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At least 325 records · Page 18

Photoabsorption Imaging at Nanometer Scales Using Secondary Electron Analysis

Optical imaging with nanometer resolution offers fundamental insights into light–matter interactions. Traditional optical techniques are diffraction limited with a spatial resolution >100 nm. Optical super-resolution and cathodoluminescence techniques have higher spatial resolutions, but these approaches require the sample to fluoresce, which many materials lack. Here, we introduce photoabsorption microscopy using electron analysis, which involves spectrally specific photoabsorption that is locally probed using a scanning electron microscope, whereby a photoabsorption-induced surface photovoltage modulates the secondary electron emission. We demonstrate spectrally specific photoabsorption imaging with sub-20 nm spatial resolution using silicon, germanium, and gold nanoparticles. Theoretical analysis and Monte Carlo simulations are used to explain the basic trends of the photoabsorption-induced secondary electron signal. Based on our current experiments and this analysis, we expect that the spatial resolution can be further improved to a few nanometers, thereby offering a general approach for nanometer-scale optical spectroscopic imaging and material characterization.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Characterization of X-Ray Diffraction System with a Microfocus X-Ray Source and a Polycapillary Optic

We present here an optimized microfocus x-ray source and polycapillary optic system designed for diffraction of small protein crystals. The x-ray beam is formed by a 5.5mm focal length capillary collimator coupled with a 40 micron x-ray source operating at 46Watts. Measurements of the x-ray flux, the divergence and the spectral characteristics of the beam are presented, This optimized system provides a seven fold greater flux than our recently reported configuration [M. Gubarev, et al., J. of Applied Crystallography (2000) 33, in press]. We now make a comparison with a 5kWatts rotating anode generator (Rigaku) coupled with confocal multilayer focusing mirrors (Osmic, CMF12- 38Cu6). The microfocus x-ray source and polycapillary collimator system delivers 60% of the x-ray flux from the rotating anode system. Additional ways to improve our microfocus x-ray system, and thus increase the x-ray flux will be discussed.

Gubarev, Mikhail↗

Monocrystalline Silicon and the Meta-Shell Approach to Building X-Ray Astronomical Optics

Angular resolution and photon-collecting area are the two most important factors that determine the power of an X-ray astronomical telescope. The grazing incidence nature of X-ray optics means that even a modest photon-collecting area requires an extraordinarily large mirror area. This requirement for a large mirror area is compounded by the fact that X-ray telescopes must be launched into, and operated in, outer space, which means that the mirror must be both lightweight and thin. Meanwhile the production and integration cost of a large mirror area determines the economical feasibility of a telescope. In this paper we report on a technology development program whose objective is to meet this three-fold requirement of making astronomical X-ray optics: (1) angular resolution, (2) photon-collecting area, and (3) production cost. This technology is based on precision polishing of monocrystalline silicon for making a large number of mirror segments and on the meta-shell approach to integrate these mirror segments into a mirror assembly. The meta-shell approach takes advantage of the axial or rotational symmetry of an X-ray telescope to align and bond a large number of small, lightweight mirrors into a large mirror assembly. The most important features of this technology include: (1) potential to achieve the highest possible angular resolution dictated by optical design and diffraction; and (2) capable of implementing every conceivable optical design, such as Wolter-I, Wolter-Schwarzschild, as well as other variations to one or another aspect of a telescope. The simplicity and modular nature of the process makes it highly amenable to mass production, thereby making it possible to produce very large X-ray telescopes in a reasonable amount of time and at a reasonable cost. As of June 2017, the basic validity of this approach has been demonstrated by finite element analysis of its structural, thermal, and gravity release characteristics, and by the fabrication, alignment, bonding, and X-ray testing of mirror modules. Continued work in the coming years will raise the technical readiness of this technology for use by SMEX, MIDEX, Probe, as well as major flagship missions.

Zhang, William W.↗

A uniform geometrical optics and an extended uniform geometrical theory of diffraction for evaluating high frequency EM fields near smooth caustics and composite shadow boundaries

A uniform geometrical optics (UGO) and an extended uniform geometrical theory of diffraction (EUTD) are developed for evaluating high frequency electromagnetic (EM) fields within transition regions associated with a two and three dimensional smooth caustic of reflected rays and a composite shadow boundary formed by the caustic termination or the confluence of the caustic with the reflection shadow boundary (RSB). The UGO is a uniform version of the classic geometrical optics (GO). It retains the simple ray optical expressions of classic GO and employs a new set of uniform reflection coefficients. The UGO also includes a uniform version of the complex GO ray field that exists on the dark side of the smooth caustic. The EUTD is an extension of the classic uniform geometrical theory of diffraction (UTD) and accounts for the non-ray optical behavior of the UGO reflected field near caustics by using a two-variable transition function in the expressions for the edge diffraction coefficients. It also uniformly recovers the classic UTD behavior of the edge diffracted field outside the composite shadow boundary transition region. The approach employed for constructing the UGO/EUTD solution is based on a spatial domain physical optics (PO) radiation integral representation for the fields which is then reduced using uniform asymptotic procedures. The UGO/EUTD analysis is also employed to investigate the far-zone RCS problem of plane wave scattering from two and three dimensional polynomial defined surfaces, and uniform reflection, zero-curvature, and edge diffraction coefficients are derived. Numerical results for the scattering and diffraction from cubic and fourth order polynomial strips are also shown and the UGO/EUTD solution is validated by comparison to an independent moment method (MM) solution. The UGO/EUTD solution is also compared with the classic GO/UTD solution. The failure of the classic techniques near caustics and composite shadow boundaries is clearly demonstrated and it is shown that the UGO/EUTD results remain valid and uniformly reduce to the classic results away from the transition regions. Mathematical details on the asymptotic properties and efficient numerical evaluation of the canonical functions involved in the UGO/EUTD expressions are also provided.

Constantinides, E. D.↗

On the convergence of the coupled-wave approach for lamellar diffraction gratings

Among the many existing rigorous methods for analyzing diffraction of electromagnetic waves by diffraction gratings, the coupled-wave approach stands out because of its versatility and simplicity. It can be applied to volume gratings and surface relief gratings, and its numerical implementation is much simpler than others. In addition, its predictions were experimentally validated in several cases. These facts explain the popularity of the coupled-wave approach among many optical engineers in the field of diffractive optics. However, a comprehensive analysis of the convergence of the model predictions has never been presented, although several authors have recently reported convergence difficulties with the model when it is used for metallic gratings in TM polarization. Herein, three points are made: (1) in the TM case, the coupled-wave approach converges much slower than the modal approach of Botten et al; (2) the slow convergence is caused by the use of Fourier expansions for the permittivity and the fields in the grating region; and (3) is manifested by the slow convergence of the eigenvalues and the associated modal fields. The reader is assumed to be familiar with the mathematical formulations of the coupled-wave approach and the modal approach.

Li, Lifeng↗

Crystalline Colloidal Arrays in Polymer Matrices

Crystalline Colloidal Arrays (CCA, also known as colloidal crystals), composed of aqueous or nonaqueous dispersions of self-assembled nanosized polymer colloidal spheres, are emerging toward the development of advanced optical devices for technological applications. The spontaneous self assembly of polymer spheres in a dielectric medium results from the electrostatic repulsive interaction between particles of uniform size and charge distribution. In a way similar to atomic crystals that diffract X-rays, CCA dispersions in thin quartz cells selectively and efficiently Bragg diffract the incident visible light. The reason for this diffraction is because the lattice (body or face centered cubic) spacing is on the order of the wavelength of visible light. Unlike the atomic crystals that diffract a fixed wavelength, colloidal crystals in principle, depending on the particle size, particle number and charge density, can diffract W, Vis or IR light. Therefore, the CCA dispersions can be used as laser filters. Besides, the diffraction intensity depends on the refractive index mismatch between polymer spheres and dielectric medium; therefore, it is possible to modulate incident light intensities by manipulating the index of either the spheres or the medium. Our interest in CCA is in the fabrication of all-optical devices such as optical switches, limiters, and spatial light modulators for optical signal processing. The two major requirements from a materials standpoint are the incorporation of suitable nonlinear optical materials (NLO) into polymer spheres which will allow us to alter the refractive index of the spheres by intense laser radiation, and preparation of solid CCA filters which can resist laser damage. The fabrication of solid composite filters not only has the advantage that the films are easier to handle, but also the arrays in solid films are more robust than in liquid media. In this paper, we report the photopolymerization process used to trap CCA in polymer matrices, the factors which affect the optical diffraction qualities of resulting polymer films, and methods to improve the efficiencies of solid optical filters. Before this, we also present the experimental demonstration, of controlling the optical diffraction intensities from aqueous CCA dispersions by varying the temperature, which establishes the feasibility of fabricating all-optical switching devices with nonlinear periodic array structures.

Sunkara, Hari B.↗

Optical transient grating pumped X-ray diffraction microscopy for studying mesoscale structural dynamics

Abstract A fundamental understanding of materials’ structural dynamics, with fine spatial and temporal control, underpins future developments in electronic and quantum materials. Here, we introduce an optical transient grating pump and focused X-ray diffraction probe technique (TGXD) to examine the structural evolution of materials excited by modulated light with a precisely controlled spatial profile. This method adds spatial resolution and direct structural sensitivity to the established utility of a sinusoidal transient-grating excitation. We demonstrate TGXD using two thin-film samples: epitaxial BiFeO 3 , which exhibits a photoinduced strain (structural grating) with an amplitude proportional to the optical fluence, and FeRh, which undergoes a magnetostructural phase transformation. In BiFeO 3 , structural relaxation is location independent, and the strain persists on the order of microseconds, consistent with the optical excitation of long-lived charge carriers. The strain profile of the structural grating in FeRh, in comparison, deviates from the sinusoidal excitation and exhibits both higher-order spatial frequencies and a location-dependent relaxation. The focused X-ray probe provides spatial resolution within the engineered optical excitation profile, resolving the spatiotemporal flow of heat through FeRh locally heated above the phase transition temperature. TGXD successfully characterizes mesoscopic energy transport in functional materials without relying on a specific transport model.

36 MATERIALS SCIENCE↗

Plasmonic Nonlinear Energy Transfer Enhanced Second Harmonic Generation Nanoscopy

Nonlinear optical response is a fingerprint of various physicochemical properties of materials related to symmetry, including crystallography, interfacial configuration, and carrier dynamics. However, the intrinsically weak nonlinear optical susceptibility and the diffraction limit of far-field optics restrict probing deep-subwavelength-scale nonlinear optics with measurable signal-to-noise ratio. Here, we propose an alternative approach toward efficient second harmonic generation (SHG) nanoscopy for SHG-active sample (zinc oxide nanowire; ZnO NW) using an SHG-active plasmonic nanotip. Our full-wave simulation suggests that the experimentally observed high near-field SHG contrast is possible when the nonlinear response of ZnO NW is enhanced and/or that of the tip is suppressed. Here, this result suggests possible evidence of quantum mechanical nonlinear energy transfer between the tip and the sample, modifying the nonlinear optical susceptibility. Further, this process probes the nanoscale corrosion of ZnO NW, demonstrating potential use in studying various physicochemical phenomena in nanoscale resolution.

36 MATERIALS SCIENCE↗

Detailed diffraction imaging of x-ray optics crystals with synchrotron radiation

Rocking curve topography at the Advanced Photon Source’s beamline 1-BM measures the x-ray reflection from large (many cm 2 ) flat crystals on a sub-mm scale with microradian angular resolution. The $(01\bar{1}1)$ reflection at 8 keV is uniform across the crystal and close to theory for three thick quartz wafers well-polished with increasingly finer grit. However, the reflection is non-uniform for some ~ 0.1mmthin, bendable crystals that are made flat by optical contact with a flat substrate. Here, these thin crystals are bent to serve in certain x-ray diagnostics of plasmas, and similar non-uniformities could then occur in bent crystals as well. The same detail in x-ray reflection in bent crystals is unachievable with the existing topography setup: one way to get the desired resolution is with a standard microfocusing approach.

47 OTHER INSTRUMENTATION↗

Exploring Divisibility and Summability of 'Photon' Wave Packets in Nonlinear Optical Phenomena

Formulations for second and higher harmonic frequency up and down conversions, as well as multi photon processes directly assume summability and divisibility of photons. Quantum mechanical (QM) interpretations are completely congruent with these assumptions. However, for linear optical phenomena (interference, diffraction, refraction, material dispersion, spectral dispersion, etc.), we have a profound dichotomy. Most optical engineers innovate and analyze all optical instruments by propagating pure classical electromagnetic (EM) fields using Maxwell s equations and gives only lip-service to the concept "indivisible light quanta". Further, irrespective of linearity or nonlinearity of the phenomena, the final results are always registered through some photo-electric or photo-chemical effects. This is mathematically well modeled by a quadratic action (energy absorption) relation. Since QM does not preclude divisibility or summability of photons in nonlinear & multi-photon effects, it cannot have any foundational reason against these same possibilities in linear optical phenomena. It implies that we must carefully revisit the fundamental roots behind all light-matter interaction processes and understand the common origin of "graininess" and "discreteness" of light energy.

Prasad, Narasimha↗

CIRS-lite, a Fourier Transform Spectrometer for Low-Cost Planetary Missions

Passive spectroscopic remote sensing of planetary atmospheres and surfaces in the thermal infrared is a powerful tool for obtaining information about surface and atmospheric temperatures, composition, and dynamics (via the thermal wind equation). Due to its broad spectral coverage, the Fourier transform spectrometer (FTS) is particularly suited to the exploration and discovery of molecular species. NASA's Goddard Space Flight Center (GSFC) developed the CIRS (Composite Infrared Spectrometer) FTS for the NASA/ESA Cassini mission to the Saturnian system. CIRS observes Saturn, Titan, icy moons such as Enceladus, and the rings in thermal self-emission over the spectral range of 7 to 1000 ell11. CIRS has given us important new insights into stratospheric composition and jets on Jupiter and Saturn, the cryo-geyser and thermal stripes on Enceladus, and the winter polar vortex on Titan. CIRS has a mass of 43 kg, contrasted with the earlier GSFC FTS, pre-Voyager IRIS (14 kg). Future low-cost planetary missions will have very tight constraints on science payload mass, thus we must endeavor to return to IRIS-level mass while maintaining CIRS-level science capabilities ("do more with less"). CIRS-lite achieves this by pursuing: a) more sensitive infrared detectors (high Tc superconductor) to enable smaller optics. b) changed long wavelength limit from 1000 to 300 microns to reduce diffraction by smaller optics. c) CVD (chemical vapor deposition) diamond beam-splitter for broad spectral coverage. d) single FTS architecture instead of a dual FTS architecture. e) novel materials, such as single crystal silicon for the input telescope primary.

Brasunas, J.↗

Synthesis of Macroscopic Single Crystals of Ge 2 Sb 2 Te 5 via Single-Shot Femtosecond Optical Excitation

Using in situ electron diffraction techniques, we demonstrate that femtosecond optical excitation above a threshold fluence of the amorphous, as-deposited, phase change material Ge 2 Sb 2 Te 5 creates large, 100 μm scale single crystals. This is 2 orders of magnitude larger than previously reported grains synthesized via photoexcitation. Transmission electron microscopy shows that these large crystals are dewetted regions with a face-centered cubic structure. Energy-dispersive X-ray spectroscopy indicates that the crystals have the same composition as the initial amorphous phase. In this work, we present a theoretical model which shows that this arises from a crossover from a nucleation-dominated crystallization regime to a growth-dominated crystallization regime, and we show that the measured grain size is consistent with Johnson–Mehl–Avrami–Kolmogorov (JMAK) crystallization theory for temperatures near the melting temperature. The ability to grow macroscopic single crystals from an amorphous material, and on arbitrary amorphous substrates, opens up a large area of potential applications, as well as new opportunities for tuning the nucleation, growth, and switching characteristics of phase-change materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Broadband Interferometer for Measuring Transmitted Wavefronts of Optical Bandpass Filters for HST (ACS)

The transmitted wavefronts of optical filters for the Hubble Space Telescope (HST) Advanced Camera for Surveys (ACS) are characterized using the Wildly and Openly Modified Broadband Achromatic Twyman Green (WOMBAT) Interferometer developed in the NASA/GSFC Optics Branch's Diffraction Grating Evaluation Facility (DGEF). Because only four of thirty-three of ACS's optical bandpass filters transmit the 633 nm light of most commercial interferometers, a broadband interferometer is required to verify specified transmitted wavefront of ACS filters. WOMBAT's design is a hybrid of the BAT interferometer developed by JPL used for HST Wide Field and Planetary Camera 2 (WFPC-2) filters and a WYKO 400 phase shifting interferometer. It includes a broadband light source, monochromator, off-axis, parabolic collimating and camera mirrors, an aluminum-coated fused silica beam splitter, flat retroreflecting mirrors for the test and reference arms, and a LTV-sensitive CCD camera. An outboarded, piezo-electric phase shifter holds the flat mirror in the interferometer's reference arm. The interferometer is calibrated through interaction between the WYKO system's software and WONMAT hardware for the test wavelength of light entering the beam splitter. Phase-shifted interferograms of the filter mounted in the test arm are analyzed using WYKO's Vision' software. Filters as large as 90 mm in diameter have been measured over a wavelength range from 200 to 1100 nm with a sensitivity of lambda/200 rms at lambda = 633 nm. Results of transmitted wavefront measurements are shown for ACS fixed band pass and spatially-variable bandpass filters for a variety of wavelengths.

Boucarut, R. A.↗

Adaptable Diffraction Gratings With Wavefront Transformation

Diffraction gratings are optical components with regular patterns of grooves, which angularly disperse incoming light by wavelength. Traditional diffraction gratings have static planar, concave, or convex surfaces. However, if they could be made so that they can change the surface curvature at will, then they would be able to focus on particular segments, self-calibrate, or perform fine adjustments. This innovation creates a diffraction grating on a deformable surface. This surface could be bent at will, resulting in a dynamic wavefront transformation. This allows for self-calibration, compensation for aberrations, enhancing image resolution in a particular area, or performing multiple scans using different wavelengths. A dynamic grating gives scientists a new ability to explore wavefronts from a variety of viewpoints.

Iazikov, Dmitri↗

Ternary molecular switching in a single-crystal optical actuator with correlated crystal strain

A growing portfolio of single-crystal optical actuators is forging a new class of photonic materials that hold prospects for quantum technologies. Ruthenium-based complexes that exhibit this phenomenon via SO 2 -linkage photoisomerisation are of particular interest since they display multiple metastable states, once induced by green light; yet, complete photoconversion into each SO 2 -isomeric state is rarely achieved. We discover a new complex, trans-[Ru(SO 2 )(NH 3 ) 4 (4-bromopyridine)]tosylate 2 , that produces 100% photoconverted η 1 -OSO isomeric crystal structures at 90 K, which fully transition into η 2 -(OS)O photoisomers upon warming to 100 K, while the dark-state η 1 -SO 2 structure is wholly recovered by heating the crystal to room temperature. Crystal structures and optical-absorption profiles of each state are captured via in-situ light-induced single-crystal X-ray diffraction and optical-absorption spectroscopy. Results show that both photoisomeric species behave as optical switches, but with distinct optical properties. The photoisomerisation process causes thermally-reversible micro- and nanoscopic crystal strain, as characterised by optical microscopy and in-situ light-induced atomic-force microscopy.

actuators↗