Nanoporous antireflection coating for high-temperature applications in the infrared.

Antireflection (AR) coatings are essential to the performance of optical systems; without them, surface reflections increase significantly at steep angles and become detrimental to the functionality. AR coatings apply to a wide range of applications from solar cells and laser optics to optical windows. Many times, operational conditions include high temperatures and steep angles of incidence (AOIs). The implementation of AR coatings is extremely challenging in these conditions. Nanoporous coatings made from high-temperature-tolerant materials offer a solution to this problem. The careful selection of materials is needed to prevent delamination when exposed to high temperatures, and an optimal optical design is needed to lower surface reflections at both the normal incidence and steep AOIs. This paper presents nanoporous silicon dioxide and hafnium dioxide coatings deposited on a sapphire substrate using oblique angle deposition by electron beam evaporation, a highly accurate deposition technique for thin films. Developed coatings were tested in a controlled temperature environment and demonstrated thermal stability at temperatures up to 800°C. Additional testing at room temperature demonstrated the reduction of power reflections near optimal for AOIs up to 70° for a design wavelength of 1550 nm. These findings are promising to help extend the operation of technology at extreme temperatures and steep angles.

Supercontinuum-laser diffuse reflectance spectroscopy in conjunction with an extended Kubelka-Munk model-a methodology for determination of temperature-dependent quantum efficiency in highly scattering and fluorescent media.

Temperature-dependent diffuse reflectance measurements on Cr-doped α-alumina monoliths have been performed using supercontinuum-laser illumination and CO2-laser heating. These measurements have been interpreted using an extended Kubelka-Munk (K-M) model describing diffuse-light propagation in highly scattering and fluorescent media to assess the temperature dependence of fluorescence quantum efficiency. Analysis of experimental results has provided a qualitative understanding of the temperature-dependent conditions for model applicability and also suggests methods for using supercontinuum-laser diffuse reflectance spectroscopy for detection of unknown fluorescent dopants.

Experimental characterization and physics-based modeling of the temperature-dependent diffuse reflectance of plasma-sprayed Nd2Zr2O7 in the near to short-wave infrared.

Supercontinuum-laser illumination in conjunction with CO2-laser heating has been implemented to measure the near to short-wave infrared (970-1660 nm) diffuse reflectance of plasma-sprayed Nd2Zr2O7 as a function of temperature. Owing to the broadband nature of this experimental technique, the diffuse reflectance of plasma-sprayed Nd2Zr2O7 has been measured at many wavelengths and has been shown to decrease with increasing temperature. A physics-based model for diffuse reflectance predicated on the crystal/electronic band structure of highly scattering semiconductor materials has been constructed to interpret the results of these measurements. Baseline materials characterization has also been performed to assist in the development of crystal/electronic band structure-optical property relationships that could be useful for the design of next-generation environmental barrier coatings. This characterization has included ambient and non-ambient x-ray diffraction as well as room-temperature, integrating-sphere diffuse reflectance spectroscopy.

Temperature-dependent diffuse reflectance spectroscopy of plasma-sprayed Cr-doped α-alumina using supercontinuum laser illumination and CO2 laser heating.

This study presents results for the high-temperature (up to 1550 K) optical properties of polycrystalline Cr-doped α-alumina materials. Diffuse reflectance spectra in the wavelength range of 510-840 nm are presented as a function of temperature to illustrate changes to the optical behavior of these materials including a previously unreported thermally activated splitting of the U-band absorption (A24→T24) in octahedrally coordinated Cr3+. Measurements were made using a unique laser-based approach for high-temperature solid-state spectroscopy, involving front-side supercontinuum laser illumination and back-side CO2 laser heating. This approach required development of samples that could withstand related thermal stresses, and measurements were made on plasma-sprayed, Cr-doped α-alumina monoliths. Measured spectra are interpreted, in part, using published optical spectra for ruby; agreement between results here with those obtained using more traditional methods serves to validate the measurement methods used for this work.

Transmittance derived line width and line shift in polycrystalline Nd:YAG.

Temperature dependent transmittance derived line width and line shift measurements are conducted on polycrystalline 1% and 6% Nd doped YAG in the 293 K-473 K range. A single crystal temperature dependent line width model is adapted for polycrystalline YAG. Comparison between line width measurement techniques was conducted, and the transmittance method is preferred for ground state line width measurements. Polycrystalline YAG material is found to have broader intrinsic line width than single crystal material. Polycrystalline YAG material should provide mode locking advantages of shorter minimum pulse length than single crystal YAG.

Lidar measurements of solid rocket propellant fire particle plumes.

This paper presents the first, to our knowledge, direct measurement of aerosol produced by an aluminized solid rocket propellant (SRP) fire on the ground. Such fires produce aluminum oxide particles small enough to loft high into the atmosphere and disperse over a wide area. These results can be applied to spacecraft launchpad accidents that expose spacecraft to such fires; during these fires, there is concern that some of the plutonium from the spacecraft power system will be carried with the aerosols. Accident-related lofting of this material would be the net result of many contributing processes that are currently being evaluated. To resolve the complexity of fire processes, a self-consistent model of the ground-level and upper-level parts of the plume was determined by merging ground-level optical measurements of the fire with lidar measurements of the aerosol plume at height during a series of SRP fire tests that simulated propellant fire accident scenarios. On the basis of the measurements and model results, the Johns Hopkins University Applied Physics Laboratory (JHU/APL) team was able to estimate the amount of aluminum oxide (alumina) lofted into the atmosphere above the fire. The quantification of this ratio is critical for a complete understanding of accident scenarios, because contaminants are transported through the plume. This paper provides an estimate for the mass of alumina lofted into the air.

Backscatter signatures of biological aerosols in the infrared.

To develop a deeper understanding of the optical signatures of both biological aerosols and potential interferents, we made field measurements of optical cross sections and compared them to model-based predictions. We measured aerosol cross sections by conducting a hard-target calibration of a light detection and ranging system (LIDAR) based on the Frequency Agile Laser (FAL). The elastic backscatter cross sections are estimated at 19 long-wave infrared (LWIR) wavelengths spanning the range from 9.23 to 10.696 µm. The theoretical modeling of the elastic backscatter cross sections is based on the measured refractive index and size distribution of the aerosols, which are used as inputs into Mie calculations. Both model calculations and experimental measurements show good agreement and also indicate the presence of spectral features based on single particle absorption in the backscatter cross sections that can be used as a basis for discrimination for both standoff and point sensors.

Chamber lidar measurements of biological aerosols.

In order to determine the performance of standoff sensors against agents, there is a need to develop methods to characterize the optical properties of biological warfare agents. The goal of this work is to develop a methodology that would allow the characterization of agent optical cross sections from the UV to the longwave IR. The present work demonstrates an optical measurement architecture based on lidar technology, allowing the measurement of backscatter and depolarization ratio from biological aerosols (either simulants or agents) released in a refereed, 1m3 chamber. Measured results on simulant materials are calibrated and compared to theoretical simulations of the cross sections.

Desorption of hydrogen from light metal hydrides: concerted electronic rearrangement and role of H···H interactions.

A theoretical study of the desorption of hydrogen from rhombic Group 1 metal hydride dimers reveals a concerted reorganisation of the electron density for the M-H and H-H moieties as the reaction coordinate is traversed and a closed-shell H···H interaction evolves into a covalent H2 bond. The central role played by homopolar dihydrogen bonding in this process is revealed and analysed.

Particle shape as revealed by spectral depolarization.

Through a series of numerical simulations we explore some scatter effects due to nonspherical particles. Specifically, we examine the link between the aspect ratio of randomly oriented, prolate spheroidal particles and the resulting linear depolarization of the scattered light in the forward and backscatter directions. The particular objective is to detect the presence of randomly oriented particles that have a systematic size and aspect ratio. Calculations show that the spectral behavior of the linear depolarization reveals the aspect ratio of the scattering particles. The concept is demonstrated using the size, shape, and refractive index of the spore form of Bacillus globigii (BG).

Modeling of the frequency- and temperature-dependent absorption coefficient of long-wave-infrared (2-25 microm) transmitting materials.

A semiempirical multiphonon model based on quantum-mechanical oscillators under a Morse potential is applied to the absorption coefficient of far-infrared transmitting materials. Known material properties are combined with absorption coefficient data to fit the empirical parameters of the model. This provides an accurate means of predicting the intrinsic absorption of the materials in their multiphonon regions. Extinction data are obtained by measuring material transmittances with a Fourier-transform spectrometer and comparing them with the lossless transmittances predicted by Sellmeier models. Where appropriate, scatter models are used to separate the extinction into loss due to scatter and absorption. Data and model parameters are presented for GaAs, GaP, ZnS, and ZnSe.