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At least 919 records · Page 51

Radio frequency passband signal generation using photonics

Devices, methods and systems for generating wideband, high-fidelity arbitrary radio frequency (RF) passband signals are described. A voltage tunable optical filter for arbitrary RF passband signal generation includes a first input configured to receive a broadband optical pulse train, a second input configured to receive a first control voltage representative of an amplitude signal, an electrooptic modulator to receive the broadband optical pulse train and the first control voltage, to modulate the broadband optical pulse train in accordance with the amplitude signal, and to produce two complementary optical outputs that form two arms of an interferometer, an optical delay component to impart an optical path difference into one of the complementary outputs of the electrooptic modulator, and a combiner or a splitter to receive two complementary optical outputs of the electrooptic modulator after impartation of the optical path difference and to produce an output interference pattern of fringes.

Gowda, Apurva Shantharaj↗

Squeezing a Prism into a Surface: Emulating Bulk Optics with Achromatic Metasurfaces

Metasurfaces promise to replace bulky prisms and lenses with 2D surfaces, revolutionizing wavefront control with technologically significant advantages in size, weight, and planar fabrication. However, conventional implementations suffer from large chromatic aberrations and cannot sustain performance over practical bandwidths of real-world signals because of the limited phase modulation margin available in a surface. How can an infinitely thin surface generate the arbitrarily large, broadband phase delay that bulk phase accumulation can provide? Here, equivalence between bulk optics and certain multiresonant metasurfaces is demonstrated, where phase delay arises from trains of multiple resonances in the effective sheet conductivities of the surface itself instead of accumulation of propagation phase. The fundamentally required electromagnetic surface conductivities of a purely achromatic metasurface are derived and general design rules for arbitrarily broadband beam steering and lensing are obtained. Both operation in transmission and reflection can be achieved in a unified way by proper alignment of the resonances, enabling 360° directionality. The arbitrary spectral bandwidth, dual reflection/transmission operation, and complete dispensability of propagation phase constitute a major advance in the state of the art of achromatic metasurfaces for wavefront manipulation.

36 MATERIALS SCIENCE↗

Structural Color Production in Melanin-Based Disordered Colloidal Nanoparticle Assemblies in Spherical Confinement

Melanin is a ubiquitous natural pigment that exhibits broadband absorption and high refractive index. Despite its widespread use in structural color production, how the absorbing material, melanin, affects the generated color is unknown. Using a combined molecular dynamics and finite-difference time-domain computational approach, here we investigates structural color generation in one-component melanin nanoparticle-based supraparticles (called supraballs) as well as binary mixtures of melanin and silica (nonabsorbing) nanoparticle-based supraballs. Experimentally produced one-component melanin and one-component silica supraballs, with thoroughly characterized primary particle characteristics using neutron scattering, produce reflectance profiles similar to the computational analogs, confirming that the computational approach correctly simulates both absorption and multiple scattering from the self-assembled nanoparticles. These combined approaches demonstrate that melanin's broadband absorption increases the primary reflectance peak wavelength, increases saturation, and decreases lightness factor. Additionally, the dispersity of nanoparticle size more strongly influences the optical properties of supraballs than packing fraction, as evidenced by the production of a larger range of colors when size dispersity is varied versus packing fraction. For binary melanin and silica supraballs, the chemistry-based stratification allows for more diverse color generation and finer saturation tuning than does the degree of mixing/demixing between the two chemistries.

broadband absorption↗

Radiative cooling and thermoregulation in the earth’s glow

Efficient passive radiative cooling of buildings requires an unimpeded view of the sky. However, vertical facades of buildings mostly see terrestrial features that become broadband-radiative heat sources in the summer and heat sinks in the winter. The resulting summertime terrestrial heat gain by buildings negates or overwhelms their narrowband longwave infrared (LWIR) radiative cooling to space, while the wintertime terrestrial heat loss causes overcooling. We show that selective LWIR emitters on vertical building facades can exploit the differential transmittance of the atmosphere toward the sky and between terrestrial objects to achieve higher summertime cooling and wintertime heating than conventionally used broadband emitters. The impact of this novel and passive thermoregulation is comparable to that of painting dark roofs white and is achievable with both novel and commonplace materials. Our findings represent new and remarkable opportunities for materials design and untapped thermoregulation of entities ranging from buildings to human bodies.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Octave-spanning terahertz quarter-wave plates based on over-coupled Fabry–Pérot resonances in reflective metal–dielectric–metal metasurfaces

Compact devices for broadband polarization control in the terahertz (THz) regime remain challenging to realize due to the intrinsic phase dispersion associated with birefringent materials and resonant structures. Here, we demonstrate achromatic THz quarter-wave plates with near-unity efficiency and operating under a wide range of incidence angles, based on over-coupled metal–dielectric–metal reflective metasurfaces. The devices operate as single-port anisotropic Fabry–Pérot cavities, in which the phase dispersion of the over-coupled resonances is engineered to maintain an approximately constant relative phase delay between orthogonal field components over a broad frequency range. Four complementary metasurface designs operating at an incidence angle of 45° collectively cover the 0.25–3 THz frequency range accessible to a typical THz time-domain spectroscopy system. Each device exhibits an approximately octave-wide operational bandwidth, with axial ratios below 3 dB and polarization-conversion efficiencies exceeding 80% across most of the operating band. Systematic structural optimization suppresses coupling to diffraction and guided-wave modes, thereby further extending the usable bandwidth while preserving the required phase relationship between orthogonal polarizations. The demonstrated metasurfaces are compatible with wafer-scale fabrication processes, and experimental results show excellent agreement with simulations. These findings establish over-coupled reflective metasurfaces as a robust, scalable, and versatile platform for broadband THz polarization control.

36 MATERIALS SCIENCE↗

Influence of Source Type on Acoustic Liner Impedance in No Flow

This paper presents findings from a study conducted under a challenge of the International Forum for Aviation Research (IFAR), which consists of partners from various national research labs around the world. A series of normal incidence impedance tube tests are performed to identify differences in acoustic impedance for various types of source excitations. These source types include single-tone, multitone, and broadband. To better understand these differences, six unique acoustic liners are tested using these source types at various sound pressure levels and frequencies. Multitone sources of up to five discrete frequencies at a time (both harmonic and nonharmonic excitations) are included. Predictions are also shown to assess capability of capturing source type in the acoustic liner design process. It is determined that impedance behavior due to single-tone and broadband source excitations is largely well-understood and predictable. Multitone source excitations, however, yield unpredictable impedance characteristics that appear highly dependent on the summed coherent waveform that is incident upon the acoustic liner. Future work on this topic is warranted to improve impedance prediction capability of multitone excitation.

acoustic liner impedance multitone prediction sour↗

Highly Anisotropic Quasi‐Direct Organic Metal Halide Hybrids: A Platform for Polarization‐Sensitive Optoelectronics

Low-dimensional organic–inorganic metal halide hybrids (OMHHs) exhibit remarkable optical properties and enhanced environmental stability. We investigate a 1D OMHH with formula C 4 N 2 H 14 PbBr 4 , consisting of Pb–Br chains separated by organic cations, which shows a large Stokes shift (0.83 eV) and broadband emission. Through first-principles calculations and polarized Raman spectroscopy, we characterize the material's vibrational properties and identify the specific phonon modes that drive exciton self-trapping. Our novel GW/Bethe-Salpeter equation force formalism reveals that low-frequency phonons (∼ 100 cm −1 , primarily involving Pb–Br motions) couple strongly with excitons, with a remarkably high Huang-Rhys factor of 137 ± 4, and gives a pathway for ultrafast structural analysis during the absorption process. This phonon-exciton coupling mechanism explains the material's broadband emission and provides a pathway for controlling optical properties through vibrations and for tuning vibrations through optical excitations. The material also exhibits highly anisotropic optical properties and electronic transport, with bands that are dispersive along the Pb–Br chains but nearly flat in perpendicular directions, resulting in direction-dependent electrical conductivity that is calculated to be an order of magnitude higher along the chain direction and consistent with measurements. These combined properties make this system an excellent platform for polarization-sensitive optoelectronic devices.

36 MATERIALS SCIENCE↗

Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

Abstract Low‐dimensional hybrid metal halides are emerging as a highly promising class of single‐component white‐emitting materials for their unique broadband emission from self‐trapped excitons (STEs). Despite substantial progress in the development of these metal halides, many challenges remain to be addressed to obtain a better fundamental understanding of the structure–property relationship and realize the full potentials of this class of materials. Here, via pressure regulation, a near 100% photoluminescence quantum yield (PLQY) of broadband emission is achieved in a corrugated 1D hybrid metal halide C 5 N 2 H 16 Pb 2 Br 6 , which possesses a highly distorted structure with an initial PLQY of 10%. Compression reduces the overlap between STE states and ground state, leading to a suppressed phonon‐assisted non‐radiative decay. The PL evolution is systematically demonstrated to be controlled by the pressure‐regulated exciton–phonon coupling which can be quantified using Huang–Rhys factor S . Detailed studies of the S ‐PLQY relation for a series of 1D hybrid metal halides (C 5 N 2 H 16 Pb 2 Br 6 , C 4 N 2 H 14 PbBr 4 , C 6 N 2 H 16 PbBr 4 , and (C 6 N 2 H 16 ) 3 Pb 2 Br 10 ) reveal a quantitative structure–property relationship that regulating S factor toward 28 leads to the maximum emission.

36 MATERIALS SCIENCE↗

Time-domain modelling and thermometry of the CH 4 v 1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

Here, we present time-domain measurements and modelling of the CH 4 v 1 vibrational Q-branch, as well as simultaneous temperature acquisition from the CH 4 and N 2 vibrational Q-branches using broadband hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS). Accurate measurements with fs/ps CARS require knowledge of the time-domain response of the probed molecule at different temperatures and pressures. In this work, a fs/ps CARS model was developed for theCH 4 v 1 Q-branch and validated using time-resolved probe delay scans at pressures between 70 and 600 Torr and temperatures between 295 and 1000 K. A simplified modified exponential energy gap model was used to determine the linewidths of the Raman transitions within the Q-branch. Total Q-branch linewidths for the entire explored parameter space were also determined from the probe delay scans. This enabled quantitative measurements of CH 4 with fs/ps CARS as well as the temperature through the hot bands of the CH 4 v 1 Q-branch. With a broadband fs laser pulse in a two-beam phase matching scheme, the N 2 Q-branch and CH 4 v 1 Q-branch were simultaneously measured in a heated cell, and the temperatures from each molecule's spectra was evaluated. Here, the fitted temperatures corresponded well with differences ranging from 4 to 17%. It was also shown that exchanging 90% of CH 4 for N 2 or Ar at 295 K and 500 Torr did not significantly impact the normalized time-domain signal prior to a 100 picosecond probe delay. Spatially resolved one-dimensional (1-D) thermometry using the CH 4 Q-branch was also demonstrated with an imaged spatial resolution of 40 µm. With the developed model, 1-D quantitative measurements of CH 4 concentration and temperature can be measured with time resolution of tens of picoseconds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploring wave propagation in heterogeneous metastructures using the relaxed micromorphic model

Metamaterials are artificial structures that can manipulate and control sound waves in ways not possible with conventional materials. While much effort has been undertaken to widen the bandgaps produced by these materials through design of heterogeneities within unit cells, comparatively little work has considered the effect of engineering heterogeneities at the structural scale by combining different types of unit cells. In this paper, we use the relaxed micromorphic model to study wave propagation in heterogeneous metastructures composed of different unit cells. We first establish the efficacy of the relaxed micromorphic model for capturing the salient characteristics of dispersive wave propagation through comparisons with direct numerical simulations for two classes of metamaterial unit cells: namely phononic crystals and locally resonant metamaterials. We then use this model to demonstrate how spatially arranging multiple unit cells into metastructures can lead to tailored and unique properties such as spatially-dependent broadband wave attenuation, rainbow trapping, and pulse shaping. In the case of the broadband wave attenuation application, we show that by building layered metastructures from different metamaterial unit cells, we can slow down or stop wave packets in an enlarged frequency range, while letting other frequencies through. In the case of the rainbow-trapping application, we show that spatial arrangements of different unit cells can be designed to progressively slow down and eventually stop waves with different frequencies at different spatial locations. Finally, in the case of the pulse-shaping application, our results show that heterogeneous metastructures can be designed to tailor the spatial profile of a propagating wave packet. Collectively, these results show the versatility of the relaxed micromorphic model for effectively and accurately simulating wave propagation in heterogeneous metastructures, and how this model can be used to design heterogeneous metastructures with tailored wave propagation functionalities.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Stabilizing dynamic subsea power cables using Bi-stable nonlinear energy sinks

This study investigates vibration mitigation of dynamic subsea cables through passive bi-stable nonlinear energy sinks (B-NESs). These devices suppress vibration energy in a broadband way, and can be regarded as extensions of classical linear tuned mass dampers (TMDs) which are narrowband devices. Through the open-source MoorDyn library, we simulated the vibrations of a vertical subsea cable equipped with a set of B-NESs. Multi-objective optimization was performed to detect the B-NES parameters for optimal mitigation of the cable vibrations. Advanced signal processing verified the efficacy of the optimized B-NESs not only to rapidly absorb and locally dissipate vibration energy, but also to nonlinearly scatter vibration energy from low to high frequencies within the cable itself. This last feature is especially beneficial for vibration mitigation of the undersea cable, as at higher frequencies the cable vibrations exhibit drastically reduced amplitudes and are more effectively dissipated by inherent structural damping and hydrodynamic radiation damping. This contrasts with traditional TMDs which can mitigate vibration only at a single frequency. Furthermore, our robustness study confirms the B-NES's effectiveness under even varying environmental conditions. Overall, the B-NES's capacity for broadband vibration mitigation renders it a promising retrofit solution for improving the performance and operational safety of dynamic power cables in offshore wind farms and other marine applications.

17 WIND ENERGY↗

Impact of Measured Spectrum Variation on Solar Photovoltaic Efficiencies Worldwide

In photovoltaic power ratings, a single solar spectrum, AM1.5, is the de facto standard for record laboratory efficiencies, commercial module specifications, and performance ratios of solar power plants. More detailed energy analysis that accounts for local spectral irradiance, along with temperature and broadband irradiance, reduces forecast errors to expand the grid utility of solar energy. Here, ground-level measurements of spectral irradiance collected worldwide have been pooled to provide a sampling of geographic, seasonal, and diurnal variation. Applied to nine solar cell types, the resulting divergence in solar cell efficiencies illustrates that a single spectrum is insufficient for comparisons of cells with different spectral responses. Cells with two or more junctions tend to have efficiencies below that under the standard spectrum. Silicon exhibits the least spectral sensitivity: relative weekly site variation ranges from 1% in Lima, Peru to 14% in Edmonton, Canada.

energy yield↗

A proposed high-intensity radiometer calibration method using concentrated solar radiation

Accurate calibration of irradiance measurement devices, or radiometers, is essential for ensuring the reliability of measurements in high heat applications such as concentrating solar power (CSP), aerospace, defense, and pulsed power systems. Despite the critical need, existing calibration standards and service providers are limited to irradiance levels below 100 kW/m 2 and specific radiation sources, which is insufficient for many applications. For instance, CSP technologies, particularly those under the Department of Energy’s Solar Energy Technologies Office (SETO) Gen 3 program, require accurate measurements of broadband irradiance at levels exceeding 2000 kW/m 2 . In even more extreme scenarios, such as re-entry vehicles, heat levels can surpass 10000 kW/m 2 . Current ISO standards, specifically ISO 14934–2 and ISO 14934–3, are constrained to lower irradiance levels and dependent on black body heat sources, limiting their applicability for high-intensity broadband irradiance measurements, particularly in concentrated solar applications. Here, to address this shortfall, the National Solar Thermal Test Facility (NSTTF) at Sandia National Laboratories (SNL) proposes a calibration method and facility capable of characterizing radiometers up to 2750 kW/m 2 using concentrated solar irradiance. Calibrating with concentrated sunlight is important for solar applications as it aligns the calibration process with the solar spectrum. This alignment is crucial for minimizing systematic errors and avoiding the need for additional corrections that may arise when radiometers designed for solar applications are calibrated using black-body or electrical sources. This paper presents the present day NSTTF characterization facility and procedure, detailing the proposed calibration method and uncertainty quantification. The presented method builds upon 1980′s NSTTF methodology and involves both theoretical and empirical methods to establish a robust relationship between gauge voltage output and irradiance intensity, quantifying both measurement and fitting errors. By addressing the limitations of existing standards and extending the characterization range, this work provides an advancement in the field of high-intensity irradiance measurement and instrumentation characterization.

Gardon gauge↗

Synchrotron infrared nano-spectroscopy and -imaging

Infrared (IR) spectroscopy has evolved into a powerful analytical technique to probe molecular and lattice vibrations, low-energy electronic excitations and correlations, and related collective surface plasmon, phonon, or other polaritonic resonances. In combination with scanning probe microscopy, near-field infrared nano-spectroscopy and -imaging techniques have recently emerged as a frontier in imaging science, enabling the study of complex heterogeneous materials with simultaneous nanoscale spatial resolution and chemical and quantum state spectroscopic specificity. Here, we describe synchrotron infrared nano-spectroscopy (SINS), which takes advantage of the low-noise, broadband, high spectral irradiance, and coherence of synchrotron infrared radiation for near-field infrared measurements across the mid- to far-infrared with nanometer spatial resolution. This powerful combination provides a qualitatively new form of broadband spatio-spectral analysis of nanoscale, mesoscale, and surface phenomena that were previously difficult to study with IR techniques, or even any form of micro-spectroscopy in general. We review the development of SINS, describe its technical implementations, and highlight selected examples representative of the rapidly growing range of applications in physics, chemistry, biology, materials science, geology, and atmospheric and space sciences.

47 OTHER INSTRUMENTATION↗

Solvation Dynamics of Wet Ethaline: Water is the Magic Component

The past two decades witnessed the development of a new type of solvent system, named deep eutectic solvents, which have become increasingly investigated because they offer new and potentially favorable properties, such as wide tunability in electrochemical, mechanical, and transport properties. Deep eutectic solvent (DES) systems are composed of at least one main solvent and an additional component that is meant to interrupt the original solvent/solvent interactions, thereby introducing lower melting points relative to each individual component. Ethaline (a 1:2 mole% mixture of choline chloride and ethylene glycol) is one of the most promising DES systems. However, it is also known to be very hygroscopic, which is a constant concern because water absorption during the use of ethaline alters its properties. Within this work, we demonstrate that modest amounts of water addition (1-10%) to ethaline are of little concern for practical use and can even lead to performance improvements, such as accelerated relaxation and solvation. In contrast, very small amounts of <1% of water lead to additional slowing of the solvent response. Thus, we suggest that the attempt to dry ethaline below 1% moisture is rather counter-productive if one attempts to achieve effective solvation and charge transport properties from DESs. This study investigates the effect of water content on the diffusional relaxation dynamics of ethaline. A set of independent spectroscopic experiments and computational simulations are aimed to provide insight into the solvent response of the DES system using femtosecond time-resolved absorption spectroscopy (fs-TA), broadband dielectric spectroscopy (BDS), nuclear magnetic resonance (NMR) diffusometry and broadband relaxometry, and molecular dynamics simulations (MDS) on ethaline with 0, 0.1, 1, 10, and 28.5wt% added water. For dry ethaline, we identify choline chloride as the rate-limiting solvation component in ethaline. However, the role of the solvent components changes gradually as water is added. Further, we provide quantitative solvent relaxation rates using the different presented time-resolved spectroscopic techniques and find remarkable agreement between them. Based on the solvent relaxation rates and combined with MDS, we develop a molecular understanding of the individual solvent components and their interactions in dry and wet ethaline with varying amounts of water content.

25 ENERGY STORAGE↗

Substitution Reactions in the Pyrolysis of Acetone Revealed through a Modeling, Experiment, Theory Paradigm

The development of high-fidelity mechanisms for chemically reactive systems is a challenging process that requires the compilation of rate descriptions for a large and somewhat ill-defined set of reactions. The present unified combination of modeling, experiment, and theory provides a paradigm for improving such mechanism development efforts. Here we combine broadband rotational spectroscopy with detailed chemical modeling based on rate constants obtained from automated ab initio transition state theory-based master equation calculations and high-level thermochemical parametrizations. Broadband rotational spectroscopy offers quantitative and isomer-specific detection by which branching ratios of polar reaction products may be obtained. Using this technique, we observe and characterize products arising from H atom substitution reactions in the flash pyrolysis of acetone (CH 3 C(O)CH 3 ) at a nominal temperature of 1800 K. The major product observed is ketene (CH 2 CO). Minor products identified include acetaldehyde (CH 3 CHO), propyne (CH 3 CCH), propene (CH 2 CHCH 3 ), and water (HDO). Literature mechanisms for the pyrolysis of acetone do not adequately describe the minor products. The inclusion of a variety of substitution reactions, with rate constants and thermochemistry obtained from automated ab initio kinetics predictions and Active Thermochemical Tables analyses, demonstrates an important role for such processes. Furthermore, the pathway to acetaldehyde is shown to be a direct result of substitution of acetone's methyl group by a free H atom, while propene formation arises from OH substitution in the enol form of acetone by a free H atom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale optical nonreciprocity with nonlinear metasurfaces

Optical nonreciprocity is manifested as a difference in the transmission of light for the opposite directions of excitation. Nonreciprocal optics is traditionally realized with relatively bulky components such as optical isolators based on the Faraday rotation, hindering the miniaturization and integration of optical systems. Here we demonstrate free-space nonreciprocal transmission through a metasurface comprised of a two-dimensional array of nanoresonators made of silicon hybridized with vanadium dioxide (VO 2 ). This effect arises from the magneto-electric coupling between Mie modes supported by the resonator. Nonreciprocal response of the nanoresonators occurs without the need for external bias; instead, reciprocity is broken by the incident light triggering the VO 2 phase transition for only one direction of incidence. Nonreciprocal transmission is broadband covering over 100 nm in the telecommunication range in the vicinity of λ = 1.5 µm. Each nanoresonator unit cell occupies only ~0.1 λ 3 in volume, with the metasurface thickness measuring about half-a-micron. Our self-biased nanoresonators exhibit nonreciprocity down to very low levels of intensity on the order of 150 W/cm 2 or a µW per nanoresonator. We estimate picosecond-scale transmission fall times and sub-microsecond scale transmission rise. Our demonstration brings low-power, broadband and bias-free optical nonreciprocity to the nanoscale.

42 ENGINEERING↗

Decoupled few-femtosecond phase transitions in vanadium dioxide

Abstract The nature of the insulator-to-metal phase transition in vanadium dioxide (VO 2 ) is one of the longest-standing problems in condensed-matter physics. Ultrafast spectroscopy has long promised to determine whether the transition is primarily driven by the electronic or structural degree of freedom, but measurements to date have been stymied by their sensitivity to only one of these components and/or their limited temporal resolution. Here we use ultra-broadband few-femtosecond pump-probe spectroscopy to resolve the electronic and structural phase transitions in VO 2 at their fundamental time scales. Our experiments show that the system transforms into a bad-metallic phase within 10 fs after photoexcitation, but requires another 100 fs to complete the transition, during which we observe electronic oscillations and a partial re-opening of the bandgap, signalling a transient semi-metallic state. Comparisons with tensor-network simulations and density-functional theory calculations show these features result from an unexpectedly fast structural transition, in which the vanadium dimers separate and untwist with two different timescales. Our results resolve the structural and electronic nature of the light-induced phase transition in VO 2 and establish ultra-broadband few-femtosecond spectroscopy as a powerful tool for studying quantum materials out of equilibrium.

Science & Technology - Other Topics↗