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DOE OSTI2017

A novel technique applying spectral estimation to Johnson noise thermometry - 317

Johnson noise thermometry is one of many important measurement techniques used to monitor the safety levels and stability in a nuclear reactor. However, this measurement is very dependent on the minimal electromagnetic environment. Properly removing unwanted electromagnetic interference (EMI) is critical for accurate drift free temperature measurements. The two techniques developed by Oak Ridge National Laboratory to remove transient and periodic EMI are briefly discussed in this paper. Spectral estimation is a key component in the signal processing algorithm used for EMI removal and temperature calculation. The cross-power spectral density is a key component in the Johnson noise temperature computation. Applying either technique requires the simple addition of electronics and signal processing to existing resistive thermometers. With minimal installation changes, the system discussed here can be installed on existing nuclear power plants. The Johnson noise system developed is tested at three locations: Oak Ridge National Laboratory, Sandia National Laboratory, and Tennessee Valley Authority (TVA) Kingston Steam Plant. Each of these locations enabled improvement on the EMI removal algorithm. The conclusions made from the results at each of these locations is discussed, as well as, possible future work. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Curium(iii) radiation-induced reaction kinetics in aqueous media

Insight into the effects of radiolytic processes on the actinides is critical for advancing our understanding of their solution chemistry because the behaviour of these elements cannot be easily separated from the influence of their inherent radiation field. However, minimal information exists on the radiation-induced redox behaviour of curium (Cm), a key trivalent transuranic element present in used nuclear fuel and frequently used as an alpha radiation source. Here we present a kinetic study on the aqueous redox reactions of Cm(III) with radicals generated through the radiolysis of aqueous media. In particular, we probe reaction kinetics in nitric acid solutions that are used as the aqueous phase component of used nuclear fuel reprocessing solvent systems. Second-order rate coefficients (k) were measured for the reaction of Cm(III) with the hydrated electron (e aq - , k = (1.25 ± 0.03) × 10 10 M -1 s -1 ), hydrogen atom (H˙, k = (5.16 ± 0.37) × 10 8 M -1 s -1 ), hydroxyl radical (˙OH, k = (1.69 ± 0.24) × 10 9 M -1 s -1 ), and nitrate radical (NO 3 ˙, k = (4.83 ± 0.09) × 10 7 M -1 s -1 ). Furthermore, the first-ever Cm(II) absorption spectrum (300–700 nm) is also reported. These kinetic data dispel the status quo notion of Cm(III) possessing little to no redox chemistry in aqueous solution, and suggest that the resulting Cm(II) and Cm(IV) transients could exist in irradiated aqueous solutions and be available to undergo subsequent redox chemistry with other solutes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Structural and Electronic Influences on Rates of Tertpyridine-Amine Co III -H Formation During Catalytic H 2 Evolution in an Aqueous Environment

In this paper, the differences in catalytic performance for a series of Co hydrogen evolution catalysts with different pentadentate polypyridyl ligands (L), have been rationalized by examining elementary steps of the catalytic cycle using a combination of electrochemical and transient pulse radiolysis (PR) studies in aqueous solution. Solvolysis of the [Co II -Cl] + species results in the formation of [Co II (κ 4 -L)(OH 2 )] 2+ . Further reduction produces [Co I κ 4 -L)(OH 2 )] + , which undergoes a rate-limiting structural rearrangement to [Co I (κ 5 -L)] + before being protonated to form [Co III -H] 2+ . The rate of [Co III -H] 2+ formation is similar for all complexes in the series. Using E 1/2 values of various Co species and pKa values of [Co III -H] 2+ estimated from PR experiments, we found that while the protonation of [Co III -H] 2+ is unfavorable, [CoII-H]+ reacts with protons to produce H 2 . The catalytic activity for H 2 evolution tracks the hydricity of the [Co II -H] + intermediate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Computational tools for the simulation and analysis of spin-polarized EPR spectra

The EPR spectra of paramagnetic species induced by photoexcitation typically exhibit enhanced absorptive and emissive features resulting from sublevel populations that differ from thermal equilibrium. The populations and the resulting spin polarization of the spectra are dictated by the selectivity of the photophysical process generating the observed state. Simulation of the spin-polarized EPR spectra is crucial in the characterization of both the dynamics of formation of the photoexcited state as well as its electronic and structural properties. EasySpin, the simulation toolbox for EPR spectroscopy, now includes extended support for the simulation of the EPR spectra of spin-polarized states of arbitrary spin multiplicity and formed by a variety of different mechanisms, including photoexcited triplet states populated by intersystem crossing, charge recombination or spin polarization transfer, spin-correlated radical pairs created by photoinduced electron transfer, triplet pairs formed by singlet fission and multiplet states arising from photoexcitation in systems containing chromophores and stable radicals. In this paper, we highlight EasySpin’s capabilities for the simulation of spin-polarized EPR spectra on the basis of illustrative examples from the literature in a variety of fields ranging across chemistry, biology, material science and quantum information science.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

A facile microwave-hydrothermal method to fabricate B doped ZnWO{sub 4} nanorods with high crystalline and highly efficient photocatalytic activity

Highlights: • High-crystallized B/ZnWO{sub 4} nanorods were fabricated via a fast microwave -hydrothermal method. • B doping effectively decreases particle size and increase in specific surface area. • The seperation of photogenerated e{sup −} and h{sup +} was largely promoted by B doping. • B/ZnWO{sub 4} exhibit super photocatalytic activity in degradation organic dyes. - Abstract: A series length of 50∼200 nm B doped ZnWO{sub 4} nanorods with high crystallinity were fabricated via a fast microwave-hydrothermal method. The effects of B doping on the physical properties of ZnWO{sub 4} nanorods were intensively characterized by N{sub 2} physical adsorption, XRD, TEM, FT-IR, XPS, ultraviolet-visible diffuse reflection spectrum (UV–vis DRS), photolunminescence spectrum (PL), transient photocurrent response (TPR). The results indicated that the doped B could replace the lattice tungsten ion in ZnWO{sub 4} crystals, which caused the lattice spacing contraction, particle size decrease, specific surface area increase. More importantly, the separation of the photogenerated electrons and holes in ZnWO{sub 4} was significantly enhanced by B doping. With doped optimum B concentration (2.42 wt%), B/ZnWO{sub 4} displayed super photocatalytic performance in dyes decomposition. The degradation rate constant (0.065 h{sup −1}) of Rhodamine B over B (2.42 wt%)/ZnWO{sub 4} is 4 times of that over ZnWO{sub 4} (0.016 h{sup −1}).

36 MATERIALS SCIENCE↗

DOE OSTI2016

Variation of excited-state dynamics in trifluoromethyl functionalized C 60 fullerenes

We report on electronically excited-state dynamics of three different trifluoromethyl C60 fullerenes (TMFs, C60(CF3)n: C60/4-1, C60/6-2, and C60/10-1, featuring four, six, and ten trifluoromethyl groups, respectively) using steady-state and time-resolved optical spectroscopy as well as ultrafast pump/probe transient absorption spectroscopy. C60/4-1 and C60/6-2 dissolved in toluene solvent show near-unity S1--T1 intersystem crossing quantum yield (..phi..ISC), ca. 1 ns S1-state lifetimes, and microsecond-timescale T1-state lifetimes, which are typical of the fullerene class. On the other hand, C60/10-1 exhibits a dominant sub-nanosecond nonradiative S1--S0 relaxation mechanism and negligible ..phi..ISC, therefore decreasing the average excited-state lifetime (..tau..avg) by about 5 orders of magnitude compared to that of C60/4-1 and C60/6-2 (..tau..avg approx. 17 us and 54 us for C60/4-1 and C60/6-2, respectively, whereas ..tau..avg approx. 100 ps for C60/10-1). These excited-state characteristics of C60/4-1 and C60/6-2 are preserved in polymer matrix, suggesting that fullerene/polymer interactions do not modulate intrinsic photophysics of trifluoromethyl-substituted fullerenes. The contrasting excited- state study results of C60/4-1 and C60/6-2 to that of C60/10-1 infer that intrinsic optical properties and excited-state dynamics can be affected by the substitution on the fullerene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Time-resolved x-ray absorption spectroscopy probe in ultrafast surface chemistry

To celebrate the scientific achievement of Jo Stöhr, I present here a personal account of the use of x-ray absorption spectroscopy to probe dynamics on surfaces using x-ray lasers. In particular, I will review the investigation of ultrafast processes in adsorbates on surfaces using an optical pump and an x-ray absorption spectroscopy probe. Here, it is shown that it is possible to gain insight into the effects of electronic excitations in metals on adsorbates as well as laser-induced vibrational motions. Furthermore, the ultrafast optical pump allows the detection of the CO precursor state in the desorption channel, species close to the transition state in CO oxidation, and the transient HCO intermediate during CO hydrogenation on Ru(0001).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Characterizing laser-heated polymer foams with simultaneous x-ray fluorescence spectroscopy and Thomson scattering at the Matter in Extreme Conditions Endstation at LCLS

Understanding the behavior of polymer foams at high energy density conditions is crucial to advance inertial fusion energy research. Here, we present a new experimental platform designed to measure the thermodynamic state of these materials at megabar pressures. At the Matter in Extreme Conditions Endstation of the Linac Coherent Light Source, we heat samples using an optical, high-intensity, femtosecond laser and dynamically probe them with ultra-short, coherent x-ray pulses of high peak brightness. We perform x-ray Thomson scattering measurements in forward and backward scattering geometries to capture both collective and non-collective electron behavior in the sample. Simultaneously, x-ray fluorescence spectroscopy is used to measure the emission from a mid-Z dopant, providing complementary information on the plasma conditions. By combining these techniques, we obtain temporally resolved temperature measurements of the transient warm dense matter states. Our initial experiments designed to benchmark the platform with carbon samples yielded data resolving the ultrafast response to laser heating with sub-picosecond resolution, measuring plasma temperatures exceeding 50 eV. These findings lay the foundation for precision studies of the dynamic evolution of laser-heated polymer foams.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2019

Revealing Nanoscale Energy Flow Using Ultrafast THz to X-ray Beams (Final Technical Report)

We developed novel spectroscopic methods and made use of them to study energy flow and material properties on nanometer length scales and ultrafast time scales. Access to short length scales was provided through the use of light beams with short wavelengths (EUV through hard x-ray spectral ranges) and/or fabricated structural elements with nanometer dimensions. Recent advances in tabletop high harmonic generation of extreme ultraviolet (EUV) pulses were exploited to measure thermal transport and acoustic vibrations using time-resolved diffraction from photoexcited periodic nanostructures, revealing new physics that arises at length scales of tens to hundreds of nm. The tabletop EUV sources as well as the FERMI free electron laser at FERMI-Elettra in Trieste were used to generate as well as measure nanoscale thermoelastic responses without the need for patterned nanostructures, with the short length scale coming from optical interference patterns formed by crossing pairs of beams in transient grating experiments. We also used EUV and optical sources to excite and monitor ultrahigh-frequency acoustic waves (coherent phonons) at ultraflat interfaces and multilayer structures, extending our measurements of the highest-frequency coherent acoustic waves observed to date. Our measurements of acoustic properties allowed direct calculation of thermal conductivities which can be compared with our measurements of thermal transport and with first-principles calculations. Terahertz-frequency acoustic measurements can also be used to reveal complex relaxation dynamics in glass-forming liquids and partially disordered solids. Acoustic measurements were used to investigate the confinement effect in ultrathin liquid layers and to characterize mechanical properties of ultrathin solid layers. The methods we developed have broad fundamental applications and may also enable new practical metrology for use in nanoelectronics, just as earlier methods we developed have found commercial applications in microelectronics metrology.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2022

Plasma electron hole kinematics. Hole tracking Particle-In-Cell simulation

The kinematics of a 1-D electron hole is studied using a novel Particle-In-Cell simulation code. A hole tracking technique enables us to follow the trajectory of a fast-moving solitary hole and study quantitatively hole acceleration and coupling to ions. We observe a transient at the initial stage of hole formation when the hole accelerates to several times the cold-ion sound speed. Artificially imposing slow ion speed changes on a fully formed hole causes its velocity to change even when the ion stream speed in the hole frame greatly exceeds the ion thermal speed, so there are no reflected ions. The behavior that we observe in numerical simulations agrees very well with our analytic theory of hole momentum conservation and the effects of “jetting.”

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1973

A pulsed xenon megawatt arc plasma source

The exhaust of the source flowing into vacuum was measured by Thomson scattering diagnosis. Mean electron temperatures and densities were found to be 4-8 eV and of order ten to the 13th power cm/3 respectively over the 8 cm exhaust diameter at 30 cm from the source. Large shot to shot variations were noted. After a transient spike passes, these conditions persist during the power time of 125 microsecond. These exhaust conditions are marginal for evaluation of a proposed near resonant charge exchange pumped laser theory.

Michels, C. J.↗

NASA NTRS1984

Preliminary flight test results of the F100 EMD engine in an F-15 airplane

A flight evaluation of the F100 Engine Model Derivative (EMD) is conducted. The F100 EMD is an advanced version of the F100 engine that powers the F15 and F16 airplanes. The F100 EMD features a bigger fan, higher temperature turbine, a Digital Electronic Engine Control system (DEEC), and a newly designed 16 segment afterburner, all of which results in a 15 to 20 percent increase in sea level thrust. The flight evaluations consist of investigation of performance (thrust, fuel flow, and airflow) and operability (transient response and airstart) in the F-15 airplane. The performance of the F100 EMD is excellent. Aircraft acceleration time to Mach 2.0 is reduced by 23 percent with two F100 EMD engines. Several anomalies are discovered in the operability evaluations. A software change to the DEEC improved the throttle, and subsequent Cooper Harper ratings of 3 to 4 are obtained. In the extreme upper left hand corner of the flight enveloped, compressor stalls occurr when the throttle is retarded to idle power. These stalls are not predicted by altitude facility tests or stability for the compressor.

Myers, L. P.↗

NASA NTRS1985

Simultaneous Solar Maximum Mission and Very Large Array (VLA) observations of solar active regions

Simultaneous observations of solar active regions with the Solar Maximum Mission (SMM) Satellite and the Very Large Array (VLA) have been obtained and analyzed. Combined results enhance the scientific return for beyond that expeted from using either SMM or VLA alone. A total of two weeks of simultaneous SMM/VLA data were obtained. The multiple wavelength VLA observations were used to determine the temperature and magnetic structure at different heights within coronal loops. These data are compared with simultaneous SMM observations. Several papers on the subject are in progress. They include VLA observations of compact, transient sources in the transition region; simultaneous SMM/VLA observations of the coronal loops in one active region and the evolution of another one; and sampling of the coronal plasma using thermal cyclotron lines (magnetic field - VLA) and soft X ray spectral lines (electron density and electron temperaure-SMM).

Lang, K. R.↗

NASA NTRS1986

Stress and efficiency studies in EFG

The goals of this program were: (1) to define minimum stress configurations for silicon sheet growth at high speeds; (2) to quantify dislocation electrical activity and their limits on minority carrier diffusion length in deformed silicon; and (3) to study reasons for degradation of lifetime with increases in doping level in edge-defined film-fed growth (EFG) materials. A finite element model was developed for calculating residual stress with plastic deformation. A finite element model was verified for EFG control variable relationships to temperature field of the sheet to permit prediction of profiles and stresses encountered in EFG systems. A residual stress measurement technique was developed for finite size EFG material blanks using shadow Moire interferometry. Transient creep response of silicon was investigated in the temperature range between 800 and 1400 C in strain and strain regimes of interest in stress analysis of sheet growth. Quantitative relationships were established between minority carrier diffusion length and dislocation densities using Electron Beam Induced Current (EBIC) measurement in FZ silicon deformed in four point bending tests.

Source record↗

NASA NTRS1991

Particle image velocimetry for the surface tension driven convection experiment using a particle displacement tracking technique

The Surface Tension Driven Convection Experiment (STDCE) is a Space Transportation System flight experiment to study both transient and steady thermocapillary fluid flows aboard the USML-1 Spacelab mission planned for 1992. One of the components of data collected during the experiment is a video record of the flow field. This qualitative data is then quantified using an all electronic, two-dimensional particle image velocimetry technique called particle displacement tracking (PDT) which uses a simple space domain particle tracking algorithm. The PDT system is successful in producing velocity vector fields from the raw video data. Application of the PDT technique to a sample data set yielded 1606 vectors in 30 seconds of processing time. A bottom viewing optical arrangement is used to image the illuminated plane, which causes keystone distortion in the final recorded image. A coordinate transformation was incorporated into the system software to correct this viewing angle distortion. PDT processing produced 1.8 percent false identifications, due to random particle locations. A highly successful routine for removing the false identifications was also incorporated, reducing the number of false identifications to 0.2 percent.

Wernet, Mark P.↗

NASA NTRS1992

Effects of a lightning discharge detected by the DE 2 satellite over Hurricane Debbie

The satellite observation of a large, about 40-mV/m, transient electric field disturbance over Hurricane Debbie in September 1982 is reported. The electric field event is viewed as a spheric disturbance from a lightning discharge in the active weather system located beneath the satellite. To elucidate this observation of upward moving electrons in the ionosphere associated with a lightning event, several mechanisms for electron acceleration by electric field with components, E(parallel), along the magnetic field are compared. 'Runaway' electrons were accelerated in about 1 ms by a downward directed E(parallel) pulse of about 1 V/m magnitude. Such fields can result from rapidly exposed, negative space charges near the tops of clouds during positive cloud-to-ground discharges. HF frequency Fourier components of the E(parallel) pulse must propagate through the low-conducting nighttime atmosphere to the ionosphere with little dissipation.

Burke, William J.↗

NASA NTRS1991

Particle image velocimetry for the Surface Tension Driven Convection Experiment using a particle displacement tracking technique

Wernet, Mark P.↗

NASA NTRS2012

Astrobiological Journeys to and from the South Polar Sea of Enceladus - Bidirectional Interactions with the Saturn Magnetosphere

The spectacularly cryovolcanic moon Enceladus is a major source of plasma for the Saturn magnetosphere via ionization of the ejected molecular species and ice grains. Field-aligned plasma flows from the Enceladus environment visibly impact the moon's magnetic footpoint in Saturn's polar auroral region, while water group and other ions from the moon emissions diffuse radially throughout the magnetosphere and may be the dominant source of oxygen for Titan's oxygen-poor upper atmosphere. But the moon-magnetosphere interaction is bidirectional in the sense that the moon surface is globally exposed to constant irradiation by the returning magnetospheric ions and by energetic electrons from the field-aligned and radially diffusing populations. The returning ion source operates both on global scales of the magnetosphere and locally for highly reactive species produced in the ejecta plume. All of these sources likely combine to produce a highly oxidized global surface layer. Since plasma electrons and ions are cooled by interaction with neutral gas and E-ring ice grains from Enceladus, the moon emissions have a governing effect on the seed populations of energetic particles that irradiate the surface. The proposed subsurface polar sea and transient crustal overturn in the south polar region could bring the polar surface oxidants into contact with hydrocarbons and ammonia to make oxidation product gases contributing to the cryovolcanic jets, a process first proposed by Cooper et al. (Plan. Sp. Sci., 2009). As has been previously suggested for Europa, the 'oxidants could contribute to enhanced astrobiological potential of Enceladus, perhaps even higher than for Europa where organic hydrocarbons have not yet been directly detected. Unlike Europa, Enceladus shows no sign of an oxygen-dominated exosphere that could otherwise be indicative of extreme surface and interior oxidation inhibiting the detectable survival and evolution of complex organics.

Cooper, John F.↗