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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 19 records

Direct Observation of Plasma-Stimulated Activation of Surface Species Using Multimodal In Situ/Operando Spectroscopy Combining Polarization-Modulation Infrared Reflection-Absorption Spectroscopy, Optical Emission Spectroscopy, and Mass Spectrometry

Nonthermal plasmas (NTPs) produce reactive chemical environments, including electrons, ions, radicals, and vibrationally excited molecules, that can drive chemistry at temperatures at which such species are thermally inaccessible. There has been growing interest in the integration of conventional catalysis with reactive NTPs to promote novel chemical transformations. Unveiling the full potential of plasma-catalytic processes requires a comprehensive understanding of plasma-catalytic synergies, including characterization of plasma-catalytic surface interactions. In this work, we report on a newly designed multimodal spectroscopic instrument combining polarization-modulation infrared reflection-absorption spectroscopy (PM-IRAS), mass spectrometry, and optical emission spectroscopy (OES) for the investigation of plasma–surface interactions such as those found in plasma catalysis. In particular, this tool has been utilized to correlate plasma-phase chemistry with both surface chemistry and gas-phase products in situ (1) during the deposition of carbonaceous surface species via NTP-promoted nonoxidative coupling of methane and (2) during subsequent activation of surface deposits with an atmospheric pressure and temperature argon plasma jet on both nickel (Ni) and silicon dioxide (SiO 2 ) surfaces. For the first time, the activation of carbonaceous surface species by a NTP on Ni and SiO 2 surfaces to form hydrogen gas and C 2 hydrocarbons was directly observed, where both PM-IRAS and OES measurements suggest that they may form through different pathways. Furthermore, this unique tool for studying plasma–surface interactions could enable more rational design of plasma-stimulated catalytic processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electron radiated power in cyclotron radiation emission spectroscopy experiments

The recently developed technique of Cyclotron Radiation Emission Spectroscopy (CRES) uses frequency information from the cyclotron motion of an electron in a magnetic bottle to infer its kinetic energy. Here we derive the expected radio-frequency signal from an electron in a waveguide CRES apparatus from first principles. We demonstrate that the frequency-domain signal is rich in information about the electron's kinematic parameters and extract a set of measurables that in a suitably designed system are sufficient for disentangling the electron's kinetic energy from the rest of its kinematic features. This lays the groundwork for high-resolution energy measurements in future CRES experiments, such as the Project 8 neutrino mass measurement.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Low-energy electro- and photo-emission spectroscopy of GaN materials and devices

In hot-electron semiconductor devices, carrier transport extends over a wide range of conduction states, which often includes multiple satellite valleys. Electrical measurements can hardly give access to the transport processes over such a wide range without resorting to models and simulations. An alternative experimental approach however exists which is based on low-energy electron spectroscopy and provides, in a number of cases, very direct and selective information on hot-electron transport mechanisms. Recent results obtained in GaN crystals and devices by electron emission spectroscopy are discussed. Using near-band-gap photoemission, the energy position of the first satellite valley in wurtzite GaN is directly determined. By electro-emission spectroscopy, we show that the measurement of the electron spectrum emitted from a GaN p-n junction and InGaN/GaN light-emitting diodes (LEDs) under electrical injection of carriers provides a direct observation of transport processes in these devices. In particular, at high injected current density, high-energy features appear in the electro-emission spectrum of the LEDs showing that Auger electrons are being generated in the active region. These measurements allow us identifying the microscopic mechanism responsible for droop which represents a major hurdle for widespread adoption of solid-state lighting.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Synthetic diagnostic for the beam emission spectroscopy diagnostic using a full optical integration

The beam emission spectroscopy (BES) diagnostic is used to measure fluctuations of electron density in the edge and core of fusion plasmas, and is a key in understanding turbulence in a plasma reactor. A synthetic BES diagnostic for the turbulence simulation code XGC1 has been developed using a realistic neutral beam model and an optical system easily adaptable to different kinds of tokamaks. The beam is modeled using multiple beam energy components, each one with a fraction of the total energy and their own mass and energy (mono-energetic components). The optical system consists of a lens focusing a bundle of optical fibers and resulting in a 2D measurement. The synthetic diagnostic gives similar correlation functions and behaviour of the turbulences than the usual methods that do not take into account the full 3D optical effects. The results, based on a simulation of XGC1, contain an analysis of the correlation (in space and time), a comparison of different approximations possible and their importance in accurately modeling the BES diagnostic.

Physics↗

Design and implementation of a portable diagnostic system for Thomson scattering and optical emission spectroscopy measurements

A diagnostic system, which has a design goal of high-portability, has been designed at Oak Ridge National Laboratory (ORNL). This project aims at providing measurements of key plasma parameters (ne, Te, ni, Ti) for fusion-relevant devices, utilizing Thomson scattering (TS) and optical emission spectroscopy (OES). The innovative design employs mostly commercial off-the-shelf instrumentation and a traveling team of researchers to conduct measurements at various magnetic-confinement plasma devices. The TS diagnostic uses a Quantel Q-smart 1500 Nd:YAG laser with a 2ω harmonic generator to produce up to 850 mJ of 532 nm laser pulses at 10 Hz. Collection optics placed at the detection port consists of an 11 × 3 optical fiber bundle, where the TS diagnostic uses an 11 × 1 subset array of the fibers, the OES diagnostic uses another 11 fibers, and the remaining fibers are available to the host institution. The detection system is comprised of two separate IsoPlane-320 spectrometers with triple-grating turrets of various line spacing and two PI-MAX 4 intensified CCD detectors, used simultaneously to measure a broad range of ion, impurity, and electron parameters. The self-contained diagnostic package also includes a data processing and storage system. The design and initial implementation of the TS-OES diagnostic system are described. The experiments from the proof-of-principle operation of the portable package on a high density (∼2.5 × 1022 m−3) and low-temperature (∼5 eV) electrothermal arc source at ORNL are also discussed.

Kafle, N. (ORCID:000000028144787X)↗

Electronic structure of ferromagnetic heavy fermion, YbPdSi, YbPdGe, and YbPtGe studied by photoelectron spectroscopy, x-ray emission spectroscopy, and DFT + DMFT calculations

Here, the electronic structures of ferromagnetic heavy fermion Yb compounds of YbPdSi, YbPdGe, and YbPtGe are studied by photoelectron spectroscopy around the Yb 4d–4f resonance, resonant x-ray emission spectroscopy at the Yb L 3 absorption edge, and density functional theory combined with dynamical mean field theory calculations. These compounds all have a temperature-independent intermediate Yb valence with large ${\rm Yb}^{3+}$ and small ${\rm Yb}^{2+}$ components. The magnitude of the Yb valence is evaluated to be YbPtGe $<$ YbPdGe $\lesssim $ YbPdSi, suggesting that YbPtGe is the closest to the quantum critical point among the three Yb compounds. Our results support the scenario of the coexistence of heavy fermion behavior and ferromagnetic ordering which is described by a magnetically-ordered Kondo lattice where the magnitude of the Kondo effect and the RKKY interaction are comparable.

30 DIRECT ENERGY CONVERSION↗

Portable diagnostic package for Thomson scattering and optical emission spectroscopy on Princeton field-reversed configuration 2 (PFRC 2)

An Advanced Research Projects Agency-Energy funded diagnostic system has been deployed to the Princeton field-reversed configuration 2 (PFRC-2) device, located at Princeton Plasma Physics Laboratory. The Portable Diagnostic Package (PDP), designed at Oak Ridge National Laboratory, allows for the measurement of Thomson Scattering (TS) for electron density and temperature and Optical Emission Spectroscopy (OES) for ion temperature, impurity density, and ion velocity. A tunable spectrometer on the PDP with three gratings provides the flexibility to measure low (1 eV) and high (1000 eV) electron temperature ranges from TS. Additionally, using a second spectrometer, the OES diagnostic can survey light emission from various ion excitation levels for wide wavelength ranges. The electron density (<2 × 10 19 m –3 ) of plasmas generated in PFRC-2 has been below the PDP TS discrimination threshold, which has made TS signal detection challenging against a high-background of laser stray light. The laser stray light was iteratively reduced by making modifications to the entrance and exit geometry on PFRC-2. Rayleigh scattering experiments on PFRC have yielded the TS discrimination sensitivity to be >1 × 10 20 m –3 for the PDP. A recently implemented narrow-band notch spectral filter that masks the second harmonic 532 nm Nd:YAG laser wavelength has increased the system’s TS light discrimination sensitivity 65 times compared to the instance when the notch filter was not implemented. The hardware implementation including design changes to the flight tubes and Brewster windows will be discussed, along with results from Rayleigh and rotational Raman scattering sensitivity analyses, which were used to establish a quantitative figure of merit on the system performance. Further, the Raman scattering calibration with the notch filter has improved the PDP electron density threshold to 1 ± 0.5 × 10 18 m –3 .

47 OTHER INSTRUMENTATION↗

Comparison of beam emission spectroscopy and gas puff imaging edge fluctuation measurements in National Spherical Torus Experiment

In this study, the close physical proximity of the Gas Puff Imaging (GPI) and Beam Emission Spectroscopy (BES) diagnostics on the National Spherical torus Experiment (NSTX) is leveraged to directly compare fluctuation measurements, and to study the local effects of the GPI neutral deuterium puff during H-mode plasmas without large Edge Localized Modes. The GPI and BES views on NSTX provide partially overlapping coverage of the edge and scrape-off layer (SOL) regions above the outboard midplane. The separation in the toroidal direction is 16°, and field lines passing through diagnostic views are separated by ∼20 cm in the direction perpendicular to the magnetic field. Strong cross-correlation is observed, and strong cross-coherence is seen for frequencies between 5 and 15 kHz. Also, probability distribution functions of fluctuations measured ∼3 cm inside the separatrix exhibit only minor deviations from a normal distribution for both diagnostics, and good agreement between correlation length estimates, decorrelation times, and structure velocities is found at the ±40% level. While the two instruments agree closely in many respects, some discrepancies are observed. Most notably, GPI normalized fluctuation levels exceed BES fluctuations by a factor of ∼9. BES mean intensity is found to be sensitive to the GPI neutral gas puff, and BES normalized fluctuation levels for frequencies between 1 and 10 kHz are observed to increase during the GPI puff.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Detection of hot electrons originating from an upper valley at ∼1.7eV above the Γ valley in wurtzite GaN using electron emission spectroscopy

Using electron emission spectroscopy, measurement and analysis were conducted on the energy distribution of vacuum emitted electrons from electrically driven InGaN/GaN green (peak wavelengths 𝜆 ≈ 515nm) light-emitting diodes (LEDs) with and without a prewell superlattice (SL). Here, we report on the detection of a high-energy upper valley at ∼ 1.7eV above the Γ valley from samples with no prewell SL. We propose that these upper valley electrons originate predominantly from trap-assisted Auger recombination (TAAR) in green LEDs, as the intensity of these peaks is found to have quadratic dependence on the carrier density 𝑛 [see Espenlaub et al., J. Appl. Phys. 126, 184502 (2019)]. The high-energy upper valley peak was not observed in the sample with a prewell SL which is attributed to gettering by the prewell SL of still unidentified impurities that act as TAAR centers.

carrier generation & recombination↗

Simultaneous detection of electronic structure changes from two elements of a bifunctional catalyst using wavelength-dispersive X-ray emission spectroscopy and in situ electrochemistry.

Multielectron catalytic reactions, such as water oxidation, nitrogen reduction, or hydrogen production in enzymes and inorganic catalysts often involve multimetallic clusters. In these systems, the reaction takes place between metals or metals and ligands to facilitate charge transfer, bond formation/breaking, substrate binding, and release of products. In this study, we present a method to detect X-ray emission signals from multiple elements simultaneously, which allows for the study of charge transfer and the sequential chemistry occurring between elements. Kβ X-ray emission spectroscopy (XES) probes charge and spin states of metals as well as their ligand environment. A wavelength-dispersive spectrometer based on the von Hamos geometry was used to disperse Kβ signals of multiple elements onto a position detector, enabling an XES spectrum to be measured in a single-shot mode. This overcomes the scanning needs of the scanning spectrometers, providing data free from temporal and normalization errors and therefore ideal to follow sequential chemistry at multiple sites. We have applied this method to study MnOx-based bifunctional electrocatalysts for the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). In particular, we investigated the effects of adding a secondary element, Ni, to form MnNiOx and its impact on the chemical states and catalytic activity, by tracking the redox characteristics of each element upon sweeping the electrode potential. The detection scheme we describe here is general and can be applied to time-resolved studies of materials consisting of multiple elements, to follow the dynamics of catalytic and electron transfer reactions.

Gul, Sheraz↗

A synthetic diagnostic for beam emission spectroscopy in the helically symmetric experiment stellarator

The Helically Symmetric Experiment (HSX) has a number of active spectroscopy diagnostics. Due to the relatively large beam width compared to the plasma minor radius, it is difficult to achieve good spatial resolution at the core of the HSX plasma. This is due to the fact that the optical sightline cuts through many flux surfaces with varying field vectors within the beam. In order to compare the experimental results with theoretical models it is important to accurately model the beam width effects. A synthetic diagnostic has been developed for this purpose. This synthetic diagnostic calculates the effect of spot size and beam width on the measurements of quantities of interest, including radial electric field, flow velocity, and Stark polarization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

FLASH SPECTROSCOPY: EMISSION LINES FROM THE IONIZED CIRCUMSTELLAR MATERIAL AROUND <10-DAY-OLD TYPE II SUPERNOVAE

Supernovae (SNe) embedded in dense circumstellar material (CSM) may show prominent emission lines in their early-time spectra (≤10 days after the explosion), owing to recombination of the CSM ionized by the shock-breakout flash. From such spectra (“flash spectroscopy”), we can measure various physical properties of the CSM, as well as the mass-loss rate of the progenitor during the year prior to its explosion. Searching through the Palomar Transient Factory (PTF and iPTF) SN spectroscopy databases from 2009 through 2014, we found 12 SNe II showing flash-ionized (FI) signatures in their first spectra. All are younger than 10 days. These events constitute 14% of all 84 SNe in our sample having a spectrum within 10 days from explosion, and 18% of SNe II observed at ages <5 days, thereby setting lower limits on the fraction of FI events. We classified as “blue/featureless” (BF) those events having a first spectrum that is similar to that of a blackbody, without any emission or absorption signatures. It is possible that some BF events had FI signatures at an earlier phase than observed, or that they lack dense CSM around the progenitor. Within 2 days after explosion, 8 out of 11 SNe in our sample are either BF events or show FI signatures. Interestingly, we found that 19 out of 21 SNe brighter than an absolute magnitude M{sub R} = −18.2 belong to the FI or BF groups, and that all FI events peaked above M{sub R} = −17.6 mag, significantly brighter than average SNe II.

74 ATOMIC AND MOLECULAR PHYSICS↗

X-ray emission spectroscopy: an effective route to extract site occupation of cations

Cation site occupation is an important determinant of materials properties, especially in a complex system with multiple cations such as in ternary spinels. In this work, we show that XES provides not only the site occupation information as EXAFS, but also additional information on the oxidation states of the cations at each site. Additionally, we show that XES is a superior and a far more accurate method than EXAFS.

Bhargava, Anuj↗

Measurement of minority carrier diffusion length in p -GaN using electron emission spectroscopy (EES)

Electron emission spectroscopy was performed on metalorganic chemical vapor deposition grown p-n – -n + junctions with p-thicknesses ranging from 50 to 300 nm, doped with [Mg] = 3.5 × 10 19 cm –3 . By measuring the decreasing emitted electron intensity from a cesiated p-GaN surface with increasing p-thickness, we were able to extract the minority carrier diffusion length of electron in p-type GaN, L e = 26 ± 3 nm. The measured value is in good agreement with literature reported values. In conclusion, the extrapolated electron current at the n – region–p-GaN interface is in reasonable agreement with the simulated electron current at the interface.

36 MATERIALS SCIENCE↗

Prototype X-ray and Gamma Detection with Cyclotron Radiation Emission Spectroscopy

Cyclotron radiation emission spectroscopy, or CRES, is a novel approach to measuring the energy of an electron. By trapping a free electron in a high magnetic field, it undergoes cyclotron motion and emits radiofrequency (RF) waves. The frequency of this RF radiation is directly related to the energy of the electron. Because many cycles of the RF emission are recorded, the energy resolution of the CRES system is on the order of a single electron volt. To make a CRES system sensitive to photons, a target gas is used to induce a photoelectric effect, producing the electron that is subsequently trapped. By adding the binding energy of the target atom, the energy of the incident photon may be reconstructed. Using a xenon target gas, photoelectric interactions dominate up to approximately 300 keV, covering not only all atomic shell X-rays of the elements, but many low-lying nuclear states as well, including key transuranic elements related to nuclear security. CRES holds the potential of maintaining single-eV resolution up to this 300-keV range, thereby surpassing current state-of-the-art detectors by a factor of 10-100. The instrumental resolution of the system is limited by the uniformity of the applied magnetic field.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Antenna arrays for neutrino mass measurements with cyclotron radiation emission spectroscopy

Cyclotron Radiation Emission Spectroscopy (CRES) is a technique for precision measurements of kinetic energies of charged particles, pioneered by the Project 8 experiment to measure the neutrino mass using the tritium end-point method. It was recently employed for the first time to measure the molecular tritium spectrum and place a limit on the neutrino mass using a cubic-centimeter-scale detector. Future direct neutrino mass experiments are developing the technique to overcome the systematic and statistical limitations of current detectors. Here, this paper describes one such approach, namely the use of antenna arrays for CRES in free space. Phenomenology, detector design, simulation, and performance estimates are discussed, culminating with an example design with a projected sensitivity of 𝑚 𝛽 < ⁢0.04 eV/𝑐 2 . Prototype antenna array measurements are also shown for a demonstrator-scale setup as a benchmark for the simulation. By consolidating these results, this paper serves as a comprehensive reference for the development and performance of antenna arrays for CRES.

Physics - Nuclear physics and radiation physics↗