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At least 55 records · Page 3

Total Internal Reflection Tomography (TIRT) for Three-Dimensional Sub-Wavelength Imaging

We will present a novel new form of near-field microscopy known as total internal reflection tomography (TIRT), which allows for true three-dimensional sub-wavelength imaging. It is based on recent theoretical advances regarding the fundamental interaction of light with sub-wavelength structures, as well as stable algorithms for the near-field inverse problem. We will discuss its theoretical underpinnings, as well describe current efforts at the NASA Glenn Research Center to implement a TIRT system for biofluid research.

Fischer, David G.↗

Super resolution for magneto-optical microscopy

Sub-diffraction limited magneto-optical microscopy, such as Kerr or Faraday effect microscopy, provide many advantages to fields of science and technology for measuring, or imaging, the magnetization structures and magnetization domains of materials. Disclosed is a method and system for performing sub-diffraction limited magneto-optic microscopy. The method includes positioning a microlens or microlens layer relative to a surface of a sample to image the surface of the sample, forming a photonic nanojet to probe the surface of the sample, and receiving light reflected by the surface of the sample or transmitted through the sample at an imaging sensor. The methods and associated systems and devices enable sub-diffraction limited imaging of magnetic domains at resolutions 2 to 8 times the classical diffraction limit.

te Velthuis, Suzanne Gabriëlle Everdine↗

High-Energy Coherent X-Ray Dffraction Microscopy of Polycrystal Grains: First Steps Towards a Multi-Scale Approach

Here, we present proof-of-concept imaging measurements of a polycrystalline material that integrate the elements of conventional high-energy x-ray diffraction microscopy with coherent diffraction-imaging techniques, and that can enable in situ strain-sensitive imaging of lattice structure in ensembles of deeply embedded crystals over five decades of length scale upon full realization. We demonstrate that the combination of these two characterization methods enables a more complete picture of the crystal-lattice strain than either method is capable of providing individually. Such complementary imaging capabilities are critical to addressing questions in a variety of research areas such as materials science and engineering, chemistry, and solid-state physics. Towards this eventual goal, the following key aspects are demonstrated: (1) high-energy Bragg coherent diffraction imaging (HE BCDI) of submicron-scale crystallites at 52 keV at current third-generation synchrotron light sources, (2) HE BCDI performed in conjunction with far-field high-energy diffraction microscopy (FF HEDM) on the grains of a polycrystalline sample in a smoothly integrated manner, and (3) the orientation information of an ensemble of grains obtained via FF HEDM used to perform complementary HE BCDI on multiple Bragg reflections of a single targeted grain. The imaged structures are seen to be 477 ± 50 nm or smaller in size, with an estimated strain resolution of 2.5 x 10 -4 . These steps lay the foundation for integration of HE BCDI, which typically provides a spatial resolution tens of nanometers, into a broad suite of well-established HEDM methods, extending HEDM beyond the few-micrometer resolution bound and into the nanoscale, and positioning the approach to take full advantage of the orders-of-magnitude improvement of x-ray coherence expected at fourth-generation light sources presently being built and commissioned worldwide.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Sub-micrometer random-pyramid texturing of silicon solar wafers with excellent surface passivation and low reflectance

Select emerging solar cell technologies, ranging from very narrow screen-printed fingers to perovskite/silicon tandems, would benefit from a reduction of the height of the standard pyramidal texture of monocrystalline silicon wafers to below 1 μm. However, fabricating such small surface features usually compromises the requisite low reflectance and high passivation quality. Through systematic design of experiments, we demonstrate that conventional alkaline-based wet-chemical etching processes can be tuned to produce dense, spatially homogeneous, and uniformly sized sub-micrometer pyramids. Precise texture size can be further controlled by adding potassium silicate to the texturing solution to effectively slow the pyramid growth rate and promote nucleation. With pyramid size distribution data—extracted from multiple atomic force microscopy images across each wafer—we demonstrate 16 nanotextures with average pyramid sizes ranging from 62 to 512 nm, with the largest having only 0.3% of its pyramids taller than 1 μm. Six of the nanotextures exhibit light trapping and surface defect densities comparable to state-of-the-art microtextured wafers. In conclusion, the best nanotexture achieved an AM1.5G-weighted reflectance of 11.8% and a minority-carrier lifetime of 3.4 ms after passivation with amorphous silicon, demonstrating that smaller textures need not deteriorate solar cell performance.

14 SOLAR ENERGY↗

In-situ spectroscopic ellipsometry for real-time characterization of the effects of high-flux helium plasmas on tungsten surfaces

Tungsten samples were exposed to He plasmas generated by an RF source (Γ i = 3.5 x 10 16 He cm -2 s -1 , ion energy = 92 eV.) The range of exposure conditions selected here is conducive to the growth of nearsurface He bubbles, and at higher fluence, the formation of W nanotendrils ranging between 50 — 100 nm in diameter. The evolution of these surface features was probed using a fixed-angle ellipsometer (280 — 1000 nm wavelength range) with direct line-of-sight to the sample. Over the parameter space explored here, changes in the two angles (p, S) that define the polarization of the reflected light followed a distinct trajectory with increasing plasma fluence. Ex-situ ellipsometry of 22 additional tungsten specimens tested at a wide range of plasma fluences and temperatures mapped onto these in-situ results well. We used helium ion microscopy and focused ion beam profiling to provide a direct calibration of the ellipsometry measurements. Our results indicate that for a reproducible process such as the growth helium-induced surface morphologies, ellipsometry is a practical in-situ diagnostic to study how fusion plasmas modify materials. To study more general effects of plasmas on surfaces, including co-deposition and sputtering, different approaches to modelling the optical properties of the exposed surfaces are also considered.

36 MATERIALS SCIENCE↗

Homogeneous condensation of gaseous mixtures of Si, Fe, O, N, and C in relative cosmic abundance and implications for astronomical condensation

The pressure versus temperature curves for homogeneous nucleation and condensation of two gaseous mixtures with nearly relative solar abundance of Si, Fe, O, N, and C in an excess of H were determined experimentally. Mixtures of CO, Fe(CO)5, H2, SiH4, and N2O in Ar were heated behind reflected shocks in a shock tube. The nucleation and condensation, which took place in the subsequent gas-dynamic expansion (cooling phase), was monitored by light scattering and turbidity. Grain morphologies and crystalline phases present in the condensates were determined by electron microscopy. These data cast doubt on the validity of both equilibrium and classical nucleation theoretical approaches to predict homogeneous condensation in a solar nebula or stellar atmosphere.

Stephens, J. R.↗

UV Shielding of Bacillus pumilus SAFR-032 Endospores by Martian Regolith Simulants

As exploration of the solar system advances with life detection missions on the horizon, the concern for planetary protection has grown considerably. When attempting to detect extraterrestrial life, the likelihood of false positives from terrestrial contamination must be minimized. The Exposing Microorganisms in the Stratosphere (E-MIST) balloon project aims to evaluate whether resilient terrestrial bacteria can survive stressors in a Mars-like environment. This is accomplished by sending Bacillus pumilus SAFR-032, an endospore-forming bacterial isolate from a spacecraft assembly facility, to the Earth's middle stratosphere (30-38 kilometers), where low temperature and pressure and high radiation and dryness conditions are similar to the surface of Mars. Previous ground and flight tests showed that the vast majority of SAFR-032 spores (99.99 percent) were inactivated by direct sunlight due to ultraviolet (UV) radiation. This observation led us to explore the role of dust shielding in changing microbial survivorship outcomes. To determine the dust particle distributions and density for potentially shielding microbes from UV radiation, samples of a Martian dust simulant were mixed with SAFR-032 spores. The dry heat sterilized simulant used was JSC MARS-1, weathered volcanic ash from Hawaii that displays many chemical and physical properties similar to the Martian soil as characterized by the Viking Lander 1, including reflectance spectrum, chemical composition, mineralogy, grain size, specific gravity, and magnetic properties. First, scanning electron microscopy was undertaken to visualize the aggregation of the spores with dust particles (i.e., shading effects), and samples of varying dust concentrations were subsequently irradiated with UVC light to test survivorship outcomes. After a relationship between dust concentration and spore survivorship was determined, a solar simulator capable of irradiating samples with a fuller UV spectrum (less than 280-400 nanometers) was used to perform a more robust middle stratosphere simulation. Taken together, we will use results from the ground-based irradiation studies to feed into experimental designs for the next E-MIST ultra-long duration polar balloon flight launched by NASA.

Stratosphere↗

Comparison of damage and ablation dynamics of multilayer dielectric films initiated by few-cycle pulses versus longer femtosecond pulses

The importance of high intensity few- to single-cycle laser pulses for applications such as intense isolated attosecond pulse generation is constantly growing, and with the breakdown of the monochromatic approximation in field ionization models, the few-cycle pulse (FCP) interaction with solids near the damage threshold has ushered a new paradigm of nonperturbative light–matter interaction. In this Letter, we systematically study and contrast how femtosecond laser-induced damage and ablation behaviors of SiO 2 /HfO 2 -based reflective multilayer dielectric thin film systems vary between FCP and 110 fs pulses. With time-resolved surface microscopy and ex situ analysis, we show that there are distinct differences in the interaction depending on the pulse duration, specifically in the “blister” morphology formation at lower fluences (damage) as well as in the dynamics of debris formation at higher fluences (ablation).

42 ENGINEERING↗

Single-particle scattering spectroscopy: fundamentals and applications

Metallic nanoparticles supporting a localized surface plasmon resonance have emerged as promising platforms for nanoscopic labels, sensors, and (photo-) catalysts. To use nanoparticles in these capacities, and to gain mechanistic insight into the reactivity of inherently heterogeneous nanoparticles, single-particle characterization approaches are needed. Single-particle scattering spectroscopy has become an important, highly sensitive tool for localizing single plasmonic nanoparticles and studying their optical properties, local environment, and reactivity. In this review, we discuss approaches taken for collecting the scattered light from single particles, their advantages and disadvantages, and present some recent applications. We introduce techniques for the excitation and detection of single-particle scattering such as high-angle dark-field excitation, total internal reflection dark-field excitation, scanning near-field microscopy, and interferometric scattering. We also describe methods to achieve polarization-resolved excitation and detection. We then discuss different approaches for scanning, ratiometric, snapshot, and interferometric hyperspectral imaging techniques used to extract spectral information. Finally, we provide a brief overview of specialized setups for in situ measurements of nanoparticles in liquid systems and setups coupled to scanning tip microscopes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Graded Buffer Bragg Reflectors with High Reflectivity and Transparency for Metamorphic Optoelectronics

A graded buffer Bragg reflector (GBBR) is a bifunctional device component that provides the reflection of a distributed Bragg reflector and the adjustable lattice constant of a compositionally graded buffer. Prior work showed that these properties can be combined with low threading dislocation density and high reflectivity. Here, we design and demonstrate complex GBBRs for specific metamorphic solar cell applications. We design buffers that provide (1) high reflectivity over a narrow bandwidth, for quantum well solar cells, (2) reflectivity over a wide bandwidth, for optically thin solar cells, and (3) low sidelobe reflection, for multijunction devices that demand low out-of-band reflection. Apodized and triple GBBRs are demonstrated, and transparency is always considered, requiring designs with carefully engineered material combinations. A GBBR with a reflection of 99% is demonstrated, as well as a triple GBBR that has over 80% reflection for 100?nm of the spectrum around 800?nm. We also analyze potential deviations in a baseline GBBR from that of a perfect DBR using transmission electron microscopy to analyze imperfections in the material and modeling to analyze the impact of imperfect refractive index data for lattice-mismatched AlGaInAs. Minimal crosshatch roughness and unintentional thickness variation occur throughout the buffer, which likely influences reflection slightly. Small deviations between the calculated AlGaInAs and utilized AlGaAs refractive index exist, giving methods for future GBBR improvement. While the GBBR designs are intended for metamorphic solar cells, the broad and high reflection may also be useful for other optoelectronic devices such as light-emitting diodes or lasers.

41 EE - Solar Energy Technologies Office (EE-4S)↗

The effect of longer-range waviness on X-ray reflectivity measurements

A model for calculating the X-ray reflectivity (XRR) of surfaces to extract both roughness and waviness features is presented. Expressions of reflectivity intensity are derived as a function of root-mean-square (RMS) roughness σ, RMS waviness σ L , and the cut-off frequency between the features ω 0 . Experiments were conducted at the Advanced Light Source at Lawrence Berkeley National Laboratory, beamline 8.3.2, on BK7 glass manufactured with a multi-step polishing process to validate the model, and were compared with atomic force microscopy (AFM), Fizeau interferometry and surface profilometry measurements. Here, the parameter results and their deviations for XRR measurements were σ = 2.9 ± 0.2 nm and σ L = 14.6 ± 0.5 nm with a wavelength cut-off of 1/(18 ± 2) µm –1 , while the results from the AFM, Fizeau and profilometry measurements were σ AFM = 3.4 ± 0.4 nm, σ L,Fizeau = 21.6 nm, σ prof = 4.0 ± 0.1 nm, and σ L,prof = 21.4 ± 0.1 nm with cut-offs for the profilometry and Fizeau measurements limited to frequencies of (1/16) µm –1 to (1/4) mm –1 .

42 ENGINEERING↗

Problems and possible solutions involved in hard target calibration of coherent Doppler lidar

The field of radiometry is surveyed with reference to coherent light, since the surfaces to be considered here are irradiated with coherent, polarized light. Definitions of some concepts are modified. In light of these modifications calibration problems are analyzed and solutions suggested. The most important task was to develop hard targets exhibiting minimal specular reflection (mirror-like and retroreflection) and following closely a Lambertian scattering curve. Bistable reflectometer experiments and integrating sphere measurements are used to physically characterize the targets. Optical and electron microscopy are used to physically characterize the targets. Since the BRDF matrix is not measured, this capability must be developed preferably for both bistatic and monostatic reflectometer measurements. The equipment is expensive and not yet developed. Calibration can be simplified if it can be proved that the BRDF matrix is diagonal for a diffuse scatterer.

Anderson, Richard↗

Light-trapping structures fabricated in situ for ultrathin III-V solar cells

Here, we describe a fully in situ method of fabricating light-scattering structures on III-V materials that generates a rough morphology via vapor phase etching and redeposition. Fully in situ methods support higher industrial throughput by utilizing the growth reactor to generate the light-trapping structures after device growth without removal from the reactor. We use HCl and PH 3 to etch and redeposit scattering morphologies on Ga 0.5 In 0.5 P in a dynamic hydride vapor phase epitaxy (D-HVPE) reactor. We show that the addition of PH 3 leads to redeposition during the vapor phase HCl etching of Ga 0.5 In 0.5 P and that HCl flow rate and time exposed to HCl-PH 3 each independently cause a linear increase in the redeposited feature size, indicating that redeposition proceeds by island growth in a III-Cl-limited, hydride-enhanced HVPE regime. Auger electron spectroscopy and scanning transmission electron microscopy with energy dispersive spectroscopy (STEM-EDS) reveal redeposition to be highly Ga-rich GaInP, i.e., Ga(In)P. The Ga-rich nature of the redeposition results from the higher thermodynamic driving force for Ga incorporation than for In during HVPE growth and the difference in the volatility of the III-Cl etch products. The resulting morphologies have high broadband scattering, as determined by normal specular reflectance and integrating sphere measurements, indicating effectiveness as light-scattering structures. In a 270-nm-thick GaAs photovoltaic device with a textured back surface, we achieve a 4.9% increase in short circuit current density (J SC ) without any loss in open-circuit voltage (V OC ) relative to a planar control using only a 60 s in situ texturing treatment.

14 SOLAR ENERGY↗

Cryo-EM structure of the Rhodospirillum rubrum RC–LH1 complex at 2.5 Å

The reaction centre light-harvesting 1 (RC–LH1) complex is the core functional component of bacterial photosynthesis. We determined the cryo-electron microscopy (cryo-EM) structure of the RC–LH1 complex from Rhodospirillum rubrum at 2.5 Å resolution, which reveals a unique monomeric bacteriochlorophyll with a phospholipid ligand in the gap between the RC and LH1 complexes. The LH1 complex comprises a circular array of 16 αβ-polypeptide subunits that completely surrounds the RC, with a preferential binding site for a quinone, designated Q P , on the inner face of the encircling LH1 complex. Quinols, initially generated at the RC Q B site, are proposed to transiently occupy the Q P site prior to traversing the LH1 barrier and diffusing to the cytochrome bc 1 complex. Thus, the Q P site, which is analogous to other such sites in recent cryo-EM structures of RC–LH1 complexes, likely reflects a general mechanism for exporting quinols from the RC–LH1 complex.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photoexcitation of Fe 3 O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Abstract Artificial photosynthesis strives to convert the energy of sunlight into sustainable, eco‐friendly solar fuels. However, systems with light‐driven water oxidation reaction (WOR) at pH=1 are rare. Broadly used [Ru(bpy) 3 ] 2+ (bpy=2,2’‐bipyridine) photosensitizer has a fixed +1.23 V potential which is insufficient to drive most water oxidation catalysts (WOCs) in acid, while Fe 2 O 3 , featuring the highly oxidizing holes, is not stable at low pH. Here, the key examples of Fe‐based metal–organic framework (MOF) water oxidation photoelectrocatalysts active at pH=1 are presented. Fe‐MIL‐126 and Fe MOF‐dcbpy structures were formed with 4,4’‐biphenyl dicarboxylate (bpdc), 2,2’‐bipyridine‐5,5’‐dicarboxylate (dcbpy) linkers and their mixtures. Presence of dcbpy linkers allows integration of metal‐based catalysts via coordination to 2,2’‐bipyridine fragments. Fe‐based MOFs were doped with Ru‐based precursors to achieve highly active MOFs bearing [Ru(bpy)(dcbpy)(H 2 O) 2 ] 2+ WOC. Materials were analyzed with X‐ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infra‐red (FTIR) spectroscopy, resonance Raman, X‐ray absorption spectroscopy, fs optical pump‐probe, electron paramagnetic resonance (EPR), diffuse reflectance and electric conductivity measurements and were modeled by band structure calculations. It is shown that under reaction conditions, Fe III and Ru III oxidation states are present, indicating rate‐limiting electron transfer in MOF. Fe 3 O nodes emerge as photosensitizers able to drive prolonged O 2 evolution in acid. Further developments are possible via MOF's linker modification for enhanced light absorption, electrical conductivity, reduced MOF solubility in acid, Ru‐WOC modification for faster WOC catalysis, or Ru‐WOC substitution to 3d metal‐based systems. The findings give further insight for development of light‐driven water splitting systems based on Earth‐abundant metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Connecting Femtosecond Transient Absorption Microscopy with Spatially Coregistered Time Averaged Optical Imaging Modalities

Multimodal all-optical imaging involving coregistered femtosecond transient absorption microscopy (TAM), time-integrated photoluminescence (PL), and steady-state modalities such as confocal reflectance and transmission offers an appealing approach to gain a comprehensive understanding of complex electronic excited-state phenomena in spatially heterogeneous systems. A unique combination of these modalities allows us to unravel not only the competing electronic excited-state dynamical processes but also the underlying morphological information with simultaneous high temporal and spatial resolution. However, correlating the various images obtained from time-resolved and time-independent modalities is generally nontrivial and particularly challenging when the electronic dynamics under study evolve in both time and space. Here, we demonstrate a new approach for rationally correlating time-resolved microscopy with coregistered time-integrated or steady-state modalities. Specifically, our approach involves an extended global lifetime analysis of the time-resolved microscopic data set to separate distinct dynamical processes taking place on commensurate time scales, and the resulting decay-associated amplitude maps (DAAMs) were applied to explore correlations with the images acquired using time-independent modalities. The feasibility of our approach was validated through analyzing a multimodal data set acquired from a thin film of chloride-containing mixed lead halide perovskites (CH 3 NH 3 PbI 3–x Cl x ) using femtosecond transient absorption, time-integrated PL, and confocal reflectance microscopies. Analysis of the results obtained enable us to gain new insight into the complex ultrafast relaxation dynamics in this highly heterogeneous system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Models and Measurements Quantify Photon Recycling, Charge-Carrier Diffusion and Photon Scattering Contributions to Photoluminescence in InP Nanowire Arrays

Nanowire arrays present many unique advantages for solar-to-chemical energy conversion. One possible advantage is that photon recycling between neighboring nanowires has the potential to increase solar energy conversion efficiencies. Here, in this work, we explore three underlying mechanisms of optical and electronic coupling between neighboring nanowires─incident photon scattering, photon recycling, and charge-carrier transport from the photoexcited nanowire to the neighboring nanowire via the underlying substrate─using single nanowire-level microscopy and spectroscopy measurements. We present a comprehensive analysis of light absorption and emission of a single nanowire at open circuit, and subsequent re-absorption and re-emission by a neighboring nanowire. We developed a novel correlated single nanowire microspectroscopy and widefield imaging methodology to spatially resolve photon communication pathways between neighboring nanowires and selectively image re-emitted and reflected photons. We developed unique multiphysics models to couple wave optics and semiconductor photophysics to especially isolate contributions from photon recycling and electronic transport to photon emission from neighboring nanowires. By systematically varying the morphologies of the nanowires modeled, we identified pathways to maximize photon recycling between neighboring nanowires. We concluded that the measured photoluminescence is more strongly influenced by the diffusion of charge carriers as compared to photon recycling in materials with moderate-to-large charge-carrier mobilities (>10 cm 2 V –1 s –1 ), and that photon recycling dictates photoluminescence intensity only when the charge-carrier mobility is low (<1 cm 2 V –1 s –1 ). The experimental and simulation platforms developed herein for photon management strategies can be leveraged by the semiconductor photocatalysis community to enhance solar-to-chemical conversion efficiencies in semiconductor nanowire arrays.

25 ENERGY STORAGE↗

Near-field imaging of optical resonances in silicon metasurfaces using photoelectron microscopy

Precise control of light–matter interactions at the nanoscale lies at the heart of nanophotonics. However, experimental examination at this length scale is challenging since the corresponding electromagnetic near-field is often confined within volumes below the resolution of conventional optical microscopy. In semiconductor nanophotonics, electromagnetic fields are further restricted within the confines of individual subwavelength resonators, limiting access to critical light–matter interactions in these structures. In this work, we demonstrate that photoelectron emission microscopy (PEEM) can be used for polarization-resolved near-field spectroscopy and imaging of electromagnetic resonances supported by broken-symmetry silicon metasurfaces. We find that the photoemission results, enabled through an in situ potassium surface layer, are consistent with full-wave simulations and far-field reflectance measurements across visible and near-infrared wavelengths. In addition, we uncover a polarization-dependent evolution of collective resonances near the metasurface array edge taking advantage of the far-field excitation and full-field imaging of PEEM. Here, we deduce that coupling between eight resonators or more establishes the collective excitations of this metasurface. All told, we demonstrate that the high-spatial resolution hyperspectral imaging and far-field illumination of PEEM can be leveraged for the metrology of collective, non-local, optical resonances in semiconductor nanophotonic structures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗