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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 1,549 records · Page 86

Project 8: Measuring the tritium beta-decay spectrum using Cyclotron Radiation Emission Spectroscopy

Abstract. The goal of the Project 8 experiment is to measure the absolute neutrino mass using tritium beta decays and a new spectroscopic technique, Cyclotron Radiation Emission Spectroscopy (CRES). The first phase of Project 8 demonstrated that CRES could be used to detect single-electron cyclotron radiation and perform precision electron spectroscopy. We are in Phase II of the experiment, performing a 100-day measurement of the endpoint of the tritium spectrum. We will demonstrate the ability to measure the last ~2 keV of the beta-decay spectrum and explore the background rate at energies just above the endpoint; CRES has the potential for extremely low backgrounds. In Phase III we will demonstrate the ability to scale up the volume of the experiment. In Phase IV we will switch the source from molecular tritium to atomic tritium, which will avoid systematic uncertainties from the final states of the molecule. I will present the current status of Project 8 Phase II and the plans for Phases III and IV.

Oblath, Noah↗

Exploring the Neutron Substructure with Advanced Polarized Helium-3 Targets (Or: How I Learned to Stop Worrying and Love Spectroscopy)

As we seek to understand the smallest, physical aspects of our universe, we cannot simply rely on our senses to probe the world around us as we did in the past. The smallest physical elements of our universe behave in strange, probabilistic ways and are completely invisible to the naked eye/ear/etc. So, we design clever experiments (such as scattering experiments) to probe these minute realms. Then, just as with the larger, observable world, we devise models and equations to describe what we think is happening. Due to the nature of the physical universe at the quantum scale and with the aid of symmetries such as Lorentz invariance, we can write down equations that describe the scattering, but the expressions contain functions, which we call ?form factors? and ?structure functions?, that we cannot compute from first principles. We can, however, formulate models that make predictions for these functions. By comparing our predictions with the observed data, we can gain insight into the validity of our models and thus a better physical understanding of what is happening at these minuscule scales. Studying the constituents inside of the nucleus of an atom adds another layer of difficulty if we can?t remove those components from the nucleus. This is the case with the neutron. When not bound in the nucleus with protons and other neutrons, the neutron will decay into a proton after about 15 minutes. So, we?re forced to study the neutron while it is still bound in the nucleus of an atom such as helium-3 (3He). For the last 1,000 years (rounding up), our group has developed high quality, polarized 3He targets made of an aluminosilicate glass. These targets are made in order to perform experiments at Jefferson Lab (JLab), experiments which let us determine the form factors and structure functions of the neutron by scattering polarized electrons from polarized neutrons (or rather polarized 3He). The specific experiments reported on in this thesis push the bounds of our understanding of the internal structure of the neutron. Good science is often about pushing experimental techniques to a new level. Toward that goal we study our polarized 3He targets both to advance the technology and to choose the best ones for our experiments. We do this using a process called nuclear magnetic resonance (NMR) to gauge the maximum polarization of a target and how fast the polarization decays with time. While these tests primarily provide us information that make analysis of our experimental scattering data possible, they also let us determine whether or not a target-cell is useful or even, dare I say, of spectacular quality. Our latest targets utilize a novel convection design allowing 3He to be polarized and quickly moved in front of the electron-beam, making it possible to use larger targets with higher electron-beam currents than ever before. This means more electrons scatter and we get more data. And by studying our targets in detail prior to using them in our experiments, we have found techniques to take effects which could have been detrimental to target quality and turn them to our advantage! It?s a real case of making lemonade out of lemons. We also use laser spectroscopy to study the absorption lines of alkali-metals in the target (potassium and rubidium, specifically). We add these alkali-metals to our target to facilitate polarizing the 3He. We can use the measurement of these pressure broadened absorption lines to determine the 3He density inside of the target with great precision. Historically, we understood the width of these lines would be dependent on the temperature of the target. Specifically, if I raise the temperature, the width should get bigger. I found that was not the case, which was very confusing at first, though very exciting now that I realize the data are self-consistent and suggestive of unexpected behavior. This thesis details the development of high quality, glass, polarized 3He targets for the 2020 An 1 /dn 2 and 2023 Gn E experiments, which utilized the first 3He convection targets and broke records in target quality. This thesis also covers the initial development of metal windows for the next-generation of 3He target-cells. Finally, this thesis documents the temperature dependence of the width of potassium (K) and rubidium (Rb) absorption lines as measured with laser spectroscopy.

Jantzi, Christopher↗

Two-Level System Spectroscopy from Correlated Multilevel Relaxation in Superconducting Qubits

Transmon qubits are a cornerstone of modern superconducting quantum computing platforms. Temporal fluctuations of energy relaxation in these qubits are widely attributed to microscopic two-level systems (TLSs) in device dielectrics and interfaces, yet isolating individual defects typically relies on tuning the qubit or the TLS into resonance. We demonstrate a novel spectroscopy method for fixed-frequency transmons based on multilevel relaxation: repeated preparation of the second excited state and simultaneous $T_1$ extraction of the first and second excited states reveals characteristic correlations in the decay rates of adjacent transitions. From these correlations we identify one or more dominant TLSs and reconstruct their frequency drift over time. Remarkably, we find that TLSs detuned by $\gtrsim 100\,\mathrm{MHz}$ from the qubit transition can still significantly influence relaxation. The proposed method provides a powerful tool for TLS spectroscopy without the need to tune the transmon frequency, either via a flux-tunable inductor or AC-Stark shifts.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗

Quasiparticle spectroscopy in tantalum films with different Ta/sapphire interfaces

One of the crucial aspects of current research in quantum information science is the identification and control of loss mechanisms in superconducting circuits. Although microwave measurements directly quantify device performance, additional techniques that probe quasiparticle excitations in superconducting films are needed to understand the microscopic mechanisms underlying dissipation and decoherence. Here, we present results from quasiparticle spectroscopy of Ta/sapphire films by measuring the Meissner-state magnetic susceptibility using a precision frequency-domain resonator specifically designed for thin films. We find direct evidence for additional low-energy excitations in samples with lower internal quality factors. These excitations are consistent with deep subgap states due to two-level systems, Yu-Shiba-Rusinov states near the gap edge, and perhaps other pair-breaking mechanisms. The developed non-destructive frequency-domain quasiparticle spectroscopy is a valuable addition to the quantum materials toolbox.

Moirangthem, Bicky Singh [Ames Lab; Iowa State U.]↗

Quasiparticle spectroscopy in tantalum films with different Ta/sapphire interfaces

One of the crucial aspects of current research in quantum information science is the identification and control of loss mechanisms in superconducting circuits. Although microwave measurements directly quantify device performance, additional techniques that probe quasiparticle excitations in superconducting films are needed to understand the microscopic mechanisms underlying dissipation and decoherence. Here, we present results from quasiparticle spectroscopy of Ta/sapphire films by measuring the Meissner-state magnetic susceptibility using a precision frequency-domain resonator specifically designed for thin films. We find direct evidence for additional low-energy excitations in samples with lower internal quality factors. These excitations are consistent with deep subgap states due to two-level systems, Yu-Shiba-Rusinov states near the gap edge, and perhaps other pair-breaking mechanisms. The developed non-destructive frequency-domain quasiparticle spectroscopy is a valuable addition to the quantum materials toolbox.

Moirangthem, Bicky Singh [Ames Lab; Iowa State U.]↗

Hyperfine structure and isotope shifts of xenon measured for near-infrared transitions with Doppler-free saturated absorption spectroscopy

Hyperfine structure and isotope shifts of Xe were investigated with Doppler-free saturated absorption spectroscopy for all transitions in the 820-841 nm spectral interval. The Xe samples were commercial gases of natural isotopic abundances. The measurements were performed by employing a widely tunable narrow line Ti:sapphire laser. The hyperfine structures for 129 Xe and 131 Xe were well resolved. For the transitions with the wavelengths in vacuum near 820.860 nm and 841.150 nm also isotope shifts of the even isotopes were clearly observed. The modeling of the shapes of the observed absorption lines qualitatively reproduces experimental spectral profiles. The measured absorption peaks of the hyperfine structure and isotope shifts of Xe isotopes present characteristic spectral fingerprints for their identification. Eventually, quantitative spectral analysis will provide isotopic abundances of natural, as well as radioactive Xe gas samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synchrotron-based ambient pressure X-ray photoelectron spectroscopy of hydrogen and helium

Contrary to popular belief, it is possible to obtain X-ray photoelectron spectra for elements lighter than lithium, namely hydrogen and helium. The literature is plagued with claims of this impossibility, which holds true for lab-based X-ray sources. However, this limitation is merely technical and is related mostly to the low X-ray photoionization cross-sections of the 1s orbitals of hydrogen and helium. Here, we show that, using ambient pressure X-ray photoelectron spectroscopy (XPS), a bright-enough X-ray source allows the study of these elusive elements. This has important implications in the understanding of the limitations of one of the most useful techniques in materials science, and moreover, it potentially opens the possibility of using XPS to directly study the most abundant element in the universe.

36 MATERIALS SCIENCE↗

Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: The NH stretching mode in ND 3 H +

High-resolution rotationally resolved spectra of the N–H stretch vibrational mode (ν1) of jet-cooled ND 3 H + ions are collected and analyzed in a sub-Doppler slit-jet infrared spectrometer. The isotopomeric ammonium ions are generated by proton transfer from H 3 + to ND 3 in a discharge of an ND 3 /H 2 gas mixture, whereby the slit jet expansion cools the nascent ND 3 H + ions into lower rotational states. Rotational assignments are confirmed by four-line combination differences that agree to within the spectrometer precision (9 MHz). Based on precision two-line ground-state combination differences and a symmetric top Hamiltonian, the B, D J , and D JK rotational constants for the ground vibrational state of ND 3 H + are determined with high precision for the first time. Approximate rotational constants for the ν 1 excited state are also determined, with a band origin at 3316.8425(19) cm -1 and in remarkable (~0.1 cm -1 ) agreement with high level anharmonic theoretical predictions by Guo and co-workers [J. Phys. Chem. A, 120, 2185 (2016)]. Our results allow us to predict several low-J pure rotational transitions of ND 3 H + , which we hope will support future studies of this important ion in laboratory and astronomical rotational spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solvent-dependent complex reaction pathways of bromoform revealed by time-resolved X-ray solution scattering and X-ray transient absorption spectroscopy

The photochemical reaction pathways of CHBr3 in solution were unveiled using two complementary X-ray techniques, time-resolved X-ray solution scattering (TRXSS) and X-ray transient absorption spectroscopy, in a wide temporal range from 100 ps to tens of microseconds. By performing comparative measurements in protic (methanol) and aprotic (methylcyclohexane) solvents, we found that the reaction pathways depend significantly on the solvent properties. In methanol, the major photoproducts are CH3OCHBr2 and HBr generated by rapid solvolysis of iso-CHBr2-Br, an isomer of CHBr3. In contrast, in methylcyclohexane, iso-CHBr2-Br returns to CHBr3 without solvolysis. In both solvents, the formation of CHBr2 and Br is a competing reaction channel. From the structural analysis of TRXSS data, we determined the structures of key intermediate species, CH3OCHBr2 and iso-CHBr2-Br in methanol and methylcyclohexane, respectively, which are consistent with the structures from density functional theory calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Excited state dynamics of cis , cis -1,3-cyclooctadiene: UV pump VUV probe time-resolved photoelectron spectroscopy

We present UV pump, vacuum ultraviolet probe time-resolved photoelectron spectroscopy measurements of the excited state dynamics of cis,cis-1,3-cyclooctadiene. A 4.75 eV deep UV pump pulse launches a vibrational wave packet on the first electronically excited state, and the ensuing dynamics are probed via ionization using a 7.92 eV probe pulse. The experimental results indicate that the wave packet undergoes rapid internal conversion to the ground state in under 100 fs. Comparing the measurements with electronic structure and trajectory surface hopping calculations, we are able to interpret the features in the measured photoelectron spectra in terms of ionization to several states of the molecular cation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Multimode two-dimensional vibronic spectroscopy. II. Simulating and extracting vibronic coupling parameters from polarization-selective spectra

We report experimental demonstrations of polarization-selection two-dimensional Vibrational-Electronic (2D VE) and 2D Electronic-Vibrational (2D EV) spectroscopies aim to map the magnitudes and spatial orientations of coupled electronic and vibrational coordinates in complex systems. The realization of that goal depends on our ability to connect spectroscopic observables with molecular structural parameters. In this paper, we use a model Hamiltonian consisting of two anharmonically coupled vibrational modes in electronic ground and excited states with linear and bilinear vibronic coupling terms to simulate polarization-selective 2D EV and 2D VE spectra. We discuss the relationships between the linear vibronic coupling and two-dimensional Huang–Rhys parameters and between the bilinear vibronic coupling term and Duschinsky mixing. We develop a description of the vibronic transition dipoles and explore how the Hamiltonian parameters and non-Condon effects impact their amplitudes and orientations. Using simulated polarization-selective 2D EV and 2D VE spectra, we show how 2D peak positions, amplitudes, and anisotropy can be used to measure parameters of the vibronic Hamiltonian and non-Condon effects. This paper, along with the first in the series, provides the reader with a detailed description of reading, simulating, and analyzing multimode, polarization-selective 2D EV and 2D VE spectra with an emphasis on extracting vibronic coupling parameters from complex spectra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of the surface layer of lithium metal using in situ spectroscopy

In this work, we have investigated the surface of lithium metal using x-ray photoemission spectroscopy and optical spectroscopic ellipsometry. Even if we prepare the surface of lithium metal rigorously by chemical cleaning and mechanical polishing inside a glovebox, both spectroscopic investigations show the existence of a few tens of nanometer-thick surface layers, consisting of lithium oxides and lithium carbonates. When lithium metal is exposed to room air (~50% moisture), in situ real-time monitoring of optical spectra indicates that the surface layer grows at a rate of approximately 24 nm/min, presumably driven by an interface-controlled process. Our results hint that surface-layer-free lithium metals are formidable to achieve by a simple cleaning/polishing method, suggesting that the initial interface between lithium metal electrodes and solid-state electrolytes in fabricated lithium metal batteries can differ from an ideal lithium/electrolyte contact.

36 MATERIALS SCIENCE↗

A new class of variable-radii diffraction optics for high-resolution x-ray spectroscopy at the National Ignition Facility (invited)

A new class of crystal shapes has been developed for x-ray spectroscopy of point-like or small (a few mm) emission sources. These optics allow for dramatic improvement in both achievable energy resolution and total throughput of the spectrometer as compared with traditional designs. This class of crystal shapes, collectively referred to as the Variable-Radii Spiral (VR-Spiral), utilize crystal shapes in which both the major and minor radii are variable. A crystal using this novel VR-Spiral shape has now been fabricated for high-resolution Extended X-ray Absorption Fine Structure (EXAFS) experiments targeting the Pb-L 3 (13.0 keV) absorption edge at the National Ignition Facility. The performance of this crystal has been characterized in the laboratory using a microfocus x-ray source, showing that high-resolution high-throughput EXAFS spectra can be acquired using this geometry. Importantly, these successful tests show that the complex three-dimensional crystal shape is manufacturable with the required precision needed to realize the expected performance of better than 5 eV energy resolution while using a 30 mm high crystal. An improved generalized mathematical form for VR-Spiral shapes is also presented allowing improved optimization as compared to the first sinusoidal-spiral based design. Finally, this new formulation allows VR-Spiral spectrometers to be designed at any magnification with optimized energy resolution at all energies within the spectrometer bandwidth.

47 OTHER INSTRUMENTATION↗

Ultrafast THz emission spectroscopy of spin currents in the metamagnet FeRh

Heterostructures of ferromagnetic (FM) and noble metal (NM) thin films have recently attracted considerable interest as viable platforms for the ultrafast generation, control, and transduction of light-induced spin currents. In such systems, an ultrafast laser can generate a transient spin current in the FM layer, which is then converted to a charge current at the FM/NM interface due to strong spin–orbit coupling in the NM layer. Whether such conversion can happen in a single material and how the resulting spin current can be quantified are open questions under active study. Here, we report ultrafast THz emission from spin–charge conversion in a bare FeRh thin film without any NM layer. Our results highlight that the magnetic material by itself can enable spin–charge conversion in the same order as that in a FM/NM heterostructure. We further propose a simple model to estimate the light-induced spin current in FeRh across its metamagnetic phase transition temperature. Our findings have implications for the study of the ultrafast dynamics of magnetic order in quantum materials using THz emission spectroscopy.

36 MATERIALS SCIENCE↗

Laser-spectroscopy testbed for impurity monitoring in liquid metal-cooled fast reactors

A significant challenge in sodium-cooled fast reactors is controlling impurities, in particular oxygen impurities, within the sodium coolant, as they can accelerate corrosion and indicate leaks. Optical methods offer the potential to rapidly detect small concentrations of both gaseous and metal impurities that accelerate corrosion, plug coolant channels, and lead to increased activation of isotopes in the coolant. We present the design and performance of an apparatus designed to enable the application of multiple optical analytical techniques, such as laser-induced breakdown spectroscopy, to detect elemental impurities in the sodium melt with high sensitivity. Here, we experimentally demonstrate the detection of characteristic sodium and oxygen spectral lines in liquid sodium, which sets the stage for the optimization of its analytical sensitivity. A robust sensor of this type integrated with the sodium cooling loop has the potential to significantly improve the safety and operational efficiency of generation IV nuclear reactors.

47 OTHER INSTRUMENTATION↗

X-ray absorption spectroscopy measurements of radiatively ionized argon gas

X-ray absorption spectroscopy is a diagnostic tool that can characterize the temperature and ionization state of a plasma. This technique requires experiments to characterize the platform, careful data calibration, and comparison with atomic models to understand the plasma parameters. We performed ionizing radiation wave experiments at the OMEGA Laser Facility that used an ∼ 80 eV X-ray source to heat an Argon (Ar) gas cell at fill pressures of 3 atm. To diagnose the Ar plasma, we used a capsule backlighter offset 10 mm from the gas cell, to produce X-rays that were absorbed by the ionized Ar gas. The absorption analysis was calibrated using the significant line structure in the backlighter spectrum, which served as independent energy fiducials enabling definitive measurements of a 50-eV shift in the energy of the Ar K-edge due to ionization. We compare the measured absorption spectra to two independent atomic models, PrismSPECT and SCRAM, and show that the observed K-edge shift in the heated gas is consistent with ionization up to Ar 4+ and temperatures of 10 eV.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Coupled valence carrier and core-exciton dynamics in WS 2 probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy

Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗