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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2

Combining Spectroscopic Ellipsometry with Transmission Spectroscopy to Derive Accurate Optical Constants for Organic Materials

A method for deriving the optical constants of organic powdered materials in the mid-infrared spectral range is introduced using variable angle spectroscopic ellipsometry and transmission spectroscopy. The approach uses pressed pellets of the powder and is applied to organic solids, which have both strong and weak infrared absorption features. Many powders have significant voids and do not press into smooth, homogenous pellets. To account for pellet non-idealities and to accurately measure both n and k, three different forms of pellets were pressed and measured: A pure analyte pellet, a mixed analyte/KBr pellet with a large analyte percentage, and a KBr transmission pellet with only a small analyte percentage. Using all three pellets in a multi-sample analysis involving both ellipsometric and transmission data, the complex refractive index (n/k) values can be derived for many organic compounds. This method is illustrated to calculate the optical constants for anhydrous lactose from 6000-400 cm-1. The transmission measurements improve the spectral fitting of weak absorption features, and the multi-sample analysis enables a better determination of the significant void space that is present in the pure pellet, leading to lower values for both n and k if not properly accounted for in the multi-oscillator model used to fit the ellipsometric data.

Optical constants, refractive index, extinction co↗

Quantitative measurement of pebble fuel anisotropy using generalized ellipsometry

The renewed development of high-temperature gas-cooled reactors has created a need to modernize pebble fuel quality control methods. One important specification in these methods is the coefficient of thermal expansion (CTE) anisotropy, which reflects graphite grain alignment and affects fuel performance. This study investigates the feasibility of using two-modulator generalized ellipsometry microscopy (2-MGEM) as a potential surrogate metric for CTE anisotropy. Graphite matrix compacts with controlled levels of anisotropy were fabricated by varying pre-pressures during forming and were subsequently characterized using both optical dilatometry and 2-MGEM. Measured responses were compared to an isotropic reference pebble produced using an industrial manufacturing process to provide a practical baseline. The resulting measurements revealed a strong quantitative correlation between the CTE anisotropy ratio and the corresponding diattenuation ratio. However, propagated measurement uncertainties in the optical method were found to limit definitive pass/fail discrimination, highlighting the need for improved precision before qualification as a quality control tool. Still, the results establish a quantitative relationship between optical and CTE anisotropy and support further development of 2-MGEM as a potential surrogate method for evaluating graphite matrix anisotropy in pebble fuel manufacturing.

Raftery, Alicia [ORNL] (ORCID:0000000259076427)↗

Delineating Confinement Regimes for Nafion Thin Films via Simultaneous QCM-D and Spectroscopic Ellipsometry

Proton-conducting ionomers used in electrodes of electrochemical devices form nanometer-scale films covering metallic catalyst surfaces, wherein they experience confinement and interfacial effects absent in the bulk polymer. This confinement alters the physical properties of the ionomer film, which is postulated to increase the density and is attributed to the transport limitations observed in fuel-cell electrodes. Despite studies showing reduced swelling, no systematic measurement has validated this phenomenon by demonstrating both densification and stiffening as the film gets thinner. Here, this study aims to fill this gap by reporting the humidity-driven changes in swelling, mass uptake, and density of Nafion ionomer films cast at varying thicknesses (10–320 nm) onto a gold-plated sensor. The films were simultaneously probed during humidification using spectroscopic ellipsometry (SE) and a quartz crystal microbalance with dissipation (QCM-D), which allowed for determination of the density and shear stiffness. The effects of confinement were prominently observed below ∼30 nm, with films showing increased density along with decreased swelling and mass uptake during hydration. In addition, the confined films show a negative excess volume upon initial water sorption, implying a larger proportion of absorbed water might bound to ionic groups in accord with notion of localized densification.

Espinet, Kevin B. [University of California, Berke↗

Electron Beam Infrared Nano-Ellipsometry of Individual Indium Tin Oxide Nanocrystals

Leveraging recent advances in electron energy monochromation and aberration correction, we record the spatially resolved infrared plasmon spectrum of individual tin-doped indium oxide nanocrystals using electron energy-loss spectroscopy (EELS). Both surface and bulk plasmon responses are measured as a function of tin doping concentration from 1–10 atomic percent. Furthermore, these results are compared to theoretical models, which elucidate the spectral detuning of the same surface plasmon resonance feature when measured from aloof and penetrating probe geometries. We additionally demonstrate a unique approach to retrieving the fundamental dielectric parameters of individual semiconductor nanocrystals via EELS. This method, devoid from ensemble averaging, illustrates the potential for electron-beam ellipsometry measurements on materials that cannot be prepared in bulk form or as thin films.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spectroscopic ellipsometry extraction of optical constants for materials from oxide covered samples: Application to the plutonium/oxides system

Spectroscopic ellipsometry is combined with scanning electron microscopy and multisample analysis of the measured oxide thickness difference from one sample at two different times during the oxide growth phase or from two separate samples to obtain the optical constants of the oxides. With the obtained thickness and optical constants of the oxides, the optical properties of the substrate material can be uniquely deduced. This methodology has been applied to obtain, the refractive indices and extinction coefficients of delta plutonium (δ-Pu) metal with 0.5 wt. % Ga in the wavelength region from 435 nm to 850 nm, without the influence of surface oxides. Lastly, the presented methodology can also be applied to metals and semiconductors from surface oxidized samples, even when the oxides do not possess a common set of optical characteristics.

36 MATERIALS SCIENCE↗

Optical constants of polycrystalline Al 0.25 Ga 0.75 P and Al 0.9 Ga 0.1 As determined by variable-angle spectroscopic ellipsometry

The optical constants of single-crystal Al x Ga 1-x P and Al x Ga 1-x As have been widely studied at various Al compositions but have not yet been thoroughly investigated as polycrystalline materials. Using variable-angle spectroscopic ellipsometry, we estimate and analyze the optical constants of polycrystalline Al 0.25 Ga 0.75 P and Al 0.9 Ga 0.1 As that were non-epitaxially deposited at deposition temperatures of either 250 or 420 °C, and with various dopant species, dopant concentrations, and V/III flux ratios. Here, for wavelengths of 350–400 nm, decreasing the V/III ratio increases the refractive index of Be-doped polycrystalline Al 0.25 Ga 0.75 P. For wavelengths >500 nm, as the targeted Be dopant concentration increases for polycrystalline Al 0.25 Ga 0.75 P, the amount the extinction coefficient increases and the indirect bandgap decreases depends on the V/III ratio. Furthermore, Si-doped polycrystalline Al 0.25 Ga 0.75 P has significantly smaller extinction coefficient values than when it is Be-doped, for the same V/III ratio and targeted doping concentration, at wavelengths >500 nm. Based on our findings, we hypothesize that the dopant species, dopant concentration, and the V/III ratio dictate various types of defect concentrations, which then affect the optical constants and indirect bandgap of polycrystalline Al 0.25 Ga 0.75 P. Additionally, for wavelengths >500 nm, we find that polycrystalline Al 0.25 Ga 0.75 P and Al 0.9 Ga 0.1 As have the lowest extinction coefficient values when deposited at 420 °C, as opposed to 250 °C. Thus, we hypothesize that the deposition temperature is the most significant factor in dictating the optical constants of these polycrystalline III-Vs. Ultimately, this work demonstrates alternative methods to tune the optical constants of polycrystalline Al 0.25 Ga 0.75 P and Al 0.9 Ga 0.1 As, as opposed to tuning the Al composition.

42 ENGINEERING↗

Assessing atomically thin delta-doping of silicon using mid-infrared ellipsometry

Hydrogen lithography has been used to template phosphine-based surface chemistry to fabricate atomic-scale devices, a process we abbreviate as atomic precision advanced manufacturing (APAM). In this work, we use mid-infrared variable angle spectroscopic ellipsometry (IR-VASE) to characterize single-nanometer thickness phosphorus dopant layers (δ-layers) in silicon made using APAM compatible processes. A large Drude response is directly attributable to theδ-layer and can be used for nondestructive monitoring of the condition of the APAM layer when integrating additional processing steps. Furthermore, the carrier density and mobility extracted from our room temperature IR-VASE measurements are consistent with cryogenic magneto-transport measurements, showing that APAM δ-layers function at room temperature. Finally, the permittivity extracted from these measurements shows that the doping in the APAM δ-layers is so large that their low-frequency in-plane response is reminiscent of a silicide. However, there is no indication of a plasma resonance, likely due to reduced dimensionality and/or low scattering lifetime.

2D material↗

Variable angle of incidence spectroscopic ellipsometry Application to GaAs-Al(x)Ga(1-x)As multiple heterostructures

The sensitivity of spectroscopic ellipsometry data to multilayer model parameters is shown to be a strong function of the angle of incidence. A quantitative study of sensitivity versus angle of incidence is performed for a GaAs-Al(x)Ga(1-x)As-GaAs substrate structure, showing that maximum sensitivity to layer thicknesses and AlGaAs composition occurs near the wavelength-dependent principal angle. These results are verified by experimental measurements on two molecular-beam epitaxy grown samples.

Snyder, Paul G.↗

Variable angle spectroscopic ellipsometry - Application to GaAs-AlGaAs multilayer homogeneity characterization

Variable angle spectroscopic ellipsometry has been applied to a GaAs-AlGaAs multilayer structure to obtain a three-dimensional characterization, using repetitive measurements at several spots on the same sample. The reproducibility of the layer thickness measurements is of order 10 A, while the lateral dimension is limited by beam diameter, presently of order 1 mm. Thus, the three-dimensional result mainly gives the sample homogeneity. In the present case three spots were used to scan the homogeneity over 1 in of a wafer which had molecular-beam epitaxially grown layers. The thickness of the AlGaAs, GaAs, and oxide layers and the Al concentration varied by 1 percent or less from edge to edge. This result was confirmed by two methods of data analysis. No evidence of an interfacial layer was observed on top of the AlGaAs.

Alterovitz, Samuel A.↗

Thin-film hermeticity - A quantitative analysis of diamondlike carbon using variable angle spectroscopic ellipsometry

This paper reports on the successful application of variable-angle spectroscopic ellipsometry to quantitative thin-film hermeticity evaluation. It is shown that, under a variety of film preparations and moisture introduction conditions, water penetrates only a very thin diamondlike carbon (DLC) top surface-roughness region. Thus, DLC is an excellent candidate for use as protective coatings in adverse chemical and aqueous environments.

Orzeszko, S.↗

Characterization of multilayer GaAs/AlGaAs transistor structures by variable angle spectroscopic ellipsometry

Variable angle of incidence spectroscopic ellipsometry (VASE) has been implemented as a means of determining layer thickness, alloy composition, and growth quality of GaAs/AlGaAs samples composed of relatively thick layers as well as superlattices. The structures studied in this work contained GaAs/AlGaAs multilayers with a superlattice 'barrier' and were grown for later formation of modulation-doped field effect transistors (MODFETs). Sample modeling was performed by treating the superlattice as a bulk AlGaAs layer of unknown composition. Extremely good data fits were realized when five layer thicknesses and two alloy ratios were allowed to vary in a regression analysis. Room temperature excitonic effects associated with the e-hh(1), e-lh(1) and e-hh(2) transitions were observed in the VASE data.

Merkel, Kenneth G.↗

Study of InGaAs based MODFET structures using variable angle spectroscopic ellipsometry

Variable angle spectroscopic ellipsometry was used to estimate the thicknesses of all layers within the optical penetration depth of InGaAs based MODFET structures. Strained and unstrained InGaAs channels were made by MBE on InP substrates and by MOCVD on GaAs substrates. In most cases, ellipsometrically determined thicknesses were within 10 percent of the growth calibration results. The MBE made InGaAs strained layers showed large strain effects, indicating a probable shift in the critical points of their dielectric function toward the InP lattice matched concentration.

Alterovitz, S. A.↗

Study of InGaAs-based modulation doped field effect transistor structures using variable-angle spectroscopic ellipsometry

Variable-angle spectroscopic ellipsometry was used to estimate the thicknesses of all layers within the optical penetration depth of InGaAs-based modulation doped field effect transistor structures. Strained and unstrained InGaAs channels were made by molecular beam epitaxy (MBE) on InP substrates and by metal organic chemical vapor deposition on GaAs substrates. In most cases, ellipsometrically determined thicknesses were within 10 percent of the growth-calibration results. The MBE-made InGaAs strained layers showed large strain effects, indicating a probable shift in the critical point of their dielectric function toward the InP lattice-matched concentration.

Alterovitz, Samuel A.↗

Atomic oxygen effects on thin film space coatings studied by spectroscopic ellipsometry, atomic force microscopy, and laser light scattering

The University of Nebraska is currently evaluating Low Earth Orbit (LEO) simulation techniques as well as a variety of thin film protective coatings to withstand atomic oxygen (AO) degradation. Both oxygen plasma ashers and an electron cyclotron resonance (ECR) source are being used for LEO simulation. Thin film coatings are characterized by optical techniques including Variable Angle Spectroscopic Ellipsometry, Optical spectrophotometry, and laser light scatterometry. Atomic Force Microscopy (AFM) is also used to characterize surface morphology. Results on diamondlike carbon (DLC) films show that DLC degrades with simulated AO exposure at a rate comparable to Kapton polyimide. Since DLC is not as susceptible to environmental factors such as moisture absorption, it could potentially provide more accurate measurements of AO fluence on short space flights.

Synowicki, R. A.↗