characterize full planetary systems around nearby solar-type stars for the first time, including rocky planets, possible water worlds, gas giants, ice giants, and faint circumstellar debris disks. It will in particular explore our nearest neighbor planetary systems and search for signs of habitability and bio-signatures in the atmospheres of rocky planets. Such high spatial resolution high contrast observations require a large (~3.5 to 8m) stable diffraction- limited optical space telescope, which also opens new unique capabilities for studying the formation and evolution of stars and galaxies. We present here some preliminary science objectives identified for HabEx by our Science and Technology Definition Team (STDT), together with a first look at the key challenges and design trades ahead.

Mennesson, Bertrand↗

DOE OSTI2021

Quasiclassical Computations of Compton-Scattered Spectra

Quality X-ray sources are crucial to fundamental physics research, medical radiology, humanities research, and materials science. While synchrotron radiation (SR) facilities produce the state-of-the-art emissions with respect to brilliance and frequency tunability, the great expense required to build, maintain, and operate these structures greatly limits their accessibility to researchers. Much of the research conducted at SR facilities, however, may be conducted with inverse Compton sources (ICS). Accelerator-based Compton scattering light sources generate high-energy, high-brilliance emissions. Compton scattering is the process by which a photon scatters o? an electron. ICS offer an affordable, in-lab alternative to SR facilities. Even though SR facilities produce greater intensity emissions, Compton sources provide the same frequency tunability at the intensities suitable for the purposes of many researchers currently fighting for time at SR facilities, i.e., ICS provides intensities suitable for contrast imaging, X-ray fluorescence, X-ray-diffraction, and X-ray spectroscopy. The focus of this work is to create computational models to simulate Compton-scattered spectra. These models have been used to build a theoretical basis for methods of improving the quality of future Compton sources and to preform diagnostic analysis of existing light sources. The theoretical basis of each model is derived from first principles. The numerical methods employed by each model are defined. A full description of the various functionalities of each code will be addressed. Furthermore, an in-depth analysis of spectral bandwidth sources is discussed. The complex physics arising from an extremely high-intensity, nonlinear laser pulse is explored in detail. Methods of frequency modulation of the incident laser, i.e., a method for correcting the nonlinear broadening effects on the scattered spectrum, will also be discussed. The work will conclude with a an exploration of the ongoing research efforts regarding regimes of operation outside of the limits of these current models.

Johnson, Erik↗