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At least 253 records · Page 14

Instrument for in situ hard x-ray nanobeam characterization during epitaxial crystallization and materials transformations

Solid-phase epitaxy (SPE) and other three-dimensional epitaxial crystallization processes pose challenging structural and chemical characterization problems. The concentration of defects, the spatial distribution of elastic strain, and the chemical state of ions each vary with nanoscale characteristic length scales and depend sensitively on the gas environment and elastic boundary conditions during growth. The lateral or three-dimensional propagation of crystalline interfaces in SPE has nanoscale or submicrometer characteristic distances during typical crystallization times. Here, an in situ synchrotron hard x-ray instrument allows these features to be studied during deposition and crystallization using diffraction, resonant scattering, nanobeam and coherent diffraction imaging, and reflectivity. The instrument incorporates a compact deposition system allowing the use of short-working-distance x-ray focusing optics. Layers are deposited using radio-frequency magnetron sputtering and evaporation sources. The deposition system provides control of the gas atmosphere and sample temperature. The sample is positioned using a stable mechanical design to minimize vibration and drift and employs precise translation stages to enable nanobeam experiments. Results of in situ x-ray characterization of the amorphous thin film deposition process for a SrTiO 3 /BaTiO 3 multilayer illustrate implementation of this instrument.

47 OTHER INSTRUMENTATION↗

Multimodal Tip-Enhanced Nonlinear Optical Nanoimaging of Plasmonic Silver Nanocubes

Optical field localization at plasmonic tip-sample nanojunctions has enabled high spatial resolution chemical analysis through tip-enhanced linear optical spectroscopies, including Raman scattering and photoluminescence. In this work, we illustrate that nonlinear optical processes, including parametric four-wave mixing (4WM), second harmonic/sum-frequency generation (SHG and SFG), and two-photon photoluminescence (TPPL), can be enhanced at plasmonic junctions and spatio-spectrally resolved simultaneously with few-nm spatial resolution under ambient conditions. More importantly, through a detailed analysis of our spectral nano-images, we find that the efficiencies of the local nonlinear signals are determined by sharp tip-sample junction resonances that vary over the few-nanometer length scale because of the corrugated nature of the probe. Namely, plasmon resonances centered at or around the different nonlinear signals are tracked through TPPL, and they are found to selectively enhance nonlinear signals with closely matched optical resonances.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bulk reconstruction and non-isometry in the backwards-forwards holographic black hole map

The backwards-forwards map, introduced as a generalization of the non-isometric holographic maps of the black hole interior of Akers, Engelhardt, Harlow, Penington, and Vardhan to include non-trivial dynamics in the effective description, has two possible formulations differing in when the post-selection is performed. While these two forms are equivalent on the set of dynamically generated states — states formed from unitary time evolution acting on well-defined initial configurations of infalling matter — they differ on the generic set of states necessary to describe the apparent world of the infalling observer. We show that while both versions successfully reproduce the Page curve, the version involving post-selection as the final step, dubbed the backwards-forwards-post-selection (BFP) map, has the desirable properties of being non-isometric but isometric on average and providing state-dependent reconstruction of bulk operators, while the other version does not. Thus the BFP map is a suitable non-isometric code describing the black hole interior including interior interactions.

3-D Image Reconstruction↗

Hierarchical Self-Assembly of Carbon Dots into High-Aspect-Ratio Nanowires

Here, we report a spontaneous and hierarchical self-assembly mechanism of carbon dots prepared from citric acid and urea into nanowire structures with large aspect ratios (>50). Scattering-type scanning near-field optical microscopy (s-SNOM) with broadly tunable mid-IR excitation was used to interrogate details of the self-assembly process by generating nanoscopic chemical maps of local wire morphology and composition. s-SNOM images capture the evolution of wire formation and the complex interplay between different chemical constituents directing assembly over the nano- to microscopic length scales. We propose that residual citrate promotes tautomerization of melamine surface functionalities to produce supramolecular shape synthons comprised of melamine-cyanurate adducts capable of forming long-range and highly directional hydrogen-bonding networks. This intrinsic, heterogeneity-driven self-assembly mechanism reflects synergistic combinations of high chemical specificity and long-range cooperativity that may be harnessed to reproducibly fabricate functional structures on arbitrary surfaces.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

High Cooperativity Using a Confocal-Cavity–QED Microscope

Cavity quantum electrodynamics (QED) with cooperativity far greater than unity enables high-fidelity quantum sensing and information processing. The high-cooperativity regime is often reached through the use of short single-mode resonators. More complicated multimode resonators, such as the near-confocal optical Fabry-Pérot cavity, can provide intracavity atomic imaging in addition to high cooperativity. This capability has recently proved important for exploring quantum many-body physics in the driven-dissipative setting. In this work, we show that a confocal-cavity–QED microscope can realize cooperativity in excess of 110. This cooperativity is on par with the very best single-mode cavities (which are far shorter) and 21 times greater than single-mode resonators of similar length and mirror radii. The 1.7-µm imaging resolution is naturally identical to the photon-mediated interaction range. We measure these quantities by determining the threshold of cavity superradiance when small optically tweezed BoseEinstein condensates are pumped at various intracavity locations. Transmission measurements of an ex situ cavity corroborate these results. We provide a theoretical description that shows how cooperativity enhancement arises from the dispersive coupling to the atoms of many near-degenerate modes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Flexible Soft X-Ray Image Sensors based on Metal Halide Perovskites With High Quantum Efficiency

Soft X-ray imaging is a powerful tool to explore the structure of cells, probe material with nanometer resolution, and investigate the energetic phenomena in the universe. Conventional soft X-ray image sensors are by and large Si-based charge coupled devices that suffer from low frame rates, complex fabrication processes, mechanical inflexibility, and required cooling below -60 °C. Here, a soft X-ray photodiode is reported based on low-cost metal halide perovskite with comparable performance to commercial Si-based device. Nanothrough network electrode minimized the optical loss due to the shadowing of insensitive layers, while a multidimensional perovskite heterojunction is generated to reduce the photo-generated carrier loss. Further, this strategy promoted a record quantum efficiency of 8 × 10 3 % without cooling, several orders of magnitude greater than the previously achieved. Flexible and curved soft X-ray imaging arrays are fabricated based on this high-performance device structure, demonstrating stable soft X-ray response and sharp imaging capabilities. This work highlights the low-cost and efficient perovskite photodiode as a strong candidate for the next-generation soft X-ray image sensors.

36 MATERIALS SCIENCE↗

Spatially co-registered wide-field nonlinear optical imaging of living and complex biosystems in a total internal reflection geometry

Nonlinear optical microscopy that leverages an objective based total internal reflection (TIR) excitation scheme is an attractive means for rapid, wide-field imaging with enhanced surface sensitivity. Through select combinations of distinct modalities, one can, in principle, access complementary chemical and structural information for various chemical species near interfaces. Here, we report a successful implementation of such a wide-field nonlinear optical microscope system, which combines coherent anti-Stokes Raman scattering (CARS), two-photon fluorescence (TPF), second harmonic generation (SHG), and sum frequency generation (SFG) modalities on the same platform. The intense optical fields needed to drive these high order nonlinear optical processes are achieved through the use of femtosecond pulsed light in combination with the intrinsic field confinement induced by TIR over a large field of view. The performance of our multimodal microscope was first assessed through the experimental determination of its chemical fidelity, intensity and polarization dependences, and spatial resolution using a set of well-defined model systems. Subsequently, its unique capabilities were validated through imaging complex biological systems, including Hydrangea quercifolia pollen grains and Pantoea sp. YR343 bacterial cells. Specifically, the spatial distribution of different molecular groups in the former was visualized via vibrational contrast mechanisms of CARS, whereas co-registered TPF imaging allowed the identification of spatially localized intrinsic fluorophores. We further demonstrate the feasibility of our microscope for wide-field CARS imaging on live cells through independent characterization of cell viability using spatially co-registered TPF imaging. Overall, this approach to TIR enabled wide-field imaging is expected to provide new insights into bacterial strains and their interactions with other species in the rhizosphere in a time-resolved and chemically selective manner.

47 OTHER INSTRUMENTATION↗

The effect of WAAM process parameters on process conditions and production metrics in the fabrication of single-pass multi-layer wall artifacts

The present work seeks to understand the impact of varying dwell time and input deposition power on part quality and overall production time for wire arc additive manufacturing. In this work, multi-layer wall geometries were deposited under different input power conditions without affecting the material deposition rate by setting traverse speed and wire feed speed constant and varying the contact tip-to-workpiece distance and the deposition power settings. Current and voltage data and optical imaging of the deposition zone were captured in situ, and wall geometry was characterized using laser scanning, so to understand the applicability of these methods for determining part height in situ. Furthermore, the present results demonstrate that alternating dwell times with lower input deposition power can result in significantly reduced overall production time and minimal material underbuilding, despite increased deposition geometry width. Furthermore, it is shown that while elimination of process dwell results in severe underbuilding of the deposition, it also yields the highest production rate for a hybrid-finished (e.g., deposited, machined) wall in terms of mm in build direction per minute and the highest buy-to-fly ratio.

36 MATERIALS SCIENCE↗

Pressure-based process monitoring of direct-ink write material extrusion additive manufacturing

As additive manufacturing (AM) has become a reliable method for creating complex and unique hardware rapidly, the quality assurance of printed parts remains a priority. In situ process monitoring offers an approach for performing quality control while simultaneously minimizing post-production inspection. For extrusion printing processes, direct linkages between extrusion pressure fluctuations and print defects can be established by integrating pressure sensors onto the print head. In this work, the sensitivity of process monitoring is tested using engineered spherical defects. Pressure and force sensors located near an ink reservoir and just before the nozzle are shown to assist in identification of air bubbles, changes in height between the print head and build surface, clogs, and particle aggregates with a detection threshold of 60–70% of the nozzle diameter. Visual evidence of printed bead distortion is quantified using optical image analysis and correlated to pressure measurements. Importantly, this methodology provides an ability to monitor the quality of AM parts produced by extrusion printing methods and can be accomplished using commonly available pressure-sensing equipment.

36 MATERIALS SCIENCE↗

Coherent diffraction imaging in the undergraduate laboratory

We present an undergraduate optics instructional laboratory designed to teach skills relevant to a broad range of modern scientific and technical careers. In this laboratory project, students image a custom aperture using coherent diffraction imaging, while learning principles and skills related to digital image processing and computational imaging, including multidimensional Fourier analysis, iterative phase retrieval, noise reduction, finite dynamic range, and sampling considerations. After briefly reviewing these imaging principles, we describe the required experimental materials and setup for this project. Our experimental apparatus is both inexpensive and portable, and a software application we developed for interactive data analysis is freely available.

Porter, J. Nicholas↗

Near-field infrared microscopy: A novel analytic mapping technique to nanocharacterize calcium silicate-based cement materials

Infrared imaging via scattering-type scanning near-field optical microscopy (s-SNOM) allows chemical mapping of organic and inorganic materials with nanoscale spatial resolution. However, its potential adaptation to the complex multiphase structure of Portland cement is yet to be explored. Here we demonstrate the successful implementation of s-SNOM to spatially resolve coexisting chemical phases in tricalcium silicate, Portland cement's main compound, with 20-nm resolution. We found that s-SNOM is sensitive to different anhydrous polymorphic phases, revealing nanoscale domains that are ‘invisible’ to other microscopic techniques. Furthermore, s-SNOM's ability to distinguish the unhydrated and hydrated phases signifies its great promise as an analytical tool to study the complex hydration process of cement. The key to s-SNOM's application was nano-modifying the surface roughness of the cement samples, allowing nanoscale infrared imaging without topographical artifacts. Our study opens a window for infrared spectral microscopy in cement and other porous inorganic materials.

36 MATERIALS SCIENCE↗

HAIMOS Ensemble Forecasts for Intra-day and Day- Ahead GHI, DNI and Ramps

The objective of this research is to develop a hybrid physics-based/data-driven forecast model to improve direct normal and global horizontal irradiance (DNI and GHI) prediction for horizons ranging from 1 to 72 hours. Project objectives also address key gaps in state-of-the-art solar forecasting: accurate probabilistic solar forecasts and the forecasting of large irradiance ramps (ramp onset and magnitude). The proposed model ensembles Numerical Weather Prediction (NWP) forecasts, determinist physics-based algorithms, and new-generation cloud cover products (high-resolution rapid refresh satellite images and Large Eddy Simulations). The result is the Hybrid Adaptive Input Model Objective Selection (HAIMOS) ensemble model. HAIMOS blends state of the art machine learning methodologies with physics-based models for cloud cover and cloud optical depth forecasts. The technical activities followed a two-pronged strategy. First, the preprocessing of data, the selection of inputs to the nonlinear approximators, the type of approximator and objective functions, and post-processing ensembling techniques included in HAIMOS were all optimized adaptively to find the best model for a specific goal (reduce DNI/GHI forecast error, improve the prediction of ramp onset, etc.). Second, a large effort was put in improving cloud identification and the forecast of cloud cover and cloud optical depth. To this end, new-generation cloud parametrization products were developed in this work. These include improved algorithms to assist in cloud identification, cloud classification and cloud parametrization from satellite images – three key factors in the accuracy of 1 to 6-hours irradiance forecasts and prediction of ramp onset. Furthermore, we also included cloud information extracted from high resolution rapid refresh satellite images (GOES-16) and Large Eddy Simulations (LES). LES was used to model the atmosphere in detail over locations of interest and produce cloud optical depth forecasts. Once these data streams were validated, they were used as input data to the HAIMOS forecast. The model was developed using data from several climatologically distinct locations with potential for high solar penetration. In the last year of the project, we conducted a validation campaign according to the guidelines stipulated by the Topic Area 1 project as described in the FOA. This effort brings, for the first time, proven machine-learning methodologies for generating state-of-the-art solar forecasts interweaved with detailed physics-based models for cloud detection, and cloud optical depth forecasts. HAIMOS will generate accurate irradiance probabilistic forecast to assist in reducing solar generation prediction error. Globally optimized solar forecast models are more likely to impact solar energy stakeholders. The goal of this project was to increase the state-of-the-art forecast skill from their present values of 10 to 35%. At the end of the project, we achieved between 30% and 50% forecast skill across a wide range of horizons for both GHI and DNI.

14 SOLAR ENERGY↗

Assessing an aqueous flow cell designed for in situ crystal growth under X-ray nanotomography and effects of radiolysis products

Nucleation and growth of minerals has broad implications in the geological, environmental and materials sciences. Recent developments in fast X-ray nanotomography have enabled imaging of crystal growth in solutions in situ with a resolution of tens of nanometres, far surpassing optical microscopy. Here, a low-cost, custom-designed aqueous flow cell dedicated to the study of heterogeneous nucleation and growth of minerals in aqueous environments is shown. To gauge the effects of radiation damage from the imaging process on growth reactions, radiation-induced morphological changes of barite crystals (hundreds of nanometres to ∼1 µm) that were pre-deposited on the wall of the flow cell were investigated. Under flowing solution, minor to major crystal dissolution was observed when the tomography scan frequency was increased from every 30 min to every 5 min (with a 1 min scan duration). The production of reactive radicals from X-ray induced water radiolysis and decrease of pH close to the surface of barite are likely responsible for the observed dissolution. The flow cell shown here can possibly be adopted to study a wide range of other chemical reactions in solutions beyond crystal nucleation and growth where the combination of fast flow and fast scan can be used to mitigate the radiation effects.

36 MATERIALS SCIENCE↗

Magnetic flux distribution, quasiparticle spectroscopy, and quality factors in Nb films for superconducting qubits

Niobium is a practical material platform for superconducting microwave circuits; however, device-level performance can vary significantly depending on film growth and processing conditions. We compare three epitaxial Nb films grown on $c-$plane sapphire substrates under nominally identical conditions, except for the deposition temperature. To correlate internal quality factors, $Q_{\mathrm {i}}$, with material properties, we combine magneto-optical imaging of magnetic flux distribution with quasiparticle spectroscopy via measurements of the London penetration depth, $λ(T)$. In the low-$Q_{\mathrm i}$ film, there is a lesser ability to screen the magnetic field and an irregular temperature variation of $λ(T)$, implying the existence of localized in-gap states. High $Q_{\mathrm i}$ films show the opposite trend. We conclude that our measurements provide an efficient method for characterizing and optimizing superconducting films for quantum informatics applications.

Datta, Amlan [Ames Lab; Iowa State U.]↗

Epidural anesthesia needle guidance by forward-view endoscopic optical coherence tomography and deep learning

Epidural anesthesia requires injection of anesthetic into the epidural space in the spine. Accurate placement of the epidural needle is a major challenge. To address this, we developed a forward-view endoscopic optical coherence tomography (OCT) system for real-time imaging of the tissue in front of the needle tip during the puncture. We tested this OCT system in porcine backbones and developed a set of deep learning models to automatically process the imaging data for needle localization. A series of binary classification models were developed to recognize the five layers of the backbone, including fat, interspinous ligament, ligamentum flavum, epidural space, and spinal cord. The classification models provided an average classification accuracy of 96.65%. During puncture, it is important to maintain a safe distance between the needle tip and the dura mater. Regression models were developed to estimate that distance based on the OCT imaging data. Based on the Inception architecture, our models achieved a mean absolute percentage error of 3.05% ± 0.55%. Overall, our results validated the technical feasibility of using this novel imaging strategy to automatically recognize different tissue structures and measure the distances ahead of the needle tip during the epidural needle placement.

60 APPLIED LIFE SCIENCES↗

Chemically sensitive fluorescence imaging of colliding microdroplets

Here, we present a simple optical capability for generating spatially resolved chemical concentration maps of mixing fluids using a chemically sensitive dye, 1-hydroxy-3,6,8-pyrenetrisulfonic acid, detected by planar laser induced fluorescence. To demonstrate an application of this capability, we investigate the collision and mixing of a pair of microdroplets in air. The two microdroplets are composed of different fluids, methanol and water, with the dye initially in the methanol droplet. When the droplets collide and mixing process develops, the fluorescence of the dye shifts from blue to green as the solvent environment changes. A series of spectral-temporal images of the collision and subsequent mixing are recorded, from which we extract the distribution of the two intermixing droplet species reflected in the spatially resolved dye spectra. Images reveal material transfer between droplets in both coalescing and non-coalescing droplet collisions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Data-Driven Approaches for Bead Geometry Prediction Via Melt Pool Monitoring

In the realm of additive manufacturing, the selection of process parameters to avoid over and under deposition entails a time-consuming and resource-intensive trial-and-error approach. Given the distinct characteristics of each part geometry, there is a pressing need for advancing real-time process monitoring and control to ensure consistent and reliable part dimensional accuracy. Here, this research shows that support vector regression (SVR) and convolutional neural network (CNN) models offer a promising solution for real-time process control due to the models’ abilities to recognize complex, non-linear patterns with high accuracy. A novel experiment was designed to compare the performance of SVR and CNN models to indirectly detect bead height from a coaxial image of a melt pool from a single-layer, single bead build. The study showed that both SVR and CNN models trained on melt pool data collected from a coaxial optical camera can accurately predict the bead height with a mean absolute percentage error of 3.67% and 3.68%, respectively.

36 MATERIALS SCIENCE↗

Controlled Assembly of Upconverting Nanoparticles for Low-Threshold Microlasers and Their Imaging in Scattering Media

Micron-sized lasers fabricated from upconverting nanoparticles (UCNP) coupled to whispering gallery mode (WGM) microresonators can exhibit continuous-wave anti-Stokes lasing useful for tracking cells, environmental sensing, and coherent stimulation of biological activity. The integration of these microlasers into organisms and microelectronics requires even smaller diameters, however, which raises threshold pump powers beyond practical limits for biological applications. To meet the need for low lasing thresholds and high fidelity fabrication methods, we use correlative optical and electron microscopy to uncover the nanoparticle assembly process and structural factors that determine efficient upconverted lasing. We show that 5 μm microspheres with controlled submonolayer UCNP coatings exhibit, on average, 25-fold lower laser thresholds (1.7 ± 0.7 kW/cm 2 ) compared to the mean values of the lowest threshold UCNP lasers, and variability is reduced 30-fold. WGMs are observed in the upconversion spectra for TiO 2 -coated microspheres as small as 3 μm, a size at which optical losses had previously prevented such observations. Finally, we demonstrate that the WGM signatures of these upconverting microlasers can be imaged and distinguished through tissue-mimicking phantoms. These advances will enable the fabrication of more efficient upconverting lasers for imaging, sensing, and actuation in optically complex environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗