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NASA NTRSDate not supplied

Exposure of Highly Reflective Far-Ultraviolet Coatings to LEO Environment for TRL Advancement for the Habitable Worlds Observatory

Over the past several years, our team at the NASA Goddard Space Flight Center (GSFC), in collaboration with the Jet Propulsion Laboratory (JPL) and the Naval Research Laboratory (NRL), have developed several new protected Al coating technologies with improved Far-Ultraviolet (FUV) reflectance performance and more robust environmental stability. These include Al protected with lithium-based fluoride (LiF) coatings such as hot deposited LiF (eLiF), XeF 2 -passivated LiF coatings (XeLiF), Li 3 AlF 6 overcoats, AlF 3 (plasma passivated), and XeF 2 passivated MgF 2 coatings (XeMgF 2 ). However, despite these developments, relatively little experimental information exists regarding the long-term stability of these coatings after simultaneous exposure to the Low Earth Orbit (LEO) environment. To evaluate their environmental durability and advance their Technology Readiness Level (TRL), representative samples of these coating technologies, Al+XeLiF, Al+eLiF, Al+Li 3 AlF 6 , Al+AlF 3 , Al+XeMgF 2 , and bare Al as reference samples, were flown onboard the International Space Station (ISS) as part of the Materials International Space Station Experiment 20 (MISSE-20). The MISSE platform is operated by Aegis Aerospace for relatively long-duration (e.g. 6 months) external exposure experiments in a space environment. The coatings were deposited on ULE and Zerodur substrates, and witness samples deposited on the same coatings runs, but on glass slides were left on Earth as control. A subset of the flight samples were fitted with MgF 2 windows to reduce direct exposure to atomic oxygen (AO) and charged particles, and still let through UV and other types of radiation on these samples. After approximately 6 months of exposure in the forward-facing (RAM) direction, the samples were returned to Earth and characterized by performing FUV/NUV/VIS/NIR reflectance measurements to quantify degradation, spectroscopic ellipsometry to evaluate coating thickness and optical constants, atomic force microscopy (AFM) to quantify surface roughness evolution during the flight in the ISS. The MgF 2 protective windows were also analyzed through FUV transmission measurements. Comparison with the witness samples left on the ground and with the flown bare Al samples (with just the naturally occurring Al 2 O 3 layer) provided a quantitative assessment of coating thickness variations, optical performance degradation, and morphological changes induced by prolonged exposure to the LEO environment.

Far Ultraviolet (FUV)↗

NASA NTRS1993

Multilayer and grazing incidence X-ray/EUV optics for astronomy and projection lithography; Proceedings of the Meeting, San Diego, CA, July 19-22, 1992

The present volume on multilayer and grazing incidence X-ray/EUV optics for astronomy and projection lithography discusses AXAF grazing incidence mirrors, the theory and high throughput optics of grazing incidence optics, multilayer mirror fabrication and characterization, and multilayer optics for X-ray projection lithography. Attention is given to the VETA-I X-ray detection system, a motion detection system for AXAF X-ray ground testing, image analysis of the AXAF VETA-I X-ray mirror, and optical constants from mirror reflectivities measured at synchrotrons. Topics discussed include the application of aberration theory to calculate encircled energy of Wolter I-II telescopes, W/C multilayers deposited on plastic films, nonspecular X-ray scattering from Si/Mo multilayers, and multilayer thin-film design as FUV polarizers. Also discussed are thin-film filter lifetesting results in the EUV, chromospheric and coronal observations with multilayer optics, present and future requirements of soft X-ray projection lithography, and the imaging Schwarzschild multilayer X-ray microscope.

Hoover, Richard B.↗

DOE OSTI2021

Giant terahertz polarization rotation in ultrathin films of aligned carbon nanotubes

For easy manipulation of polarization states of light for applications in communications, imaging, and information processing, an efficient mechanism is desired for rotating light polarization with a minimum interaction length. Here, we report giant polarization rotations for terahertz (THz) electromagnetic waves in ultrathin ( ∼ <#comment/> 45 n m ), high-density films of aligned carbon nanotubes. We observed polarization rotations of up to ∼ <#comment/> 20 ∘ <#comment/> and ∼ <#comment/> 110 ∘ <#comment/> for transmitted and reflected THz pulses, respectively. The amount of polarization rotation was a sensitive function of the angle between the incident THz polarization and the nanotube alignment direction, exhibiting a “magic” angle at which the total rotation through transmission and reflection becomes exactly 90°. Our model quantitatively explains these giant rotations as a result of extremely anisotropic optical constants, demonstrating that aligned carbon nanotubes promise ultrathin, broadband, and tunable THz polarization devices.

Baydin, Andrey (ORCID:0000000225673506)↗

NASA NTRS2023

Cryolite Overcoated Aluminum Reflectors for Far-Ultraviolet Spectroscopy

Aluminum (Al) mirrors are conventionally protected with metal-fluoride coatings (e.g., MgF2, LiF, or AlF3) immediately after deposition to prevent oxidation and preserve its far-ultraviolet (FUV) spectral efficiency. However, the resulting FUV reflectance of the aluminum reflector is limited by the metal-fluoride overcoat film index of refraction, morphology, stoichiometry, and its absorption cut-off in the lower end of the FUV spectra. Cryolite (sodium hexafluoroaluminate, Na3AlF6) emerges as a potential candidate to preserve the aluminum FUV reflectance due to its relatively lower index of refraction in the visible to ultraviolet; therefore, allowing for the thin-film design of highly spectral efficient reflectors over a wide spectral range. We investigate the use of cryolite in aluminum reflector FUV coating design. The deposited aluminum reflector overcoated with cryolite will be examined in terms of spectral efficiency and environmental durability. The deposited cryolite overcoat will be evaluated in terms of optical constants and structural properties. Preliminary results have shown that the use of cryolite as an overcoat to protect aluminum would yield unprecedented results as an optimal Hydrogen Lyman-alpha (HLyα) spectral line reflector, with experimental reflectance values >96%.

optical coatings↗

NASA NTRSDate not supplied

Cryolite Overcoated Aluminum Reflectors for Far-Ultraviolet Spectroscopy

Aluminum (Al) mirrors are conventionally protected with metal-fluoride coatings (e.g., MgF 2 , LiF, or AlF 3 ) immediately after deposition to prevent oxidation and preserve its far-ultraviolet (FUV) spectral efficiency. However, the resulting FUV reflectance of the aluminum reflector is limited by the metal-fluoride overcoat film index of refraction, morphology, stoichiometry, and its absorption cut-off in the lower end of the FUV spectra. Cryolite (sodium hexafluoroaluminate, Na 3 AlF 6 ) emerges as a potential candidate to preserve the aluminum FUV reflectance due to its relatively lower index of refraction in the visible to ultraviolet; therefore, allowing for the thin-film design of highly spectral efficient reflectors over a wide spectral range. We investigate the use of cryolite in aluminum reflector FUV coating design. The deposited aluminum reflector overcoated with cryolite will be examined in terms of spectral efficiency and environmental durability. The deposited cryolite overcoat will be evaluated in terms of optical constants and structural properties. Preliminary results have shown that the use of cryolite as an overcoat to protect aluminum would yield unprecedented results as an optimal Hydrogen Lyman-alpha (HLyα) spectral line reflector, with experimental reflectance values >96%.

optical coating↗

NASA NTRS2002

A New Method for Estimating the Single Scattering Phase Functions of Regolith Grains

Hapke's photometric model has been widely used in solar system remote sensing applications for nearly two decades. Recently, Hapke extended his model to describe the coherent-backscatter opposition effect and multiple-scattering by particles with anisotropic single particle phase functions (SPPF's). A practical difficulty for retrieving Hapke's model parameters from typical planet, satellite, and asteroid photometry data sets is that the model employs a large number of adjustable parameters (at least eight) that can be reliably constrained only for a small number of planetary data sets in which both disk-resolved and whole-disk observations are available from opposition to very large phase angles. The present work aims to reduce the number of adjustable parameters and preserve (or even enhance) the model's accuracy and usefulness by expressing Hapke's parameters in terms of more fundamental physical properties on which they mutually depend. The most difficult part of this task, described here, is to develop a simple method for computing the effective SPPF for structurally complex regolith grains from optical constants, grain-size distribution, and average regolith porosity. The development of light-scattering models for irregularly shaped particles is a large, complex subject and many sophisticated methods, such as Discrete Dipole Approximation (DDA) and Monte-Carlo simulations, have been explored elsewhere. Many of these methods are computationally intensive and probably impractical for routine substitution in Hapke's model. Here, progress is reported in developing a practical, semi-empirical method for estimating the directional scattering behavior (i.e. SPPF) of irregular regolith grains. The method employs Optical Transfer Function (OTF) techniques to model how the structural complexity of regolith particles broaden and attenuate the angular distribution of scattered light relative to that expected from ideal spherical particles of equivalent size and composition.

Helfenstein, P.↗

NASA NTRS1991

Polycyclic aromatic hydrocarbon optical properties and contribution to the acceleration of stellar outflows

The optical constants of four polycyclic aromatic hydrocarbon (PAH) molecules (benzene, pyrene, pentacene, and coronene) are determined from their measured laboratory absorption spectra. The Planck mean of the radiation pressure cross section is computed for each molecule and for amorphous carbon (AC) grains, and semiempirically estimated for large PAH molecules up to 400 carbon atoms. Assuming that PAHs are present in carbon-rich stellar outflows, the radiation pressure forces acting on them are calculated and compared with the radiation forces on AC particles. The results show that PAHs possess very different optical properties from AC grains. Small PAHs may experience an 'inverse greenhouse' effect in the inner part of the envelope, as they decouple from the gas close to the photosphere. The radiation pressure force on PAHs is always much less than the force at work on AC grains, and PAH molecules do not affect significantly the dynamics of the outflow.

Cherchneff, Isabelle↗

NASA NTRS1998

Analysis of Physical Properties of Dust Suspended in the Mars Atmosphere

Methods for iteratively determining the infrared optical constants for dust suspended in the Mars atmosphere are described. High quality spectra for wavenumbers from 200 to 2000 1/cm were obtained over a wide range of view angles by the Mariner 9 spacecraft, when it observed a global Martian dust storm in 1971-2. In this research, theoretical spectra of the emergent intensity from Martian dust clouds are generated using a 2-stream source-function radiative transfer code. The code computes the radiation field in a plane-parallel, vertically homogeneous, multiply scattering atmosphere. Calculated intensity spectra are compared with the actual spacecraft data to iteratively retrieve the optical properties and opacity of the dust, as well as the surface temperature of Mars at the time and location of each measurement. Many different particle size distributions a-re investigated to determine the best fit to the data. The particles are assumed spherical and the temperature profile was obtained from the CO2 band shape. Given a reasonable initial guess for the indices of refraction, the searches converge in a well-behaved fashion, producing a fit with error of less than 1.2 K (rms) to the observed brightness spectra. The particle size distribution corresponding to the best fit was a lognormal distribution with a mean particle radius, r(sub m) 0.66 pm, and variance, omega(sup 2) = 0.412 (r(sub eff) = 1.85 microns, v(sub eff) =.51), in close agreement with the size distribution found to be the best fit in the visible wavelengths in recent studies. The optical properties and the associated single scattering properties are shown to be a significant improvement over those used in existing models by demonstrating the effects of the new properties both on heating rates of the Mars atmosphere and in example spectral retrieval of surface characteristics from emission spectra.

Snook, Kelly↗

DOE OSTI2024

Optical Modeling of Polysilicon: TOPCon PV

Determine how film thickness changes with different deposition methods. Analyze relationship between film thickness and optical constants. The deposition rate of intrinsic polysilicon is higher during initial deposition then begins to slow down as deposition time increases. Longer depositions of polysilicon are more crystalline in structure than shorter depositions. N-type doping of polysilicon is more crystalline in structure than p-type doping, despite similar film thicknesses.

Bruggeman effective media approximation↗

DOE OSTI2020

Parametric study of optical transmission through plasmonic hole arrays modulated by the phase transition of vanadium dioxide

We have performed comprehensive electromagnetic simulations and preliminary experiments to explore the effects of geometrical and material parameters on the extraordinary optical transmission (EOT) through periodic arrays of subwavelength holes in a bilayer stack consisting of a gold or silver film atop a vanadium dioxide film (Au/Ag + VO 2 ), where the latter undergoes a semiconductor-to-metal phase transition. Using the finite-difference time-domain (FDTD) and finite-element methods (FEM), we vary iteratively the array periodicity, VO 2 film thickness and hole diameters, as well as the refractive index inside the VO 2 -layer holes and the VO 2 optical constants. For each variation, we compare the metallic-to-semiconducting ratios of the zero-order transmission ( T 00 ) peaks and find sharp maxima in these ratios within narrow parameter ranges. The maxima arise from Fabry-Perot and Fano-type resonances that minimize T 00 in the semiconducting phase of the perforated bilayers. At a fixed array period, the primary factors controlling the VO 2 -enabled EOT modulation are the VO 2 thickness, diameter of the VO 2 -layer holes, and absorption in the two VO 2 phases. Besides uncovering the origins of the higher metallic-phase T 00 , this study provides a protocol for optimizing the performance of the bilayer hole arrays for potential uses as dynamically tunable nano-optical devices.

Donev, Eugenii U. (ORCID:000000030555219X)↗

DOE OSTI2022

Optical properties of Mo and amorphous MoOx, and application to antireflection coatings for metals

To form antireflection (AR) coatings to hide metal architecture in display technologies, we deposited thin films of metal Mo and oxide MoOx by sputtering targets of various compositions using pure Ar sputter gas. The optical constants [n,k] of these samples were measured by the direct numerical solution of reflectance and transmittance at each wavelength point measured. We find that 50 nm films are uniform in the growth direction, but for thicker 100 nm samples, evidence exists for nonuniform growth, where the top 20 nm appears to be metal rich. From these [n,k], negative Tauc bandgap energies show these oxides are semi-metals. We then identified the specific composition (x) that optimizes the AR response for a host of metals (Al, Cu, Ag, Au). Finally, two methods were used to understand why these MoOx materials function well as AR media, including (i) using phasor rays and (ii) developing a universal expression for the AR condition that applies to both dielectric and metal substrates. In (i), we find two characteristics for AR of metals: (a) its optical thickness should be roughly π3, not the π2 for dielectrics, since for MoOx, their [r^ij,t^ij] Fresnel phases differ from the usual [180°, 0°] of dielectrics; and (b) the medium incorporates a k-dominant strategy whose function is to absorb the energy that is reflected at the AR/metal interface. In (ii), the universal AR condition is found to be r^01+r^12z^=0. For dielectrics, this reduces to the well-known nAR=nairnsub condition. However, for metals, a concise analytic expression is lacking since this expression is highly nonlinear but is easily solved by numerical methods.

Tsu, David V. (ORCID:0000000295903418)↗

NASA NTRS2011

Aromatic Structure in Simulates Titan Aerosol

Observations of Titan by the Cassini Composite Infrared Spectrometer (CIRS) between 560 and 20 per centimeter (approximately 18 to 500 micrometers) have been used to infer the vertical variations of Titan's ice abundances, as well as those of the aerosol from the surface to an altitude of 300 km [1]. The aerosol has a broad emission feature centered approximately at 140 per centimeter (71 micrometers). As seen in Figure 1, this feature cannot be reproduced using currently available optical constants from laboratory-generated Titan aerosol analogs [2]. The far-IR is uniquely qualified for investigating low-energy vibrational motions within the lattice structures of COITIDlex aerosol. The feature observed by CIRS is broad, and does not likely arise from individual molecules, but rather is representative of the skeletal movements of macromolecules. Since Cassini's arrival at Titan, benzene (C6H6) has been detected in the atmosphere at ppm levels as well as ions that may be polycyclic aromatic hydrocarbons (PAHs) [3]. We speculate that the feature may be a blended composite that can be identified with low-energy vibrations of two-dimensional lattice structures of large molecules, such as PAHs or nitrogenated aromatics. Such structures do not dominate the composition of analog materials generated from CH4 and N2 irradiation. We are performing studies forming aerosol analog via UV irradiation of aromatic precursors - specifically C6H6 - to understand how the unique chemical architecture of the products will influence the observable aerosol characteristics. The optical and chemical properties of the aromatic analog will be compared to those formed from CH4/N2 mixtures, with a focus on the as-yet unidentified far-IR absorbance feature. Preliminary results indicate that the photochemically-formed aromatic aerosol has distinct chemical composition, and may incorporate nitrogen either into the ring structure or adjoined chemical groups. These compositional differences are demonstrated in the aerosol mass spectra shown in Figure 2. The aromatic aerosol also demonstrates strong chemical reactivity when exposed to laboratory air, indicating substantial stored chemical potential. Oxidatoin and solubility studies wil be presented and implicatoins for prebiotic chemistry o nTitan will be discussed.

Trainer, Melissa G.↗

DOE OSTI2023

Photonics in Multimaterial Lateral Heterostructures Combining Group IV Chalcogenide van der Waals Semiconductors

Abstract Lateral heterostructures combining two multilayer group IV chalcogenide van der Waals semiconductors have attracted interest for optoelectronics, twistronics, and valleytronics, owing to their structural anisotropy, bulk‐like electronic properties, enhanced optical thickness, and vertical interfaces enabling in‐plane charge manipulation/separation, perpendicular to the trajectory of incident light. Group IV monochalcogenides support propagating photonic waveguide modes, but their interference gives rise to complex light emission patterns throughout the visible/near‐infrared range both in uniform flakes and single‐interface lateral heterostructures. Here, this work demonstrates the judicious integration of pure and alloyed monochalcogenide crystals into multimaterial heterostructures with unique photonic properties, notably the ability to select photonic modes with targeted discrete energies through geometric factors rather than band engineering. SnS‐GeS 1− x Se x ‐GeSe‐GeS 1− x Se x heterostructures with a GeS 1− x Se x active layer sandwiched laterally between GeSe and SnS, semiconductors with similar optical constants but smaller bandgaps, were designed and realized via sequential vapor transport synthesis. Raman spectroscopy, electron microscopy/diffraction, and energy‐dispersive X‐ray spectroscopy confirm a high crystal quality of the laterally stitched components with sharp interfaces. Nanometer‐scale cathodoluminescence spectroscopy provides evidence for a facile transfer of electron–hole pairs across the lateral interfaces and demonstrates the selection of photon emission at discrete energies in the laterally embedded active (GeS 1− x Se x ) part of the heterostructure.

2D layered crystals↗

DOE OSTI2020

Anisotropic index of refraction and structural properties of hexagonal boron nitride epilayers probed by spectroscopic ellipsometry

The anisotropic index of refraction of 200 μm thick boron-10 enriched hexagonal boron nitride (h-BN) freestanding epilayers grown by metalorganic chemical vapor deposition has been measured using spectroscopic ellipsometry in the UV (4.0–5.1 eV) spectral range. It was found that the index of refraction for the polarization mode with an electric field perpendicular to the c-axis (ordinary, n o ) is much higher than that with an electric field parallel to the c-axis (extraordinary, n e ). By inclusion of turbostratic- (t-) phase layers within h-BN having an average inclination angle (θ) with respect to the ideal c-plane, a simple method for quantifying θ has been deduced. Our results revealed that the presence of t-phase layers decreases the optical anisotropy of h-BN and that a signature of improved crystalline quality is an increase in the ordinary index of refraction (n o ) as a result of the average incline angle θ approaching 0° and predicted that n o = 2.7 and n e = 1.5 at 280 nm for single crystalline h-BN epilayers. More importantly, our results demonstrated that spectroscopic ellipsometry is an effective technique for characterizing the crystalline quality of h-BN epilayers with the advantages of being noninvasive and highly sensitive.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Imaging plasma formation in isolated nanoparticles with ultrafast resonant scattering

We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations

In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. Unfortunately, kinematical models are often inaccurate even for relativistic electron probes, especially for dense, oriented single crystals where strong channeling and multiple scattering effects are present. This article introduces and demonstrates dynamical scattering models tailored for quantitative analysis of UED experiments performed on single-crystal films. As a case study, we examine ultrafast laser heating of single-crystal gold films. Comparison of kinematical and dynamical models reveals the strong effects of dynamical scattering within nm-scale films and their dependence on sample topography and probe kinetic energy. Applying to UED experiments on an 11 nm thick film using 750 keV electron probe pulses, the dynamical models provide a tenfold improvement over a comparable kinematical model in matching the measured UED patterns. Also, the retrieved lattice temperature rise is in very good agreement with predictions based on previously measured optical constants of gold, whereas fitting the Debye–Waller factor retrieves values that are more than three times lower. Altogether, these results show the importance of a dynamical scattering theory for quantitative analysis of UED and demonstrate models that can be practically applied to single-crystal materials and heterostructures.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Robust method for broadband efficiency enhancement of electron photocathodes using optical interferences

In this work, we demonstrate the key features of an interference cathode using both simulations and experiments. We deposit Cs 3 Sb photocathodes on Ag to produce an interference enhanced photocathode with 2–5× quantum efficiency (QE) enhancement using a robust procedure that requires only a smooth metal substrate and QE monitoring during growth. We grow both an interference cathode (Ag substrate) and a typical photocathode (Si reference substrate) simultaneously to confirm that the effects are due to optical interactions with the substrate rather than photocathode composition or surface electron affinity differences. Growing the cathodes until the QE converges shows both the characteristic interference peaks during growth and the identical limiting case where the cathode is “infinitely thick,” in agreement with simulations. We also grow a cathode until the QE on Ag peaks and then stop the growth, demonstrating broadband QE enhancement.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Nonlinear optical properties of lanthanum titanate glasses prepared by levitation melting

Lanthanum titanate glasses (17 La 2 O 3 -83 TiO 2 ) are fabricated via aerodynamic levitation melting. Here, nonlinear refraction and absorption were measured with the Z scan technique using ps optical pulses at 532 nm wavelength with peak intensities in the range of 0.25–2.5 GW/cm 2 . The two-photon absorption coefficient (β) and the effective nonlinear refraction coefficient (⁠$n^{eff}_{2}$) are found to be, respectively, 2.19 cm/GW and 152 × 10 -16 cm 2 /W (85 × 10 -13 esu). The Raman gain is measured to be 106 × 10 -11 cm/W. The nonlinearity strength is found to be nearly 60 times larger in lanthanum titanate glasses relative to silica.

36 MATERIALS SCIENCE↗