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Results for “core level spectroscopy”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Si-based materials for lithium-ion batteries XI. 70% surface-modified Si/C/perfluorooctene-carbon black/lithiated polyacrylic acid electrode

X-ray photoelectron spectroscopy was used to analyze a 70% Si/C/perfluorooctene-carbon black/lithiated polyacrylic acid electrode fabricated at the Cell Analysis, Modeling, and Prototyping (CAMP) Facility, Argonne National Laboratory. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.83 401 nm). A survey spectrum together with O 1s, C 1s, and Si 2p are presented. The spectra indicate the principal core level photoelectron and Auger electron signals with only minor sodium, copper, calcium, and lithium signals and show the expected silicon-carbon, carbon-fluorine, and silicon-fluorine species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure.

25 ENERGY STORAGE↗
DOE OSTI2020

Si-based materials for lithium-ion batteries II. Surface-modified Si/C/polyethylene glycol powder

X-ray photoelectron spectroscopy was used to analyze Si/C/polyethylene glycol powder obtained from Paraclete Energy, Inc. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.834 01 nm). An initial survey spectrum together with O 1s, C 1s, and Si 2p are presented. A final survey spectrum was collected to ascertain the amount of beam-induced damage, which appears to be minimal. Finally, the spectra indicate the principal core level photoelectron and Auger electron signals, with only minor calcium and nitrogen signal, and show the expected silicon-carbon species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure.

25 ENERGY STORAGE↗
DOE OSTI2022

Time-Resolved Optical Pump-Resonant X-ray Probe Spectroscopy of 4-Thiouracil: A Simulation Study

We theoretically monitor the photoinduced ππ* → nπ* internal conversion process in 4-thiouracil (4TU), triggered by an optical pump. The element-sensitive spectroscopic signatures are recorded by a resonant X-ray probe tuned to the sulfur, oxygen, or nitrogen K-edge. We employ high-level electronic structure methods optimized for core-excited electronic structure calculation combined with quantum nuclear wavepacket dynamics computed on two relevant nuclear modes, fully accounting for their quantum nature of nuclear motions. We critically discuss the capabilities and limitations of the resonant technique. For sulfur and nitrogen, we document a pre-edge spectral window free from ground-state background and rich with ππ* and nπ* absorption features. The lowest sulfur K-edge shows strong absorption for both ππ* and nπ*. In the lowest nitrogen K-edge window, we resolve a state-specific fingerprint of the ππ* and an approximate timing of the conical intersection via its depletion. A spectral signature of the nπ* transition, not accessible by UV–vis spectroscopy, is identified. The oxygen K-edge is not sensitive to molecular deformations and gives steady transient absorption features without spectral dynamics. Here, the ππ*/nπ* coherence information is masked by more intense contributions from populations. Altogether, element-specific time-resolved resonant X-ray spectroscopy provides a detailed picture of the electronic excited-state dynamics and therefore a sensitive window into the photophysics of thiobases.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Si-based materials for lithium-ion batteries III: Surface-modified Si/C/polyvinylidine difluoride powder

X-ray photoelectron spectroscopy was used to analyze Si/C/polyvinylidine difluoride powder obtained from Paraclete Energy Inc. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.834 01 nm). An initial survey spectrum together with F 1s, O 1s, C 1s, and Si 2p are presented. A final survey spectrum was collected to ascertain the amount of beam-induced damage, which appears to be minimal. Finally, the spectra indicate the principal core level photoelectron and Auger electron signals with only minor nitrogen signal and show the expected silicon-carbon and silicon-fluorine species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure.

25 ENERGY STORAGE↗
NASA NTRS2018

Constraints on the chemical enrichment history of the Perseus Cluster of galaxies from high-resolution X-ray spectroscopy

High-resolution spectroscopy of the core of the Perseus Cluster of galaxies, using the Hitomi satellite above 2 keV and the XMM–Newton Reflection Grating Spectrometer at lower energies, provides reliable constraints on the abundances of O, Ne, Mg, Si, S, Ar, Ca, Cr, Mn, Fe, and Ni. Accounting for all known systematic uncertainties, the Ar/Fe, Ca/Fe, and Ni/Fe ratios are determined with a remarkable precision of less than 10 per cent, while the constraints on Si/Fe, S/Fe, and Cr/Fe are at the 15 per cent level, and Mn/Fe is measured with a 20 percent uncertainty. The average biases in determining the chemical composition using archival CCD spectra from XMM–Newton and Suzaku typically range from 15 to 40 per cent. A simple model in which the enrichment pattern in the Perseus Cluster core and the protosolar nebula are identical gives a surprisingly good description of the high-resolution X-ray spectroscopy results, with X^2=10.7 for 10 degrees of freedom. However, this pattern is challenging to reproduce with linear combinations of existing supernova nucleosynthesis calculations, particularly given the precise measurements of intermediateα-elements enabled by Hitomi. We discuss in detail the degeneracies between various supernova progenitor models and explosion mechanisms, and the remaining uncertainties in these theoretical models. We suggest that including neutrino physics in the core-collapse supernova yield calculations may improve the agreement with the observed pattern ofα-elements in the Perseus Cluster core. Our results provide a complementary benchmark for testing future nucleosynthesis calculations required to understand the origin of chemical elements.

A Simionescu↗
DOE OSTI2021

Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser

Femtosecond carrier dynamics in layered 2H-MoTe2 semiconductor crystals have been investigated using soft x-ray transient absorption spectroscopy at the x-ray free-electron laser (XFEL) of the Pohang Accelerator Laboratory. Following above-bandgap optical excitation of 2H-MoTe2, the photoexcited hole distribution is directly probed via short-lived transitions from the Te 3d5/2 core level (M5-edge, 572–577 eV) to transiently unoccupied states in the valence band. The optically excited electrons are separately probed via the reduced absorption probability at the Te M5-edge involving partially occupied states of the conduction band. A 400 ± 110 fs delay is observed between this transient electron signal near the conduction band minimum compared to higher-lying states within the conduction band, which we assign to hot electron relaxation. Additionally, the transient absorption signals below and above the Te M5 edge, assigned to photoexcited holes and electrons, respectively, are observed to decay concomitantly on a 1–2 ps timescale, which is interpreted as electron–hole recombination. The present work provides a benchmark for applications of XFELs for soft x-ray absorption studies of carrier-specific dynamics in semiconductors, and future opportunities enabled by this method are discussed.

2D materials↗
DOE OSTI2020

Si-based materials for lithium-ion batteries IV: Surface-modified Si/C/perfluorooctene powder

X-ray photoelectron spectroscopy was used to analyze nano-Si/C/perfluorooctene powder obtained from Paraclete Energy Inc. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.834 01 nm). An initial survey spectrum together with F 1s, O 1s, C 1s, and Si 2p are presented. A final survey spectrum was collected to ascertain the amount of beam-induced damage, which appears to be minimal. Finally, the spectra indicate the principal core level photoelectron and Auger electron signals with only minor nitrogen signal and show the expected silicon-carbon, carbon-fluorine, and silicon-fluorine species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure.

25 ENERGY STORAGE↗
NASA NTRS2003

Ultrasonic Spectroscopy of Stainless Steel Sandwich Panels

Enhanced, lightweight material systems, such as 17-4PH stainless steel sandwich panels are being developed for use as fan blades and fan containment material systems for next generation engines. In order to improve the production for these systems, nondestructive evaluation (NDE) techniques, such as ultrasonic spectroscopy, are being utilized to evaluate the brazing quality between the 17-4PH stainless steel face plates and the 17-4PH stainless steel foam core. Based on NDE data, shear tests are performed on sections representing various levels of brazing quality from an initial batch of these sandwich structures. Metallographic characterization of brazing is done to corroborate NDE findings and the observed shear failure mechanisms.

Cosgriff, Laura M.↗
DOE OSTI2022

Technical and personal remembrances of David A. Shirley in studies of surface magnetism, photoelectron spectroscopy, EUV lithography, and hydrogen storage

This article describes the influence of Professor David A. Shirley on the research science of one of his Ph.D. students in the diverse areas of surface magnetism, x-ray photoelectron spectroscopy (XPS), spin-resolved XPS (SRXPS), extreme ultraviolet (EUV) lithography, and hydrogen storage materials science. Examples are given from the author's work on Cr(001) surface magnetism, XPS, and SRXPS studies of multiplet-splitting in core-level photoemission from Fe. In addition, Dave's influence in understanding the radiation-induced deposition of carbon on EUV optics is described, along with the use of XPS in deciphering how hydrogen storage materials are modified by repeated hydrogen adsorption/desorption cycling. The current status of these particular topics is briefly summarized. These technical remembrances are combined with some fond personal stories about Dave, in recognition of his passing on March 29, 2021.

Klebanoff, L. E.↗
DOE OSTI2020

Si-based materials for lithium-ion batteries VIII. 90% surface-modified Si/C-lithiated polyacrylic acid electrode

X-ray photoelectron spectroscopy was used to analyze a 90% Si/C-lithiated polyacrylic acid electrode fabricated at the Cell Analysis, Modeling, and Prototyping Facility (CAMP), Argonne National Laboratory. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.834 01 nm). An initial survey spectrum together with O 1s, C 1s, and Si 2p are presented. A final survey spectrum was collected to ascertain the amount of beam-induced damage, which appears to be minimal. Finally, the spectra indicate the principal core level photoelectron and Auger electron signals with only minor lithium signal and show the expected silicon-carbon species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure as well contributions related to the binder material.

25 ENERGY STORAGE↗
DOE OSTI2020

Si-based materials for lithium-ion batteries IX: 70% surface-modified Si/C/polyethylene glycol-carbon black/lithiated polyacrylic acid electrode

X-ray photoelectron spectroscopy was used to analyze a 70% Si/C-carbon black/polyethylene glycol/lithiated polyacrylic acid electrode fabricated at the Cell Analysis, Modeling, and Prototyping Facility (CAMP), Argonne National Laboratory. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.834 01 nm). An initial survey spectrum together with O 1s, C 1s, and Si 2p are presented. A final survey scan was collected to ascertain the amount of beam-induced damage, which appears to be minimal. Finally, the spectra indicate the principal core level photoelectron and Auger electron signals with only minor copper and lithium signals and show the expected silicon-carbon species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure as well as contributions related to the binder material.

25 ENERGY STORAGE↗
DOE OSTI2020

Role of Alkali-Metal Cations in Electronic Structure and Halide Segregation of Hybrid Perovskites

The ability to control or prevent phase segregation in perovskites is crucial to realizing stable and tunable mixed-halide optoelectronic devices. Here, we systematically examine the impact of alkali-metal-cation (Cs + and K + ) concentration on the band structure, chemical composition, phase segregation, and polycrystalline microstructure on formamidinium-dominated mixed-halide mixed-cation perovskite films. It was found that the incorporation of Cs + and K + cations decreases the work function and the core levels of all components shift toward higher binding energy consistent with n-doping the perovskite film, which facilitates electron transfer to the electron transport layer TiO 2 . A concentration-dependent film structure was observed by X-ray photoemission spectroscopy and grazing incidence wide-angle X-ray scattering where the halides and cations are distributed evenly across perovskite films at low metallic cation concentration (5%). A high metal-cation ratio (20%) leads to halide segregation within the perovskite film and the surface becomes bromide-poor, whereas the bromide and metal cations diffuse more deeply within the film. These differences in electronic properties, element distribution, and film morphology were reflected in the device performance where the power conversion efficiency of low-metallic-cation concentration (5% of Cs + and K + ) perovskite solar cells is ≈5% higher than the high-concentration ones (20%). This study provides valuable chemical and physical insight into the underlying trade-offs in the careful tuning of electrical properties and film structure to optimize multication and mixed-halide hybrid perovskites.

36 MATERIALS SCIENCE↗
NASA NTRS1988

(1 + 1) resonant enhanced multiphoton ionization via the A2Sigma(+) state of NO - Ionic rotational branching ratios and their intensity dependence

Rotational branching ratios resulting from the (1 + 1) resonant enhanced multiphoton ionization spectroscopy of NO via the 0-0 transition of the A-X band for the four possible branches that can be assigned as R(21.5) are explored using calculation performed in the frozen-core approximation at the Hartree-Fock level. The four different branches, of which three are distinctly different in the perturbative limit, have rather different branching ratios. The mixed R12 + Q22(21.5) branch, which is not intense and has the lowest transition energy, appears to give the best agreement with experimental branching ratio for parallel detection. The agreement is less satisfactory for perpendicular detection. Neither the effect of finite-acceptance angle of the photoelectron detector nor high intensities can explain the discrepancy.

Rudolph, H.↗
DOE OSTI2020

Si-based materials for lithium-ion batteries VII. 70% surface-modified Si/C-carbon black/lithiated polyacrylic acid electrode

X-ray photoelectron spectroscopy (XPS) was used to analyze a 70% Si/C-carbon black/lithiated polyacrylic acid electrode fabricated at the Cell Analysis, Modeling, and Prototyping Facility (CAMP), Argonne National Laboratory. The spectra were obtained using incident monochromatic Al K α radiation at 1486.6 eV (0.834 01 nm). An initial survey spectrum together with O 1s, C 1s, and Si 2p are presented. A final survey spectrum was collected to ascertain the amount of beam-induced damage, which appears to be minimal. Finally, the spectra indicate the principal core level photoelectron and Auger electron signals with only minor copper, nitrogen, calcium, and lithium signals and show the expected silicon-carbon species related to the surface modification process in addition to oxidized carbon and silicon due to atmospheric exposure as well contributions related to the binder material.

25 ENERGY STORAGE↗
NASA NTRS1995

A search for interstellar CH3D: Limits to the methane abundance in Orion-KL

A search has been performed for interstellar CH3D via its J(K) = 1(0) - 0(0) transition at 230 GHz and its J(K) = 2(0) - l(0) and J(K) = 2(1) - 1(1) lines at 465 GHz using the NRAO 12 m and CSO 10 m telescopes towards Orion-KL. This search was done in conjunction with laboratory measurements of all three transitions of CH3D using mm/sub-mm direct absorption spectroscopy. The molecule was not detected down to a 3 sigma level of T(A) less than 0.05 K towards Orion, which suggests an upper limit to the CH3D column density of N less than 6 x 10(exp 18)/sq cm in the hot core region and a fractional abundance (with respect to H2) of less than 6 x 10(exp -6). These measurements suggest that the methane abundance in the Orion hot core is f less than 6 x 10-4, assuming D/H approximately 0.01. Such findings are in agreement with recent hot core chemical models, which suggest CH4/H2 approximately 10(exp -4).

Womack, Maria↗
DOE OSTI2024

Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic Signatures

X-ray photoelectron spectroscopy (XPS) is a powerful characterization technique that unveils subtle chemical environment differences via core– electron binding energy (CEBE) analysis. We extend the development of realspace pseudopotential methods to calculating 1s, 2s, and 2p 3/2 CEBEs of third-row elements (S, P, and Si) within the framework of Kohn–Sham density-functional theory (KS-DFT). The new approach systematically prevents variational collapse and simplifies core-excited orbital selection within dense energy level distributions. However, careful error cancellation analysis is required to achieve accuracy comparable to all-electron methods and experiments. Combined with real-space KS-DFT implementation, this development enables large-scale simulations with both Dirichlet boundary conditions and periodic boundary conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Atomically Dispersed Zn/Co–N–C as ORR Electrocatalysts for Alkaline Fuel Cells

Hydrogen fuel cells have drawn increasing attention as one of the most promising next-generation power sources for future automotive transportation. Developing efficient, durable, and low-cost electrocatalysts, to accelerate the sluggish oxygen reduction reaction (ORR) kinetics, is urgently needed to advance fuel cell technologies. Herein, we report on metal–organic frameworks-derived nonprecious dual metal single-atom catalysts (SACs) (Zn/Co–N–C), consisting of Co–N 4 and Zn–N 4 local structures. These catalysts exhibited superior ORR activity with a half-wave potential (E 1/2 ) of 0.938 V versus RHE (reversible hydrogen electrode) and robust stability (ΔE 1/2 = –8.5 mV) after 50k electrochemical cycles. Moreover, this remarkable performance was validated under realistic fuel cell working conditions, achieving a record-high peak power density of ~1 W cm –2 among the reported SACs for alkaline fuel cells. Operando X-ray absorption spectroscopy was conducted to identify the active sites and reveal catalytic mechanistic insights. The results indicated that the Co atom in the Co–N 4 structure was the main catalytically active center, where one axial oxygenated species binds to form an O ads –Co–N 4 moiety during the ORR. In addition, theoretical studies, based on a potential-dependent microkinetic model and core-level shift calculations, showed good agreement with the experimental results and provided insights into the bonding of oxygen species on Co–N 4 centers during the ORR. Furthermore, this work provides a comprehensive mechanistic understanding of the active sites in the Zn/Co–N–C catalysts and will pave the way for the future design and advancement of high-performance single-site electrocatalysts for fuel cells and other energy applications.

25 ENERGY STORAGE↗
DOE OSTI2021

Observation of Hydrodynamic Flows in Imploding Fusion Plasmas on the National Ignition Facility [plus supplemental information]

Inertial confinement fusion implosions designed to have minimal fluid motion at peak compression often show significant linear flows in the laboratory, attributable per simulations to percent-level imbalances in the laser drive illumination symmetry. In this work, we present experimental results which intentionally varied the mode 1 drive imbalance by up to 4% to test hydrodynamic predictions of flows and the resultant imploded core asymmetries and performance, as measured by a combination of DT neutron spectroscopy and high-resolution x-ray core imaging. Neutron yields decrease by up to 50%, and anisotropic neutron Doppler broadening increases by 20%, in agreement with simulations. Furthermore, a tracer jet from the capsule fill-tube perturbation that is entrained by the hot-spot flow confirms the average flow speeds deduced from neutron spectroscopy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗