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At least 793 records · Page 44

Oxide-nitride heteroepitaxy for low-loss dielectrics in superconducting quantum circuits

Superconducting qubits show great promise for the realization of fault-tolerant quantum computing, but lossy, amorphous dielectrics limit current technology. Identifying highly crystalline and stoichiometric dielectrics with intrinsically low microwave loss is therefore a central materials challenge, yet experimentally validated platforms remain scarce. In this work, we integrate a crystalline dielectric into a heteroepitaxial TiN/$γ$-Al$_2$O$_3$/TiN trilayer grown via pulsed laser deposition. Correlative high-resolution imaging, diffraction, and spectroscopy measurements confirm the single-crystal quality and chemical integrity of all layers, with minimal defects and limited anion interdiffusion across the oxide-nitride interfaces. Using microwave lumped-element resonators with parallel-plate capacitors, we report the first direct measurement of the dielectric loss of epitaxial $γ$-Al$_2$O$_3$, for which we find a low intrinsic two-level system loss, $δ_{\text{TLS}}^0 = (2.8 \pm 0.1) \times 10^{-5}$. These results establish heteroepitaxial oxides on transition metal nitrides as an attractive materials platform for superconducting quantum circuits, particularly for integration into compact device architectures such as merged-element transmons and microwave kinetic inductance detectors.

Garcia-Wetten, David A. [Northwestern U.]↗

Contributions to the BeEST sterile neutrino search

Sterile neutrinos are hypothetical right-handed leptons that have been postulated as extensions to the Standard Model to help explain the origin of neutrino masses and the matter-antimatter asymmetry in the Universe. Sterile neutrinos with keV-scale masses are also a promising candidate for dark matter. LLNL and the Colorado School of Mines are developing an experiment to search for sterile neutrinos by measuring the \Beryllium-7 Electron capture in Superconducting Tunnel junctions (STJs)" (the \BeEST" Experiment). When 7 Be implanted into STJ radiation detectors decays by electron capture, the neutrino escapes and the energy of the recoiling 7 Li nucleus can be measured with high accuracy. Using conservation of energy and momentum, the mass of the emitted neutrino can then be found. Sterile keV neutrinos would generate additional peaks in the spectrum, and the experiment uses high-resolution STJs to observe such a potential signal. During my internship, I contributed to different aspects of the BeEST experiment. I designed a UHV setup for X-ray spectroscopy analysis with STJs. It will allow high-resolution X-ray spectroscopy of different materials to examine the broadening in the BeEST spectra, the origins of which are unknown but may be related to material effects inside the STJ detectors. The design accounts for the specific demands of the BeEST project, but provides a degree of flexibility that makes it useful for other potential STJ projects. Additionally, to test the accuracy of the electronics and data analysis routine, an arbitrary waveform generator (AWG) will be used to generate simulated spectra that contain sterile neutrino signals of a specified mass and admixture. For this I programmed an AWG to output random STJ signals whose amplitudes follow the appropriate user-de ned probability distribution. The AWG signals can be input into the 32-channel preamplifier to simulate any spectrum of interest and test the uniformity of the amplifier chain, as well as the sensitivity of the data analysis.

42 ENGINEERING↗

High-Sensitivity Low-Energy Ion Spectroscopy with Sub-Nanometer Depth Resolution Reveals Oxidation Resistance of MoS 2 Increases with Film Density and Shear-Induced Nanostructural Modifications of the Surface

For decades, density has been attributed as a critical aspect of the structure of sputter-deposited nanocrystalline molybdenum disulfide (MoS 2 ) coatings impacting oxidation resistance and wear resistance. Despite its importance, there are few examples in the literature that explicitly investigate the relationship between the density and oxidation behaviors of MoS 2 coatings. Aging and oxidation are primary considerations for the use of MoS 2 coatings in aerospace applications as they inevitably experience prolonged storage in water and oxygen-rich environments prior to use. Oxidation that is either limited to the first few nanometers or through the bulk of the coating can result in seizure due to high initial coefficients of friction or component failure from excessive wear. High-sensitivity low-energy ion spectroscopy (HS-LEIS) and Rutherford backscattering spectrometry (RBS) are both used to understand the extent of oxidation throughout the first ~10 nanometers of the surface of pure sputtered nanocrystalline MoS 2 coatings after high-temperature aging and how it is impacted by the density of coatings as measured by RBS. Results show that low-density coatings (ρ = 3.55 g/cm 3 ) exhibit a more columnar microstructure and voiding, which act as pathways for oxidative species to penetrate and interact with edge sites, causing severe surface and subsurface oxidation. Furthermore, HS-LEIS of surfaces sheared prior to oxidation reveals that the oxidation resistance of low-density MoS 2 coatings can be significantly improved by shear-induced reorientation of the surface microstructure to a basal orientation and elimination of pathways for oxygen into the bulk through compaction of surface and subsurface voids.

36 MATERIALS SCIENCE↗

Fabry-Perot interferometer development for rocket engine plume spectroscopy

This paper describes a new rugged high-resolution Fabry-Perot interferometer (FPI) designed for rocket engine plume spectroscopy, which is capable of detecting spectral signatures of eroding engine components during rocket engine tests and/or flight operations. The FPI system will make it possible to predict and to respond to the incipient rocket engine failures and to indicate the presence of rocket components degradation. The design diagram of the FPI spectrometer is presented.

Bickford, R. L.↗

In-beam 𝛾-ray spectroscopy toward the proton dripline: The curious case of 32 Ar

High-resolution in-beam 𝛾-ray spectroscopy was used to study excited states of the neutron-deficient nucleus 32 Ar populated in fast-beam induced four- and six-nucleon removal reactions from 36,38 Ca. One new 𝛾-ray transition and indications for an additional two were found, allowing for a glimpse at the level scheme beyond the 2$^{+}_{1}$ state. The nature of the new 1900⁢(4)-keV transition is discussed in the context of the known energy spectrum of the mirror nucleus 32 Si and shell-model calculations using the FSU and SDPF-M cross-shell effective interactions. Its resulting parent state at 3767⁢(5)⁢keV, more than 1.3 MeV above the proton separation energy, is tentatively assigned to have mixed 𝑠⁢𝑑-shell and 2p-2h character. It might either be the mirror of the 𝐽 𝜋 = 2$^{+}_{2}$ state of 32 Si at 4230.8⁢(8)⁢keV, but with a decay branch favoring a transition to the 2$^{+}_{2}$ over the ground state, or the mirror of the 4983.9⁢(11)-keV state with quantum numbers 0 + . Furthermore, the resulting mirror-energy differences of −473⁢(5) and −1218⁢(5)⁢keV are both sizable when compared to systematics; in the latter case the result would, in fact, be among the largest reported to date in the nuclear chart or suggest the potential existence of an additional, hitherto unidentified, low-lying 0 + state of 32 Si.

20 ≤ A ≤ 38↗

Surface preparation method for investigating the three-dimensional electronic structure of perovskite nickelates

The investigation of the electronic structures on perovskite oxides using surface-sensitive spectroscopy techniques is often hindered by their “uncleavable” nature, typically requiring expensive and complex in situ experimental setups that integrate the capabilities of sample synthesis and spectroscopy measurement under ultrahigh vacuum condition. Here, we address this challenge by developing an ozone-annealing process that yields atomically flat surfaces on perovskite oxide thin films, making them suitable for high-resolution angle-resolved photoemission spectroscopy measurements. Using this method, we present a three-dimensional electronic structure study of Nd 1−𝑥 ⁢Sr 𝑥 ⁢NiO 3 (𝑥=0 and 0.175) thin films with unprecedented accuracy. The experimentally determined low-energy fermiology exhibits quantitative agreements with two-band tight-binding simulations, which is further validated by first-principles calculations considering the material's actual crystal structure. This work provides an accessible approach for ex situ ARPES measurements on perovskite oxides and other strongly correlated oxides, including the recently discovered high-𝑇 c nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

SIMS and HR-XPS characterization of lithiated graphite from the magnetic fusion device RFX-mod

Lithium wall conditioning has improved the performance of many magnetic fusion devices. Li conditioning in the RFX-mod device was performed by: (1) a single Li pellet injector and (2) a multi-Li pellet injector during He plasma discharges; (3) a Li evaporator after He glow discharge cleaning and He plasma discharge exposure. This report compares the spatial and depth distributions of Li deposited on polycrystalline graphite witness samples at different locations in RFX-mod and the elemental and chemical compositions of the resulting surfaces. The sample surfaces were analyzed ex situ using secondary ion mass spectrometry (SIMS) and high-resolution X-ray photoelectron spectroscopy (HR-XPS). The results showed that Li pellet injection provided a relatively uniform toroidal coverage while Li evaporation produced highly localized Li deposition. A Li 1s HR-XPS peak at 56.5 eV binding energy (BE) characteristic of lithium-intercalated graphite was only observed with the sample exposed to Li evaporation. All of the samples exhibited a HR-XPS C 1s peak at 285.1–285.2 eV BE that is largely attributed to hydrogenated graphite. This finding suggests that hydrogenation of fresh graphite occurs during He plasma discharge exposures. Finally, our results have implications for density control and the selection of Li conditioning techniques in magnetic fusion devices.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The Transition-Edge-Sensor Array for the Micro-X Sounding Rocket

The Micro-X sounding rocket program will fly a 128-element array of transition-edge-sensor microcalorimeters to enable high-resolution X-ray imaging spectroscopy of the Puppis-A supernova remnant. To match the angular resolution of the optics while maximizing the field-of-view and retaining a high energy resolution (< 4 eV at 1 keV), we have designed the pixels using 600 x 600 sq. micron Au/Bi absorbers, which overhang 140 x 140 sq. micron Mo/Au sensors. The data-rate capabilities of the rocket telemetry system require the pulse decay to be approximately 2 ms to allow a significant portion of the data to be telemetered during flight. Here we report experimental results from the flight array, including measurements of energy resolution, uniformity, and absorber thermalization. In addition, we present studies of test devices that have a variety of absorber contact geometries, as well as a variety of membrane-perforation schemes designed to slow the pulse decay time to match the telemetry requirements. Finally, we describe the reduction in pixel-to-pixel crosstalk afforded by an angle-evaporated Cu backside heatsinking layer, which provides Cu coverage on the four sidewalls of the silicon wells beneath each pixel.

Eckart, M. E.↗

Report of the facility definition team spacelab UV-Optical Telescope Facility

Scientific requirements for the Spacelab Ultraviolet-Optical Telescope (SUOT) facility are presented. Specific programs involving high angular resolution imagery over wide fields, far ultraviolet spectroscopy, precisely calibrated spectrophotometry and spectropolarimetry over a wide wavelength range, and planetary studies, including high resolution synoptic imagery, are recommended. Specifications for the mounting configuration, instruments for the mounting configuration, instrument mounting system, optical parameters, and the pointing and stabilization system are presented. Concepts for the focal plane instruments are defined. The functional requirements of the direct imaging camera, far ultraviolet spectrograph, and the precisely calibrated spectrophotometer are detailed, and the planetary camera concept is outlined. Operational concepts described in detail are: the makeup and functions of shuttle payload crew, extravehicular activity requirements, telescope control and data management, payload operations control room, orbital constraints, and orbital interfaces (stabilization, maneuvering requirements and attitude control, contamination, utilities, and payload weight considerations).

Source record↗

A position-sensitive germanium detector for gamma-ray astronomy

The critical problem in high-resolution cosmic gamma-ray spectroscopy in the energy range from 0.02 to 10 MeV is the limited spectral sensitivity of the detectors used. This results from the small effective area of the detectors and the high background noise due to induced radioactivity and scattering in the detectors' high-energy particle environment. The effective area can be increased by increasing the number of detectors, but this becomes prohibitive because of the size and expense of the resulting instrument. We have taken a new approach: a segmented large-volume germanium gamma-ray detector which can effectively discriminate against internal background yet maintain the high spectral resolution and efficiency of conventional coaxial Ge detectors. To verify this concept, a planar detector divided into two segments has been fabricated and laboratory measurements agree well with Monte Carlo calculations. A large coaxial detector which will be divided into five segments is being built using the techniques developed for the planar detector. Monte Carlo calculations show that the sensitivity (minimum detectable flux) of the segmented coaxial detector is a factor of 2-3 better than conventional detectors because of the reduction in the internal background.

Varnell, L. S.↗

Hyperspectral X-ray Imaging with TES Detectors for Nanoscale Chemical Speciation Mapping

We are developing an imaging capability (“Hyperspectral X-ray Imaging”) for mapping chemical information (molecular formula, phase, oxidation state, hydration) that is based on ultra-high-resolution X-ray emission spectroscopy with large transition-edge sensor microcalorimeter arrays in the scanning electron microscope. By combining microcalorimeter arrays with hundreds of pixels, high-bandwidth microwave frequency-division multiplexing, and fast digital electronics for near real-time data processing, our goal is to enable measurements using laboratory-scale instrumentation rather than synchrotron beamlines. Our application focus here is on mapping the chemical form of uranium compounds on the nanoscale. Furthermore, we will present our approach to developing the Hyperspectral X-ray Imaging capability, progress toward a 128-pixel microwave multiplexed X-ray fluorescence instrument at LANL, and the path to high-throughput nanoscale chemical mapping.

47 OTHER INSTRUMENTATION↗

High-count-rate effects in event processing for the XRISM/Resolve X-ray microcalorimeter. II. Energy scale and resolution in orbit

The Resolve instrument on the X-ray Imaging and Spectroscopy Mission (XRISM) uses a 36 pixel microcalorimeter designed to deliver high-resolution, non-dispersive X-ray spectroscopy. Although it is optimized for extended sources with low count rates, Resolve observations of bright point sources are still able to provide unique insights into the physics of these objects, as long as high-count-rate effects are addressed in the analysis. These effects include the loss of exposure time for each pixel, changes in the energy scale, and changes in the energy resolution. To investigate these effects under realistic observational conditions, we observed the bright X-ray source, the Crab Nebula, with XRISM at several offset positions with respect to the Resolve field of view and with continuous illumination from 55 Fe sources on the filter wheel. For the spectral analysis, we excluded data where exposure-time loss was too significant to ensure reliable spectral statistics. The energy scale at 6 keV shows a slight negative shift in the high-count-rate regime. The energy resolution at 6 keV worsens as the count rate in electrically neighboring pixels increases, but can be restored by applying a nearest-neighbor coincidence cut (“cross-talk cut”). We examined how these effects influence the observation of bright point sources, using GX 13+1 as a test case, and identified an eV-scale energy offset at 6 keV between the inner (brighter) and outer (fainter) pixels. Users who seek to analyze velocity structures on the order of tens of km s–1 should account for such high-count-rate effects. These findings will aid in the interpretation of Resolve data from bright sources and provide valuable considerations for designing and planning for future microcalorimeter missions.

X-rays: general↗

A simple vacuum suitcase for enabling plasma facing component characterization in fusion devices

We have demonstrated a vacuum suitcase to transport samples in vacuo to a surface analysis station for characterization of tokamak plasma facing components (PFCs). This technique enables surface analysis at powerful, dedicated stations that are not encumbered by design constraints imposed on them by a tokamak. The vacuum suitcase is an alternative solution to characterizing PFCs using diagnostics that are designed and built around a tokamak. The vacuum suitcase, called the Sample Exposure Probe (SEP), features mobile ultra-high vacuum pumping. Active pumping under high vacuum enables sample transfer between the Lithium Tokamak eXperiment-β (LTX-β) and a high resolution X-ray Photoelectron Spectroscopy (XPS) system that is situated close by. A thermocouple inserted in the back of the sample head measures heat flux from the plasma during exposure, and together with a button heater, allows the sample to match the LTX-β PFCs in high temperature operations. As vacuum conditions are better during transfer and analysis than in the tokamak, less contamination is introduced to the samples. XPS scans on a dedicated analysis station enable peak identification due to higher resolution and signal to noise ratio. A similar probe could be implemented for other fusion devices. As a result, the SEP is the first vacuum suitcase implementation for fusion applications that incorporates active pumping.

47 OTHER INSTRUMENTATION↗

Infrared Near-Field Spectroscopy of Gold Nanotriangle Fabry-Pérot Resonances

Here, in this work, we characterize the near-field response of individual gold nanotriangles over a broad, visible-to-infrared, spectral region (200–1500 meV) using high-resolution electron energy-loss spectroscopy (EELS) performed inside of a scanning transmission electron microscope (STEM). We begin by experimentally imaging the spatial and spectral extent of each nanotriangle’s plasmonic Fabry-Pérot modes and measuring the evolution of their resonance energies with increasing edge length; thereby providing detailed information on infrared plasmon dephasing times and dispersion relations. Numerical electromagnetic simulations of the electron probe are used to interpret these experimental results and to compare the near-field electromagnetic enhancement factors of gold nanotriangles and nanorods of equal resonant energy. Taken together, this combined experimental and theoretical study provides unique insights relevant to designing noble metal plasmonic nanoparticle systems for solar energy harvesting and sensing applications in the near- and mid-infrared.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-speed assembly language (80386/80387) programming for laser spectra scan control and data acquisition providing improved resolution water vapor spectroscopy

An assembly language program using the Intel 80386 CPU and 80387 math co-processor chips was written to increase the speed of data gathering and processing, and provide control of a scanning CW ring dye laser system. This laser system is used in high resolution (better than 0.001 cm-1) water vapor spectroscopy experiments. Laser beam power is sensed at the input and output of white cells and the output of a Fabry-Perot. The assembly language subroutine is called from Basic, acquires the data and performs various calculations at rates greater than 150 faster than could be performed by the higher level language. The width of output control pulses generated in assembly language are 3 to 4 microsecs as compared to 2 to 3.7 millisecs for those generated in Basic (about 500 to 1000 times faster). Included are a block diagram and brief description of the spectroscopy experiment, a flow diagram of the Basic and assembly language programs, listing of the programs, scope photographs of the computer generated 5-volt pulses used for control and timing analysis, and representative water spectrum curves obtained using these programs.

Allen, Robert J.↗

Electronic structure of a nodal line semimetal candidate TbSbTe

The 𝐿⁢𝑛⁢SbTe (𝐿⁢𝑛 = Lanthanides) family, like isostructural ZrSiS-type compounds, has emerged as a fertile playground for exploring the interaction of electronic correlations and magnetic ordering with the nodal line band topology. Here, we report on a detailed electronic band structure investigation of TbSbTe, corroborated by electrical transport, thermodynamic, and magnetic studies. Temperature-dependent magnetic susceptibility and thermodynamic transport studies indicate the onset of antiferromagnetic ordering below 𝑇 𝑁 ∼ 5.8K. The electronic band structure study, carried out with high-resolution angle-resolved photoemission spectroscopy measurements aided with density functional theory–based first-principles calculations reveal presence of a nonsymmorphic symmetry-protected Dirac crossing in the Γ-X high-symmetry (HS) direction, which is part of a nodal line along the X-R HS direction. Another Dirac crossing occurs along the Γ-X direction at a relatively higher binding energy, which occurs from $\tilde{𝒞}$ 2⁢𝜈⁢ 𝒫 symmetry which is gapped in the theoretical calculations with the effect of spin-orbit coupling considered. Parallel to this direction, our theoretical calculations and experimental results exhibit strongly momentum-dependent surface bands. In this study, we open an avenue to further uncover the intricate interplay among symmetry-protected topological band structure, spin-orbit coupling, and magnetism in this material and the 𝐿⁢𝑛⁢SbTe family, in general.

Angle-resolved photoemission spectroscopy↗

Observation of bound valence excited electronic states of deprotonated 2-hydroxytriphenylene using photoelectron, photodetachment, and resonant two-photon detachment spectroscopy of cryogenically cooled anions

Polycyclic aromatic hydrocarbons (PAHs) are common atmospheric pollutants, and they are also ubiquitous in the interstellar medium. Here, we report the study of a complex O-containing PAH anion, the deprotonated 2-hydroxytriphenylene (2-OtPh–), using high-resolution photoelectron imaging and photodetachment spectroscopy of cryogenically cooled anions. Vibrationally resolved photoelectron spectra yield the electron affinity of the 2-OtPh radical as 2.629(1) eV and several vibrational frequencies for its ground electronic state. Photodetachment spectroscopy reveals bound valence excited electronic states for the 2-OtPh– anion, with unprecedentedly rich vibronic features. Evidence is presented for a low-lying triplet state (T1) and two singlet states (S1 and S2) below the detachment threshold. Single-color resonant two-photon photoelectron spectroscopy uncovers rich photophysics for the 2-OtPh– anion, including vibrational relaxation in S1, internal conversion to the ground state of 2-OtPh–, intersystem crossing from S2 to T1, and a long-lived autodetaching shape resonance about 1.3 eV above the detachment threshold. The rich electronic structure and photophysics afforded by the current study suggest that 2-OtPh– would be an interesting system for pump–probe experiments to unravel the dynamics of the excited states of this complex PAH anion.

Chemistry↗

Monitoring of catalyst performance in CO2 lasers using frequency modulation spectroscopy with diode lasers

Closed-cycle CO2 laser operation with removal of O2 and regeneration of CO2 can be achieved by catalytic CO-O2 recombination. Both parametric studies of the optimum catalyst formulation and long-term performance tests require on line monitoring of CO, O2 and CO2 concentrations. There are several existing methods for molecular oxygen detection. These methods are either intrusive (such as electrochemical method or mass spectrometry) or very expensive (such as CARS, UV laser absorption). Researchers demonstrated a high-sensitivity spectroscopic measurement of O2 using the two-tone frequency modulation spectroscopy (FMS) technique with a near infrared GaAlAs diode laser. Besides its inexpensive cost, fast response time, nonintrusive measurements and high sensitivity, this technique may also be used to differentiate between isotopes due to its high spectroscopic resolution. This frequency modulation spectroscopy technique could also be applied for the on-line monitoring of CO and CO2 using InGaAsP diode lasers operation in the 1.55 microns region and H2O in the 1.3 microns region. The existence of single mode optical fibers at the near infrared region makes it possible to combine FMS with optical fiber technology. Optical fiber FMS is particularly suitable for making point-measurements at one or more locations in the CO2 laser/catalyst system.

Wang, Liang-Guo↗