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NASA NTRS2004

Imaging of gamma-Irradiated Regions of a Crystal

A holographic technique has been devised for generating a visible display of the effect of exposure of a photorefractive crystal to gamma rays. The technique exploits the space charge that results from trapping of electrons in defects induced by gamma rays. The technique involves a three-stage process. In the first stage, one writes a holographic pattern in the crystal by use of the apparatus shown in Figure 1. A laser beam of 532-nm wavelength is collimated and split into signal and reference beams by use of a polarizing beam splitter. On its way to the crystal, the reference beam goes through a two-dimensional optical scanner that contains two pairs of lenses (L1y, L2y and L1x,L2x) and mirrors M1 and M2, which can be rotated by use of micrometer drives to make fine adjustments. The signal beam is sent through a spatial light modulator that imposes the holographic pattern, then through two imaging lenses L(sub img) on its way to the crystal. An aperture is placed at the common focus of lenses Limg to suppress high-order diffraction from the spatial light modulator. The hologram is formed by interference between the signal and reference beams. A camera lens focuses an image of the interior of the crystal onto a charge-coupled device (CCD). If the crystal is illuminated by only the reference beam once the hologram has been formed, then an image of the hologram is formed on the CCD: this phenomenon is exploited to make visible the pattern of gamma irradiation of the crystal, as described next. In the second stage of the process, the crystal is removed from the holographic apparatus and irradiated with rays at a dose of about 100 krad. In the third stage of the process, the crystal is remounted in the holographic apparatus in the same position as in the first stage and illuminated with only the reference beam to obtain the image of the hologram as modified by the effect of the rays. The orientations of M1 and M2 can be adjusted slightly, if necessary, to maximize the intensity of the image. Figure 2 shows such an image that was formed in a crystal of Fe:LiNbO3.

Dragoi, Danut↗

NASA NTRS2007

Efficient Generation of Truncated Bessel Beams using Cylindrical Waveguides

In this paper we address efficient conversion between a Gaussian beam (a truncated plane wave) and a truncated Bessel beam of agiven order, using cylindrical optical waveguides and whispering gallery mode resonators. Utilizing a generator based on waveguides combined with whispering gallery mode resonators, we have realized Bessel beams of the order of 200 with a conversion efficiency exceeding 10 %.

laser beam shaping↗

DOE OSTI2023

Temperature-Dependent Optical and Structural Properties of Chiral Two-Dimensional Hybrid Lead-Iodide Perovskites

Layered hybrid halide perovskites gain chirality via the incorporation of chiral organic cations in the spacer layer. These so-called chiral two-dimensional (2D) halide perovskites have attracted considerable interest recently for chiral optoelectronic, spintronic, and ferroelectric applications. However, the effect of temperature on these materials, especially how the structure changes with temperature and its impact on the chiral optoelectronic properties, remains an open question. Here, we study the effect of temperature change on chiral optoelectronic and structural properties through temperature-dependent circularly polarized photoluminescence (CPPL) microscopy and synchrotron powder X-ray diffraction as well as pair distribution function analysis to elucidate the intrinsic chiral optoelectronic and structural variations for R-, S-, and racemic-methylbenzylamine lead iodide. Here our results show that the temperature-induced band gap changes indicate a strong electron–phonon coupling compared to the thermal-induced lattice expansion in chiral 2D perovskites. From powder diffraction measurements, a monotonic lattice expansion is observed on heating with no structural phase transitions over 90–360 K detected for the three samples studied herein. Locally, a strongly anisotropic and even negative expansion in some components of the instantaneous Pb–I pair-distance distribution is suggestive of coupling between dynamical intralayer distortions and lattice expansion. This work provides insights into the fundamental understanding of the temperature effect on chiral optoelectronic and structural properties of chiral 2D perovskites, which can lead to new chiral materials design strategies for future chiral optoelectronic applications.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Unprecedented lattice volume expansion on doping stereochemically active Pb 2+ into uniaxially strained structure of CaBa 1- x Pb x Zn 2 Ga 2 O 7

Lone pair cations like Pb 2+ are extensively utilized to modify and tune physical properties, such as nonlinear optical property and ferroelectricity, of some specific structures owing to their preference to adopt a local distorted coordination environment. Here we report that the incorporation of Pb 2+ into the polar “114”-type structure of CaBaZn 2 Ga 2 O 7 leads to an unexpected cell volume expansion of CaBa 1- x Pb x Zn 2 Ga 2 O 7 (0 ≤ x ≤ 1), which is a unique structural phenomenon in solid state chemistry. Structure refinements against neutron diffraction and total scattering data and theoretical calculations demonstrate that the unusual evolution of the unit cell for CaBa 1- x Pb x Zn 2 Ga 2 O 7 is due to the combination of the high stereochemical activity of Pb 2+ with the extremely strained [Zn 2 Ga 2 O 7 ] 4- framework along the c -axis. The unprecedented cell volume expansion of the CaBa 1- x Pb x Zn 2 Ga 2 O 7 solid solution in fact is a macroscopic performance of the release of uniaxial strain along c -axis when Ba 2+ is replaced with smaller Pb 2+ .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Liquid crystalline behavior and photoluminescence of lanthanide decanoate nanoparticles synthesized by microwave radiation

Luminescent lanthanide decanoate nanoparticles (LnC 10 NPs; Ln = Pr, Nd, Sm, Eu, Gd, Er) with spherical morphology (<100 nm) have been synthesized via a facile microwave (MWV) method using Ln(NO 3 ) 3 ·xH 2 O, ethanol/water, and decanoic acid. These hybrid nanomaterials adopt a lamellar structure consisting of inorganic Ln 3+ layers separated by a decanoate anion bilayer and exhibit liquid crystalline (LC) phases during melting. The particle size, crystalline structure, and LC behavior were characterized using transmission electron microscopy (TEM), differential scanning calorimetry (DSC), and powder X-ray diffraction (ambient and heated). Thermal analysis indicated the formation of Smectic A LC phases by LnC 10 nanoparticles, with the smaller lanthanides (Ln = Sm, Gd, Er) displaying additional solid intermediate and Smectic C phases. The formation of LC phases by the smaller Ln 3+ suggests that these nanoscale materials have vastly different thermal properties than their bulk counterparts, which do not exhibit LC behavior. In this work, photoluminescence spectroscopy revealed the LnC 10 NPs to be highly optically active, producing strong visible emissions that corresponded to expected electronic transitions by the various Ln 3+ ions. Under long-wave UV irradiation (λ = 365 nm), bright visible luminescence was observed for colloidal suspensions of Nd, Sm, Eu, Gd, and ErC 10 NPs. To the best of the authors’ knowledge, this is the first reported synthesis of nanoscale metal alkanoates, the first report of liquid crystalline behavior by any decanoate of lanthanides smaller than Nd, and the first observation of strong visible luminescence by non-vitrified lanthanide alkanoates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Nonmonotonic-potential description of polarization effects, fusion, and nuclear rainbows in elastic scattering of 6 Li + 12 C at 4.5–600 MeV

The experimental differential cross-section (CS) and analyzing power (AP) data of the 6 Li + 12 C elastic scattering over a wide laboratory energy scale (4.5MeV≤𝐸 lab ≤600MeV) are analyzed within the framework of the optical model (OPM) using nonmonotonic (NM) nucleus–nucleus potentials. The real part of the NM potentials is derived from the Pauli-embodied energy density-functional (EDF) formalism with the sudden approximation. The real part of the noncentral spin-orbit and tensor terms, as well as the imaginary parts, are treated phenomenologically. The effect of the radius of sensitivity on the CS and AP data is found to be more important at lower energies. The diffractive and refractive scattering with Airy structures in the whole angular region of the elastic scattering across the studied energy range is successfully described within the OPM using the NM 6 Li + 12 C potential. The near- and far-side (N and F) decomposition of the total elastic-scattering amplitudes has also been studied using our NM potentials. The evolution of the Airy minima in the angular distributions, coupled with the fitting of the AP data, provides an accurate description of Airy minima of different orders. The OPM calculations with the NM potentials describe exceptionally well the CS, vector analyzing power (VAP), and tensor analyzing power data at 𝐸 lab =9.0,19.24,20,30, and 50MeV. In agreement with our past successful descriptions of CS and the opposite signs of the VAP data for the 6 Li and 7 Li elastic scattering using NM potentials in OPM, the present results appear to provide a better fit, so far, than those obtained from the coupled-channels method. The fusion cross sections of 6 Li + 12 C have been predicted in the energy range (4.5MeV≤𝐸 lab ≤20MeV), fitting the experimental data well in the range 𝐸 lab =2.97–11.77MeV. The EDF potential without any energy dependence and renormalization is also found to describe satisfactorily the experimental CS and AP data at energies up to several hundreds of MeV.

6 ≤ A ≤ 19↗

DOE OSTI2024

Atmospheric clearing of solid-particle debris using femtosecond filaments

Through nonlinear self-focusing, femtosecond pulses can propagate several kilometers beyond diffraction limits, forming an ionization channel in air known as a laser filaments. It has been demonstrated that in the wake of the filament, aerosols can be effectively cleared to improve the transmission of subsequent laser pulses or secondary light sources, pertinent to applications in atmospheric sensing. However, the current understanding of aerosol clearing is founded on interactions with droplets to simulate fogs and clouds and thus does not extend to solid particles or atmospheric debris. Using optical trapping, we isolate both graphite and silica microparticles and directly measure the subsequent displacement caused by the filament using time-resolved shadowgraphy. The shock wave from the filament is demonstrated to propel particles away from the filament, directly contributing to atmospheric debris clearing. Particles exposed to the laser light in either the intense filament core or the surrounding energy reservoir are axially displaced along the beam path. Furthermore, it is found that the optomechanical properties of the particle largely influence the axial displacement induced by laser exposure through mechanisms such as radiation pressure, mass ejection from ablation or optical damage, and particle deagglomeration.

42 ENGINEERING↗

NASA NTRS1991

High quality flame deposited diamond films for infrared optical windows

The IR absorption in polycrystalline diamond films deposited in oxygen-acetylene flames is characterized using FTIR. The one-phonon absorption coefficient in the region from 7 to 12 microns that is related to extrinsic defects in the diamond films shows a strong dependence on the flame conditions as well as the substrate temperature. A high degree of diamond crystalline perfection, as judged from the undetectable one-phonon absorption, is achieved under the optimized deposition conditions for our flame setup. This is further supported by the sharp Raman peak at 1332/cm as well as the high purity in crystal orientation according to the X-ray diffraction pattern measured for the high quality diamond films.

Tzeng, Y.↗

NASA NTRS2007

Extended-Range Ultrarefractive 1D Photonic Crystal Prisms

A proposal has been made to exploit the special wavelength-dispersive characteristics of devices of the type described in One-Dimensional Photonic Crystal Superprisms (NPO-30232) NASA Tech Briefs, Vol. 29, No. 4 (April 2005), page 10a. A photonic crystal is an optical component that has a periodic structure comprising two dielectric materials with high dielectric contrast (e.g., a semiconductor and air), with geometrical feature sizes comparable to or smaller than light wavelengths of interest. Experimental superprisms have been realized as photonic crystals having three-dimensional (3D) structures comprising regions of amorphous Si alternating with regions of SiO2, fabricated in a complex process that included sputtering. A photonic crystal of the type to be exploited according to the present proposal is said to be one-dimensional (1D) because its contrasting dielectric materials would be stacked in parallel planar layers; in other words, there would be spatial periodicity in one dimension only. The processes of designing and fabricating 1D photonic crystal superprisms would be simpler and, hence, would cost less than do those for 3D photonic crystal superprisms. As in 3D structures, 1D photonic crystals may be used in applications such as wavelength-division multiplexing. In the extended-range configuration, it is also suitable for spectrometry applications. As an engineered structure or artificially engineered material, a photonic crystal can exhibit optical properties not commonly found in natural substances. Prior research had revealed several classes of photonic crystal structures for which the propagation of electromagnetic radiation is forbidden in certain frequency ranges, denoted photonic bandgaps. It had also been found that in narrow frequency bands just outside the photonic bandgaps, the angular wavelength dispersion of electromagnetic waves propagating in photonic crystal superprisms is much stronger than is the angular wavelength dispersion obtained by use of conventional prisms and diffraction gratings and is highly nonlinear.

Ting, David Z.↗

DOE OSTI2024

Piezochromic Behavior of 2,4,6-Triphenylpyrylium Tetrachloroferrate

In advanced photonics, there is a growing interest in piezochromic luminescent materials that exhibit multicolor switching, driven by their potential applications in optical recording, memory, and sensors. Here, the piezochromic behavior of 2,4,6-triphenylpyrylium tetrachloroferrate (Py-FeCl 4 ) under high pressures from 0 to 9 GPa is reported. The observed multicolor changing properties of Py-FeCl 4 (yellow–orange–red–maroon–black) are found to be fully reversible upon decompression to ambient conditions. The mechanism of Py-FeCl 4 piezochromism is investigated via Raman, infrared, and UV–vis spectroscopy combined with powder X-ray Diffraction. The absence of structural phase transitions as well as the abrupt shifts of bandgap values together with characteristic Raman and IR peaks within 0-9 GPa suggests that the Py-FeCl 4 multicoloring switching behavior is driven by an electron transfer between the inorganic FeCl 4 – anion and the organic pyrylium cation. The obtained results demonstrate that Py-FeCl 4 dye is a good candidate for developing high-pressure sensing technologies designed to function in extreme environments. Moreover, due to the inherent role of molecular-structure relationships in the pyrylium salt's photophysical properties, findings suggest the potential discovery of piezochromic behavior in other pyrylium compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

FeSi 4 P 4 and CoSi 3 P 3 : Hidden Gems of Ternary Tetrel Pnictides with Outstanding Nonlinear Optical Properties

Metal silicon phosphides have shown promise as nonlinear optical materials. To be practically useful and cheap, earth-abundant 3d transition metals are preferred over their scarcer and more expensive 4d and 5d counterparts. Here, we developed a synthetic method to produce polycrystalline bulk powders and millimeter-sized single crystals of ternary compounds FeSi 4 P 4 and CoSi 3 P 3 . Both studied compounds have noncentrosymmetric and chiral crystal structures with ordered Si/P arrangements as was confirmed by single-crystal X-ray diffraction and solid-state NMR. Despite the presence of the transition metal, FeSi 4 P 4 and CoSi 3 P 3 are semiconductors with direct band gaps of 1.3 and 1.6 eV, respectively, indicating low-spin d 6 electronic configuration for octahedral Fe 2+ and Co 3+ . Relative to reported sulfide materials, FeSi 4 P 4 and CoSi 3 P 3 small band gap semiconductors demonstrate an outstanding combination of second-harmonic generation (SHG) activity and laser damage threshold (LDT). Both studied materials are phase-matchable with a 2.09 μm laser and not only exhibit 2.5–3.0 times stronger SHG signal than that of the state-of-the-art AgGaS 2 standard but also demonstrate an LDT response of 2.3–2.5 times higher than that of AgGaS 2 (at 1.09 μm laser with a pulse width of 10 ns)-which is unprecedented for small band gap semiconductors.

36 MATERIALS SCIENCE↗

NASA NTRS1992

Transmission Of Power Via Combined Laser Beams

Laser Diode Array (LDA) appears to be most efficient means of transferring power from Earth to satellites and between satellites, in terms of mass and size, of various laser configurations. To form large-scale-array amplifier (LSAA), element LDA's must generate well-defined diffraction-limited beams. Coherent matching of phases among LDA's enables system to generate good beam pattern in far field over thousands of kilometers. By passing beam from master laser through number of LDA amplifiers simultaneously, one realizes coherence among amplified output beams. LSAA used for transmission of power with efficiency of approximately 80 percent into receiver of moderate size at 5,000 km. Also transmits data at high rates by line-of-sight rather than fiber optics.

Kwon, Jin H.↗

NASA NTRS2009

Spatial Modulation Improves Performance in CTIS

Suitably formulated spatial modulation of a scene imaged by a computed-tomography imaging spectrometer (CTIS) has been found to be useful as a means of improving the imaging performance of the CTIS. As used here, "spatial modulation" signifies the imposition of additional, artificial structure on a scene from within the CTIS optics. The basic principles of a CTIS were described in "Improvements in Computed- Tomography Imaging Spectrometry" (NPO-20561) NASA Tech Briefs, Vol. 24, No. 12 (December 2000), page 38 and "All-Reflective Computed-Tomography Imaging Spectrometers" (NPO-20836), NASA Tech Briefs, Vol. 26, No. 11 (November 2002), page 7a. To recapitulate: A CTIS offers capabilities for imaging a scene with spatial, spectral, and temporal resolution. The spectral disperser in a CTIS is a two-dimensional diffraction grating. It is positioned between two relay lenses (or on one of two relay mirrors) in a video imaging system. If the disperser were removed, the system would produce ordinary images of the scene in its field of view. In the presence of the grating, the image on the focal plane of the system contains both spectral and spatial information because the multiple diffraction orders of the grating give rise to multiple, spectrally dispersed images of the scene. By use of algorithms adapted from computed tomography, the image on the focal plane can be processed into an image cube a three-dimensional collection of data on the image intensity as a function of the two spatial dimensions (x and y) in the scene and of wavelength (lambda). Thus, both spectrally and spatially resolved information on the scene at a given instant of time can be obtained, without scanning, from a single snapshot; this is what makes the CTIS such a potentially powerful tool for spatially, spectrally, and temporally resolved imaging. A CTIS performs poorly in imaging some types of scenes in particular, scenes that contain little spatial or spectral variation. The computed spectra of such scenes tend to approximate correct values to within acceptably small errors near the edges of the field of view but to be poor approximations away from the edges. The additional structure imposed on a scene according to the present method enables the CTIS algorithms to reconstruct acceptable approximations of the spectral data throughout the scene.

Bearman, Gregory H.↗

DOE OSTI2024

Electron-beam-based Compton scattering x-ray source for probing high-energy-density physics

The physics basis for an electron-beam-based Compton scattering x-ray source is investigated for single-shot experiments at the major high-energy-density facilities, such as the Omega Laser Facility, National Ignition Facility, and Z pulsed power facility. A source of monoenergetic ( δ ε / ε < 5 % ) 10- to 50-keV x rays can be produced by scattering of a short-pulse optical laser by a 23- to 53-MeV electron beam and collimating the scattered photons. The number and spectrum of scattered photons are calculated as a function of electron packet charge, electron and laser pulse duration, laser intensity, and collision geometry. A source delivering greater than 10 10 photons in a 1-mm-radius spot and 100-ps time resolution is plausible with the available electron gun and laser technology. Applications of this source for x-ray diffraction, x-ray imaging, x-ray absorption fine structure, and x-ray absorption spectroscopy in high-energy-density physics experiments are described, demonstrating significant advancements compared to the present state of the art. Published by the American Physical Society 2024

47 OTHER INSTRUMENTATION↗

NASA NTRS2003

Laboratory and In-Flight In-Situ X-ray Imaging and Scattering Facility for Materials, Biotechnology and Life Sciences

We propose a multifunctional X-ray facility for the Materials, Biotechnology and Life Sciences Programs to visualize formation and behavior dynamics of materials, biomaterials, and living organisms, tissues and cells. The facility will combine X-ray topography, phase micro-imaging and scattering capabilities with sample units installed on the goniometer. This should allow, for the first time, to monitor under well defined conditions, in situ, in real time: creation of imperfections during growth of semiconductors, metal, dielectric and biomacromolecular crystals and films, high-precision diffraction from crystals within a wide range of temperatures and vapor, melt, solution conditions, internal morphology and changes in living organisms, tissues and cells, diffraction on biominerals, nanotubes and particles, radiation damage, also under controlled formation/life conditions. The system will include an ultrabright X-ray source, X-ray mirror, monochromator, image-recording unit, detectors, and multipurpose diffractometer that fully accommodate and integrate furnaces and samples with other experimental environments. The easily adjustable laboratory and flight versions will allow monitoring processes under terrestrial and microgravity conditions. The flight version can be made available using a microsource combined with multilayer or capillary optics.

Source record↗

DOE OSTI2021

Tunable Broad Light Emission from 3D “Hollow” Bromide Perovskites through Defect Engineering

We report hybrid halide perovskites consisting of corner-sharing metal halide octahedra and small cuboctahedral cages filled with counter cations have proven to be prominent candidates for many high-performance optoelectronic devices. The stability limits of their three-dimensional perovskite framework are defined by the size range of the cations present in the cages of the structure. In some cases, the stability of the perovskite-type structure can be extended even when the counterions violate the size and shape requirements, as is the case in the so-called "hollow" perovskites. In this work, we engineered a new family of 3D highly defective yet crystalline "hollow" bromide perovskites with general formula (FA) 1-x (en) x (Pb) 1-0.7x (Br) 3-0.4x (FA = formamidinium (FA + ), en = ethylenediammonium (en 2+ ), x = 0-0.44). Pair distribution function analysis shed light on the local structural coherence, revealing a wide distribution of Pb-Pb distances in the crystal structure as a consequence of the Pb/Br-deficient nature and en inclusion in the lattice. By manipulating the number of Pb/Br vacancies, we finely tune the optical properties of the pristine FAPbBr 3 by blue shifting the band gap from 2.20 to 2.60 eV for the x = 0.42 en sample. A most unexpected outcome was that at x > 0.33 en incorporation, the material exhibits strong broad light emission (1% photoluminescence quantum yield (PLQY)) that is maintained after exposure to air for more than a year. This is the first example of strong broad light emission from a 3D hybrid halide perovskite, demonstrating that meticulous defect engineering is an excellent tool for customizing the optical properties of these semiconductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1993

The interaction of atomic oxygen with copper: An XPS, AES, XRD, optical transmission, and stylus profilometry study

The University of Alabama in Huntsville (UAH) experiment A-0114 was designed to study the reaction of material surfaces with low earth orbits (LEO) atmospheric oxygen. The experiment contained 128 one-inch circular samples; metals, polymers, carbons, and semiconductors. Half of these samples were exposed on the front of the Long Duration Exposure Facility (LDEF) and remaining on the rear. Among metal samples, copper has shown some interesting new results. There were two forms of copper samples: a thin film sputter-coated on fused silica and a solid piece of OFHC copper. They were characterized by x-ray and Auger electron spectroscopies, x-ray diffraction, and high resolution profilometry. Cu 2p core level spectra were used to demonstrate the presence of Cu2O and CuO and to determine the oxidation states.

Raikar, Ganesh N.↗

DOE OSTI2021

Multifunctional two-dimensional metal-organic frameworks for radionuclide sequestration and detection

Two lanthanide containing porous coordination polymers, [Ln2(bpdc)6(phen)2] · nH2O (1) and [Ln2(bpdc)6(terpy)2] · 3H2O (2) (Ln = either Pr, Nd or Sm-Dy); bpdc: 2,2'-bipyridine-5,5'-dicarboxylic acid, phen: 1,10-phenanthroline, and terpy: 2,2':6',2''-terpyridine, have been hydrothermally synthesized and structurally characterized by powder and single crystal X-ray diffraction. The crystallographic analyses reveal compounds 1 and 2 feature Ln3+ containing dimeric nodes that form a porous two-dimensional (2D) and non-porous three-dimensional (3D) framework, respectively. Each material is stable in aqueous media between pH 3-10 and exhibits modest thermal stability to ~400ºC. Notably, a portion of the phen and bpdc ligands in 1 can be removed thermally, without compromising the crystal structure, causing the surface area and pore volume to increase. The optical properties of 1 and 2 with Gd3+, Sm3+, Tb3+, and Eu3+ were explored in the solid-state using absorbance, fluorescence, and lifetime spectroscopies. The analyses reveal a complex blend of metal and ligand emission in the materials containing Sm3+ and Tb3+, while those featuring Eu3+ are dominated by intense metal-based emission. Compound 1 with Eu3+ displayed promise for the capture and detection of the uranyl cation, (UO2)2+, from aqueous media. In short, uranyl capture was observed at pH 4 and the adsorption thereof was detectable via vibrational and fluorescence spectroscopies and colorimetrically as the off-white color of 1 turned yellow with uptake. Finally, both 1 and 2 with Eu3+ produce bright red emission upon irradiation with Cu ka X-ray radiation (8.04 keV) and are candidate materials for applications in solid-state scintillation.

Surbella, Robert G.↗

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