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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Electron thermalization and relaxation in laser-heated nickel by few-femtosecond core-level transient absorption spectroscopy

Direct measurements of photoexcited carrier dynamics in nickel are made using few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy at the nickel M 2,3 edge. It is observed that the core-level absorption line shape of photoexcited nickel can be described by a Gaussian broadening (σ) and a red shift (ω s ) of the ground-state absorption spectrum. Theory predicts and the experimental results verify that after initial rapid carrier thermalization, the electron temperature increase (ΔT ) is linearly proportional to the Gaussian broadening factor σ, providing quantitative real-time tracking of the relaxation of the electron temperature. Measurements reveal an electron cooling time for 50 nm thick polycrystalline nickel films of 640 ± 80 fs. With hot thermalized carriers, the spectral red shift exhibits a power-law relationship with the change in electron temperature of ω s ∝ ΔT 1.5 . Rapid electron thermalization via carrier-carrier scattering accompanies and follows the nominal 4-fs photoexcitation pulse until the carriers reach a quasithermal equilibrium. Entwined with a <6 fs instrument response function, carrier thermalization times ranging from 34 fs to 13 fs are estimated from experimental data acquired at different pump fluences and it is observed that the electron thermalization time decreases with increasing pump fluence. Here, the study provides an initial example of measuring electron temperature and thermalization in metals in real time with XUV light, and it lays a foundation for further investigation of photoinduced phase transitions and carrier transport in metals with core-level absorption spectroscopy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films

The authors discuss the use of in situ optical absorption to probe point defect equilibria and kinetics in oxides, with particular attention to thin films and high-temperature measurements evaluating changes in oxygen content. The introduction notes the effect of point defects on oxide behavior, including differences in thin films versus bulk materials, and describes methods to evaluate point defect equilibria and kinetics; advantages of optical absorption among these methods are highlighted. Section 2 provides an overview of how optical absorption and point defect concentrations are related, including various possible structural and electronic origins of defect-mediated absorption changes corresponding to oxygen content changes. Section 3 traces the development of historical understanding of optical absorption in nonstoichiometric oxides and emergence of thin film applications and measurement approaches that resulted. Section 4 details the procedure for determining surface exchange coefficients from optical transmission relaxation measurements and provides specific examples of how this approach uniquely has enabled new insights into thin film surface exchange behavior with and without current collectors. Section 5 provides examples of optically derived diffusivity measurements and comparisons of bulk and thin film defect equilibria. Section 7 outlines potential opportunities and future developments in this area, and Section 7 concludes the manuscript.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Enhanced absorption of monolayer molybdenum disulfide (MoS{sub 2}) using nanostructures with symmetrical cross resonator in the visible ranges

In order to enhance the absorption of monolayer molybdenum disulfide (MoS{sub 2}), a novel nanostructure with symmetrical cross resonator based on MoS{sub 2} in the visible wavelength ranges has been proposed. At a resonant wavelength of 623 nm, the absorption of monolayer MoS{sub 2} in the absorption structure is as high as 82%, much higher than the bare MoS{sub 2} in the air. The electric field around monolayer MoS{sub 2} is enhanced by the guided mode resonance, thereby enhancing the absorption of monolayer MoS{sub 2} in the structure. The relevant parameters of the proposed structure are adjusted to achieve the tunability of the resonant wavelength in the visible ranges and the high-efficiency absorption of monolayer MoS{sub 2} in the structure, which is of great significance for the applications of MoS{sub 2}-based optoelectronic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

The simulation on absorption properties of metamaterial/GaAs/electrode layer hybrid structure based Terahertz photoconductive detector

Terahertz (THz) photodetectors have attracted great attention from scientists worldwide for their application in security checking, biomedical treatment and astronomical observation of remote stars and distant galaxies. As a typical THz detector, extrinsic GaAs based photoconductive detector is facing critical technical bottlenecks in the epitaxial growth of sufficiently thick and high-quality GaAs absorption layer. In this work, a novel THz photoconductive detector based on metamaterial/GaAs/electrode layer hybrid structure was designed and simulated. By setting the periodic split ring resonator (SRR) structure as 88 μm pitch with 8 μm width, the absorption peaks exist at the wavelength of about 142 and 367 μm, which originate from the resonant cavity and the SRR dipole resonance effect, and the novel device shows a significant enhancement compared with the conventional GaAs photoconductive detector. Thus, the necessary thickness of GaAs absorption-layer is largely reduced, and the resonant absorption peak can be modulated by changing the thickness of absorption layer. This work provides a novel device structure which can solve the critical epitaxial growth bottleneck of GaAs photoconductive detector and used for the astronomical observation, security check, etc.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Control of optical absorption and fluorescence spectroscopies of natural melanin at different solution concentrations

The source of the optical properties of natural melanin persists as an impressive conundrum, hindering a thorough comprehension of the complicated photo-protective contribution of these extensive natural pigments and the pragmatic design of revolutionary bioinspired materials for optoelectronic functionalities. Melanin is a natural pigment distributed in vivo, and provides protection from the sun rays, exhibiting a strong wide-band UV–visible absorption. In the present study, we investigated the optical properties of natural melanin at different pH concentrations within the framework of experimental techniques, namely, UV–visible absorption, Fourier transform infrared spectroscopy (FTIR), and fluorescence spectroscopies. The results indicate that the optical absorption and fluorescence of natural melanin are enhanced within the near-UV and visible regimes with an increase in the solution concentration, are dependent on the pH level, and can impact the emergence of a broad band of visible absorption. The variations in the optical absorption spectra of natural melanin solutions at various pH levels will demonstrate novel rational strategies for controlling their optical properties for potential optoelectronic applications.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2019

Process intensification in a spinning disk absorber for absorption heat pumps

Absorption heat pumps are often an efficient machine for recovering of low-grade waste heat to cooling applications. However, they suffer from slow transfer processes and consequently large equipment size. This paper presents an experimental investigation of a novel absorber that utilizes a combination of a spinning disk and manifold-microchannel technology to intensify the absorption process. The rotation of the disk improves solution-side absorption performance, while an adaption of manifold-microchannel technology provides water-side enhancement. The enhanced spinning disk absorber was tested in an experimental setup using aqueous lithium bromide as the working fluid. Experimental results are compared with key performance metrics reported in the existing literature. The overall heat transfer increased by a factor of 4.7, and absorption rate increased by a factor of 4 to 10 folds over those in conventional tube absorbers. The results suggest that the spinning disk reactor could substantially reduce the size of absorber in the absorption machines. Better thermal and mass transfer performance can also enable air cooling with higher heat sink temperature than the one available through cooling towers.

42 ENGINEERING↗
DOE OSTI2021

Electromagnetic wave absorption of multifunctional cementitious composites incorporating polyvinyl alcohol (PVA) fibers and fly ash: Effects of microstructure and hydration

Highlights: • The cementitious composite shows excellent wide-band electromagnetic wave absorption in a frequency range of 2–18 GHz. • The PVA fibers and the fly ash change the dielectric properties of the cementitious composite by Debye polarization. • The iron oxide of the cementitious binders contributes to the magnetic properties of the composites. • The impacts of the microstructure and the hydration of the cementitious composite on its microwave absorption are analyzed. This paper devises a novel method for the adjustment of the pore structure and the hydration of cement to improve the electromagnetic wave absorption of the cementitious composites incorporating polyvinyl alcohol (PVA) fibers and fly ash in a frequency range of 2–18 GHz. The underlying mechanism of the absorption is investigated to explore the possibility of the structural and functional integration of these composites. The electromagnetic parameters of the prepared cementitious composites and those of the raw materials are analyzed in a frequency range of 0.5–18 GHz. Moreover, the pore structure and the chemical environment of the cementitious composites are examined by mercury intrusion porosimetry (MIP), back-scattered electron detector (BSE), and X-ray photoelectron spectroscopy (XPS). The results indicate that the PVA fibers and the high-volume fly ash have a positive effect on electromagnetic wave absorption of the cementitious composites through the adjustment of their pore structure and hydration.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Turbulence-induced bias in time-averaged laser absorption tomography of correlated concentration and temperature fields with a first-order correction

The influence of correlated scalar fluctuations on time-averaged laser absorption tomography measurements of temperature and species in a piloted turbulent premixed flame was examined using a coupled spectroscopic and fluid-dynamic analysis. To understand bias associated with turbulence, spatio-temporally resolved temperature and species mole fraction profiles predicted by large eddy simulations (LES) were used to synthetically generate time-resolved line-of-sight absorption measurements at short time scales (microsecond) to reflect the unsteady nature of a canonical jet burner across various transverse measurement planes. Inversion methods were employed on the time-averaged line-of-sight data to produce radially-resolved temperature and mole fraction profiles, analogous to those produced by laser absorption tomography performed on a time-averaged axisymmetric flowfield. It is shown that bias in the measurements compared to true time-averaged scalar fields is a function primarily of temperature dependence in absorptivity and non-zero correlation between temperature and species concentration scalars. Finally, a first-order correction to tomography measurements is proposed to account for the bias based on estimated correlations and the known spectroscopic parameters of the probed absorption transitions.

42 ENGINEERING↗
DOE OSTI2023

Temperature and anion ligand field dependence of LnCl 3 (Ln = Nd, Dy, Sm) electronic absorption spectra in LiCl–KCl eutectic molten salt

A comprehensive knowledge of the coordination, bonding, and speciation of elements in molten salt mixtures is necessary to understand and predict the chemical and physical properties of the salt. Absorption spectroscopy can yield information about the chemistry of species of interest in alkali halide molten salt mixtures by revealing information about the electronic structure and transitions of those species. In this study, ultraviolet (UV), visible (vis), and near-infrared (NIR) absorption spectroscopy was used to examine changes to the electronic structure of trivalent Nd, Sm, and Dy in LiCl–KCl eutectic molten salt with changes in temperature and the anion composition of the melt. With increasing temperature, changes to spectral features suggest a distortion of the coordination complexes. Changes to lineshape with the substitution of alternative halide anions were examined and analyzed, revealing differences in the coordination for I – versus F – with the lanthanides. Gaussian peak fitting was used to show that the changes in lineshape with the progressive addition of F – anions can be explained by the superposition of a set of absorption bands from complexes with all Cl – anion ligands and a set of blueshifted absorption bands from complexes containing both F – and Cl – anion ligands. Finally, this work yields a new method to analyze and interpret change to electronic absorption spectra for f-block elements dissolved in alkali halide molten salts as well as new observations of the interactions of larger and smaller halide anions with lanthanides in Cl – -based molten salts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Early- and late-time dynamics of laser-produced plasmas by combining emission and absorption spectroscopy

Optical emission spectroscopy and laser absorption spectroscopy are two highly complementary techniques for diagnosing plasmas, specifically in the determination of important parameters such as temperature and density. In this work, we characterized a laser-produced plasma by combining emission and tunable absorption spectroscopy. Plasmas are produced by focusing pulses from a frequency quadrupled Nd:YAG laser onto a glass target containing a minor concentration of aluminum in an ambient atmosphere of ~100 Torr N 2 . Here, emission spectroscopy is used to investigate the line behavior of Al and Ca, electron density, and excitation temperature at times = 5 μs, while absorption spectroscopy is used to investigate the line behavior of Al and Ca, species density, and kinetic temperature at times = 5-100 μs. A comparison is made between the excitation temperature measured from emission using the Boltzmann plot method and the kinetic temperature measured from absorption; the implications of this comparison on local thermodynamic equilibrium and line-of-sight averaging are discussed. By combining the two methods of optical emission and laser absorption spectroscopy, a comprehensive characterization of the plasma over the entire lifetime of its evolution is possible, leading to a greater understanding of the plasma behavior including particle condensation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Absorption spectroscopy based high-speed oxygen concentration measurements at elevated gas temperatures

A sensor built upon tunable diode laser absorption spectroscopy (TDLAS) has been developed for concentration measurements in high-temperature (up to 800 K) gas streams; while the sensor measures gas oxygen and water concentration, temperature and pressure, this work focuses on the challenges and solutions to transient oxygen measurement. A 760-nm diode laser was used to probe a pair of oxygen absorption transitions, and a Herriott cell based multi-pass arrangement was utilized to compensate for the extremely weak oxygen absorption as well as the high gas temperature. This multi-pass arrangement provides a 4297.4-mm absorption path length across a 76.2-mm diameter duct, and an O 2 detection limit ([O 2 ] where SNR=1) of ca. 0.1%. Laboratory validation of the HITRAN spectral parameters of the chosen absorption transitions was performed over a range of high temperatures and oxygen concentrations relevant to engine-exhaust applications. The insensitivity of the Herriott cell arrangement to vibrations and spatial temperature gradients was demonstrated. Conclusions from applications to single- and multi-cylinder engine exhaust are presented and demonstrate the new sensor’s ability to measure fast intra-cycle gas-property transients, and provide insights relevant to advancing internal-combustion-engine technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Interference-Limited Absorption in Dense Molecular Nanolayers Near Reflecting Surfaces

We investigate linear resonant absorption by a dense ensemble of molecules confined to a sub-wavelength layer in two geometries: (i) a free-standing film in a homogeneous space and (ii) the same film placed at a controlled distance from a reflecting surface. In both cases, increasing the effective light–matter coupling (via molecular density/oscillator strength) produces a nonmonotonic response: absorption rises to an optimum and then decreases as the film becomes increasingly radiatively bright and reflective. Finite-difference time-domain simulations and analytical transfer-matrix calculations agree quantitatively and yield compact ridge conditions for the optimum. We interpret the trends using a scattering/port picture: the isolated film is a symmetric two-port system (reflection and transmission), which bounds single-sided resonant absorption to ≤50% in the ultrathin limit (reflecting transition saturation), whereas adding a mirror suppresses transmission and converts the structure into an effectively one-port absorber. In the mirror-backed geometry, interference can cancel reflection, and unity absorption is obtained at critical coupling, when radiative leakage is balanced by intrinsic molecular loss. These results clarify fundamental limits and design rules for collective absorption in dense molecular layers near dielectric or metallic boundaries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Chemical Interface Damping Revealed by Single-Particle Absorption Spectroscopy

Plasmon-induced interfacial charge separation is a promising way to efficiently extract energetic carriers through direct plasmon decay. This mechanism of charge transfer has been investigated by single-particle scattering spectroscopy, which measures the homogeneous plasmon line width. The line width is broadened by charge transfer, generally known as chemical interface damping. However, conflicting reports exist regarding the effect of chemical interface damping on the corresponding single-particle absorption spectrum, which is needed to accurately determine absolute light conversion efficiencies. This work aims to resolve this question by directly correlating absorption and scattering spectra of individual gold nanorods in the presence and absence of a charge-accepting interface. We find that for TiO 2 coated nanorods, the absorption line width is indeed broadened due to chemical interface damping but is overall narrower than the scattering line width. Here, chemical interface damping is furthermore found to increase with larger resonance energies. The observed differences in line widths between absorption and scattering are elucidated within the context of an analytically tractable model describing the lowest energy optically bright and higher-order optically dark plasmon modes of the nanorod, including bulk, radiative, and chemical interface damping effects. Taken together, these results establish that single-particle absorption spectroscopy is capable of revealing interfacial charge injection by direct plasmon decay.

absorption↗
DOE OSTI2021

Ultrafast time-resolved x-ray absorption spectroscopy of ionized urea and its dimer through ab initio nonadiabatic dynamics

Investigating the early dynamics of chemical systems following ionization is essential for our understanding of radiation damage. However, experimental as well as theoretical investigations are very challenging due to the complex nature of these processes. Time-resolved x-ray absorption spectroscopy on a femtosecond timescale, in combination with appropriate simulations, is able to provide crucial insights into the ultrafast processes that occur upon ionization due to its element-specific probing nature. In this theoretical study, we investigate the ultrafast dynamics of valence-ionized states of urea and its dimer employing Tully's fewest switches surface hopping approach using Koopmans' theorem to describe the ionized system. We demonstrate that following valence ionization through a pump pulse, the time-resolved x-ray absorption spectra at the carbon, nitrogen, and oxygen K-edges reveal rich insights into the dynamics. Excited states of the ionized system give rise to time-delayed blueshifts in the x-ray absorption spectra as a result of electronic relaxation dynamics through nonadiabatic transitions. Moreover, our statistical analysis reveals specific structural dynamics in the molecule that induce time-dependent changes in the spectra. For the urea monomer, we elucidate the possibility to trace effects of specific molecular vibrations in the time-resolved x-ray absorption spectra. For the urea dimer, where ionization triggers a proton transfer reaction, we show how the x-ray absorption spectra can reveal specific details on the progress of proton transfer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Laser absorption measurements of electron density in nanosecond-scale atmospheric pressure pulsed plasmas

We report on time-resolved measurements of electron number density by continuous-wave laser absorption in a low-energy nanosecond-scale laser-produced spark in atmospheric pressure air. Laser absorption is a result of free-free and bound-free electron excitation, with the absorption coefficient modeled and evaluated using estimates of the time-variation in electron temperature and probe laser absorption path length. Plasma electron number densities are determined to be as high as n e = 7 x 10 19 cm -3 , and decay to 1/e of their peak values over a period of about 50 ns following plasma formation using a 20 mJ, 10 ns pulse width frequency-doubled Nd:YAG laser. The measured plasma densities at later times are shown to be in reasonable agreement with Stark broadening measurements of the 3s[ 5 S o ]-3p[ 5 P] electronic transition in atomic oxygen at 777 nm. This study provides support for the use of such continuous wave laser absorption for time resolved electron density measurements in low energy spark discharges in air, provided that an estimate of the electron temperature and laser path length can be made by accompanying diagnostics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition

Black carbon (BC) absorbs solar radiation, leading to a strong but uncertain warming effect on climate. A key challenge in modeling and quantifying BC’s radiative effect on climate is predicting enhancements in light absorption that result from internal mixing between BC and other aerosol components. Modeling and laboratory studies show that BC, when mixed with other aerosol components, absorbs more strongly than pure, uncoated BC; however, some ambient observations suggest more variable and weaker absorption enhancement. We show that the lower-than-expected enhancements in ambient measurements result from a combination of two factors. First, the often used spherical, concentric core-shell approximation generally overestimates the absorption by BC. Second, and more importantly, inadequate consideration of heterogeneity in particle-to-particle composition engenders substantial overestimation in absorption by the total particle population, with greater heterogeneity associated with larger model–measurement differences. We show that accounting for these two effects—variability in per-particle composition and deviations from the core-shell approximation—reconciles absorption enhancement predictions with laboratory and field observations and resolves the apparent discrepancy. Furthermore, our consistent model framework provides a path forward for improving predictions of BC’s radiative effect on climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Influence of Microstructure on the Absorption of Tritium into Gold-Plated 316 Stainless Steel

The interaction of tritium with metal surfaces is the initial step in the overall absorption of tritium by the substrate metal. As a result, limiting the adsorption of tritium to the surface may effectively reduce the quantity of tritium absorbed by a metal when it is in contact with tritium gas. To limit tritium adsorption, many tritium users electroplate gold onto the substrate metal. The gold layer is expected to reduce tritium adsorption, and subsequently absorption, by reducing water adsorption. The present work shows a comparison between tritium inventories in nonplated 316 stainless steel to the inventories in 316 stainless-steel samples electroplated with gold by various commercial vendors and laboratories. Of the various gold-plated samples, only one type of plating shows ~25% reduction in tritium inventory, relative to non-plated steel samples. The degree of tritium absorption appears to be significantly influenced by the porosity, texture, and completeness of the gold layer. Incomplete and/or porous layers lead to increased absorption, while gold layers with smaller surface features lead to similar tritium inventories as non-plated samples. Furthermore, reduced tritium absorption was observed only for complete gold layers with small surface features.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

H i 21-cm absorption in radio-loud AGN with double-peaked [O iii ] emission

ABSTRACT Different physical processes in galaxy evolution, such as galaxy mergers that lead to coalescence of dual Active Galactic Nuclei (AGN) and outflows emanating from the narrow line region, can leave their imprint on the optical spectra of AGN in the form of double-peaked narrow emission lines. To investigate the neutral gas in the centres of such AGN, we have conducted a pilot survey of H i 21-cm absorption, using the upgraded Giant Metrewave Radio Telescope (uGMRT), in radio-loud AGN whose optical spectra show double-peaked [O iii] emission lines at z ≤ 0.4 (median z ≈ 0.14). Among the eight sources for which we could obtain clean spectra, we detect H i 21-cm absorption in three sources (detection rate of $38^{+36}_{-20}$ per cent) and find tentative indication of absorption in two other sources. The detection rate of H i 21-cm absorption is tentatively higher for the systems that show signatures of interaction or tidal disturbance (≳ 50 per cent) in the ground-based optical images than that for the systems that appear single and undisturbed (≈25 per cent). This is consistent with the high incidence of H i 21-cm absorption observed in z ≤ 0.2 galaxy mergers. Higher spatial resolution spectroscopy is required to confirm the origin of the H i absorbing gas, i.e. either gas infalling on to the radio-loud AGN, outflowing gas ejected by the AGN, or gas in rotation on the galactic-scale or circumnuclear discs.

79 ASTRONOMY AND ASTROPHYSICS↗