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DOE OSTI2022

High-Cooperativity Coupling of Rare-Earth Spins to a Planar Superconducting Resonator

The interfacing of a superconducting microwave resonator with rare-earth-doped crystals presents a promising hybrid quantum system for applications including spin-assisted transducers and memories. The coupling strength between the spins of the rare-earth ions and the microwave photons is characterized by the cooperativity. Here, we report an ultrahigh cooperativity of C~650 between rare-earth spins and a planar superconducting microwave resonator that features a highly uniform magnetic field for harnessing the strong anisotropic coupling strength of erbium-doped yttrium orthosilicate. This cooperativity rivals that from a bulk dielectric resonator and may pave a path for efficient coupling of spins with microwave photons on an integrated platform.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Optimal coupling of Ho W 10 molecular magnets to superconducting circuits near spin clock transitions

A central goal in quantum technologies is to maximize GT 2 , where G stands for the coupling of a qubit to control and readout signals and T 2 is the qubit’s coherence time. Furthermore, this is challenging, as increasing G (e.g., by coupling the qubit more strongly to external stimuli) often leads to deleterious effects on T 2 . Here, we study the coupling of pure and magnetically diluted crystals of Ho W 10 magnetic clusters to microwave superconducting coplanar waveguides. Absorption lines give a broadband picture of the magnetic energy level scheme and, in particular, confirm the existence of level anticrossings at equidistant magnetic fields determined by the combination of crystal field and hyperfine interactions. Such “spin clock transitions” are known to shield the electronic spins against magnetic field fluctuations. The analysis of the microwave transmission shows that the spin-photon coupling also becomes maximum at these transitions. The results show that engineering spin-clock states of molecular systems offers a promising strategy to combine sizable spin-photon interactions with a sufficient isolation from unwanted magnetic noise sources.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

High-volume tunable resonator for axion searches above 7 GHz

In this research, we present results from an experimental demonstration of a tunable thin-shell axion haloscope whose geometry decouples its overall volume from its resonant frequency, thereby evading the steep sensitivity degradation at high frequencies. An aluminum 2.6-l (41⁢λ 3 ) prototype, which tunes from 7.1 to 8.0 GHz, was fabricated and characterized at room temperature. An axion-sensitive, straightforwardly tunable TM 010 mode is clearly identified with a room-temperature quality factor, Q, of approximately 5000. The on-resonance E-field distribution is mapped and found to agree with numerical calculations. Anticipating future cryogenic operation, we develop an alignment protocol relying only on rf measurements of the cavity, maintaining a form factor of 0.57 across the full tuning range. These measurements demonstrate the feasibility of cavity-based haloscopes with operating volume V $\gg$ λ 3 . We discuss plans for future development and the parameters required for a thin-shell haloscope exploring the postinflationary axion parameter space (approximately 4 to 30 GHz) at Dine-Fischler-Srednicki-Zhitnitsky sensitivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

Probing the Atomic Scale Mechanisms of Time Dependent Dielectric Breakdown in Si/SiO 2 MOSFETs (June 2022)

Here we report on an atomic-scale study of trap generation in the initial/intermediate stages of time-dependent dielectric breakdown (TDDB) in high-field stressed (100) Si/SiO2 MOSFETs using two powerful analytical techniques: electrically detected magnetic resonance (EDMR) and near-zero-field magnetoresistance (NZFMR). We find the dominant EDMR-sensitive traps generated throughout the majority of the TDDB process to be silicon dangling bonds at the (100) Si/SiO2 interface (Pb0 and Pb1 centers) for both the spin-dependent recombination (SDR) and trap-assisted tunneling (SDTAT) processes. We find this generation to be linked to both changes in the calculated interface state densities as well as changes in the NZFMR spectra for recombination events at the interface, indicating a redistribution of mobile magnetic nuclei which we conclude could only be due to the redistribution of hydrogen at the interface. Additionally, we observe the generation of traps known as E’ centers in EDMR measurements at lower experimental temperatures via SDR measurements at the interface. Our work strongly suggests the involvement of a rate-limiting step in the tunneling process between the silicon dangling bonds generated at the interface and the ones generated throughout the oxide.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Polarization-separated double-imaging spectroscopy for weakly-ionized plasma diagnostics

Laser Thomson scattering, which provides thermal properties of electrons, has been extensively utilized in plasma diagnostics. However, being a non-resonant linear light scattering technique, it often encounters several challenges in weakly-ionized plasma diagnostics due to spectral overlap with different scatterings induced from other existing species, including Mie, Rayleigh, and rotational Raman scatterings. To address this challenge, we propose an imaging spectroscopy technique, polarization-separated double-imaging spectroscopy (PoDIS), which selectively separates specific scatterings based on their polarization characteristics. Using an atmospheric plasma jet as a plasma source for demonstration, we show that PoDIS can effectively separate rotational Raman and Thomson scatterings from a superimposed spectrum without prior knowledge or assumptions about the thermal properties of neutrals or electrons. This separation enables independent fitting of the rotational Raman and Thomson scattering spectra, allowing for precise determination of the thermal properties of neutral particles and electrons separately.

Bak, Junhwi [Texas A&M University, College Station↗

DOE OSTI2024

Institute for Catalysis in Energy Processes (ICEP) (Final Report)

The Institute for Catalysis in Energy Processes (ICEP) was a multi-PI program located at the Northwestern University Center for Catalysis and Surface Science from 2006-2024. Over several renewal cycles and several organizing themes, ICEP addressed fundamental questions in catalysis science. In turn, the scientific questions addressed were directly relevant to the efficient use of the nation’s resources to produce fuels and commodity chemicals, harness alternate energy sources for chemical reactions such as light or electricity, reduce emissions and waste, and minimize the impact of our use of plastics. Selective oxidation, (oxidative) dehydrogenation, deNOx, CO 2 reduction, hydrogen release, polymer decomposition / depolymerization, and many other reactions of intense interest to the US Department of Energy were studied in the center. Major ICEP strengths were in catalyst synthesis, in measurements that elucidated catalyst properties, in reaction mechanisms and kinetics, and in predictive theory and modeling. ICEP researchers were often the inventors or developers of materials and methods that were brought to bear on the Institute’s catalytic systems. Key characterization tools advanced through this project included resonance Raman and related techniques, sum frequency generation, and X-ray standing wave spectroscopy. Center members relied extensively on computational tools such as density functional theory and microkinetic modeling to fully investigate catalyst structures and catalytic mechanisms. ICEP researchers were early developers of atomic layer deposition (ALD) for catalyst synthesis and were early pioneers of metal organic frameworks for catalysis. ICEP innovations are found in areas of intense research such as single-atom catalysts, catalytic deconstruction of plastics, and catalytic MOFs, to name a few. Research areas initiated by ICEP indirectly led to DOE EFRCs, startup companies, and other achievements. Over its 18 years of existence, ICEP involved two different PIs (Stair and Notestein) and 24 senior investigators across several academic disciplines at Northwestern University. There were tight collaborations with Argonne National Laboratory, including specialized equipment and experiments permanently located there. The center supported ~400 person-years of effort by graduate students and postdocs, either directly through DOE support or indirectly by leveraging independent support provided to the trainees, e.g. through the NSF GRFP or internal fellowships. The project resulted in 328 manuscripts and numerous conference presentations.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Covalent integration of polymers and porous organic frameworks

Covalent integration of polymers and porous organic frameworks (POFs), including metal-organic frameworks (MOFs), covalent organic frameworks (COFs) and hydrogen-bonded organic frameworks (HOFs), represent a promising strategy for overcoming the existing limitations of traditional porous materials. This integration allows for the combination of the advantages of polymers, i.e., flexibility, processability and chemical versatility etc., and the superiority of POFs, like the structural integrity, tunable porosity and the high surface area, creating a type of hybrid materials. These resulting polymer-POF hybrid materials exhibit enhanced mechanical strength, chemical stability and functional diversity, thus opening up new opportunities for applications across a large variety of fields, such as gas separation, catalysis, biomedical applications, environmental remediation and energy storage. In this review, an overview of synthetic routes and strategies on how to covalently integrate different polymers with various POFs is discussed, especially with a particular focus on methods like polymerization within, on and among POF structures. To investigate the unique properties and functions of these resultant hybrid materials, the characterization techniques, including nuclear magnetic resonance spectroscopy (NMR), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), transmission electron microscopy (TEM) and scanning electron microscopy (SEM), gas adsorption analysis (BET) and computational modeling and machine learning, are also presented. The ability of polymer-POFs to manipulate the pore environments at the molecular level affords these materials a wide range of applications, providing a versatile platform for future advancements in material science. Looking forward, to fully realize the potential of these hybrid materials, the authors highlight the scalability, green synthesis methods, and potential for stimuli-responsive polymer-POF materials as critical areas for future research.

Hossain, Md Amjad↗

NASA NTRS1971

Experimental and computer studies of the radiation effects in silicon solar cells

A summary of selected experimental results obtained on lithium-diffused bulk silicon is presented. Particular emphasis is placed on the radiation-induced degradation and thermal annealing of minority carriers in bulk silicon because solar cell output is related to the minority carrier lifetime. The temperature dependence of the minority carrier lifetime indicates the density and energy levels of the recombination centers and provides clues to their identity. Electron spin resonance and infrared absorption techniques are used to investigate the introduction and anneal of three specific radiation induced defects, which are thought to contribute to the recombination process.

Leadon, R. E.↗

NASA NTRS1972

Niobium hyperfine structure in crystal calcium tungstate

A study of the niobium hyperfine structure in single crystal calcium tungstate was made by the combination of the technique of electron paramagnetic resonance and electron nuclear double resonance (EPR/ENDOR). The microwave frequency was about 9.4 GHz and the radio frequency from 20MHz to 70 MHz. The rare earth ions Nd(3+), U(3+), or Tm(3+) were added as the charge compensator for Nb(5+). To create niobium paramagnetic centers, the sample was irradiated at 77 deg K with a 10 thousand curie Co-60 gamma source for 1 to 2 hours at a dose rate of 200 K rads per hour and then transferred quickly into the cavity. In a general direction of magnetic field, the spectra showed 4 sets of 10 main lines corresponding to 4 nonequivalent sites of niobium with I = 9/2. These 4 sets of lines coalesced into 2 sets of 10 in the ab-plane and into a single set of 10 along the c-axis. This symmetry suggested that the tungsten ions are substituted by the niobium ions in the crystal.

Tseng, D. L.↗

NASA NTRS1974

Electron paramagnetic resonance of several lunar rock samples

The results are presented of investigating lunar rock samples returned by the Luna 16 automatic station, using electron paramagnetic resonance (EPR). The EPR technique makes it possible to detect paramagnetic centers and investigate their nature, with high sensitivity. Regolith (finely dispersed material) and five particles from it, 0.3 mm in size, consisting mostly of olivine, were investigated with EPR.

Marov, P. N.↗

NASA NTRS1975

Vector plotting as an indication of the approach to flutter

A binary flexure-torsion analysis was made to check theoretically a method for predicting flutter which depends on plotting vectorially the amplitudes of response relative to the exciting force and extracting the relevant damping rate. The results of this calculation are given in graphs both of the vector plots themselves and of the estimated damping rate against forward speed. The estimated damping rates are compared with calculated values. The method has the advantage that in a flight flutter test damping can be estimated from continuous excitation records: the method is an extension of the Kennedy and Pancu technique used in ground resonance testing.

Broadbent, E. G.↗

NASA NTRS1977

Apollo-Soyuz O/3P/ and N/4S/ density measurement by UV spectroscopy

The densities of O(3P) and N(4S) at 225 km were determined during the Apollo-Soyuz Test Project by a resonance absorption-fluorescence technique in which O I and N I line radiation produced and collimated on board the Apollo was reflected from the Soyuz back to the Apollo for spectral analysis. The two spacecraft maneuvered so that a range of observation angles of plus or minus 25 deg with respect to the normal to the orbital velocity vector was scanned. The measurements described were made at night on two consecutive orbits at spacecraft separations of 150 and 500 m. The results indicate an O density of 1.15 billion per cu cm (plus or minus 30%), agreeing with mass-spectrometric measurements made under similar conditions, and an N density of 5.6 to 11.2 million per cu cm, in good agreement with recent measurements but suggesting a smaller diurnal variation than predicted by present models.

Donahue, T. M.↗

NASA NTRS1977

Depositional history of core section 74001 - Depth profiles of maturity, FeO, and metal

Samples from every 0.5-cm interval of soil in core section 74001 have been studied by ferromagnetic resonance (FMR) and magnetic techniques. The values of the FMR maturity index show that the 74001 samples are very immature (the index ranges from 0.14 to 0.29 units) and have not seen appreciable, if any, surface exposure since their deposition. In fact, the small amount of fine-grained metal in the 74001 samples is probably not acquired as a result of their exposure to the micrometeoroid flux at the lunar surface. Thus, the black-glass soil of 74001 was deposited very rapidly, probably in a single episode or several closely spaced episodes of lunar fire fountaining. The average concentration of FeO and its standard deviation for all the 74001 samples are 22.5 + or - 0.3 wt.%. Since the FeO concentration is so uniform, no large variations in the major-element chemistry of 74001 are expected, with the possible exception of the volatile elements. The concentration of coarse-grained metal, which is measured magnetically, and its standard deviation are 0.15 + or - 0.01 wt.%. The coarse-grained metal probably precipitated contemporaneously with the silicate and oxide phases in the black-glass droplets.

Morris, R. V.↗

NASA NTRS1978

Validity of modifying Mie theory to describe scattering by nonspherical particles

A calculation procedure has been developed (Chylek et al., 1976) for determining the scattering properties of irregularly shaped, randomly oriented particles. The procedure uses a modified form of the Mie theory for spheres with equivalent cross-sectional areas. The validity of the procedure is examined with reference to the work of Welch and Cox (1978). Particular consideration is given to: (1) the assumption that surface waves constitute the only major difference between scattering by spherical and nonspherical particles, (2) the identification of certain properties of the Mie coefficients with surface waves, and (3) the technique of removing surface waves from the Mie theory. It is concluded that the idea of determining the scattering properties of random orientations of irregular particles by eliminating surface waves from the Mie expansion is valid. It is also found that the technique for removing the resonances leads to the introduction of substantial fictitious absorption.

Acquista, C.↗

NASA NTRS1978

Reactions of OH/+/ and H2O/+/ ions with some diatomic and simple polyatomic molecules

The rate constants and product distributions of the reactions of OH(+) and H2O(+) with some diatomic and simple polyatomic molecules were studied by ion cyclotron resonance (ICR) mass spectrometric techniques. Reaction rates with CO, NO, O2, N2, CO2, H2S, N2O, H2CO, CH4 and CD4 were measured. Charge transfer and proton transfer were generally observed in cases for which the reaction channel is exothermic, but processes involving rearrangement were not found.

Karpas, Z.↗

NASA NTRS1979

The reaction N/4S/ + O3 - An upper limit for the rate constant at 298 K

The reaction of N(4S) atoms with ozone was examined at 298 K using discharge flow and flash photolysis techniques, both coupled with resonance fluorescence detection of N(4S). No reaction was detected in either system, and an upper limit of 5 x 10 to the -16th cu cm/molecule/s was estimated for the rate constant. This is 1000 times lower than the presently accepted value of 5.7 x 10 to the -13th cu cm/molecule/s which is based on a discharge flow-mass spectrometric study of the reaction. Potential complications in the latter experiment are discussed.

Stief, L. J.↗

NASA NTRS1984

Ion-molecule reactions in unsaturated hydrocarbons - Allene, propyne, diacetylene, and vinylacetylene

Ion-molecule reactions in allene, propyne, diacetylene, and vinylacetylene (1-buten-3-yne) have been studied at near-thermal energies by the technique of ion cyclotron resonance mass spectrometry. Rate coefficients and branching ratios are reported for the reactions of C3Hn(+) (n = 1-4) with allene and propyne and for the reactions of C4Hn(+) (n = 0-5) with diacetylene and vinylacetylene. Branching ratios are also given for the reactions of C4Hn(+), C5Hn and C6Hn(+) with propyne and for reactions of C6Hn(+) with diacetylene and vinylacetylene. More than 90 percent of the reactive channels lead to product ions having a larger carbon skeleton than the reactant ion. Evidence for ions with the same m/e ratio having differing reactivities was obtained for C3Hn(+), C6H7(+), and C7H7(+). Ion reaction sequences in allene and propyne were followed at higher pressures (0.0001 torr) to investigate secondary, tertiary, and higher order processes.

Anicich, V. G.↗

NASA NTRS1990

Flow diagnostics by resonant holographic interferometry

This paper describes a resonant-holographic-interferometry (RHI) technique for nonintrusive flow diagnostics, that relies on the index of refraction variation close to a spectral line. This technique makes it possible to obtain interferograms that are species-selective along with quantitative full-field information for the species under study. The application of the RHI technique to flow fields is analyzed together with measurements of flow parameters such as velocity, pressure, and temperature. The advantages of RHI technique over other nonintrusive diagnostic techniques, such as LIF and planar LIF, are discussed.

Sirota, J. M.↗