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DOE OSTI2023

Comparison of methods to derive infrared optical constants for organic materials for optical modeling

Reflectance spectroscopy, especially at infrared wavelengths, is often used for contact, standoff, and remote sensing of solid materials. The reflectance spectra of solids, however, are complex, relying on many factors, even for the same material. Such phenomena can be modeled if the optical constants as a function of wavelength or wavenumber, n(?) and k(?), are known. Methods to measure the optical constants of solids, however, are challenging, particularly for powdered materials. For powdered materials, a pressed pellet of the neat material is often used when a crystalline specimen is not available. In this work, three techniques, including ellipsometry, single-angle reflectance and KBr transmission spectroscopy, are applied to an organic material, acetaminophen, for comparison, and the effects on the modeled spectra are shown.

ellipsometry, infrared (IR) spectroscopy, FTIR, hy↗

DOE OSTI2023

X-ray wavefront sensor development at the Advanced Light Source

At Lawrence Berkeley National Laboratory's Advanced Light Source, we are developing x-ray wavefront sensors to support the creation and operation of beamlines with diffraction-limited quality. Our new approach to rapid, intermittent wavefront sensing operates in reflection at glancing incidence angles and is compatible with the high-power densities of modern beamlines. For soft x-ray applications especially, the wavefront sensor can operate upstream of the exit slit in a vertically dispersed beam. This single-shot technique supports lateral shearing interferometry and Hartmann wavefront sensing; it can be adapted to speckle-based techniques as well. The reflected beam is directed to an off-axis YAG crystal that produces scintillated visible light. A small mirror reflects the light to a microscope and camera, and the measured wavefront shape information can be used as feedback to adaptive x-ray mirror elements. A compact array of gratings enables measurement across a broad range of photon energies or wavefront curvatures. We describe recent demonstrations at soft x-ray and hard x-ray wavelengths measuring an adaptive x-ray mirror, and a toroidal focusing mirror.

Goldberg, Kenneth A↗

DOE OSTI2024

Static metrology of the meter-scale deformable heliostat

This paper describes a heliostat metrology system which is developed based on deflectometry, utilizing a static perforated panel instead of conventional dynamic monitor displays to provide incident rays. The developed method is named static screen deflectometry (SSD). This robust and scalable method is especially valuable for outdoor tests of large reflectors used in concentrating solar-thermal power (CSP) systems. The developed method has been successfully demonstrated on a 2.4 𝑚 × 3.3 𝑚 float glass deformable reflector bent to focus sunlight at 113 𝑚 distance throughout a day. From images obtained from a camera at 50𝑚 distance, the reflector surface was measured to an accuracy of less than 1 𝑚𝑟𝑎𝑑 rms slope error in the full test scope.

14 SOLAR ENERGY↗

DOE OSTI2020

Spatially resolved characterization of optical and recombination losses for different industrial silicon solar cell architectures

In this work, spatially resolved characterization methods are used to identify loss mechanisms for common p -type silicon solar cell architectures, including multicrystalline aluminum back surface field (Al-BSF), monocrystalline Al-BSF, monocrystalline passivated emitter and rear cells (PERC), and bifacial monocrystalline PERC. The characterization methods used in this work include suns-V OC , photoluminescence imaging, and spatially resolved external quantum efficiency and reflectance measurements. The optical and recombination losses are driven by the material properties, cell processing conditions, and device architecture. These losses are quantified and categorized in terms of underlying mechanisms (e.g., front reflectance, escape reflectance, front recombination, and parasitic optical absorption and recombination in the bulk and rear). The ability to create images of these loss parameters can be used to gain more insight into the materials and manufacturing processes used to produce solar cells, and examples are given in this work to illustrate how these images can help reveal the origin of defects.

14 SOLAR ENERGY↗

DOE OSTI2022

Are there echoes of gravitational waves?

In several approaches to evading the information paradox, the semiclassical black hole is replaced by an Exotic Compact Object (ECO). It has been conjectured that gravitational waves emitted by the merger of ECOs can reflect off the ECOs and produce a detectable ‘echo’. We argue that while a part of the wave can indeed reflect off the surface of an ECO, this reflected wave will get trapped by a new closed trapped surface produced by its own backreaction. Thus, no detectable signal of the echo will emerge to infinity. The only assumption in this analysis is that causality is maintained to leading order in gently curved spacetime. Thus, if echoes are actually detected, then we would face a profound change in our understanding of physics.

Astronomy & Astrophysics↗

DOE OSTI2022

Evaluation of WRF simulation of deep convection in the US Southern Great Plains

The Southern Great Plains (SGP) exhibits a relatively high frequency of periods with extremely high rainfall rates (RR) and hail. Here, seven months of 2017 are simulated using the Weather Research and Forecasting (WRF) model applied at convection permitting resolution with the Mibrandt-Yau microphysics scheme. Simulation fidelity is evaluated, particularly during intense convective events, using data from ASOS stations, dual-polarization RADAR, gridded data sets and observations at the DoE Atmospheric Radiation Measurement site. The spatial gradients and temporal variability of precipitation and the cumulative density functions for both RR and wind speeds exhibit fidelity. Odds ratios >1 indicate WRF is also skillful in simulating high composite reflectivity (cREF, used as a measure of widespread convection) and RR > 5 mmhr –1 over the domain. Detailed analyses of the ten days with highest spatial coverage of cREF >30 dBZ show spatially similar reflectivity fields and high RR in both RADAR data and WRF simulations. However, during periods of high reflectivity, WRF exhibits a positive bias in terms of very high RR (> 25 mmhr –1 ) and hail occurrence, and during the summer and transition months, maximum hail size is underestimated. For some renewable energy applications fidelity is required with respect to the joint probabilities of wind speed and RR and/or hail. While partial fidelity is achieved for the marginal probabilities, performance during events of critical importance to these energy applications is currently not sufficient. Further research into optimal WRF configurations in support of potential damage quantification for these applications is warranted.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

A Regime-Oriented Approach to Observationally Constraining Extratropical Shortwave Cloud Feedbacks

The extratropical shortwave (SW) cloud feedback is primarily due to increases in extratropical liquid cloud extent and optical depth. Here, we examine the response of extratropical (35°–75°) marine cloud liquid water path (LWP) to a uniform 4-K increase in sea surface temperature (SST) in global climate models (GCMs) from phase 5 of the Coupled Model Intercomparison Project (CMIP5) and variants of the HadGEM3-GC3.1 GCM. Compositing is used to partition data into periods inside and out of cyclones. The response of extratropical LWP to a uniform SST increase and associated atmospheric response varies substantially among GCMs, but the sensitivity of LWP to cloud controlling factors (CCFs) is qualitatively similar. When all other predictors are held constant, increasing moisture flux drives an increase in LWP. Increasing SST, holding all other predictors fixed, leads to a decrease in LWP. The combinations of these changes lead to LWP, and by extension reflected SW, increasing with warming in both hemispheres. Observations predict an increase in reflected SW over oceans of 0.8–1.6 W m -2 per kelvin SST increase (35°–75°N) and 1.2–1.9 W m -2 per kelvin SST increase (35°–75°S). This increase in reflected SW is mainly due to increased moisture convergence into cyclones because of increasing available moisture. The efficiency at which converging moisture is converted into precipitation determines the amount of liquid cloud. Thus, cyclone precipitation processes are critical to constraining extratropical cloud feedbacks

58 GEOSCIENCES↗

DOE OSTI2021

Clarifying remotely-retrieved precipitation of shallow marine clouds from the NSF/NCAR Gulfstream V

Precipitation is a key process within the shallow cloud lifecycle. The Cloud System Evolution in the Trades (CSET) campaign included the first deployment of a 94 GHz Doppler radar and 532 nm lidar. Despite a larger sampling volume, initial mean radar/lidar retrieved rain rates (Schwartz et al. 2019) based on the upward-pointing remote sensor datasets are systematically less than those measured by in-situ precipitation probes in the cumulus regime. Subsequent retrieval improvements produce rainrates that compare better to in-situ values, but still underestimate. Retrieved shallow cumulus drop sizes can remain too small and too few, with an overestimated shape parameter narrowing the raindrop size distribution too much. Three potential causes for the discrepancy are explored: the gamma functional fit to the dropsize distribution, attenuation by rain and cloud water, and an underaccounting of Mie dampening of the reflectivity. A truncated exponential fit may represent the dropsizes below a showering cumulus cloud more realistically, although further work would be needed to fully evaluate the impact of a different dropsize representation upon the retrieval. The rain attenuation is within the measurement uncertainty of the radar. Mie dampening of the reflectivity is shown to be significant, in contrast to previous stratocumulus campaigns with lighter rain rates, and may be difficult to constrain well with the remote measurements. An alternative approach combines an a priori determination of the dropsize distribution width based on the in-situ data with the mean radar Doppler velocity and reflectivity. This can produce realistic retrievals, although a more comprehensive assessment is needed to better characterize the retrieval errors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Standoff Detection of Oil and Powder Mixtures at 12 Meters Using a Tunable Quantum Cascade Laser-Based System with a Close Focus Telescope and Uncooled Infrared Detector

We have designed and demonstrated a quantum cascade laser (QCL) based standoff system that utilizes an uncooled mercury cadmium telluride (MCT) detector with lock-in signal processing for chemical identification at a distance of 12.5 meters in indoor ambient light conditions. In the system, a tunable quad-QCL operating (1 MHz) in quasi-continuous wave mode between 8.45 and 10.03 μm (~1182 to 1000 cm –1 ) serves as the active mid-infrared source for remotely interrogating mineral, powder, and thin film oil samples including powder mixtures (6, 12.5, 25, and 50%) of crystalline quartz (SiO 2 ) in KBr. Light as reflected from a given sample is collected using a 10-inch (25.4 cm) Dall Kirkham telescope and coupled with ZnSe optics to an uncooled MCT detector. Furthermore, the mixture dependence of the highly transparent KBr and strongly absorbing quartz was found to fit a modified version of the Schatz reflectance model for compacted powder mixtures. All reflectance spectra reported are relative to an Au-coated diffuse reflector. A NIST traceable polystyrene standard reflector was also used to determine the QCL wavelength tuning range and calibration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Determining fast-S and slow-S propagation directions with SV-P data produced by buried explosives and recorded with vertical geophones

We have evaluated the concept of practicing S-wave reflection seismology with legacy 3D seismic data generated by a P-wave source and recorded with only vertical geophones. This type of S-wave imaging is based on the principle that seismic P-wave sources not only produce a downgoing illuminating P wavefield, but they also simultaneously produce a downgoing illuminating SV wavefield that, in almost all cases, is suitable for S-wave reflection imaging. The S-mode used in this study is the SV-P, or converted-P, mode. This mode involves a downgoing illuminating SV wavefield and an upgoing reflected P-mode that is recorded by vertical geophones. In flat-layered stratigraphy, the lengths of the SV and P raypaths in SV-P imaging are identical to the lengths of the SV and P raypaths in P-SV imaging with P-sources and 3C geophones. P-SV imaging of deep rocks has been practiced for more than two decades; SV-P imaging is a new concept. SV-P data should provide the same options for investigating deep rocks as do P-SV data. We have determined one of the equivalences between SV-P data extracted from vertical-geophone data and P-SV data extracted from horizontal geophones: that both modes react to azimuth-dependent variations in the S velocity in anisotropic rocks. Azimuthal variations in the SV-P traveltime can be used to define the polarization direction of the fast-S-wave mode, which is also the azimuth of the maximum horizontal stress (SHmax). Our investigation demonstrates a noninvasive method for monitoring changes in the SHmax azimuth across a CO 2 storage reservoir, or any targeted porous rock, as fluids are cycled into, and then out of, that rock’s pore space.

Geochemistry & Geophysics↗

DOE OSTI2022

Neural net detection of seismic features related to gas hydrates and free gas accumulations on the northern U.S. Atlantic margin

Bottom-simulating reflections (BSRs) that sometimes mark the base of the gas hydrate stability zone in marine sediments are often identified based on the reverse polarity reflections that cut across stratigraphic layering in seismic amplitude data. On the northern U.S. Atlantic margin (USAM) between Cape Hatteras and Hudson Canyon, legacy seismic data have revealed pronounced BSRs south of the deepwater extension of Hudson Canyon and more subtle ones from offshore Delaware south to Cape Hatteras, where the reflections sometimes follow stratigraphic layering. Using high-resolution seismic data acquired during the 2018 Mid-Atlantic Resource Imaging Experiment and a supervised neural net, we identify seismic features associated with gas hydrates and/or the top of gas between Hudson Canyon and Cape Hatteras. Using seismic attributes especially sensitive to the presence of gas, we train a neural network algorithm on seismic data from an area with strong BSRs and then apply the model to the rest of the data set. The results indicate that gas hydrate and/or shallow free gas are significantly more widespread on the northern part of the USAM than previously known. Seismic indicators of gas extend landward from the 2000 m isobath to the upper continental slope in sectors with (offshore Virginia) and, to a lesser extent, without (offshore New Jersey) pervasive upper slope methane seeps. Higher sand content and intermediate sediment thickness, factors related to the container size and gas charge in a petroleum systems framework, are associated with more robust gas indicators.

Geochemistry & Geophysics↗

DOE OSTI2022

Incoherent range-based holography of far-distant objects using LIDAR

Los Alamos National Laboratory has developed an incoherent, long-range, sub-centimeter resolution (LIDAR) with which we achieve centimeter-scale reflection holography at extremely long ranges. The system consists of a pulsed laser and photon-counting receiver. This combination yields round-trip time of flight data to illuminate parts of the object of interest. The aggregation of these data for many LIDAR pulses yields a plot with a range on the X axis and reflectance on the Y axis, which we refer to as a range profile. Observing that the range profile is a projection of the reflection map of the object onto the view vector, we collect profiles from a variety of viewing angles and invert these data to form an image. We adapt imaging algorithms from the field of computer aided tomography to suit our application and present results from imaging demonstrations at a 10 km range.

Hoffmann, Mitchell P. (ORCID:0000000170551324)↗

DOE OSTI2022

Simons Observatory: broadband metamaterial antireflection cuttings for large-aperture alumina optics

Here we present the design, fabrication, and measured performance of metamaterial antireflection cuttings (ARCs) for large-format alumina filters operating over more than an octave of bandwidth to be deployed at the Simons Observatory (SO). The ARC consists of subwavelength features diced into the optic’s surface using a custom dicing saw with near-micrometer accuracy. The designs achieve percent-level control over reflections at angles of incidence up to 20°. The ARCs were demonstrated on four 42 cm diameter filters covering the 75 to 170 GHz band and a 50 mm diameter prototype covering the 200 to 300 GHz band. The reflection and transmission of these samples were measured using a broadband coherent source that covers frequencies from 20 GHz to 1.2 THz. These measurements demonstrate percent-level control over reflectance across the targeted pass-bands and a rapid reduction in transmission as the wavelength approaches the length scale of the metamaterial structure where scattering dominates the optical response. The latter behavior enables use of the metamaterial ARC as a scattering filter in this limit.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2026

Design of a broadband, high-power, off-axis spiral polarization reflector

Spirally polarized beams are known to produce a strong longitudinal field under high numerical aperture focusing. Here, we report on the design of a reflective optical element with an off-axis geometry that is capable of transforming a uniformly polarized beam into a predominantly spirally polarized beam. By utilizing the retardance present in Fresnel reflection, our device can operate over a broad range of wavelengths. The output polarization and intensity structure of a beam passing through the reflector are calculated using polarization and scalar ray tracing. Vector diffraction is used to calculate the polarization and intensity structure under $f/0.656$ focusing. The off-axis reflective design is well-suited for high-power laser applications and could enable current and future laser-based particle accelerators to achieve strong longitudinal fields at focus.

Black, A. Nicholas [Univ. of Rochester, NY (United↗

DOE OSTI2022

New method for the determination of photoabsorption from transmittance measurements in the extreme ultraviolet

We have developed a new method for the determination of photoabsorption at extreme ultraviolet wavelengths longer than 20 nm, where reliable refractive index values are sparse or non-existent. Our method overcomes the obstacle of multiple reflections that occur inside thin films in this spectral range, which up until now has prevented the accurate determination of photoabsorption from transmittance measurements. We have derived a mathematical expression that is independent of internal reflection amplitudes, while taking advantage of the transmittance oscillations stemming from such reflections. The method is validated on measurements of aluminum thin films. This advance will enable accurate refractive index values for many important materials for optical instrumentation, thus facilitating high-priority research on topics including coherent light sources, planetary and solar physics, and semiconductor manufacturing.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Correcting thermal-emission-induced detector saturation in infrared spectroscopy

We found that temperature-dependent infrared spectroscopy measurements (i.e., reflectance or transmittance) using a Fourier-transform spectrometer can have substantial errors, especially for elevated sample temperatures and collection using an objective lens. These errors can arise as a result of partial detector saturation due to thermal emission from the measured sample reaching the detector, resulting in nonphysical apparent reduction of reflectance or transmittance with increasing sample temperature. Here, we demonstrate that these temperature-dependent errors can be corrected by implementing several levels of optical attenuation that enable convergence testing of the measured reflectance or transmittance as the thermal-emission signal is reduced, or by applying correction factors that can be inferred by looking at the spectral regions where the sample is not expected to have a substantial temperature dependence.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Multislice forward modeling of coherent surface scattering imaging on surface and interfacial structures

To study nanostructures on substrates, surface-sensitive reflection-geometry scattering techniques such as grazing incident small angle X-ray scattering are commonly used to yield an averaged statistical structural information of the surface sample. Grazing incidence geometry can probe the absolute three-dimensional structural morphology of the sample if a highly coherent beam is used. Coherent surface scattering imaging (CSSI) is a powerful yet non-invasive technique similar to coherent X-ray diffractive imaging (CDI) but performed at small angles and grazing-incidence reflection geometry. A challenge with CSSI is that conventional CDI reconstruction techniques cannot be directly applied to CSSI because the Fourier-transform-based forward models cannot reproduce the dynamical scattering phenomenon near the critical angle of total external reflection of the substrate-supported samples. To overcome this challenge, we have developed a multislice forward model which can successfully simulate the dynamical or multi-beam scattering generated from surface structures and the underlying substrate. The forward model is also demonstrated to be able to reconstruct an elongated 3D pattern from a single shot scattering image in the CSSI geometry through fast-performing CUDA-assisted PyTorch optimization with automatic differentiation.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2023

Impact of substrates and quantum effects on exciton line shapes of 2D semiconductors at room temperature

Exciton resonances in monolayer transition-metal dichalcogenides (TMDs) provide exceptionally strong light–matter interaction at room temperature. Their spectral line shape is critical in the design of a myriad of optoelectronic devices, ranging from solar cells to quantum information processing. However, disorder resulting from static inhomogeneities and dynamical fluctuations can significantly impact the line shape. Many recent works experimentally evaluate the optical properties of TMD monolayers placed on a substrate and the line shape is typically linked directly to the material’s quality. Here, we highlight that the interference of the substrate and TMD reflections can strongly influence the line shape. We further show how basic, room-temperature reflection measurements allow investigation of the quantum mechanical exciton dynamics by systematically controlling the substrate reflection with index-matching oils. By removing the substrate contribution with properly chosen oil, we can extract the excitonic decay rates including the quantum mechanical dephasing rate. The results provide valuable guidance for the engineering of exciton line shapes in layered nanophotonic systems.

2D semiconductor↗